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Electrical Generation of Surface Phonon Polaritons: S.de-Liberato@soton - Ac.uk
Electrical Generation of Surface Phonon Polaritons: S.de-Liberato@soton - Ac.uk
sub-diffraction photonic modes in the mid-infrared. They also support longitudinal phonons, which
couple efficiently with electrical currents through the Fröhlich interaction. As we have shown in
previous theoretical and experimental works, these two degrees of freedom can hybridize forming
longitudinal-transverse polaritons. Here we theoretically demonstrate that longitudinal-transverse
polaritons can be efficiently generated by electrical currents, leading to resonant narrowband pho-
tonic emission. This approach can therefore be utilised to electrically generate far-field mid-infrared
photons in the absence of dipole-active electronic transitions, potentially underpinning a novel gen-
eration of mid-infrared optoelectronic devices.
a) 1000 b) 1000
j=u 1.5
Wavenumber (cm−1 )
950 950 1
j=m
900
n=2 n = 20.5
j=l
850 850 0
0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1
In-plane Wavevector (×108 m−1 ) In-plane Wavevector (×108 m−1 )
FIG. 3: Density of states and modal dispersions for a 3C-SiC film of thickness 2nm characterised by Eq. 1,
sandwiched in a Si cladding (c = 11.71). In panel a), representing the prediction of a local theory, the black dashed
line shows the bulk LO phonon frequency ωL and the dot-dashed green line the local SPhP dispersion
ωqSP (Appendix A 1). In panel b), representing the prediction of a nonlocal theory, the black dashed lines shows the
L LTP
localised LO phonon frequencies ωq,n and the dot-dashed green lines the LTP frequencies ωq,j . In both panels blue
solid lines mark edge of the light-cone in the cladding.
Density of LTPs ×10−2 cm Density of Photons ×10−6 cm
0 0.2 0.4 0.6 0.8 1 1.2 1.4 1.6 1.8 2 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
a) 1,000
Wavenumber (cm−1 ) b)
950
900
950
900
950
900
950
900
FIG. 4: Comparison of LTP and photonic steady-state populations generated by thermal and electrical processes. In
the first column we plot the LTP density, while in the second column we plot the photonic density, obtained by
multiplying the LTP density by the photon fraction ξq,j from Eq. 6. The first row (a,b) shows data obtained
considering purely thermal emission, obtained setting both the lattice and the electronic temperatures to the same
equilibrium device temperature Tl = Te = 600K. The other three rows show instead data obtained considering
electronic temperature Te = 1000K and lattice temperatures equal to Tl = 0K (c,d), Tl = 300K (e,f), and Tl = 600K
(g,h). Other parameters as in Fig. 3. In all panels the blue-solid line indicates the light-cone edge in the cladding,
and the dot-dashed green lines indicate the real LTP frequencies. Note that the color in the figure has been
saturated to allow the thermal and the much larger electrical populations to be plotted on the same color scale.
7
a) a) 2
Lower Polariton
Tl = 0K
4 Td 1
0.5 Tl = 0K
2
Tl = 300K
Tl = 600K
0
0 500 1,000 1,500 2,000
0
0 500 1,000 1,500 2,000 Electronic Temperature (K)
b) b)
Lower Polariton
Tl = 300K 2
1.5
4 Td
1
0.5 Tl = 0K
2
Tl = 300K
Tl = 600K
0
1 2 3 4 5
0 Thickness (nm)
0 500 1,000 1,500 2,000
c)
FIG. 6: Figure of merit η (2) . In panel (a) we plot it as a
Lower Polariton Tl = 600K function of the electronic temperature Te , for an active
6 Middle Polariton region of thickness 2nm. In panel (b) we plot the same
Upper Polariton quantity as a function of the thickness for a constant
Figure of Merit η (1)
1. Local Response of Thin Polar Films where U, L are coefficients describing the contribution of
the SPhPs at either interface. After applying boundary
In this work we consider a trilayer waveguide, consist- conditions on the tangential component of the electric
~ q · r we recover the following dispersion relation
field E
ing of a polar film of thickness d sandwiched between
semi-infinite positive dielectric cladding layers, occupy- αc
( αc − 1)e−αd 1+ α c
U 0
ing the region −d < z < 0. The system is translationally αc
αc
= .
