What Is Negative Capacitance - PDF

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Question Asked 10th Oct, 2016

Narendar Vadthiya
National Institute of Technology, Warangal
hat is negative capacitance?
hat is negative capacitance? What are the negative capacitance Similar questions and discussions
evices? Application of negative capacitance?
lectric Capacitance Capacitance-Voltage Electrochemistry Capacitance What is deep trap and shallow trap in
semiconductors?
Question 12 answers
Asked 4th Apr, 2015
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Rohul Adnan
In perfect semiconductors, there exist a band
gap (forbidden band) composed of valence
band (bottom) and conduction band (top).
When defects are introduced (such as
r Answers (1)
impurities, vacancies, interstitial), there exist
allowed energy states somewhere in the band
gap. The states that are close to the band
Petr Viscor 11th Nov, 2016 edges (either conduction band or valence
EIS Laboratory
band), then we call them shallow traps. If the
states are close to the middle of band gap,
ear Narendar,
then we call them deep traps. My questions
st to Yuri's suggestion. This (googling) is always a good starting point, are 1) are the deep (or shallow) traps differen
ut it can often mislead. it seems that there exist a whole number of for both hole and electron? 2) when people
ctive (!!) devices, where one talks about negative capacitance. This is not mention deep traps, should not they specify
ally interesting, because it does not address the real problem, namely, whether the deep traps belong to electron or
.Is there a physical process in condensed phase, where the electrical hole? Thank you in advance for your help and
sponse is correctly described by the negative capacitance ?" Remember feedback.
at if there is an inductive process (be that standard self-induction and/or
netic induction - ballistic transport or superconductivity) taking place in View
our system under test SUT), it can be misinterpreted as a negative What is the estimated value for Subthresho
apacitance. Swing (mV/dec) ?
he only serious attempt to attack this "problem" to my knowledge has Question 13 answers
een made by A.Jonscher (see the attached article) . We confirmed some Asked 2nd Feb, 2017
his results, but do not agree with others.
Reza Meshkin
yself, I have not had time yet to write about the phenomenon, but my What is the estimated value of Subthreshold
eliminary conclusion is that it is indeed a real physical effect. With the Swing for the Log(Id)-Vgs graph that is
ep voltage input (Heaviside), the usual current output from the any SUT attached here.
non-increasing, that is, it either decreases with time and/or is constant
th time( for time-> "infinity"). There are though apparently situations, this graph is result of the paper :
here, within some time interval, the responding current increases. This
http://ieeexplore.ieee.org/document/682656
en causes the "negative capacitance effect".
?tp=&arnumber=6826562
e have seen this type response (numerical solutions of Maxwell
quations) even in the ultra pure, defect free, single crystal Silicon View
amples with Schottky-Schottky electrical contacts. The effect becomes How to convert a potential collected with
ronger if the sample contains a deep defect level. It is then seen also reference to Ag/AgCl to Reversible Hydroge
xperimentally. Electrode?
hope this will help you on the way. Question 18 answers

Asked 4th Apr, 2014
ith best regards
Aneeya Kumar Samantara
etr
NegativeCapacitance02.pdf · 282.91 KB I have collect a cyclic voltammetric data by
0 Recommendations taking Ag/AgCl as the reference electrode. Bu
I want to convert this one to Potential with
respect to Reversible Hydrogen Electrode.
Please suggest me the required conversion
equation. 0.5M H2SO4 was taken as the
wers (108) 1 2 supporting electrolyte.
Yurii V Geletii View

10th Oct, 2016
Emory University Why is the dielectric constant for metals
infinity?
o your homework yourself. Google will help you! Good luck
Question 33 answers
Recommendations Asked 4th Apr, 2014
Petr Viscor 11th Nov, 2016 Jahid Akhtar
EIS Laboratory See above
ear Narendar,
View
st to Yuri's suggestion. This (googling) is always a good starting point, What free software do you use to analyze
ut it can often mislead. it seems that there exist a whole number of XRD data?
ctive (!!) devices, where one talks about negative capacitance. This is not
Question 162 answers
ally interesting, because it does not address the real problem, namely,
.Is there a physical process in condensed phase, where the electrical Asked 5th May, 2013
sponse is correctly described by the negative capacitance ?" Remember M. Yusuf Hakim Widianto
at if there is an inductive process (be that standard self-induction and/or
There is many free software to analyze XRD
netic induction - ballistic transport or superconductivity) taking place in
data but what is the best, if I have raw, dat, cp
our system under test SUT), it can be misinterpreted as a negative
apacitance. sd , rd data?
he only serious attempt to attack this "problem" to my knowledge has View

een made by A.Jonscher (see the attached article) . We confirmed some Why slope of electrochemical impedance
his results, but do not agree with others. spectroscopy (EIS) should be 1 (45 degree
between imaginary Z and real Z) for Li-ion
yself, I have not had time yet to write about the phenomenon, but my
battery?1
eliminary conclusion is that it is indeed a real physical effect. With the
ep voltage input (Heaviside), the usual current output from the any SUT Question 14 answers
non-increasing, that is, it either decreases with time and/or is constant
Asked 7th Jul, 2017
th time( for time-> "infinity"). There are though apparently situations,
here, within some time interval, the responding current increases. This Firoz Khan
en causes the "negative capacitance effect". Why the angle between imaginary part of
impedance (Zim) and real part (Zre) of
e have seen this type response (numerical solutions of Maxwell impedance in low frequency region should be
quations) even in the ultra pure, defect free, single crystal Silicon 45 degree for Li-ion battery and it should be 9
amples with Schottky-Schottky electrical contacts. The effect becomes degree for capacitor?
ronger if the sample contains a deep defect level. It is then seen also
xperimentally. If there are three materials A, B and C. The
angles between Zim and Zre are 35, 55 and 6
hope this will help you on the way. degree for materials A, B, and C, respectively.
Among these materials, which one is best an
ith best regards which one is second best for Li-ion batteries?
etr
View
NegativeCapacitance02.pdf · 282.91 KB How to calculate the Subthreshold Swing
0 Recommendations (mV/dec) with Silvaco?
Narendar Vadthiya 11th Nov, 2016 Question 8 answers
National Institute of Technology, Warangal
Asked 2nd Feb, 2017
hank you so much Petr Viscor, Reza Meshkin
How we can calculate the SS with Silvaco for
hat you said is correct, I had gone through googlig but, unable to find
hich is correct one. I hope this paper will help me to understand the an existing Id-Vgs graph (log file that is plotte
egative Capacitance". with tonyplot) ?
h k f d l bl ti
hanks for your concern and valuable suggestions. View
What the difference between dielectric
Maxim Ershov 11th Nov, 2017 permittivity and dielectric constant or
Diakopto Inc. tangent loss?
arendar - Question 25 answers

Asked 7th Jul, 2015
he paper that Petr has uploaded actually tells it all, about the origin of
Pooja Gautam
egative capacitance, from mathematical viewpoint (Fourier transform of
e transient current in response to applied voltage step). Microscopic I am studying some lecturer but confused . so
hysical mechanisms leading to a non-monotonically decreasing current please give me answer easy way.
aveform (for example - increasing waveform) are different in different
evice types. View
How is ResearchGate dealing with copyrigh
should say that there is a different "negative capacitance" (NC) effect
issues when posting our papers?
at is being actively researched in the last decade or so - related to
rroelectric materials, with polarization switching. This is a quite different Question 260 answers
pe of phenomena, and I am not sure if "negative capacitance" term is the
Asked 9th Sep, 2012
ght one here, since in ferroelectric switching the charge changes abruptly
iscontinuously) with switching / voltage, and hence a derivative (of Bashar Altakrouri
harge with respect to voltage = C) is not defined, strictly speaking. But I am wondering if there are any copyright
C term is used there, introducing quite a confusion, in my opinion. issues when we post our published papers on
ResearchGate? Is there any rule we should
axim Ershov follow or we can simply upload the papers an
hope that we do not really break the
Recommendation
publisher's copyrights. I will be more than
Vasili Ivanovich Dimitrov 11th Nov, 2017 happy to know more about this.
Tel Aviv University
ear Naendar, View
oth by definition (*The capacitance, C is the ability of a body to store an

ectric charge*) and formalization (*The capacitance, C, is defined as the
tio of the magnitude of the charge on either conductor to the potential Got a technical question?
fference between the conductors*) capacitance conceptually can’t be Get high-quality answers from experts.
egative conception.
Ask a question
o, actually this is nothing but slang that is used by non-educated
uthors.
et, sometime it may be used (in the gauche *non-scientific* discourse) in

e comparative sense, i.e. if 2 bodies have capacitance C1 and C2 while
1>C2, than the difference ΔC= C1-C2>0 may be read (but only read!) as
e negative capacitance of the second body relatively the first one.
his way, negative capacitance as an entity simply doesn’t exist. Don’t be

onfused.
ood luck.
Dimitrov
S. Well, RG isn’t area for *child’s questions*. So, following Prof. Geletii,
ad first any text-book (or Google).
D.
Vasili Ivanovich Dimitrov 11th Nov, 2017

Tel Aviv University
ear Naendar,
oth by definition (The capacitance, C is the ability of a body to store an

ectric charge) and formalization (The capacitance, C, is defined as the
tio of the magnitude of the charge on either conductor to the potential
fference between the conductors) capacitance conceptually can’t be
fference between the conductors) capacitance conceptually can t be
egative conception.
o, actually this is nothing but slang that is used by non-educated

uthors.
et, sometime it may be used (in the gauche *non-scientific* discourse) in

e comparative sense, i.e. if 2 bodies have capacitance C1 and C2 while
1>C2, than the difference ΔC=C1-C2>0 may be read (but only read!) as
egative capacitance of the second body relatively the first one.
his way, negative capacitance as an entity simply doesn’t exist. Don’t be

onfused.
ood luck.
Dimitrov
S. Well, RG isn’t area for *child’s questions*. So, following Prof. Geletii,
ad first any text-book (or Google).
D.
Maxim Ershov 11th Nov, 2017

Diakopto Inc.
ome references on negative capacitance:
A. K. Jonscher, "The physical origin of negative capacitance", J. Chem.

oc. Faraday Trans. II, vol. 82, pp. 75-81, 1986.
M. Ershov, H. C. Liu, L. Li, M. Buchanan, Z. R. Wasilewski, A. K. Jonscher,

egative capacitance effect in semiconductor devices", IEEE Trans.
lectron Devices, vol. 45, no. 10, pp. 2196-2206, Oct. 1998.
Petr Viscor 11th Nov, 2017

EIS Laboratory
ear Narendar and Vasilij Ivanovich,
Vasilij I would say that in my view, it is not fair to critisize Narendar for
sking this question. Firstly, it is not childish, but relevant and intriguing
nd secondly, as Maxim points out, it seems to be a real effect and not "a
ang, used by the un-educated authors".
is a purpose, again in my view, of RG forum to discuss this type of non-

vial (but also trivial must be welcomed !!) questions and I am always
appy to see this here.
egative capacitance (and again, Maxim might be right that one should
erhaps call it different name) is a dynamic effect when one measures
ectrical response in materials (non-linearity migh be playing a role). As I
ave already indicated a year ago, it is apparently a result of response
urrent being non-monotonic, going through a minimum (in time) and then
creasing before becoming time independent. This happens even in
erfect monocrystals with residual deep defects and/or under dc bias
oltage load. As an example, I will leave you with a plot of complex
apacitance, measured in a perfect monocrystalline Silicon sample
chottky-Schottky contacts) dc biased to -0.1 Volt.
th best regards
etr
NegativeCapacitance01.docx · 23.57 KB
Vasili Ivanovich Dimitrov 11th Nov, 2017
Tel Aviv University
eaf Petr Viscor.
our remark indirectly confirms my point of view. The decrease of

apacitance (minimum what are you talking about) is of relative nature
nd in fact is nothing but the interim capacitance drop at subsequent time
as compare to previous time t1. In this comparative sense it may be
ad as negative phenomenon. But absolute negative value C= ̶ |c| simply
oesn’t exist (like negative mass or viscosity or temperature in Kelvin
cale, etc.) ̶ this was the essense of my remark.
o, certainly the very conception of “negative capacitance” is nothing but

islead parlance. That is the physical point of view.
nother situation occurs in computational math. when one solve

umerically Navier ̶ Stokes equation. It is well ̶ known that a negative term
at may be read as “negative viscosity” appears in the computational
rmula. Yet, it should be absolutely clear that this term is of artificial
ature providing only the very stability of the computing circuit on the
hole. Physically it is meaningless.
egards, V. Dimitrov

