.
Surfa<:.: S<:ience 247 (1991) 125-132
Nonh-Holland
Image potential states at surfaces
P.M. Echenique
Departamento de Física de '''fateriales. Facultad de Química.
and
M.E. Uranga
Departamento de Matemática Aplicada. Escuela Técnica Superior de Ingenieros
Received 21 may 1990; acc.:pted for publication 30 May 1990
Tbe main physics of image potential induced surface states is presented in a simple manner.
~ is compared with theoretical predictions. The role of image states in STM. as a two-dimensional
noise at disorded surfaces is discussed.
1. Introduction
That electrons can be localized at surfaces has
been recognized for a long time. The electrons in
such state cannot penetrate into the bulk when the
material (solid or liquid) shows a negative electron
affinity and do not have enough energy to escape
into the vaccum because'its own image potential.
i.e.. the potential created by the polarization charge
it induces at the surface. In fact the Coulombic
tail of the image potential of l/z aIlows an in-
finite Rydberg-type series to exist.
Hydrogenic states of this kind were studied in
liquid helium [1]. in the case of a surface polaron
- [2]. and in metals were such states can arise if a
gap in the direction normal to the surface contains
the vacuum level.
Johnson and Smith [3] pointed out tha't these
states could be observed by angle-resolved inverse
photoemission. Inverse photoernission (or brems-
strahlung spectroscopy) [4,5] is well suited for
probing bound stat~s directly by measuring the
* 1nvited lecture presented by P.M. Echenique.
0039-6028/91/$03.501) 1991 - Els.:vier Science Publishers B.V. (North-Holland)
125
*
Universidad del País Vasco. Apdo /072. 20080 San Sebastián. Spain
Industriales. Universidad del País Vasco. Bilbao. Spain
Recent experimental data on .Iifetime
electron gas ando as a source of a 1//
energy and momentum of an incident electron and
the energy of the emitted photon. In the last years
two photon experiments have provided good reso-
lution data bn binding energies and effective
masses [6]. and even lifetime data [7.9] has been
extracted. Energy loss experiments have produced
[10] some data on the binding energy of image
states on simple surfaces.
2. Phase shift model
A simple way of understanding the physics
involved in image states is provided by the phase
shift model [11,\2]. This model has been widely
employed to give a transparent picture of surface
states wbich can be used either for precise numeri-
cal calculations. or for simple analytic approxima-
tions. In this picture the surface state is considered
as a wave trapped between the bulk crystal and
. the surface barrier. This assumes a region of con-
stant potential between the crystal and the surface
barrier but since tbis need only be infinitesimally
wide. this places no restriction on the arguments
we are about to make.
:1
¡
¡
126 P.M. Echenique. M.E. Uranga / Image pOlenlialslales al surfaces

Thc
Summing the repeated scattering, taking into spending time on the crystal or the barrier side
sta tic ti
account all paths via the scattering formalism of [11]:
magnitu
Pendry and Gurman [13] the condition for a dlf>o
-o:: liquid h
surface state becomes dE .. s.de 1'1'12dz,
1barner close to
thus the
-ddEIf>co::
det{l- ReRo} =0, (1)
¡cryslal side
1
'1' 1
2 dz
' (4) ten ths (
away ( -
where I is the identity matrix and Re and R o are '1' being the wavefunction describing the elec- an elect
the crystal and barrier reflection matrices. tronic state. It is worthwhile to stress the point surface
A simple. approximation containing the essen- that variation of either If>cor If>ois an important and Eb
tial physics consists in reducing the problem to a element in producing a surface state: the greater = -0.8.
one-dimensional one; then the sum of the re- the variation the greater ihe chance of sweeping is reasol
peated scattering gives for the total amplitude of through the 27Tcondition. Thus Echenique and The (
the wavefunction at the surface Pendry referrred to a surface state induced prim- the crys
arily by a rapid variation of If>c as a crystal penmen
1 induced sta te, and that induced by a rapid varia- so-calleó
(2)
1 - rore ~i(4)B+4>c)' tion of If>oas a barrier induced state. We stress g?'-"':'~p.
the point that the two sorts of states are described tht gap,
where rco; If>coare the modulus and the phase of by condition (3). v~ fn
the crystal and the surface barrier reflectivity re- ga'fF.'íf t
spectively. The conditions for a surface state are gap, as
them 3. Binding energy metals,
eV/n2;
(3) A useful expression for If>Bis the WKB solu- proximat
rero=l, If>o + If>c= 27Tn.
- 21/z,
tion [14] for the classical image potential situation