invariant in the xy plane. Modes of the system are char- αc + 1 (αc
αc − 1)e
−αd L 0
acterized by a 2D in-plane wavevector q, and out-of-plane (A5)
wavevectors given by This equation is satisfied when the determinant of the
matrix is zero, which leads to the transcendental disper-
p
α = |q|2 − ω 2 /c2 , sion relation
p
αc = |q|2 − c ω 2 /c2 , (A1) 1 − r2 e−2αd = 0, (A6)
respectively in the film and the cladding, where (c ) is in which r is the Fresnel reflection coefficient
the dielectric function in the film (cladding) and c is the αc − αc
r= . (A7)
speed of light in vacuum. In all the Paper in-plane 2D αc + αc
vectors are bold, and three dimensional vectors are indi-
cated either listing the in- and out-of-plane components After manipulation Eq. A6 can be recast in the form [48]
in squared parenthesis or, when notationally clear, with
αc c α
an arrow symbol. The full 3D wavevector of the mode in 2 − tanh (αd) + = 0. (A8)
c α αc
the layers is thus written as [q, α], and similarly we write
the full 3D coordinate [r, z]. Although in the thin film limit Eq. A8 can simplify dra-
Each interface between the polar film and cladding matically [58] in this work we cannot utilise this ap-
supports a surface phonon polariton with electric field proximation as it breaks down at the larger wavevec-
components at the upper and lower interfaces given by tors under study. The SPhP frequency ωqSP utilised in
10
LTP
the main body is found by numerical solution of Eq. A8. polaritons (LTPs) [48] with frequencies ωq,j
This yields a complex modal frequency as a function of X
LTP ˆ† ˆ
wavevector q, which leads to the loss rate ĤLTP =~ ωq,j dq,j dq,j , (A14)
q,j
γ
γqM = = ωqSP = , (A9)
2 described by creation operators
X
in the wavevector region under study [58], a consequence dˆq,j = αq,j âq + βq,j,n b̂q,n , (A15)
of strong confinement in the polar layer. Note that we n
neglect the frequency and polarization dependence of the
phononic loss rate. in which j indexes the polariton branch, and the Hopfield
coefficients αq,j , βq,j,n preserve the unitary nature of the
transformation
2. Nonlocal Response of Thin Polar Films X
|αq,j |2 + |βq,j,n |2 = 1. (A16)
n
The nonlocal optics of the system can be derived semi-
analytically considering the dispersion of LO phonons This ensures that the resulting LTP modes are also
in the polar film [48]. In the typical quadratic model bosonic, whose creation and annihilation operators sat-
of phonon dispersion [45] the dispersive LO phonon fre- isfy the commutation relation
quency takes the form h i
dˆq,j , dˆ†q0 ,j 0 = δq,q0 δj,j 0 , (A17)
ωq~L 2 = ωL2 − βL2 |q|2 + qz2 , (A10)
and j indexes the different LTP branches.
where ωL is the frequency at zero-wavevector, ~q = [q, qz ] The homogeneous lineshape of the j th LTP branch can
is the 3D wavevector and βL is a characteristic veloc- be written as a Lorentzian
ity. In a planar layer enforcing Pekar boundary condi-
LTP
tions, as when the Reststrahlen bands in the layer and 1 γq,j
ρLTP
q,j (ω) = , (A18)
the cladding do not overlap, this leads to discrete, lo- LTP )2 + (γ LTP )2
π (ω − ωq,j q,j
calised LO phonon modes with frequencies
q where the homogeneous LTP linewidth can be written
L
ωq,n = ωL2 − βL2 (ξn2 + |q|2 ), (A11) from Eq. A15 as a weighed sum of the different involved
scattering channels as
where ξn is the quantized out-of-plane wavevector defined LTP
γq,j = γ + |αq,j |2 γqM − γ . (A19)
in Eq. 4 in the main text.