EIS Laboratory
ear Vasilij Ivanivich,
t me agree and disagree with you :
I agree that the phenomenon of "negative capacitance" is of dynamical

ature and NOT of static nature , something you discuss in your remark,
th which I have no problem.
It is a known EXPERIMENTAL fact that when measuring optical

operties of metals, the real part of the dielectric response function goes
egative at low frequencies. This is not an artefact of some mathematical
umerical analysis.
For linear and causal response processes, it also a known fact that the
sponse functions, such as dielectric response function (~capacitance of
e system) is time(frequency) dependent and as one moves from high
equencies through the transition, the real part diverges to minus infinity
nd re-occurs from plus infinity below the given optical resonant transition
ramers-Kronig integral relation between the real and imaginary part of
e response).
What about if we re-name this "negative capacitance" a "part of

ynamical (time/frequency dependent) dielectric response of a system" ?
hen we do not use the same name for two different things, but believe
e , it is real enough and it is seen in experiments, not in numerical
nalysis. It also has Farad as unit.
The problem with this dynamic phenomenon is that it is often not

early resolved and it might be due to some measurements errors. But as
ndrew Jonscher pointed out (and he certainly knew what he was talking
bout) , we should not be scared to discuss this effect, even if running the
sici that we will be proven wrong. We, experimentalists , we see this too
ten and usually we measure it well above the noise level and after
minating inductive effects.
conclusion, I think we talk about two different things, the static and the
ynamic capacitance.
ith best regards
etr
Diakopto Inc.
etr -
hink that another source of confusion regarding negative capacitance is

at the most of the people were exposed to the concept of capacitance in
ectrostatics - where the charges can accumulate only on the (surfaces
) conductors, and do not flow through the space between the
onductors (dielectrics). In electrostatics, indeed, capacitance cannot be
egative (excluding some special cases, like moving boundaries of the
onductors with voltages etc.). Also, in electrostatics, capacitance is
rectly related to electric field energy.
more general case - semiconductors, dielectrics with losses, metals,

nd so on - the concept of capacitance is generalized, and capacitance is
efined through complex admittance:
=dI(omega)/dV(omega)
omega) = Im(Y(omega))/omega
this case, capacitance is determined by various complex physical

henomena - carrier transport, injection, capture/emission, etc. It is not
lated to energy, and it is not determined by DC changes of charges in
sponse to applied voltage step. The changes of charges may be
stributed all over space, and it may be impossible and unphysical to
ssociate them with this or that conductor (terminal, contact,...).
his more general definition of capacitance coincides with C=dQ/dV

efinition in the case of electrostatics (no carrier movement between
onductors).
he problem is that this generalized concept of frequency-dependent

apacitance (and admittance) is not discussed in the textbooks - although
equency-dependent dielectric permittivity (or susceptibility) is being
scussed widely.
axim

EIS Laboratory
ear Maxim,
s, I agree and this is precisely what I was trying to point out to Vasilij. In
ct, it is just one possible representation of the electromagnetic (well,
ectrical) response to external perturbation, on the same footing as the
ptical spectroscopies, the only difference being the classical frequency
nge (from dc to ~1 THz).
my analysis of the response, I usually relate it to the space-time

hanges/evolution in the local total electrical charge density ro(x,t).
terestingly enough, it kind of ressembles , the density functional method
electron band structure calculations.
ith best regards
etr

Diakopto Inc.
ear Peter -
s, agreed, this time-dependent "response function" or frequency-

ependent "transfer function" (the one is being Fourier transform of the
ependent transfer function (the one is being Fourier transform of the
her) are very general and useful things. In different areas of
hysics/engineering they are called different things:
complex admittance (complex frequency-dependent conductivity and

apacitance)
reuqnecy-dependent dielectric function
complex frequency-dependent capacitance (real part is the capacitance,

nd imaginary part is G/omega)
he space-time evolution of the charges and related processes

rapping/emission, injection, extraction, etc.), different in different
hysical systems, can be used to explain the specifics of the transient or
equency-dependent response (like negative capacitance). But in most
ases it's impossible to assign these changes to specific contact - these

e things distributed all over space.
egards,
axim

EIS Laboratory
ear Maxim,
is always nice to see that one's view agree with the view of a colleague. I
ope that Narendar has a benefit of our discussion also.
ou write further :
.But in most cases it's impossible to assign these changes to specific

ontact - these are things distributed all over space..."
ere, I do not know whether I understand. If, by contact, you mean metal
ectrodes - sample interface regions, then I have to say that this is not
mpossible, although it may be a difficult task. In fact, the numerical
nalysis of the electrical response IS a boundary value problem and for
mple systems (like a monocrystal, glass and/or simple liquid), the
odelling of boundary response is relatively easy. This is not so for more
omplicated systems, like polycrystals, spatially inhomogeneous systems
uman tissue) etc..
o , although various physical processes may be distributed in various

patial regions, we can model these, using reasonable simplifications.
ith best regards
etr
Maxim Ershov 12th Dec, 2017

Diakopto Inc.
ear Peter -
s, "contact" is a term usually used in semiconductor device community

denote an equipotential system (usually a highly conductive one - a
onductor / metal), which voltage / potential is well defined, and which
an be used to control a device - either by applied voltage or by injected
urrent.
egarding my comment on difficulty to attribute a change of charge to a

pecific contact, when a step voltage is applied to one of the contacts -
hat I mean is that the definition of capacitance C=dQ/dV is (strictly) valid
( )
nly in the case of electrostatics, when there is no DC current between
ontacts. This definition should not be used in systems with non-zero DC
onductivity.
electrostatics, dQ is the change of charge on one of the contacts, does

ot matter on which one (in a two-terminal devices) - one contact gets
harge increment +dQ, and the other -dQ. The sum of the two charge
crements is zero.
devices with non-zero conductivity, the charges (mobile charges -

ectrons and holes, as well as "fixed" charges - traps, impurities, defects,
c.) are spread all over the space between the contacts/terminals, and
e incremental change of the charge distribution dQ(x) (x is the
oordinate - 1D, 2D, or 3D) cannot be attributed, in general case, to one or
e other contacts. That was my point.
egards,
axim
Petr Viscor 12th Dec, 2017

EIS Laboratory
ear Maxim,
hink, I understand what you meant. What I mean by contact is indeed the
terface plane, separating the metal electrode and the sample (System
nder Test - SUT). In this way, the boundary conditions can be well defined
nd modelled.
he important point is though that the external charges, applied to the

ample and sitting within the Debye screening length on the metal
ectrodes sides of the interface planes that form and keep the external
pplied voltage constant, do not enter at all the calculation of the space-
me evolution of the total and local electrical charge density ro(x,t). This
uantity is the el.charge denisty within the sample, while the external
pplied charges enter the calculation/simulation of the response only
rough the value of the applied dc voltage.
herefore, as you point out correctly, ro(x,t) describes all the charges
roughout the entire sample, be those localised and/or delocalised (finite
obility).
nce the corresponding currents j(x,t) are known(calculated), the space

tegral of those gives the response of the system J(t) to the applied
oltage step Vo (for example) and the LaPLace transform of the J(t)/Vo is
en the frequency dependent (in general) admittance of the sample.
hen divided by (iw), you get representation of the response in terms of
e complex capacitance C [Farad] , a perfectly well defined quantity,
espective whether the system is a pure dielectric, pure conductor and/or
mixture of both.
o, at no point one is attributing the charge ro(x,t) to charges at one or the

her electrode. ro(x,t) is just response of the system to the applied
oltage which, in turn, is faciliated by the charges at the electrodes.
o me it seems that we do not really disagree here. I just want to stress

at the measured/transformed response in terms of complex
apacitance has also very definite simple physical meaning in certain
equency regions, like geometrical capacitance of the bulk of the sample,
eometrical capacitance of the interface regions of SUT and/or the
rength (density) of the deep level that relaxes towards
quilibrium/steady state, when the external voltage is applied.
nd of course and under special circumstances, the real part of this

omplex capacitance can go even negative (our previous discussion).
o p e capac ta ce ca go e e egat e (ou p e ous d scuss o ).
ith best regards
etr
Recommendation
Ioannis Samaras 12th Dec, 2017
Aristotle University of Thessaloniki
ear Petr Viscor,
k, this[1] is (among others) a "perfectly well defined quantity"; however,

is defined quantity is NOT, always, a weighty "(complex) capacitance C
Farad]"[1], apart the archetypal case study, of an ideal C (model) and some
lated feeble models. In practice, we are exceedingly spreading this
nciful calculation[1] to some "near C" cases (R//C), e.g. the turn up of the
[1]
mag. part, also. To sum things up, the result, from this calculation,
hould be taken under some precautions, and a possible (but bizarre)
ase, with a Creal<0, is not more than, a fragile hint for a further
vestigation[2], e.g. it should be never treated as an unyielding proof for a
onsequential "negative C", scenario.
From Petr Viscor, above : ...When divided by (iw), you get representation of the response in terms
the complex capacitance C [Farad] , a perfectly well defined quantity, irrespective whether the
stem is a pure dielectric, pure conductor and/or a mixture of both.
This is the best case scenario. However, the experimental errors could be the commonplace
se, as a proposal reasoning.

EIS Laboratory
ear Ioannis,
t us not misunderstand each other here. :
One thing is a transform C(w)=Y(w)/(i*w) and/or Y(w)=1/Z(w) and so

n.. and other thing is: Does this complex function has a clear simple
hysical meaning. Yes, it does in certain frequency ranges , but the rest is
st part of the response, expressed in units of Farad.
From the fact that in most cases in passive systems, the response is
elayed in time relative to the perturbation, Z(w) and thereby also
w), C(w), L(w), M(w) ,..(and other functional forms of the same
sponse) are complex quantities.
In fact, one need not talk about complex capacitance, one can just use
e word "response" or complex impedance. But I think we agree here.
Real part of complex Capacitance (and of complex dielectric response

nction) in metallic Drude systems like Au, Cu or Pt are also negative at
w frequencies, so the so called negative capacitance is not really
omething unique to semiconductors/insulators/glasses.
I can only agree with you that for the time being, it must be still
onsidered as "fragile hint", mostly, as Andrew Jonscher often stressed,
ecause peoples are often "shy" to talk about this subtle effect. My point
as anything BUT an attempt to "..proof for negative C scenario...". I would
e seriously misunderstood here. What I say is only that the phenomenon
seen in some experiments and I would add here that it suprisingly
nough comes out also in the corresponding numerical solutions of

overning set of Maxwell equations.
For illustration, I attach a figure. It is a measurement of the electrical

sponse and of the corresponding theoretical calculation in ultra pure
sponse and of the corresponding theoretical calculation in ultra pure
onocrystalline Silicon sample with Schottky-Schottky contacts. The
her examples I believe are in the two books by A.Jonscher on Dielectric
elaxation in Materials and Universal response.
ith best regards
etr
Vasili Ivanovich Dimitrov 12th Dec, 2017
Tel Aviv University
ear colleagues (involved persons and all, whom to it may concern).
o be open, I wasn’t going to continue discussion on the capacitance, but

eems this is my turn for “childish question”. The plot that was referred to
etr Viscor (minimum at H=10−3) is nothing but local extremum (no
atter how small it is and what is the ratio real/imaginary terms).
es, in a physics we are dealing with some counter-phenomena

cceleration/deceleration (breaking), melting/freezing,
sistance/conductivity, etc.). Yet, nobody defines conductivity as a
egative resistance”.
ormally, any number (rational, irrational, no matter) is characterized by