221 metals q\
Because of flux conservation re and ro must be -0.85 e'
(5)
equal to unity. This means that the energy (E) lf>o(E)= ( V-2E ~1 ) 7T, for such
and momentum parallel to the surface (kp) of the where E is the energy measured from the vacuum more tigt
waves must be such that there are no propagating faces. Th
level, as E approaches the vacuum leve!, the phase
states within the crystal and no possibility of flux
varies very rapidly with energy. Many
escaping from the crystal into vacuum, i.e., a gap cated mI
In a real crystal, when image states exist, one
in the projected band structure and energy below the barri,
the vacuum leve!. has usually a band gap several electron volts wide
while the Rydberg series lies within an eV below results C0
This still leaves condition (3) for the phases to
be satisfied and this will only happen for certain
the vacuum level (21 = ~ in this case) therefore discussed
because of the rapid variation of the barrier phase o ¡th
values of energy and momentum. In particular the treII..~ th
reflectivity we can take 1>e as a constant and
crystal phase If>ewill vary at most by 7Tfor the
obtain for the binding energy ener:A
energy values we are concerned with here. Clearly surfa~1
if this would also hold for the barrier phase reflec- _ 2
tivity, condition (3) on the phases will have one or Eb = _ 2\ (6) applied ti
2(n+a)'; 11=1.2..... gaps asso
no solutions (this is actually the case for a step
where not paraIl
model of the surface barrier). Ir If>o,however, We sh(
varies rapidly with energy, as is the case for the 1 Es- 1 review 01
image potential, there is a good chance that many 2\ = "4 Es + 1'
(7)
solutions can be found. importan,
model re;
The variation of the phase with energy is di- (8)
a = i (1- ~e). systematil
rectly related to the probability of the electron