The SPhP mode considered in Appendix A 1 and these
localised LO phonons interact through shared electro- 3. Quantization of the LO Mode
mechanical boundary conditions [45]. In the trilayer un-
der study we previously derived the analytical form of
In this Paper we aim to describe interactions between
this coupling Ωn,q , given by Eq. 5 [48]. Using this result
electrons and localised LO phonon modes through the
the interacting system can be described in the rotating
Fröhlich interaction. To do this we require the Hamilto-
wave approximation by the quadratic Hamiltonian
nian modeling the interaction of the two systems. Given
X X an electronic charge density operator ρ̂ we can write
ĤLTP =~ ωqSP â†q âq + L
ωq,n b̂†q,n b̂q,n Z h i
q n
ĤInt = − d2 r dz ρ̂ (r, z) φ̂ (r, z) + ĵ (r, z) · Â (r, z) ,
+ Ωq,n âq b̂†q,n + â†q b̂q,n , (A12) (A20)
where φ̂ is the electric potential arising from LO phonon
in which â†q (b̂†q,n ) are the annihilation operators for the modes, ĵ is the electric current density operator and Â
is the electromagnetic vector potential. The first term
SPhP (nth LO phonon) mode, obeying bosonic commu- of this Hamiltonian describes the interaction between an
tation rules electronic charge and the induced LTP charge in the lat-
h i tice, while the second describes interaction between elec-
âq , â†q0 = δq,q0 ,
tronic currents and the electromagnetic tranverse fields.
h i
The former one is dominant for low-frequency currents
b̂q,n , b̂†q0 ,n0 = δq,q0 δn,n0 . (A13)
and in this Paper we will consider only this component,
using the Fröhlich Hamiltonian
The quadratic bosonic Hamiltonian in Eq. A12 can be Z
diagonalized using a multimode Hopfield-Bogoliubov di-
agonalization into a spectrum of longitudinal-transverse ĤFrö = − d2 r dz ρ̂ (r, z) φ̂ (r, z) . (A21)
11
In a local model the discontinuity in the out-of-plane elec- Appendix B: Electron Gas
tric field at the boundaries of the polar layer leads to a
finite induced charge which, due to the transverse nature Electrons interact with LO phonons through the
of the electric field, is unable to spread into the interior Fröhlich Hamiltonian in Eq. A21. Introducing the
of the polar layer. In our nonlocal model instead, charge fermionic annihilation operators ĉ~k with 3D momentum
induced at the edge of the polar layer is able to spread ~k = [k, k], describing electrons in the conduction band,
into the interior, manifesting as a source of LO phonons.
the free electron Hamiltonian is given by
This charging is entirely encoded in the LO phonon fields
and their corresponding scalar potential. X
The electric potential at fixed in-plane wavevector q in Ĥ = ε~k ĉ~† ĉ~k , (B1)
k
branch n with out-of-plane wavevector ξn given by Eq. 4 ~
k
is proportional to
where the free-electron energy is ε~k = ~2 |~k|2 /2m∗ and m∗
iq·r
uq,n (r, z) = sin [ξn (z + d/2)] e . (A22) is the effective electron mass in the cladding region. We
consider a Si cladding region and we will thus consider
To parameterize the Hamiltonian Eq. A21 it is necessary the conductivity effective mass m∗ = 0.26me , where me
to quantize the phonon field. This can be carried out is the free-electron mass. The electronic creation and
from the corresponding electric field annihilation operators obey Fermionic anti-commutator
~ q,n (r, z) = −Bq,n ∇uq,n (r, z) , rules
E (A23)
{ĉ~k , ĉ~† 0 } = δ~k,k~0 , (B2)
where Bq,n is a constant to be determined by the quan- k
tization procedure. Utilizing the results of Refs. [49, 63],
where we developed a quantum theory on local and non- and have free plane-wave wavefunctions of form
local polar media, 1 ik·r ikz
Z 2 ψ~k (r, z) = √ e e , (B3)
L2 2 LA
20 ∞ ωq,n ωL − ωT
3
d r ~ q,n |2
|E
L
~ωq,n L 2 − ω 2 + β 2 (|q|2 + ξ 2 ) 2