WO features, i.e. attribute (sign) and value (modulus) |X|. Now I’m talking
n the attribute. So, we read -X as a negative number -X<0, while +X is
ositive number +X>0. Usually, for positive number, we omit sign, hence
e read X (no sign) as a positive number.
o you see that 10(−10), 10(−100), 10(−Googol) (no matter) still are>0.
hese are positive figures! Reread the very definition. By definition, ”The
apacitance is the ABILITY…, etc.”
o, the “childish question” is as follow: “Are you enable to image a

egative ability”?
et me to confess - I’m unable.
o cover the issue, I believe that it’s proper time and place to remember
and René Descartes (Renatus Cartesius). I cite “…Define the sense of
he words, and you will clean up the World from the half of the possible
elusions …” - end of the citation).
other words - ‘define the definitions’. You don’t like definition? Are you
sagree?
K, no objection - change it promptly! But up today, for me “negative

bility/capacitance” is nothing but something like “negative temperature”
n Kelvin scale) or “fried ice”.
orry, but I’m out of the further discussion.
egards to all.
Dimitrov.
Recommendation
EIS Laboratory
ear Vasili Ivanovich,
seems to me that we two still talk about different things. In the

tachment, I am trying to express my view as simply and as clearly as
ossible, in order that we might agree on something. Otherwise, we have
agree to disagree at least at this point
agree to disagree, at least at this point.
ith best regards
etr
Pouya Dianat 12th Dec, 2017
Drexel University
ear all,
apacitance may generally be viewed as the density of potential energy

ored in a dielectric medium due to certain formation of charge. In
uantum mechanics, and at certain critical densities of charge carriers,
g. electrons, the associate capacitance may become negative. It means
at at these conditions, removal of a unit of charge (dq<0) will result in an
nhancement in the voltage (dV>0), therefore C=dq/dV<0. This additional
nergy come is due to exchange and correlation energies of a quantum
echanical system of electrons, which is released and stored in the
electric with removal of charge from the system.
Recommendation
EIS Laboratory
ear Pouya Dianat,
is is an interesting suggestion and it would be interesting to try to

esign an experiment to test this.
owever, the apparent negative capacitance effect I am referring to above,

a dynamical classical phenomenon (the numerical simulations are
sing Classical Electrodynamics equations) and the charges involved are
ewed as classical particles (even the electrons - semi-classical
pproximation and/or quasi-particle concept of L.Landau).
ith best rgards
etr
Alexandru Marius Panait 6th Jun, 2018

National Institute for Aerospace Research "Elie
Carafoli"
ear colleagues,
om a strictly electronic point of view whenever any of you said "dynamic

apacitance" I could not hear anything but "impedance" . Which can of
ourse become negative , zero, or take an arbitrary value. If we mix them
p, we get a fine mess. Yes there are a number of strongly non-linear
aterials, yes lately we got those meta-materials with interesting (global)
operties, etc. But as far as I remember, the definition for capacitance is
e electrostatic one while once we talk about dynamic effects we talk
bout impedance.Think of the so-called dielectric constant -and the fact
at it really is not so constant but a function of frequency and material
ectric (and quantic ) properties.For not-so-small frequency spans and a
eat many situations we can approximate its behavior to a constant
ough. So yes, in a matter of speaking, one can get a "variable capacity" if
e frequencies are variable and high enough , and in some circuits the
ehavior of certain elements can simulate a "negative capacitance"- of
ourse it is just a complex impedance ..being itself. But yes if you want to
guess you can stick a label on it saying "negative capacitance". But it is
fact impedance- with a large C value, that happens to be negative at
at particular point, and yes, it does happen to impedances once in a
hile in say oscillators and scintillating tubes etc From my point of view
hile in, say, oscillators and scintillating tubes etc. From my point of view,
apacitance is a static construct, while impedance is a complex-valued
onstruct , positive or negative or indeed zero- that can contain resistance,
ductance and capacitance terms and may locally become Z=-C*i for
xample . That does not change the definition of capacitance- a static
oncept related to variations of voltage with charge. Yes there are
aterials and devices that sometimes exhibit negative impedance and it
ight just be capacitive at that particular instant under those conditions-
ut the definition of capacitance does not allow by itself negative values.
you want a (silly) analogy, it is like your financial balance - a construct by

efinition made up of all your income (necessarily positive or God forbid,
ro) and subtracting all your debt. In nasty cases the balance can be
egative but that does not mean that your salary ,for example, is minus
ome number) euros.Impedance can be negative and made up of only a
apacitive term, in some cases- but it does not make the capacity itself
egative. In the cases where metals under low frequency or
etamaterials or various strongly non-linear materials are discussed,
apacity might be a function but if we stick to classical definitions, it is
ositively defined. The effect of a locally negative function involving terms
sembling capacity is a complex impedance. If the material is strongly
on-linear one might argue that the capacitance of the material does
mply not exist (* it does but is a function of frequency and other special
onditions depending on material but in a classic sense we cannot say a
apacitor with that material as a dielectric will have a capacity of.. xxx
rads but that we built a sensor for.. frequency, temperature or whatever
at has a variable capacitance output ). In a way think of a piezoelectric
aterial. At rest it has a capacitance. Strike it with an impact hammer and
e capacity varies- sometimes decreases- while generating a very very
mall current by re-arranging charge carriers.Local negative slope for
apacitance- negative impedance yes, negative capacitance never. That is
y take on the problem.
Petr Viscor 6th Jun, 2018

EIS Laboratory
ear Alexandru,
ou are both right and wrong:
You are right that the electrical response is measured as frequency

ependent complex impedance. That is what I was talking about.
You are wrong if you claim that the term capacitance reflects static
ectrostatics. In any material , the response can be viewed in a number of
vial transforms, all of which convey the same information :
w) [Ohm]->Y(w)=1/Z(w) [Siemens]-> C(w)= Y(w)/(i*w) [Farad]. The

omplex capacitance C(w) is just generalisation of the dc limit C(w->0).
You are wrong when you state that it is only in "active" special devices
at you see "negative capacitance" (the negative real part of the
easured complex capacitance C(w)).
The "negative capacitance" is seen in passive devices when the output

easured current (Heaviside step voltage input) increases with time in a
ertain time interval. This is confirmed in the "exact" numerical solutions
Maxwell equations for samples with Schottky-Schottky contacts. Also
esence of deep levels in semiconducting materials leads to observation
this effect.
ith best regards
etr
Recommendation
Alexandru Marius Panait 6th J 2018
Alexandru Marius Panait 6th Jun, 2018
National Institute for Aerospace Research "Elie
Carafoli"
hank you dear Petr for your insight in the matter- indeed whenever
scussing special materials and combinations thereof there are such
fects. That Schottky double junction is such a construct.
ome schools of thought consider the capacitance as a static construct

nly and the generalization a matter of impedance- others embrace your
efinition. Of course your arguments are solid and, I might add, a little
ore..modern than the rigid concepts we were once taught :) . Special
fects in doped crystals , Schottky double junctions and advanced
emiconductor physics are indeed the bleeding edge of the art and I, for
ne, am happy to learn new things every day. Thank you for the
arification, I will look deeper into the matter and will come back .
uddha said you cannot see the truth unless you have no opinion, and a
ing is not wrong or right, it just is. Methinks- if only things were that
mple...After this I have no opinion and therefore nothing more to say-
ntil I find one....).
Petr Viscor 6th Jun, 2018

EIS Laboratory
ear Alexandru,
am happy that I might have helped you on the way. please feel free to
ome back to discuss further.
hink budha was a wise man, but the sentense should probably go as
llows :
ou can not see the truth unless you HAVE an opinion". Then I would
nderstand the message.
ou are right "a thing just IS..", but only until you start investigating. Then,
least in science, you might have a correct or incorrect description of
is "..thing.." - part of ther Objective Reality. the judge is the empirical
vidence (experiment and/or observation).
th best regrads
etr
Michael Partenskii 12th Dec, 2018

Lechem Lab
slightly different look at NC problem, originated from studies of

ectrical double layers:
ease review the story described in the following publications.
rticle Influence of the metal electrode on the capacitance of the c...
rticle Density functional approach to the metal-solid electrolyte i...
tps://arxiv.org/ftp/physics/papers/0208/0208048.pdf
rticle The question of negative capacitance and its relation to ins...
rticle Limitations and strengths of uniformly charged double-layer ...
rticle Relaxing gap capacitor models of electrified interfaces
ease also read the answer below
Maxim Ershov 12th Dec, 2018

Diakopto Inc.
ichael -
is indeed a different take on NC effect.
ormally, in electrostatics, and in semiconductor (or, more generally -

ectronic devices) devices, it is implicitly assumed that the geometry of
e system (conductors, dielectrics, the boundaries, etc.) is fixed. This is a
etty good approximation in electronic / semiconductor devices.
lowing the system to change its geometry immediately leads to new

teresting effects, in particular - NC effect. It's interesting to see how
asily NC appears in a simplest system - a parallel plate capacitor, with
ne plate fixed, and another connected to a mechanical spring.
axim
Recommendation
Ioannis Samaras 12th Dec, 2018
so, a microphone inside an op[1]-feedback circuit might be based on the

bove[2] parallel (with a moving CpP) plate, electro-mechanical capacitor
), such as a mechanical spring-CpP, composite EC-model.
operational preamplifier, with a positive-feedback circuit.
Maxim Ershov, proposal neg-C-model, above.
Michael Partenskii 12th Dec, 2018

Lechem Lab
axim Ershov:
ormally, in electrostatics, and in semiconductor (or, more generally -

ectronic) devices, it is implicitly assumed that the geometry of the
ystem (conductors, dielectrics, the boundaries, etc.) is fixed. This is a
etty good approximation in electronic / semiconductor devices. "
--------------------------------------
esponse:
hanks, Maxim. To the readers not familiar with this field, we owe an
xplanation. In the context of our discussion, your statement quoted
bove may lead to confusion. Thus, someone may erroneously assume
at electro-mechanical models with variable dimensions ("geometry")
ave no relation to the properties of interfaces important for
ectrochemistry or electronics, because the geometry of experimentally
udied devices is reasonably assumed to be fixed.
et us clarify the picture using electrochemical applications as an

xample.
hile the macroscopic dimensions of electrochemical cells are indeed

xed, there are significant changes in the "geometry" of charge
stributions induced at atomic scales by the electrode charge. For this
ason, the interfacial electric double layer (EDL) is theoretically described
s a microscopic capacitor with movable plates ( variable effective
ickness h ). In some cases, h significantly decreases with charging, and
is leads to the predictions of negative differential capacitance (NC).
hus, despite the fixed dimensions ("geometry") of the macroscopic cell
lectrodes, electrolyte, boundaries , etc), the "geometry" changes of EDL
e profound. Exactly these changes are responsible for NC, which is
e focus of our discussion.
he electroelastic models serve to illustrate the origin of this

henomenon Their "spring" is a metaphor for all forces involved in the
henomenon. Their spring is a metaphor for all forces involved in the
quilibrium of interface polarized by the field of electrode (Coulomb,
ntropic, exchange and correlation - you name!). Their movable "plates"
e conceptually associated with the centroids of microscopic charge
stributions (electrons, holes, ions, polarization charges).
other words, these toy models mimic the variable geometry of EDL.
hey allowed to understand the origin of NE and analyse possibility of its
bservation. More importantly, they allowed to predict and analise
stabilities and phase transitions in EDLs associated with the onset of
C.
he elastic capacitor (EC) was the first model demonstrating NC in

olated system with controlled surface charge density. It also
emonstrates NC-related charging instability in EC connected to the
otential source (battery). A more advanced model is the squishy (elastic)
apacitor (SEC) with lateral flexibility of its plates, demonstrates NC-
lated lateral instability in the isolated system
rticle "Squishy capacitor" model for electrical double layers and t...
Some other interesting properties can be demonstrated by more

dvanced EC models.
equency (f)-dependent response of these models is affected by "NC -

lated" peculiarities such as the "mode softening" in the vicinity of critical
oint (vertical asymptote of C) . As a result, EC behaves as a classical
xed gap capacitor at high f, and sharply deviates from this (displaying
rongly non-linear response) in the low f limit (this was mentioned in
rticle Self-consistent electron theory of the metal-solid electroly...
nd some later publications). This result is apparently related to the

operties observed in your collaborative studies
rticle Negative Capacitance Effect in Semiconductor Devices
nd others.Thanks for your comment that motivated my reading.
eviously I had a perception that NC in semiconductor devices is a
eculiar interpretation of certain behaviors of impedance, and has no
lation to the equilibrium characteristics of real interfacial capacitors.
ow it looks like these fields are closer than I thought.
____________________
annis, other conventional examples of electro-elastic behaviors are the

ectro-compression of lipid bilayers and piezoelectricity, electrostriction,
ectric actuators. Thanks for your comment.
Recommendation
Alexandr Vladimirovich Kobelev 12th Dec, 2018
Institute of Metal Physics
wonder, is it possibe to stay within classical mechanics and

ectrodynamics to understand NC phenomenon, or one must involve
xchange, correlation and etc features of quantum theory? I hope, the
nswer is positive.