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.,

I
'-- - - -

P.M. Echenique, M.E. Vranga / Image potential states at surfaces
side The coupling constant Z\ and therefore the
static dielectric constant Es fixes the order of
magnitude of the binding energy. In the case of
liquid helium the static dielectric constant is very
close to unity (1.0572 for 4He and 1.0428 for 3He),
thus the binding energy is of the order of a few
(4) tenths of meV (- 3.73/n2 meV); the state is far
away (- 100 Á) from the surface. For the case of
elec- an electron attracted by its image potential to the
Joint surface of an ionic crystal, such as LiF Es= 8.65
rtan t and Eb:::: -0.5/n2 eVo For metals Es= - 00; Eb
eater = -0.85/n2 eVoIn the last two cases the electro n
:ping is reasonably close to the surface - 2.3Á.
and The details of the binding are fixed by (])c,i.e.,
>nm- the crystal scattering. In metals and in most ex-
)'stal perimental cases the image states appear in the
ana- so-called Shockley inverted gap case, where the
.tress gap is p-like at the bottom and s-like at the top of
ribe~ the gap, then a is greater than zero since (])c
e variés from O at the bottom to 17at the top of the
gap. Ir the vacuum level occurs at the top of the
gap, as it occurs in the [111] faces of some fcc
metal s, then (])c::::17, a = O and Eb = -0.85
eV/n2; while if the vacuum level occurs ap-
solu- proximately at the rniddle of the gap, such a
?:l/Z, situation arises in the [100] faces of the same fcc
metals quoted above, (])c= 117,a = 0.25 and Eb =
(5) -0.85 eV/(n + 0.25)2. Therefore one expects that
for such fcc "metals the image states would be
:uum more tigthly bound in the [111] than in the [100]
Jhase faces. This has been found experimentally [6,7,15).
Many more calculations using more sophisti-
.one cated models both for the crystal scattering and
wide the barrier one have been presented [16,30). Their
>elow results corrobora te the basics of the physical model
-efore discussed above.
:>hase Srnith [31) has presented an elegant study of the
_ ar'-..- trends that should be expected for the binding
~ energies and effective masses for a variety of
~ surface states on different surfaces. He has also
(6) applied the phase shift formalism to the case of
gaps associated with a reciprocal lattice vector g
not parallel to the surface normal.
We should hke to emphasise as stressed in the
(7) review of Echenique and Pendry [32) that the
importance of the one-dimensional phase shift
model relies on the correct description of the
(8) systematics and trends of the binding energies of
- ---
m
both crystal induced and image potential induced
surface states. For accurate quantitative calcula-
tions it is well established [31] that surface-state
energies (and the work-function) are correctly re-
produced only in calculations which have been
performed self-consistently. The scattering for-
malism of Pendry and co-workers [13), or equiv-
alent ones, can still be used for accurate calcula-
tions via eq. (1). We insist, however, that the
importance of the one-dimensional phase-shift
model is to provide a simple explanation of sys-
tematic trends. Even within this simple model
some further assumptions have to be made to
justify the use of a two-band nearly-free-electron
model, outside the gap region (Au(111» [33), or
for cases in which the states at the gap are pre-
dorninantly d-like. Perhaps it is not surprising that
the biggests discrepancies reported between the
simple phase shift model (with a nearly free elec-
tron (])c) and the experimental values have been,
in the n = 1 state of Au [27,31) where the state is
nearly 2 eV above the top of the gap; and in
Ni(lll) [34-36] where the states at the bottom of
the gap are predominantly d-like. As pointed out
by Steinmann [15] even if a better calculation of
(])c could resol ve the disagreement about the n =1
state, it is questionable whether it could account
for the binding energy of the n = 2 state, which is
higher than the hydrogenic value. A careful analy-
sis of the positioos of the image plane rnight have
some bearing on these cases since one would ex-
pect that the d-baod character will tend to dis-
place the ceotroid of the induced charge density
towards the material compared with the results of
the jellium model. A similar conclusion has been
reached by Pitarke et al. [37) io their analysis of
the influence of the shape and image potential 00
the oscillations of current versus voltage in STM.
4. Effective mass
lo the preceding section we have coocerned
mainly with surface slates at the bottom of the
surface band, and \Ve have nol takeo into account
aoy possible variation (other Ihan the implicit tk;
free-electron-like one) with the direction parallel
to the surface. Within the one-cleclron picture of a
A
.
I
128 P.M. Echenique. M.E. Uran/{a / Ima/{e potential.<tates at surfaces