EIS Laboratory
ear Alexandr,
see Negative Capacitance (not inductance) both in experiments and in

e corresponding Classical Electrodynamics simulations. The fit is often
uite "impressive". I stil work on the precise cause, the non-linearity and
oundary conditions being the most likely candidates. Not to forget the
elayed response of some mobile charges relative to the majority mobile
harges.
ith best regards
etr

ear Petr,
onlinearity is to me quite reasonable way to get NC. Look for, please, the
onmonotonic relaxation of mechanical stress, or deformation.
BookKobelev_Nelenejnye_vyazkouprugie_English.pdf · 9.37 MB
EIS Laboratory
ear Alexandr,
ank you for the reference to your work on visco-elastic properties of

ological tissues.
here are similarities between electrical and mechanical relaxational

henomena and in phenomena like glass transition, melting, creep ,they
e even related.
will read your work with interest, but right now I have a problem with the
oncept of geometry caused non-linearity (p.210 of the book).
can not see how a combination of ideal springs(constant, time

dependent elasticity) and ideal dampers(constant, time independent
scosity) can lead to genuinely non-linear behaviour .
dielectric relaxation, this type of models (variouis topological nets,

omprising ideal resistors(viscous flow) and capacitors(elastic
eformation)) give rise to the distribution of various Debye-like relaxation
mes that can be fitted to the (non-linear) experimental results. This
ough does not mean that they(relaxation times) have a physical
terpretation. The explanation, in my view, should be looked for in the
on-linear nature of the "ideal springs" themselves. In atomic systems this
ads to a genuine non-linear behavior (Fermi, Pasta, Ulam paradox).
ith best regards
etr

ear Petr,
hanks for prompt reply to my note.
It's a true thing that electrical cirquit with capasitors and resistors may
ve much more opportunities in modeling than network of springs and
amps. I'm not enough expirienced in this field.
Two exponential pattern in relaxing is quite common in nuclear

agnetic and electron paramagnetic resonance, with spin-spin, and much
ore rapid spin-lattice relaxation as a physical origin of it. They are usualy
uick at first and then in time scale it goes a long tail, still being
onotonically decreasing.
In nonlinear systems, however, we can observe nonmonotonic relaxing

uantity (after step-wise Heaviside excitation). The derivative is at first
ositive, nul in maximum, and then, negative.
Nonmonotonic_relaxation3.pdf · 2.18 MB
EIS Laboratory
ear Alexandr,
your points :
wonder whether they do (R,C elements in electrical response as

ompared to springs and dampers in mechanical response). All these
ements are based on the ideal response, that is to say R(ideal,
me/frequency independent conductivity) and corresponding damper
deal, time/frequency independent viscosity) are both purely dissipative,
hile C(ideal, time/frequency independent permitivity) and corresponding
amper (ideal, time/frequency independent bulk modulus) are both purely
on-dissipative (90 degrees out of phase to applied force). In both cases
e characteristic response time is given either by conducto-permitivity
laxation time tau= permitivity/conductivity or Maxwell visco-elasticity
laxation time tau=viscosity/bulk modulus .
ow, I am not an expert in mechanical relaxation , but I believe the

xpressions are correct. In conclusion therefore I also believe that various
pological networks should give similar type of response.
Not only two, in principal there can be even more of simple exponential
laxations (Debye relaxations) working in parallel/series.
Yes, and it is this I was referring to. You can get this type of response, if
e system is spatially non-homogenoeus, but still built with ideal
omponents. That we see in the electrical response, but in most cases,
e required spatial in-homogeneities (spatial variations of Rs and Cs -
spatial variations of the corresponding conducto-permitivity relaxation
mes) are out of reasonable physical limits . For example the system will
ave to be composed of series impedances (each impedance consisting
parallel R(x) and C(x)) going from almost perfect insulator
onductivity->0) to almost perfect metal ( permittivity->0 idealisation
ough !!) . In conclusion here I therefore agree with your reference main
oint "...spatial non-homogeneity.." as being the cause of non-monotonic
laxation .
ith best regards
etr

ear Petr,
s a great pleasure to hear from you, very interesting for me, but i was
ngaged in that some years ago.
he idea was that some (even 2D topology) construction composed of

ear Hook springs with different stiffness may have nonlinear behavior in
ress-strain curve. Rhombic model with more soft transversal diagonal
pring demonstrates 'toughening' effect as if its Young's modulus
crease with stretching. This effect is quite common in biological tissues
nd play important role in natural behavior. Btw, coiled spring, as a
ominent human investigation, has similar toughening after 'unfolding' of
oils when stretching modulus works, while it is rather complinable in
tial coiled state when shear modulus works.
s to nonlinear capacitor, i remember Misha Paryenskii's (my school

ate) spring - in parallel - capacitor model which he envolved early in NC
oblem for electrolytes.
ood wishes in new year,
espect,
p ,
Kobelev
obelev@imp.uran.ru

EIS Laboratory
ear Alexandr,
is interesting to envisage a single block with an internal structure

hombic model), encompassing a number of different ideal Hook's
prings with varying Bulk (Young) modulus. I have to think of the electrical
sponse analogy.
owever, in the linear response regime (all elements are stil ideal) it
eems to me that the response is again that of a distribution of
haracteristic relaxation times (Maxwell visco-elastic relaxation times) .
nd morover, in order to get time/frequency dependent behaviour,
ampers (dash-pots) have to be present as well.
he mechanical response has always intrigued me, perhaps it is time to

et more involved in the matter. the Glass Transition phenomenon I have
entioned, does indeed involve both (inclusive NMR).
l the best wishes for the year 2019 to you as well !!
ith best regards
etr

ear Petr,
i worry you with my replies, please, tell me to have a break, don't

esitate. l'm pleased conversating weekendless.
What do you mean of Young's modulus being not constant? By hands?

s to my mind, each nonlinearity is due to internal topological structure, at
ach scale, and it may be fractal.
If my memory serves me, linear Newton's damper can be attached to

ook's spring in two ways: in parallel (Kelvin-Foigt model), and then it has
o relaxation at all, only hysteresis loop, and in series (Maxwell model),
hich fits well to mimic relaxation, but it has no equilibrium state, with
finite creep.
It's quite easy to programm both purely elastic, or posessing viscosity,

omplex (2D, or 3D) graphs to get response to uniaxial stretching, or
erhaps, shear loading. I hope, i'm ready. Dependent on the goal,
omething may be easy in mechanics, smth in electrical cirquits.
ood luck,
Kobelev
Michael Partenskii 1st Jan, 2019

Lechem Lab
exander: is it possible to stay within classical mechanics and

ectrodynamics to understand NC phenomenon or one must involve
xchange, correlation and etc features of quantum theory? .
exander, the answer depends on what do you mean by understanding

he " NC phenomenon ". And primary, on to which phenomenon are you
ferring to? Please describe the observations and we will try to discuss
ferring to? Please, describe the observations, and we will try to discuss
eir possible interpretation.
ith best regards.
Alexandr Vladimirovich Kobelev 1st Jan, 2019

ear Michael,
eople believe the NC phenomenon exists, i can hardly imagine that its
echanism in one case differs from the other. Let's take the electrolyte
oundary, for instanse.
est wishes,
Petr Viscor 1st Jan, 2019

EIS Laboratory
ear Michael,
your comment to Alexandr :
By understanding I believe Alexandr means a sufficiently precise

escription of the phenomenon of Negative (dynamic) Capacitance using
assical Electrodynamcis and Classical Mechasnics. I believe this to be
deed the case, apart from the energies of the electrically active particles
These might have to be calculated quantum mechanically.
As to the observations, please have a look at the enclosed WD. I have

hosen two cases, both for the "perfect" system, namely defect free
onocrystalline Silicon, where almost everything is known to a high
egree of accuracy.
ith best regards
etr
NegDynCapSilicon01.docx · 47.43 KB
Lechem Lab
hank you, Petr, for sending the real stuff for case study. Sorry if my
uestions are immature.
) Do you apply a constant component of voltage (should I say "non-zero

as"?) in you experiments?
) What is the equivalent circuit of your setting?
) Could you please reflect on the assumptions made to derive the sign
nd value of C from the measured imaginary component of impedance ? (
understand the relation for regular RC (RCL) circuit, but your case is
fferent).
) In your response, you asked for the classical example of the NC, and
dded "(dynamic)". Why?
S You can contact me at moshep@brandeis.edu with anything that does

ot fit in the frames of public forum. Otherwise, we can use some
ollaborative tool (say GDocs) for more private discussion.
i h l kii
Lechem Lab
hank you. Alexander. I am not aware of any unambiguous measurement

NC at the electrochemical interfaces which does not mean that they do
ot exist. If you find an example, similar to one sent by Peter, we can
clude it in our case study.
ith best regards. M
S If the private setting suits you better, you are welcome to use my email
a collaborative tool.

ear Michael,
Please, have a glance at Oleg's old paper.
May i scetch down my general view. With my poor awareness, i left all
gh-level activities in the field to you, and to much yonger Petr. As to my
bilities, i hope i can model NC analogue in massless viscomechanics.
he capacitor equals spring, resistor - dashpot, (and induction coil works
s inertion mass). The fish is, to me, in friction, which needs dinamics, and
nonlinearity. They both lead to nonmonotonic relaxation (see, pls.
viously attached file). According to cited by Petr paper, which i'v read a
eak later, it may serve as an origin (they mentioned there 'positive
erivative', but it's completely unstable case).
Memorizing one of ancient Kourovka's, and Kurkin's question to your

port, the problem arises with NC prohibition by some conservation law.
he answer was, i remember, in periods in time domain, with NC, while
rther the right things restore.
ood wishes,
exa
ZfurP.pdf · 756.25 KB
Lechem Lab
asha, evolution of our views on NC is reflected in the following
ublications.
rticle Influence of the metal electrode on the capacitance of the c...
rticle Self-consistent electron theory of the metal-solid electroly...
rticle The admissible sign of the differential capacity, instabilit...
rticle Limitations and strengths of uniformly charged double-layer ...
m am sorry for self-references, but this is the most concise way to

spond to your questions, explicit and implied.
y comments and questions to your paper are too technical, and do not
atisfy the Q&A form of this public forum. So, it is better to discuss them
private setting.

isha, i've send you reply at your private address ...@gmail.com.
etr may also contact me privately, if needed.
Kobelev
Petr Viscor 1st Jan, 2019

EIS Laboratory
ear Michael(Misha),
our questions are definitely NOT immature . Her I try to answer them :
) Do you apply a constant component of voltage (should I say "non-zero

as"?) in you experiments?
ot always, but the data I have sent you actually were measured under
cBias Voltage (~0.1 to 1.0 Volt). I know though that I have somewhere
e data without dcBias and still showing Neg. Cap. effects.
2) What is the equivalent circuit of your setting?
do not have a good approximate linear equivalent R,C,L circuit for these
fects, but I am sure that one can be made, although ideal inductance
ement would have to be involved and that would have no physical
terpretation (simple). The response is not inductive.
my simulations I solve the complete set of Maxwell equations in real

pace-time and then La Place transform them to get frequency dependent
dmittance/Impedanca/Capacitance etc.. The agreement between the
ata and the numerical simulations are quite good in the case of one or
wo deep levels in perfect semiconductor (monocrystalline Silicon).
3) Could you please reflect on the assumptions made to derive the sign
nd value of C from the measured imaginary component of impedance ? (
understand the relation for regular RC (RCL) circuit, but your case is
fferent).
s is clear from the above, I just solve the equations and get the
mpedance.
he convention that I follow when working with R,C.L networks is
w)=Z1(w) + i*Z2(w). That gives -90 degrees for the purely capacitive
sponse and +90 degrees for purely inductive response. I hope I have
nderstood your question correctly.
4) In your response, you asked for the classical example of the NC, and
dded "(dynamic)". Why?
NC-A classical phenomenon
have not finished the analysis of this phenomenon ( there is also a truly
egative phase, inductive response in some of these samples, which is
ue to ballistic transport - kinetic inductance effects that complicate
ings), but for the time being I can explain the data at hand just through
assical electrodynamics and elements of classical mechanics ´(forces
n the particles ). Therefore I do not believe that it is a pure Quantum
echanical effect.
NC - A dynamical effect
ere I want to make a distinction between a dc concept of a capacitance

nd a dynamic measurement of a capacitance in order to avoid some
itical comments like ...there is absolutely no NC in Nature... This kind of
omments have occurred here.
hen things settle in time (time >infinity) I stil believe that

hen things settle in time (time->infinity) I stil believe that
(charge)/V(voltage) = C(capacitance of the system). T least in the linear
sponse regime.
ith best regards
etr