solid the dispersion of Eh(kp) can only be due to effective mass through the shift in potential energy these tI
a scattering with the ion cores of the surface, i.e., 8V( z). allows
variation of the crystal reflectivity with k p or a momen
8V(z)k;
variation of the dynamic image potential with the V(z. kp) = V(z, O) + '). (9) leading
electron parallel velocity. such el'
A rough estimate of the effective mass correc- for a rH
tion (m * = 1 + 8m) can then be obtained by using of Ih.: (
4.1. Crysta/ effects the undispersed surface plasmon to represent the value o
surface response and taking the value of 8 V( z) at for Ihe
Echenique and Pendry suggested that for small the position of maximum probability density possiblt
kp the effective mass should be very close to 8V( zmax)' This gives, for a hydrogenic wavefunc- centre e
unity. The qualitative reason is that even for the tion to represent the first image state at 2.5%
crystal
most tightly bound Rydberg states the wavefunc- correction for rs = 2.67 (Cu) and 3.5% correction
rapidly
tion lies mainly in the vacuum, and the electron for r, = 3 [40,41]. certain
moves in a regíon with no potential variation The use of a more adequate surface response broader
parallel to the surface. In variance with this idea function including particle-hole excitation does governe
Garcia. et al. [38] suggested that image-potential not change the above conclusions [22,42]. Analo-
absorpt
surface states are strongly affected by surface cor- gous result is obtained when explicit inclusion of
rugations. This implies a relation between E h and the wavefunction penetration into the crystal is
8E a:
effective mass m* which does not agree with the taken into account [22].
accurate two-photon photoemission measurements ~J
of Giesen et al. [7,34] showing that the binding Therefo
energy is independent of m* within error bars of 5. Lifetimes pace WI
- 0.03 eVoMoreover the [100] surfaces orientation n. AII n
exhibits a more pronounced surface corrugation So far we have concentrated on the binding are in ¡:
but as mentioned above the binding energy of energy and effective mass of the sta te. and we member
image states in such surface is less than in the have assumed that the modulus of the crystal find ag
[111]. reflectivity re is unity. In fact flux can escape wavefur
A multiple scattering calculation for the energy from the state. The electron in such a state is not crystal ,
infinitely long-lived but can in principIe, make a fected \
dispersion of the first image state ~inding energy
in the [100] silver surface performed by Pendry et Iransition to other states, i.e.. to an empty crystal r
al. [39] gíves an effective electron mass equal to current-carrying state of the crystal. For finite l/S. A t:
unity. When effective masses are defined outside momentum parallel to the surface additional in-
the region of small kp' significant deviations from elastic channels are present !eading to an extra 8E a:-
unity appear: Giesen et al. have explained [7] broadening. In principie one could think that in
satisfactorily the experimentally observed effective metals electron-electron interaction w0uld result
masses using a one-dimensional phase-shift model in decay processes that broaden surface states to .-.....
with explicit inclusion of the shrinking width of resonances. This interaction may be so se\"ere dS to
the gap and the behaviour approaching band destroy all but the lowest member of Ihe Rydherg
edges. A comparison between the results of the senes. r~.
by b:fie
simple phase shift model and the experimental As the energy normal to the surface. ap- separale
ones has recently presented by Steinmann [15]. proaches the vacuum leve!. Ihe stales get closer in the ~ta:,
energy6.EJ. a: l/n} but at the same time the centre the ener
of gravity of the resonant sta te charge distrihution Ihe initi
4.2. Dynamica/ image potentia/ effects moves further away from the surface, having less the em~
probability of coupling to surface excilations. When ti
From the definition of local effective potential hence the energy broadening of the levels becomes lO Ihe ':
one could for operational purposes define a local smaller. Echenique and Pendry [11] proved th:1I wiJth .!

...
...

I
 --- --

P.M. Echenique, M.E. (jranga (/muge PQlenlial Slales al surfa('es

129

:rgy these two effects compensa te in such a way that state decays into a state localized in the surface
allows resonant levels to be resolved. For the having the same z-dependent wavefunction but
moment we shall not discuss in detail the processes with a different k-parallel component (intraband
(9) leading to an energy broadening, and represent transition). The results of two calculations of the
such effects by an absorptive potential 1:;, which energy broadening r(1); r(2) for the two processes
rec- for a bulk free electron of the same energy can be described above are given in ref. [43.44] and in the
,;Ing of the order of 0.5-1 eV (depending on the actual review of Echenique and Pendry [32].
the value of the energy). ClearIy if these values held Typical values of model calculations of Pl)
.) at for the image states, no Rydberg series will be and r(2), with no wavefunction penetration are of
1sity possible. What saves the day is the location of the the order of 5 meV for the case of a silver surface
unc- [43]. When penetration of the wavefunction is
centre of gravity of the surface state outside the
2.5% taken into account the halfwidth increases, while
crystal because' these inelastic' processes decay
;tion the one associated to the momentum parallel re-
rapidly in strength outside the surface. Beyond a
certain range. zC' they can be neglected, and the mains of the same order. For a 30% penetration of
onse broadening, SE.J. of an image state wiII be the wavefunction de Andres et al. [44] quote 33
does meV for !r(1) in Ag, which is about a factor 10
governed by its overIap with this region of finite
1alo- absorption: greater than the value obtained with no wavefunc-
n of tion penetration. We should like to emphasize that
al iSI ZC 2 a4lB 1 in spit(: of their complexity the calculations of the
j
SE .J.'a:. -00 I'1'I dz a:. aE a:.3"
n
(10)
lifetime of image states use very simplified models
~
~ for the surface response that might not be very
Therefore the broadening scales as 1/n3 and keeps adequate tó describe appropriately the response
pace with the leve! separation in the limit of large function of materials such as Cu or Ag. The
n. All resonances converging on a given threshold calculations [43,44] use simplified models for the
Iding are in principIe resolvable. If we can see the first surface response, based either on the specular
j we members of a series the rest should follow. We model of Ritchie and Marusak [45] for the surface
)'stal find again the same idea. the Rydberg state's response, together with the small w expansion fo
;cape wavefunctions are effectively decoupled from the the bulk RPA dielectric response function of Pers-
s not crystal wavefunctions and therefore would be af- son and Andersson [47] for the case of an electron
Ike a fected very little by scattering processes at the totally outside the crystal [43]. At the energies
mpty crystal region. This, of course, is exact only for high involved preliminary analysis [48] indicates that
finite n's. A typical value of SE.J. can be obtained: the use of the experimentally derived undispersed
11 in- response functlon may lead to energy widths.
-1: a4lclaE
I
extra greater by a factor of 2 ar more than the ones
8E.J. a:. a4lB/aE
at in obtained using the respon se functions quoted
result -1:¡ 50 meV above. Recent experimental data by Schoenlein et
¡es to (11 ) al. [8] and Nielsen et al. [49] on Ag(lOO) .have
32(gap width)n3 n3
as l, measured a lifetime of about 25::!: 10 fs [8] or
~ .g More detailed calculations have been presented 20::!:5 fs [49]. These correspond to a line width of
~.

by Echenique. Flores and co-workers [43,44]. They
. ap- separate two contributions. First they calcmate for
ser ID the state at the bottom of the surface state band
;en tre the energy broadening related to transitions from
)ution the initial image state to a final state defined by
g less the empty. current-carrying states of the metal.
ltions, When the Rydberg states have momentum parallel
::omes to the surface, an extra contribution to the energy
j that width arises from a process in which the initial
about 35::!:la meV which is more than twice the
calculated' value with no wave-penetration [43].
Nielsen et al. [49] and Steinmann [15] have sug-
gested that the discrepancy is presumably due to
an additional decay channel, e.g., surface imper-
fections. This is .an interesting suggestion that
should be explored. but also one should take into
account the abbve comments on the wavefunction
penetration and on the innuence of the different