Lechem Lab
ear Petr, your response is very interesting, and provokes many

uestions.Here is just a few.
In studies of electrochemical double layers with no Faradic current

cross the interface, the charge Q is essentially the electron charge
calized at atomic scales near the surface of a (metallic) electrode. What
the composition of Q in your experiments: its components, origin,
pacial distribution? There are obvious differences due to differences in
ebye lengths of semiconductors , but are there other, dynamics -related
fferences?
The differential capacitance dQ/dV , not the integral capacitance Q/V ,

usually used in Electrochemical studies of interfaces. This is similar to
sing instantaneous rather than average velocity describing the
echanical motion. Why does your response mention only the integral
apacitance?
I have doubts (likely, because of the lack of understanding and

ducation in this field) that Z2(w) can be safely named in general "the
urely capacitive response". This title is indeed adequate for RCL circuits ,
nd actually originates from this local and linear limit. But is it true in
eneral? (sic: I do not mean the trivial issue of filtering out the induction )
(On your response 4.2 regarding the dynamic measurement of a

apacitance). What exactly is measured dynamically? Is it some quantity
at exists at rest?
Describing the model, you mention deep electron states in Si. Can you
ill consider your model "classical"? (I believe that this only sounds
ontradictory, and you certainly have a good answer).
his is already getting complicated. I have to stop here avoid further

ess. :)
ertainly, there are more questions, but, as I mentioned in response to

exander, they are technical and suggest further discussion. This will be
detraction from the Q&A format of this forum. So, I would appreciate if
e can continue this in a collaborative setting, such as Google docs. You
e welcome to reach me at moshep@brandeis.edu.
Petr Viscor 2nd Feb, 2019

EIS Laboratory
ear Misha,
have just completed an answer to your questions and just before sending
off, it bloody disappeared from my screen.. Sorry, I will try again and will
end it as suggested, to your e.mail. it might though take a week or so,
ecause I am abroad.
ith best regards
etr
Maxim Ershov 2nd Feb 2019

a s o 2nd Feb, 2019
Diakopto Inc.
his is an interesting and fruitful discussion, please post your exchange

ere :)
ne more thought on negative capacitance -
e analogy between electrical and mechanical effects says that

apacitance in electricity is equivalent to stiffness coefficient (k) in
echanics.
nergy in capacitor: E=CV^2/2
nergy in mechanical spring: E=kx^2/2
oltage across a capacitor: V=Q/C
splacement of a spring: x=F/k (Hooke's law)
nd so on.
terestingly, negative stiffness in mechanical world has been engineered

nd used for a long time now. Once, at an exhibit of a conference (I don't
member which one), I came across a company called Minus-K
echnology, that makes products based on negative stiffness effect
ables to reduce mechanical vibrations - for example, for probe stations
r microelectronics):
tps://www.minusk.com/
e there similar examples of using negative capacitance in engineering /

chnology?
here are a lot of papers and information on negative impedance circuits,

r example:
tps://en.wikipedia.org/wiki/Negative_impedance_converter
owever, I have not heard much about their practical applications (for
xample - to reduce RC delays in ICs).

EIS Laboratory
ear Maxim,
K, I will do it, I just have to remember to save the text not to loose it
gain.
our example of negative Young modulus is interesting.
nd you are right, there is a lot of parallelism/analogy between visco-

asticity and conducto-permittivity. Probably the "same type" of equations
escribing the dynamics.
ith best regards
etr
Alexandr Vladimirovich Kobelev 2nd Feb, 2019

hanks to Maxim for referring, but i can't realy imagine the mecamizm of
egative stiffness (NS). That anti-noise tablet with NS must be completely
nstable: it produses force negative in sign with deformation, at stretching
gives force which increases stretching, and at compression we go to
ollapse. The same thing with capasitance always lead to prohibition of it
stable case and it may work only after shunting with "normal" elements
stable case, and it may work only after shunting with normal elements.
oming back to initialy asked question about devices based on NC

henomenon, the list in wiki Negative Impedance article gives hundred of
uch examples in electrocirquits. In electrochemistry, biochemistry and
ectrolyte field i am unaware of devices, only traces of NC in
ectrocapillarity of melted copper/ oxide melt interface with adsorption,
nd examples, given in Micael Partenski's contribution to this discussion.
ood luck to all of us,
Kobelev

EIS Laboratory
o Maxim, Alexandr and Michael :
I believe that the examples given in Wiki on NC "devices" are related to

active devices, not the passive ones that we discuss here (?!).
From the Electrical Impedance Spectroscopy measurements on various
systems andfrom the following following analysis, my impression is
that one deals with what I call "delayed response".
An example is again a deep level in Silicon monocrystalline sample with
good metal electrodes. Here, if the emmission and capture rates for
electrons between the deep level and conduction band and the deep
level and valence band are appreciably different, the equilibrium/steady
state is established first there, where the rates are largest and at a later
stage follows the "slower channel". This leads to an increase of the the
total measured current through the sample within a characteristic time
window. But it then settles to a constant value and stays there to time-
>infinity !
Interestingly enough , the same phenomenon happens (much weaker
though) just with Schottky-Schottky system without deep level. Non-
linearity and assymetry are probably the main cause.
ith best regards
etr
Maxim Ershov 2nd Feb, 2019

Diakopto Inc.
ear Alexander - I think negative stiffness is a negative component, that is

dded to a positive (normal) stiffness, to produce effectively very small
ositive stiffness (small capacitance in electricity) - to minimize
brations.
his page explains the basics, very briefly (I did not try to understand it
lly):
tps://www.minusk.com/content/technology/how-it-
orks_passive_vibration_isolator.html
pparently, the stiffness (or a part of it) can be negative only under certain
rcumstances (frequency range, etc.) - similar to capacitance, that can be
egative only within certain frequency range and within other limits
emperatures, applied voltages, etc.).
constant negative capacitance would lead to an (unphysical)

xponential voltage increase on the capacitor.
axim
Maxim Ershov
Diakopto Inc.
y the way, a very quick search on "negative stiffness" reveals a volume of

aterial on this effect, for example:
tps://www.comsol.com/blogs/can-a-stiffness-be-negative/
tps://www.me.utexas.edu/~ppmdlab/files/Kashdan_Paper11_FINAL.pdf
e may learn something useful from mechanical world, to apply and use
is information in the electrical world! :)

Diakopto Inc.
ear Petr -
s, circuits reproducing effective negative capacitance (or, more

enerally, negative impedance) are based on opamps, that contain
ansistors.
the context of electronic devices and their negative capacitances -

orrect, we are talking about what we can call "passive" devices, although
do not see a fundamental difference between transistors and simpler
evices - p-n junctions, Schottky diodes, etc. - when these "simpler"
evices display a complex dynamics, that leads to a delayed current
sponse to applied voltage excitations (a fundamental requirement for
e onset of negative capacitance, as first explained by Andrew Jonscher).
eferring to an earlier question/discussion - I believe that, in general, a

henomenon of negative capacitance has nothing to do with whether
ere are classical or quantum effects involved in the dynamics of the
ectrical system. Fundamental microscopic mechanisms can be quite
fferent, either quantum or classical (or combination of thereof), and the
ain requirement is the delay between current and voltage transient
gnals.
axim

ear Maxim,
egative additive to in general positive stiffness means decrease of

oung's module with deformation. As Petr said, it may come from 'active'
omponent, which means nonlinear feedback effect. We may imagine of
ourse, computer-based, or from special electric scheme component with
pposite phase. It looks like well known method of noise reduction by
mmidiate adding to the signal one with it's inverted phase. The thing is
ow to do it mechanically, and i know how to get increase of stiffness with
retching in this way.
ith good wishes,
Kobelev

ear Maxim,
anks a lot for the comsol site. Just reading, it's interesting.
it the 'Femlab' designer?

Kobelev
Michael Partenskii 2nd Feb, 2019

Lechem Lab
hanks, Maxim, for the analogy , and Sasha, Petr for further insightful
omments. Apparently, this kind of analogies reflect similar nature of the
operties such as dielectric and magnetic susceptibilities, various elastic
onstants”, compressibility, capacitance… you name! (I can not find it
ow, but Petr, I belive, has already mentioned this relation in our
rum).They are all related to thermodynamic response functions, and
ence to stability of matter , second derivatives of different energy
nctions (by thy way, negative Poisson ratio, which is not directly related
stability and not thermodynamically forbidden, is still counter-intuitive
nd fascinating !). Their divergence indicates "criticality". Negativity is a
onundrum raised in practically all such cases (see for example Kirzhnits
al in respect to static dielectric response eps(k)). Probably the most
mous is the issue of negative compressibility in van der Waals phase
agrams. Thrilled by its analogy with NC, we discussed it in
sing "squishy capacitor model" for illustration.
he Comsol forum example looks like a nice version of Euler buckling

stability. Thanks, Maxim, for the pointer.

Lechem Lab
his response is edited. I removed some confusing and lengthy parts
the original post. MP
---------------------------------------------------------------------------------
axim: "I think negative stiffness (NS) is a negative component, that is

dded to a positive (normal) stiffness, to produce effectively very small
ositive stiffness (small capacitance in electricity) - to minimize
brations".
ear Maxim, how do you add (negative) stiffness to stiffness? If we target

e analogy with capacitance, it would be appropriate to consider two
asic connections: parallel and serial. Using your own k <-> C analogy , the
erial connection of two elastic elements would result in the gross elastic
onstant K = k1x k2/(k1 + k2). Did you mean to make it smaller by
hoosing proper k1< 0? Otherwise, did you mean parallel
onnection?
aturally, stiffness is not exactly k, but it is unlikely to make a big

fference.
ut is it really possible to add k1<0 to the device? Let me mention in this

spect a story from the live of NC.
e discussed a similar case, with (potentially, in some charge range)

egative capacitor (c1) and a positive capacitor (c2) connected in series
.B). This was important because of the conventional assumption that
e positive c2 "buffers" NC and stabilizes the system if total C>0. It was
hown, however, that this assumption is false: as soon as c1 approaches
itical point (right before it becomes negative), system becomes unstable
d ii ih 0
nd transitions to a new state with c1>0.
eturning now back to stiffness and using your analogy, we may expect
at just before k1 becomes negative, the system looses stability and
ansits to a new stable state with positive k1. In other words, it seems
nlikely that one can control stiffness by connecting positive and negative
omponents. "Unlikely" does not mean "impossible" - I simply do not know
ow, and I can be wrong.
S: Surely there are many other ways of controlling stiffness. My doubts

nly concern the addition of NS element for this purpose.

ear Maxim and Misha,
being not so smart enough in electrical engineering, reading article by

enrik Soennerlind in Comsol blog, reveal at last the block, composed of
ormal elastic Hook's springs, posessing NS in the dependence of force
l) prodused by elongation .The nul point in the middle is the begining of
stability domain. It looks like a variety of 3D networks springs - rigid rods
th rapid flip-flop effect in rod's orientation. Who can give electric
nalogue of such mechanics?
est wishes,
Kobelev
F(l).JPG · 23.84 KB

Lechem Lab
asha: Who can give electric analogue of such mechanics?
ear Sasha. This sounds like an interesting challenge. However, I do not

early understand its goals.
his is a wonderful article on the role of models and their purpose.
tps://nemenmanlab.org/~ilya/images/9/99/Rosenblueth-wiener-
945.pdf I remember reading a while ago that its authors had a very
opular seminar on interdisciplinary modeling (started by Rosenblueth).
some point, they decided to stop this project because (I am quoting
om memory) " anything can be a model of anything else, but the best
odel of one cat is another cat"
odel of one cat is another cat .
he question is what is the mechanical problem that you want to solve

th the help of electric analogs?

ear Misha,
hanks a lot for poniting to Weiner (that same, sic!) notes on modeling
hilosophy, i agree of course, that it is mechanism of our (and i believe
her animals) way of brain-governed behavior, except the modeling for
odeling and couple of cats, which is added for conspiracy, i wonder.
he purpose of my effort i believe is to imagine NC 'in mechnical way'. It's

ot by chance you and Jordan use spring (mechanical mirror of capacitor)
your squiszy model.
capavitor's gap varies with charging, it may not only decrease natutaly
a Coulomb attraction, but some times increase due to some nonlinear
onstable understandable 'on fingers' way. Other possibility is unstable
ecreasing charge with voltage.
oods, not nessesary 'material',
r you, relatives and neibours.
asha

Lechem Lab
K. : "The purpose of my effort i believe is to imagine NC 'in mechnical

ay'. It's not by chance you and Jordan use spring (mechanical mirror
capacitor) in your squiszy model. "
asha, initially (with Vitaly Feldman and Misha Voroibjev) we used electro-
astic models to understand the counter-intuitive and puzzling outcomes
semi-microscopic models of Double Layer (EDL) where electrons were
udied in spirit of Density Functional approach. Elastic capacitor helped
s to elucidate the nature of NC (which microscopically was already
ssociated with the displacement of the "plates" - centroids of charge
stributions on both "sides" of EDL) , grasp its relation to (in)stability of
terface, and, later, to introduce other models addressing some extra NC-
lated features and possibilities.
he elastic spring was used as a component of capacitor, responsible for

e charge-induced gap variation, because we needed to demonstrate that
C is compatible with some (restricted) type of equilibrium; the restriction
as later termed "sigma-control"*. The spring itself (or the stabilizing
rce) may contain a lot of possible behaviors. For instance, it can be
ulti-stable, and cause instabilities even under sigma control. Such
stabilities naturally enrich the DL behavior patterns under q- or Phi-
ontrol. An example of such behavior was demonstrated by "Amper -
ook" capacitor model
rticle On the non-linear response to charging of a relaxing capacitor
ut even this toy model was aimed to demonstrate some

icroscopically-discovered behaviors (where the distance of the solvent
olecules' closest approach to electrode was a variable parameter
etermined from equilibrium , additionally contributing to gap variation).
uch more behaviors may be introduced by playing with springs (and the
ate's gap-dependent potential energy in general), but we always avoided
g p p p gy g ), y
aking it an end in itself.
By the way, we considered a similar combination (and mutual effect) of

wo types of phase transitions in super-ionic conductors, a field-induced
ansition in the electrolyte and NC -related instability in DL, in our work
th Yuri Kharkats.
K: " If capacitor's gap varies with charging, it may not only decrease
aturally via Coulomb attraction, but some times increase due to some
onlinear unstable understandable 'on fingers' way. "
is well established that the gap is non-monotonous function of charge

heck, for instance, "lattice saturation" entropy effects in ionic layer,
ading to expansion of the gap with charging). It can contract or expand
epending on electrode charge and other parameters [temperature,
oncentrations, etc]). There is vast literature on this subject, from old ages
recent studies of, say, ionic liquids. A variety of behaviors are also
lated to the "dipolar" component of DL. They all are "non-linear" and not
ecessary unstable.
We were not interested in modeling all these behaviors, focusing only

n NC.
K: "Other possibility is unstable decreasing charge with voltage".
ossibility of what? This statement seems vague. Can you explain clearly
hat does it mean. Please, try to be specific. Describe the phenomenon,
o that we would be able to discuss it productively.

ear Misha, may be i'm wrong.
Explain me pls simple thing (i read that early articles quite breafly and
ng time ago, so poorly remember the details) about DL: charge at
apacitor planes exists, external voltage does not. If we apply voltage

pposite in sign to make charge nul, and then restore it, can we name it
C?
So, equivalent scheme of transistors, resistors, etc, for DL electric

ehavior with NC can't be seen? And i wish it. Much simpler previous case
two springs also?
At last, may be i misunderstand smth, NC of flat capasitor (and cilinder

ne) can be obtained by a) varying gap width in "unnatural" way keeping
ormal charge course, or b) keeping permanent gap by opposite course of
harge at external electric polirizing. This can be done via electrotech
rquits with feedback as in impedance meters.
orry for my nonspecific abstractal flow.
ood luck,
asha

Lechem Lab
asha, I can not grasp all the details of your questions, but you can surely
oogle the answers. I believe that some of this is related to the "zero
harge point", but in case of ideal surface-inactive electrolytes you can
afely assume (at least for the sake of discussion and mutual
nderstanding) that V(Q=0) =0.
this point, to avoid unnecessary complexity, I would avoid references to

mpedance and feedback- just deal with basic physics - charging C with
xed portions of Q, or applying fixed V.
would be fair, if in addition to new questions you added some answers

my previous question as well. :)

ear Misha,
ood question MAY value much.
K, settled.
est wishes, Sasha

Lechem Lab
hank you, Sasha. I am trying :)

Lechem Lab
K: 1) Explain me pls simple thing (i read that early articles quite

eafly and long time ago, so poorly remember the details) about DL:
harge at capacitor planes exists, external voltage does not. If we apply
oltage opposite in sign to make charge nul, and then restore it, can we
ame it NC?
asha, I believe that I understand now your question (except for the early
ticles that you read. Are they still available? Can you send a link?)
respect to the essence of the question, consider a thought experiment,

o that all physics is on the table. Assume that you have a polarized film
etween the plates of capacitor, with P the surface density of polarization
ipole moment per unit area). Then if the plates are grounded (V=0), they
e charged . Let's name this charge density S0. Assume for simplicity
at P is frozen -does not depend on the field from the plates. ( You can
dditionally introduce dielectric constants eps inside the gap but the
hysics will stay the same). If you apply a voltage dV, the charge will
hange by dS exactly like in a classical high school capacitor. The
apacitance C = dS/dV = constant(V). If you now apply voltage -dV, the
harge decrement is - dS, and C stays the same. In other words, in this
mple picture the equilibrium charge at V=0 has no effect on capacitance.
aturally, C is strictly positive. In your question, "and then restore it"
orresponds directly to the second step of this experiment, no matter how
xactly the charge was changed at the first step.
est wishes. M

hank you Misha, after some time I've just get myself this unswer. My
ope was that exsistance of unpolarized DL may be the reason of NC. I've
st in mind that for lipid membrains in instance it's due to dipolar
olecules arranged in a DL. The porige boil in my pot irrespective to
nything, it's my fault, what can I do? :(
ake it easy as given with me, your old and true mate.
asha
S if it is saved, please, sent me back privately address of YouTube clip of
aradoxical English sillables usage (my reply to your 'chastushki', in
rses, by some guy, I've lost)

Lechem Lab
K: My hope was that existence of unpolarized DL may be the reason of

C. I've lost in mind that for lipid membranes in instance it's due to
polar molecules arranged in a DL.
, Sasha. Please clarify. Seemingly, I understand each word separately,

ut not jointly. How "existence of unpolarized DL may be the reason of
C",
nd what is the relation to lipids. Just provide a simple model. You can do
in "mechanical way" if you like. Btw, there is no deficit of polar molecules
the interfaces. For instance, so called "dipolar models" of the compact
yers are focused on the electric response of the polar water molecules
contact with electrode. So, if you have same polaritity- related ideas, we
an discuss them. We have some modest experience in this field :
rticle Electron and molecular effects in the double layer for the m...
rticle Model for a metal—electrolyte interface: elastically bonded ...

ear Misha,
guess it was my unfruitful idea. Due to my lack of education i often

oduce paradoxial things believing that they may lead to sucsess.
the surface of metal DL model of TF the internal Coulomb potential

hich give expon tail of el distribution can not be deminished by any
xternal voltage (may be not?). In lipid membrane DL the same?
do this conversation believing that my fulish activity may help someone

revise his position ones more, that is vry important as to me, or perhaps
get profit to us all.
ith love,
asha
S that finnish gue is funny in all his clips. Till now i do not find lost
nglish paradoxial verses about spelling and pronounsiation
Recommendation
Lechem Lab
K, Sasha. Thanks for your time.

Lechem Lab
etr: "I have just completed an answer to your questions and just before
ending it off, it bloody disappeared from my screen.. Sorry, I will try again
nd will send it as suggested, to your e.mail. it might though take a week
so, because I am abroad."
ear Petr. Sorry I missed this note. I am waiting for you response and feel
ateful for our productive dialogue. Wherever you post your response,
ease send also a copy to my brandeis address as you planned.
hank you.
isha

EIS Laboratory
ear Misha,
have just returned from abroad and will shortly send the promised
nswer to your questions.
ith best regards
etr

Lechem Lab
hank you, Petr.

EIS Laboratory
ear Misha,
ere is the promised reply to your questions :
ear Petr, your response is very interesting, and provokes many

uestions.Here is just a few.
In studies of electrochemical double layers with no Faradic current

cross the interface, the charge Q is essentially the electron charge
calized at atomic scales near the surface of a (metallic) electrode. What
the composition of Q in your experiments: its components, origin,
pacial distribution? There are obvious differences due to differences in
ebye lengths of semiconductors , but are there other, dynamics -related
fferences?
etr: if there is no Faradaic current across the electrolyte-metal electrode

terface, it means that there is no electron transfer (no REDOX reactions
xist) and the electrical charges are only those, present in the electrolyte.
most cases these are not electrons ,but rather ions of various kinds. In
y case n.1 (Monocrystalline Silicon), these charges are
ectrons(conduction band) and missing electrons/holes (valence band).
some other electrically active energy levels are present (like a shallow or
eep level) , then there is also a contribution from these localised charges
+ or B- for example). There is no double layer present at the interface in
is case. In my case n.2 (aqueous chloride solutions), apart from Na+
nd Cl- ions for example, there are also polar water molecules and it is
ese that form the “Helmholtz first layer” (physisorption). Their strong
pole moment get aligned so that at the positively charged electrode, it is
ghtly negatively charged oxygen that is “stuck” to the surface of the
etal electrode and the whole molecule becomes imobile. As a
onsequence the dielectric constant of these water molecules falls from
psr~80 to a value characteristic of ice ~3.0 Also in this case there is no
ouble layer. The spatial variations of the total, local electrical charge
ensity is given by one of the Maxwell equations (Poison equation).
The differential capacitance dQ/dV , not the integral capacitance Q/V ,

usually used in Electrochemical studies of interfaces. This is similar to
sing instantaneous rather than average velocity describing the
echanical motion. Why does your response mention only the integral
apacitance?
etr: There is only one response. To an applied time varying voltage

w)=Vo*cos(wt) - input, the system responds through the measured
ectrical current I(w)=Io(w)*cos(wt+phi(w)) – output. Your
Q=I(w)*dt=C(w)*dV(w). No mystery here, just that the response, the
apacitance C(w) is frequency/time dependent. At time->infinity, this
uantity becomes frequency/time independent and you get your “integral”
apacitance. I prefer to call it static capacitance.
I have doubts (likely, because of the lack of understanding and

ducation in this field) that Z2(w) can be safely named in general "the
urely capacitive response". This title is indeed adequate for RCL circuits ,
nd actually originates from this local and linear limit. But is it true in
eneral? (sic: I do not mean the trivial issue of filtering out the induction )
etr: it was only in the example given. The impedance of purely capacitive
stem is Z(w)=0+1/(i*wC). It could be of course also purely inductive
w)= 0+i*wL, or it could be a mixture of both. I am sorry if I did not
xpress this more clearly. Purely capacitive response is not a title
dequate only for RCL circuits, it is fully legitimate assignment for a purely
apacitive response of a real system, like for example a piece of sapphire
thin the frequency range DC to some GHz .
(On your response 4.2 regarding the dynamic measurement of a

apacitance). What exactly is measured dynamically? Is it some quantity
at exists at rest?
etr: By dynamic I mean that the measurement is done as a function of

me/frequency. When the measured quantity dQ/dV is time/frequency
dependent, then C becomes time/frequency independent constant and it
erefore exists at rest also.
Describing the model, you mention deep electron states in Si. Can you
ill consider your model "classical"? (I believe that this only sounds
ontradictory, and you certainly have a good answer).
etr: You are right, it does sound contradictory. My point here has been
at in general, the energies of the various electrically charged particles
hould be known if we want to describe the electrical response correctly,
ecause the electro-magnetic response process takes place in energy-
pace-time. And in general, you can define the relevant energies only
rough quantum mechanical calculation. However, in electrolytes, like
queous chloride solutions, I can approximate these energies (for
xample energy of Na+ ion respective to the vacuum level) through some
ermodynamical arguments/measurements.
will send this also to your e-mail, but Maxim asked us to continue here.
ith best regards
etr