~
,

I
I
130 P.M. Echenique. M.E. Uranga / /mage po/ential sta/es a/ surfaces

models of the response function. A calculation simplified model of Louis et al. [52], but because cient (e
along these lines is in progress [48]. the exponential dependence of the tunneling life- functiol
Very recently Schoenlein et al. [50] have re- time this should be a good value for any real another
ported the first time-resolved studies of higher situation.
phase i
order image potential states on Ag(lOO).
expericI
They measure the lifetime of the n = 2 image
state on Ag(100) to be - 180 fs, substantially 7. Two-dimensional electron gas
befort: .
high de
longer (- a factor of 7) than that of the n = 1
delay ir
state. This result is in agreement with the original Image states represent a very simple and funda- tor is c(
prediction of Echenique and Pendry [11] (see eqs. mental class of surface states which is useful in
surface
(14) and (15». The n3 scaling prediction is exact studying the two-dimensional (20) electron gas disordel
only for high n 's. More recent calculations by de [54]. To obtain a 20 Ferrni electro n gas a high of enco;
Andres et al. [51] using a many-body self-energy electron density is needed. In liquid helium the
whose p
formalism predict n3 lifetime scaling for states binding energy is weak (- meV) and an instability the elecl
n ~ 5. For lower order states, the model predicts a of the 20 electron gas develops when the density disorder
lifetime scaling less than n3, with is increased [55]. In metals the binding energy is of tum to
the order of 1 eV but a problem arises due to the
('Tn_2/'Tn= 1) =:::4. produce
processes that contribute to the energy width of w- res
The hydrogenic model of de Andres et al. as the image state. The interband transition (decay wOI1cers
stressed by Schoenlein et al. [50] overestimates into allowed bulk states) contribution to the en-
'Tn_1 since it neglects wavefunction penetration ergy width is high and comparable to the in- h~
m~~re
into the bulk. Thus one expects the ratio of life- traband (decay into image sÜltes having smaller
times 'Tn_2/'T"=1to be between four and eight, parallel momentum within the band) contribution. d4>B('
which is in good agreement with the experimental
measurements of Schoenlein et al. [50]. In the case
This means that electrons may not be able to ( dE
thermalize to the bottom of the 20 band because The con
of silver (and copper) (111) surfaces the n = 2 they decay into bulk states and the high density lifetimes
image state lies in the continuum and therefore needed to obtain a Ferrni electron gas would not tions th.
the surface state presents an elastic linewidth, be achieved. In insulators, such as diamond or For quit
originating from the lack of total reflectivity, Le., LiF, relatively strong binding appears (a large cut-off f
re < 1. This elastic half width for the n = 2 state of enough dielectric constant) and the escape outside measure
Cu and Ag has been estimated to be around 25 the band into buIk states is prevented by the insulatOl
meV [44]. electronic structure. Amau and Echenique [56]
have evaluated variationaIfy that the intraband
energy halfwidth is 150 meV for parallel momen- Aclrnowlt
6.STM tum of 0.15 (Á -1). They conclude that if one
The :
could populate the first image-state electron band
Louis et al. have presented an analysis of the Flores, J
up to parallel momentum of k p = 0.13 Á -1 then a . ~
conduction process through image surface states density of about 1013 cm - 2 could be a.ttained, Sl( an.
in scanning tunneling microscopy [52,53]. For low enough to think in terms of a20 Ferrni electron Rese3:il
electric fields the Auger inverse lifetime discussed gas [57]. ibert~'J.
above, becomes larger than the tunneling lifetime Guipuzk,
CAICYl
ando therefore, the tunneling process controls the
current while for large fields a saturation occurs, 8. Disordered surfaces
since the Auger process is not fast enough as to Referenc
allow new electrons to come from the tip into the Pendry [58] has suggested toat image states at
crystal, thus further increases of the field do not the surfaces of insulators may playa central role [1]W.T.~
lead to an increase in the tunneling current. The in the generation of 1/1 noise at the surfaces of M.("..
transition occurs at fields around 0.40 V/ Á in the these materials. The phase of the reflection coeffi- V.B.S

..

~
!,
¡.¡
~j

~
 .

P.M. Echenique, M.E. Uranga I lmage po/en/ia} sta/es a/ surfaces Dt

cause [2] J. Sak, Phys. Rey. B 6 (1972) 3981.

cient (eq. (4» is related to the amount of wave-
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! real 2527.
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y is of
to the
. disorder induced localized state to eventually re-
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[11] P.M. Echenique and J.B. Pendry, J. Phys. C 11 (1978)
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P.M. Echenique, PhD Thesis Cambridge Uniyersity, 1976.
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jd<PB(E)d<PB(E+W)
)_.!.
ution. 5199.
( )
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