EIS Laboratory
ear Maxim,
ou write:
yes, circuits reproducing effective negative capacitance (or, more

enerally, negative impedance) are based on opamps, that contain
ansistors.
the context of electronic devices and their negative capacitances -

orrect, we are talking about what we can call "passive" devices, although
do not see a fundamental difference between transistors and simpler
evices - p-n junctions, Schottky diodes, etc. - when these "simpler"
evices display a complex dynamics, that leads to a delayed current
sponse to applied voltage excitations (a fundamental requirement for
he onset of negative capacitance, as first explained by Andrew Jonscher).
he "fundamental" difference is that in active devices there are internal

nergy sources, at least as I understand this type of classification. But I
uess one could argue that putting a field across a sample and forcing the
ample out of equilibrium into a steady state could be considered as
nergy source, though external.
ndrew Jonsher in the article that you I believe, were a co-author (see my
omment here a couple of years back), did not explain, but suggested that
the response current for some reason starts to increase within some
me interval, this could lead to negative capacitance. In my example of a
eep level in Si, this is what happens for some values of capture/emission
tes between a deep level and the conduction and valence bands. The
her example is a perfect Schottky-Schottky samle under moderate dc
oltage bias, the third are simple aqueous chloride solutions and the
urth is ultra pure Silicon Schottky-Ohmic system, again under moderate
c bias voltage, although here it is not the negative capacitance, but rather
netic inductance effect (ballistic transport).
Referring to an earlier question/discussion - I believe that, in general, a

henomenon of negative capacitance has nothing to do with whether
here are classical or quantum effects involved in the dynamics of the
ectrical system. Fundamental microscopic mechanisms can be quite
fferent, either quantum or classical (or combination of thereof), and the
main requirement is the delay between current and voltage transient
gnals.
es, under certain set of bulk electrical material parameters and for given
oundary conditions , defining the system under observation, the
umerical solution of Maxwelll equations (Classical Electrodynamics !)
ves the negative capacitance effect in agreement with experiment. One
as to be careful though to first exclude all other possible causes.
ith best regards
etr

Lechem Lab
ear Petr, thank you! There is a lot to digest Unfortunately, I did not receive
e email to which I can privately respond with silly and technical
uestions, and have and ongoing dialogue.
or now, one general question (I put it here, but it is also addressed to

axim, and other experts in this field).
he capacitance of electrical double layer (EDL) is a conventionally

efined equilibrium characteristic. Majority of its theoretical studies are
cused on equilibrium charge distributions at the interface. NC (in
quilibrium) is prohibited by thermodynamics*. However , NC can legally
ppear in the models implying restricted equilibrium- uniform controllable
urface charge density distribution ( overwhelming majority of EDL
eories belong to this class) . Prediction of NC in such models indicates
harging instabilities/phase transitions under the physically accessible
onditions (when the potential V or the total charged Q is controlled).
hese transitions lead to discontinuous behavior of C and other critical
eculiarities. These properties are well illustrated by electroelastic toy
odels. For our discussion it is only important that their impedance has a
ro- frequency limit if studied far from a critical point, and displays
omplex nonlinear behavior in critical region.
ccording to the response there is no EDL present in cases of your

ccording to the response, there is no EDL present in cases of your
terest. So (please correct if I am wrong), C is a purely dynamic property
lated to the phase shift between AC voltage and current. In other words,
I may, it does not have static equilibrium limit.
uestion: is there any prohibition/restriction on the sign of "your" C ? If

s, please formulate it. If not, and NC is not forbidden, why is it an issue
all? Why is NC surprising and deserves special attention?
believe that it does, and the question is not rhetorical. Still, if the sign of
is not related to stability, why +2 is less peculiar than - 2?)
----------------------------
ow the correction to my question that you have addressed before.
he following part was very poorly crafted:
. In studies of electrochemical double layers ... the charge Q is

ssentially the electron charge localized at atomic scales near the
urface of a (metallic) electrode. "
ere I meant the following. In conventional picture of EDL, there is a

harge Q" on the electrode and a "counter-charge" -Q distributed in
ectrolyte. I was trying to say that in this picture Q, the "electron excess
harge" is localized at atomic distances near the surface of electrode (in
ell-defined region), and asked you how the "charge of electrode" is
efined and distributed in your systems. Apparently, you have answered by
lling that there is no EDL in your case.
Because C is a second derivative of a corresponding thermodynamic

otential

EIS Laboratory
ear Misha,
will send a copy to your e-mail address.
ow to your question:
There is no restriction as to the space-time evolution of the total local

ectrical charge density in the neighborhood of the interface as a
sponse to Heaviside voltage step input, apart from the interface itself
locking ,Schottky contacts).
NC is not a static effect, it is a dynamic effect (time dependent currents

owing through the sample) of bulk electrical charge density responding
step voltage input under certain conditions of material parameters and
oundaries.
My view at present is that NC has nothing to do with some kind of

rious surface processes, but it is a simple result of the solution to
axwell equations, given the conditions I have just mentioned above.
It is misleading to talk about "capacitance of the double layer", the only

ing one talk about really is the total and local electrical charge density
hanging in time and space. Due to finite temperature fluctuations, this
charge is not discontinuous across the interface.
Negative Capacitance effect is a "problem" since its cause (see the

aper by A.Jonscher and Maxim and others that I have attached to my
omment for 2 years back) implies that the response is not Kramers-
onig compatible.
ith best regards

etr

Lechem Lab
orry, Petr. I was re-editing my question, while you responded to the

iginal version. Please, read my update (it comes from the heart :) ), while
am reading your original response. Thanks!
-------------
0 minutes later
fter reading your response I see that it already deals with some of my
pdates. Kramers-Kronig reference immediately caught my eye. So, here
C contradicts the law of Entropy. Makes perfect sense - I have to read
e references. First thing to check is if C in your approach a well-defined
sponse function. Thanks again.
S:
V: "Due to finite temperature fluctuations, this el.charge is not

scontinuous across the interface."
agree. It is not discontinuous already due to quantum nature of electrons

he charge distributions overlap. And you are right that charge
uctuations in electrolyte induce "image" currents in electrode. Still, I
elieve that in time-averaged picture (in static regime) the EDL is a nice
orking model. Regretfully, there is no molecular dynamic studies that
qually treat metal electrons and species of electrolyte, to account for
uctuations of charge distribution on both sides of interface.

Lechem Lab
ear Maxim
your IEEE article, is this a typo (p.2): "On the other hand, it should not be
rge enough that the transient current is properly resolved." ? Otherwise,
hat does it mean?

EIS Laboratory
ear Misha,
st a couple more comments so that we do not misunderstand each

her :
First thing to check is if C in your approach a well-defined response

unction. Thanks again.
ell, it is as well defined as the linear response theory defines it (ratio of

utput/input). Complex capacitance C(w) is obtained as a trivial transform
the measured complex impedance Z(w) (well defined response
nction):
w)=Y(w)/i*w [Farad] and Y(w)=1/Z(w) [Siemens].
Just to make sure, if we take the external voltage source into account,
e system (a piece of Silicon for example) can be considered
ermodynamically as an open system, allowing the current to increase
or a while).
The solutions for the space-time evolution of the total, local electrical
harge density I get by solving Maxwell equations are continuous up to
harge density I get by solving Maxwell equations are continuous up to
e interface (from the sample side). But I assume a perfect metal
ectrodes surface charge that creates a constant voltage drop across the
ample. The experiment is a constant voltage experiment. There are no
mage charge or forces (those I actually consider as a fallacy in the
scussions concerning the charge distributions across the interfaces).
y view is that the fluctuations "smooth out" the distributions. Also
mportant is the fact that we deal with macroscopic Maxwell equations (in
andau sense - Electrodynamics of Continuous Media).
ith best regards
etr

Lechem Lab
hanks, Petr!
nfortunately it happened to me too: I wrote a response, and then lost it.
general, I wanted to say, that reading your answers helped to

nderstand much better your field (also represented here by Maxim), and
ome questions just disappeared. The most important was realization
at you are not focused on the interfacial phenomena/properties
ncluding double layers), but consider macroscopic "bulk" phenomena.
he borders are accounted for by "classical" boundary conditions, and
stead of surface charge distributions you calculate transient currents
enerated by voltage step, or the harmonic response.
nother difference is that all this is typically done in presence of

onductive current (while we consider "ideally polarized electrode").
still need your guidance:
V: 5. Negative Capacitance effect is a "problem" since its cause (see the

aper by A.Jonscher and Maxim and others that I have attached to my
omment for 2 years back) implies that the response is not Kramers-
onig compatible.
he paper is very interesting and insightful, but I did not find anything
bout KK - NC contradiction . Please let me know where in the paper it
as is implied.
hank you.
isha

EIS Laboratory
ear Misha,
am happy that at least some of my comments/observations/views have

elper to clarify some of your questions.
Boundary conditions. You are right, they are essential, but need not be
alculated quantum mechanically. I use electrochemical potential of the
etal electrode and of the bulk sample to define them. Alternatively one
an use the current boundary conditions. The microscopic description
omes later in the analysis, when interpreting Helmholtz layer
apacitance, Faraday electron transfer current etc.
KK contradiction is not in Andrew Jonscher paper as far as I know. It is

consequence of response current increasing in time. In linear esponse
eory this current should be a non-increasing function of frequency. You
an see this when you consider the real and imaginary parts of the
easured complex capacitance. The real part of the capacitance at a
f (di l t i f ti ) i i t l th
ven frequency (dielectric response function) is an integral over the
maginary part from infinite frequency to that given frequency and
erefore it must be a non-decreasing function when you go from infinity
zero frequency. NC does not follow this.
ith best regards
etr
Ioannis Samaras 2nd Feb, 2019

ear Petr, and Michael,
you address a pure non-faradaic process[1] taking place on a (one side

at) WE[2] and two (the same) REs, but in a side to side topology (with
spect to the WE), then
one RE1 help to record a Zc1, we have a common, normal, Cap.1 (C1>0)
ase;
owever, the other side (RE2) based Z, will help to record a -Zc1 (Zc2=-Zc1)
lue, e.g. a nominally "abnormal" Cap.2 (C2=-C1<0) value.
ctually, C2 (-C1<0) has nothing,
xceedingly, abnormal,
least in this, thought experiment, example.
http://ilmuwantekkim.lecture.ub.ac.id/2016/11/difference-of-faradaic-and-nonfaradaic-
ocesses/
Say, found, initially, at zero DC-potential (steady state) value, so that a Z value has only a non-
adaic current based source, e.g. a more simple (and clear) measurement.
Recommendation
ear Ioannis,
ust in time you flow in a new stream into NC discussion. In

ectrocapillary studies of melted Cu / oxide melt interface we considered
ome Red-Ox reactions at the interface in that case.
dsorption/desorption processes result in potential (voltage) regions with
C.
eturning to initial point of our discussion, how long do you evaluate the
ay we get the NC devices?
ncerely,
Kobelev
Recommendations
Ioannis Samaras 2nd Feb, 2019
ear Alexandr Vladimirovich Kobelev,
our electro-capillary studies could be referred as a good, non-thought

xperiment, (among others) example(s).
so, a certain state of your (and other similar) interface(s) might be used
s a quite stable impedance (Z-)memory, as a memristive device. The
eneral (devices' family) brand name is, already here, between us, the
emristor[1,2].
further discussion, about the give out on "how long, or how strong will
e supported, do you evaluate... etc." is, rather, a marketing issue[3], also.
Memristive Devices for Computing: Mechanisms, Applications and Challenges

p://www.hpl.hp.com/techreports/2013/HPL-2013-48.pdf
Memristors - How it works! see frames after 20m https://www.youtube.com/watch?

sLJyijsA2A
https://www.memristor.org/electronics/flash-storage/284/ocz-1-tb-terabyte-ssd-solid-state-disk-
ve-colossus
Recommendations
ear Ioannis,
hank you very much for this new for me 'memristor' item. I'd like to study
e subject, grateful to your advise.
eksandr
Recommendation
Lechem Lab
V: In linear response theory this current should be a non-increasing

nction of frequency.
ear Peter,
ay be this is why I was always interested in situations where the non-

earity is important. For example, mode softening and strong low-
equency dispersion in Elastic Capacitor in the vicinity of NC range is
ssentially non-linear effect. Are you dealing with linear regime in your
nalysis? If you do, then how do you explain the breach of K-K?
Recommendation
EIS Laboratory
ear Ioannis and Misha,
do not follow the usual approach to electro-chemistry of the electrolyte-

etal electrode interfaces. I feel that the "normal" 3 electrode
onfiguration for electrochemical impedance measurements are not only
n-necessary, but often can be source of errors. Why ? Because one
troduces extra "unknown" interfaces into the problem and for a given
olution, one does not really know, where the "zero" potential exactly is.
hat is also reason why I do not really understand Ioannis's argument

bout Negative Capacitance effect. Could you clarify for me what is the
eometry of the electrodes and what are the quantities Zc1 and Zc ?. If
ey are the measured complex electrical impedances between Working
ectrode and Reference Electrode 1 (let us say to the left from WE) and
etween WE and RE 2 (to the right from WE), then you have two , almost
nrelated impedance systems.
my approach I use the two electrode configuration with a very well and
ecisely defined geometry - a small glass container (diameter of some
2cm and the length ~0.5 cm) that is Pt sealed on both sides. Two outlets
nable the solution to be put in and taken out and the cell properly cleaned
etween various measurement.. In this type of cell, the two interfaces are
ssumed to be identical, namely Platinum-solution interface. Under dc
oltage Bias there comes an assymetry, but this is taken care of by
axwell equations automatically. What we still do not have at present is
xplicit incorporation of the possible REDOX reactions into the system of
quations. However, the impedance data suggest that down to low
equencies where the interface is really felt, the mozt systems behave as
e interfaces would be prefectly blocking - no electron charge transfer
cross the interfaces.
he Negative Capacitance effect does not occur in these systems as a

le.
ith best regards
etr
Petr Viscor
EIS Laboratory 2nd Feb, 2019
ear Misha,
Almost all the systems where one measures electrical impedance are
on-linear. However, one can measure the response (the complex
ectrical impedance Z(w)) within linear response regime by applying a
ufficiently small perturbation (ideally zero, but then there is no
easurable response). The compromise is e.V~kT.
Is my analysis linear ? No, I do not linearise the set of Maxwell

quations that I am solving numerically. In other words, the whole problem
posed as as a set of non-linear differential equations of parabolic type
th well defined boundary conditions.
ith best regards
etr

Lechem Lab
ear Petr, thanks for your timely response. As your system is non-linear*,
ere is no K-K (or any other restrictions) on the sign of the "C-component"
impedance. If this is correct, them "NC" is not prohibited. And it is even
xperimentally observed. So, could you please elucidate the goal of your
udy. Do you want to build a transparent (and consistently treated)
xample of how NC happens, or there is still something general to be
oven or disproved? Or, can we say that, being permissible, the
ppearance of NC is still surprising? If so, then why?
understood you notion, that the perturbation in your study is small [but
ill large enough for response to be observable :)]. I am just saying that
s you well aware) the nolinear systems are full of surprises, and they
ay "over-react" in response to small signals. Apparently, you feel safe
om such disastrous events (or have a good insurance policy :) ), while
e, dealing with EDLs that you "despise" (just kidding), feel always at the
dge of catastrophe (both in conventional and mathematical senses).
ow a technical question from reading your earlier response:
V: But I assume a perfect metal electrodes surface charge that creates a

onstant voltage drop across the sample. The experiment is a constant
oltage experiment.
etr, when you say "constant voltage drop", what does it mean ?
orry, I am sure that this is purely semantic misunderstanding on my part,

nd your answer will help me to understand your setting.
y p y g
V: There are no image charge or forces (those I actually consider as a

llacy in the discussions concerning the charge distributions across the
terfaces).
he term "Image charges" was used in my comment as a metaphor for the

hielding of the field of external charges by metal electrons. It is not a
llacy and it is quite accurate at distances > 2-3 AA from the surface.
owever, I agree that one should be cautious in using this terminology and
pproach. The conundrum lies in the danger of double- counting, because

equilibrium the surface charge on electrode is actually built of the same
mages". Hence, it would be wrong to consider images as an addition to
e "surface charge density".
hank you.
isha
n our study of EDLs the non-linearity is crucial. For example, linear

eatment of electric response (say to the field of charged ( Q) electrode)
ways keeps centroids of induced charge distributions frozen in space
nd independent of Q. In our area of study this kills the NC appearance
ven in theories based on Sigma - control (while NC in this artificially
stricted equilibrium is not generally forbidden). It's worth noting,
owever, that the electric field in EDLs at metal/electrolyte interface can
cally reach enormous values (up to 10 V/nm !) , and the response is
ssentially non-linear. I am not sure that this is an issue in your study
here (as you've mentioned) the role of EDLs is not important and the
terfaces are accounted for via the classical boundary conditions .

Lechem Lab
ear Petr, I just reiterated some of my previous questions (see the

odified text above.
est

EIS Laboratory
ear Misha,
".. So, could you please elucidate the goal of your study. .."
y goal is to put the analysis of the electromagnetic response in

ondensed phase within classical range of frequencies (dc to THz) on a
ew qualitative level ("first principles approach"), using Quantum
echanics, Thermodynamics and Classical Electrodynamics as the three
ssential ingrediens. Negative Capacitance phenomenon is just one of the
omewhat exotic results of this analysis, consistent with experimental
vidence.
"..Do you want to build a transparent (and consistently treated) example

f how NC happens, or there is still something general to be proven or
sproved?
he cause (causes) of NG needs a more extensive investigation which I

ave not done so far.
".. Petr, when you say "constant voltage drop", what does it mean ? .."
constant voltage experiment is when you apply a Heaviside step voltage

cross the sample at time zero and measure /calculate the time response
he current)
he current).
" The term "Image charges..."
he response of the system to external electrical field is to "shield"

mobile charge screening polarisation) it so that inside the system, the
eld becomes zero and current eventually stops. I do not know why
eoples call this "image" charges. When an electron in vacuum
pproaches a metal surface, The so called "image force" is completely
egligible (density of electrons inside is 10*27 per m*-3 !) and the
pparent decrease of the potential has nothing to do with this.
".. I am just saying that (as you well aware) the nonlinear systems are full
f surprises, and they may "over-react" in response to small signals..."
agree and for the time being, I would use this term "over-react" rather
en "delayed response" (A.Jonscher). Your description is more precise.
ith best regards
eter

Lechem Lab
hanks, Petr.
rst, I must tell that this setting is very inconvenient for more-or-less
tense discussion, and awfully time-consuming . Instead of working in
e same document, we have to create a new one every time we sneeze,
nd then copy-paste phrases from the previous... For some reason my
uggestion to work in GDocs was not supported.
y Response
Clarified. Thanks.
OK. I thought that your target is NC.
So, "constant voltage drop" = "voltage step". Done.
Images is one of the most beautiful concepts in electrostatics. I

ompletely misunderstood your objection. Btw, high electron density in a
etal is exactly the reason why its boundary is equipotential, which
akes images to work so simply and nicely.
I thought that "delayed response" is about non-locality, phase shift, etc.

ut, with your motivation, I see that this is a part of what happens in
itical region: reaction to a small perturbation is a long-lasting story
rocess). Would be interesting to know how the author defines this term.
guess, it will require some extra reading
l the best.

EIS Laboratory
ear Misha,
your e-mail address : moshep@brandeis.edu ?
will try to send my answer(s) also there
etr
EIS Laboratory
ear Misha,
your points :
I am aware of this way (image force approach) to calculate potentials

nd charge distributions in electrostatics, but I am referring to "..Image
rce lowering of the potential barrier at metal-semiconductor interface.."
is here I use the word "Fallacy" because there is no empirical evidence of
is effect. Peoples, when they do not know precisely how the interface
ok in their experiment, refer to the measured barrier height as being
fected by this force. The quantum mechanical calculations (charge
ensity functional method for example) reveal that is force is not affecting
nything that could be identified in the corresponding experiment (internal
hoto-effect) or as in my case, the Electrical Impedance Spectroscopy
xperiment.
It looks interesting, I can not comment because I do not know what

stem it refers to. A word of caution, oscillations are typically result of
umerical errors encountered in the numerical analysis of non-linear
sponse. But this is probably an experiment ?!
ith best regards
etr

Lechem Lab
hanks, Petr.
Well, then we were talking about different things. I meant very ordinary
ectron shielding (screening) of external charges at conductive surface.
peaking about self-consistent calculations of surface barrier, I am not

ure what r u referring to. The "image" energy is due to electron's
teraction with the surrounding "hole" (which lags behind e when it moves
ut) and it is implicitly present in any QM treatment consistently
ccounting for exchange-correlation.
he picture showed very accurate solution of a non-linear toy model. I

move it because it is not self-explanatory and provokes more questions
an gives answers.
he address is correct. Best.
S I am going to be a poor communicator for a while, with strongly non-

ear delays :(
PS
1 2
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Question Asked 10th Oct, 2016

hope this will help you on the way. Question 18 answers

Yurii V Geletii View

he only serious attempt to attack this "problem" to my knowledge has View

arendar - Question 25 answers

ear Naendar, View

oth by deﬁnition (*The capacitance, C is the ability of a body to store an

et, sometime it may be used (in the gauche *non-scientiﬁc* discourse) in

his way, negative capacitance as an entity simply doesn’t exist. Don’t be

Vasili Ivanovich Dimitrov 11th Nov, 2017

oth by deﬁnition (The capacitance, C is the ability of a body to store an

o, actually this is nothing but slang that is used by non-educated

et, sometime it may be used (in the gauche *non-scientiﬁc* discourse) in

his way, negative capacitance as an entity simply doesn’t exist. Don’t be

Maxim Ershov 11th Nov, 2017

ome references on negative capacitance:

A. K. Jonscher, "The physical origin of negative capacitance", J. Chem.

M. Ershov, H. C. Liu, L. Li, M. Buchanan, Z. R. Wasilewski, A. K. Jonscher,

Petr Viscor 11th Nov, 2017

ear Narendar and Vasilij Ivanovich,

is a purpose, again in my view, of RG forum to discuss this type of non-

our remark indirectly conﬁrms my point of view. The decrease of

o, certainly the very conception of “negative capacitance” is nothing but

nother situation occurs in computational math. when one solve

Petr Viscor 11th Nov, 2017

ear Vasilij Ivanivich,

t me agree and disagree with you :

I agree that the phenomenon of "negative capacitance" is of dynamical

It is a known EXPERIMENTAL fact that when measuring optical

What about if we re-name this "negative capacitance" a "part of

The problem with this dynamic phenomenon is that it is often not

ith best regards

hink that another source of confusion regarding negative capacitance is

more general case - semiconductors, dielectrics with losses, metals,

this case, capacitance is determined by various complex physical

his more general deﬁnition of capacitance coincides with C=dQ/dV

he problem is that this generalized concept of frequency-dependent

Petr Viscor 11th Nov, 2017

my analysis of the response, I usually relate it to the space-time

ith best regards

Maxim Ershov 11th Nov, 2017

s, agreed, this time-dependent "response function" or frequency-

complex admittance (complex frequency-dependent conductivity and

reuqnecy-dependent dielectric function

complex frequency-dependent capacitance (real part is the capacitance,

he space-time evolution of the charges and related processes

ases it's impossible to assign these changes to speciﬁc contact - these

Petr Viscor 11th Nov, 2017

.But in most cases it's impossible to assign these changes to speciﬁc

o , although various physical processes may be distributed in various

ith best regards

Maxim Ershov 12th Dec, 2017

s, "contact" is a term usually used in semiconductor device community

egarding my comment on diﬃculty to attribute a change of charge to a

electrostatics, dQ is the change of charge on one of the contacts, does

devices with non-zero conductivity, the charges (mobile charges -

Petr Viscor 12th Dec, 2017

et, sometime it may be used (in the gauche non-scientiﬁc discourse) in

et, sometime it may be used (in the gauche non-scientiﬁc discourse) in