ωq,n T L n where L is the electronic quantization length along z and
L
A the sample surface. By inverting Eq. A15 to write
= sgn ωq,n ,
(A24) the LO phonon operators in terms of the LTPs we can
rewrite Eq. A21 as
L
where ωq,n is the mode frequency, given in this case be
Eq. 3. For the Fabry-Pérot modes under study, consid- (2π)2 X
ĤFrö = ~κq,k,k0 ,j δ (k0 − k − q)
ering that ξn = nπ/d we can find A
~
k,q,~
k0 ,j
Z h i
~ q,n |2 = |Bq,n |2 Ad ω 2 − ω 2 ,
d3 r|E (A25) × ĉ~† ĉ~k0 dˆ†q,j + ĉ~† 0 ĉ~k dˆq,j ,
k k
2 L q,n
2βL (B4)
with A the device in-plane area. After substituting
Eq. A25 back into Eq. A24 we recover the quantization in which ~k = [k, k] is the incoming electronic wavevector
constant and ~k 0 = [k0 , k 0 ] is the outgoing one. Integrating over
s s the in-plane component of the out-going wavevector k0
L
~ωq,n βL2 we put the Fröhlich Hamiltonian in the form
Bq,n = ρ 2 L2
, (A26)
0 q,n Ad ωL − ωq,n X h i
ĤFrö = ~κq,k,k0 ,j ĉ~† ĉ~k+~q dˆ†q,j + ĉ~† ĉ~k dˆq,j ,
L k k+~
q
in which, compared to the local case ωq,n = ωL , we ac- ~
k,k0 ,q,j
quired a dispersive Fröhlich constant (B5)
L2
ωq,n clearly describing the dressed Fröhlich process in Fig. 2c,
ρq,n = ∞ 2 . (A27)
ωL2 − ωT where the electron-LTP coupling coefficient has form
Finally, we can write the second-quantized form of the eX
LO phonon potential κq,k,k0 ,j = Bq,n βq,j,n Ξk,k0 ,n , (B6)
~ n
X h i
φ̂ (r, z) = Bq,n uq,n (r, z) b̂q,n + b̂†−q,n , (A28) with the electron-phonon overlap integral given by
q,n
Z 0
1 0
which parameterizes the LO phonon contribution to Ξk,k0 ,n = dz ei(k−k )z sin [ξn (z + d/2)] . (B7)
Eq. A21. L −d
12
Note that in systems containing free charges the di- the drift velocity, and the temperature of the electron
electric function differs from Eq. 1, and is instead given gas.
by We are able to write the balance equations between elec-
tronic energy ε and drift velocity ν as [65]
ωL2 − ω (ω + iγ) X nj e2 1
(ω) = ∞ 2 − ∗ , ∂ε ~ωL
ωT − ω (ω + iγ) 0 mj ω (ω + iΓ) = −eEν − , (C1a)
j=e,h
∂t τε (Te , Tl )
(B8)
where Γ is a characteristic free carrier scattering rate, ∂ν eE ν
=− ∗ − , (C1b)
nj is the carrier density, m∗j is the carrier conductivity ∂t m τm (Te , Tl )
effective mass, and j refers to electrons e, or holes h. In
SiC the relatively high frequencies of the Reststrahlen where E is the scalar electric field, τε (Te , Tl ) (τm (Te , Tl ))
band mean that even at large charge densities the shift in is the energy (momentum) relaxation time dependent on
dielectric function is minimal [64]. Deviations are most both the electron and lattice temperatures. In the steady
severe near to ωL where the Lorentz dielectric function state these equations can be directly solved
vanishes. Note that the predominant effect is a small ~ωL
blue shift in SPhP frequencies. This would actually be eEν = − , (C2)
beneficial for the effect we aim to describe, as the SPhP τε (Te , Tl )
mode would move toward ωL where electron-phonon eE ν
∗
=− , (C3)
coupling is strongest. m τm (Te , Tl )
allowing the electric field or drift velocity to be eliminated
τm (Te , Tl )
Appendix C: Thermalized Electron Model m∗ ν 2 = ~ωL , (C4a)
τε (Te , Tl )
Electrons interacting with the polar nanolayer consid- e2 E 2 ~ωL
= , (C4b)
ered in this Paper are assumed to propagate under the m∗ τm (Te , Tl ) τε (Te , Tl )
influence of an applied electric field polarized perpendic-
ular to the nanolayer. An average electron propagates Although it is not strictly possible to define a relaxation
at the drift velocity, which is limited through momentum time for the polar interaction, a consequence of the in-
relaxation with the crystal lattice. The lattice also pro- elastic and non velocity-randomising nature of the inter-
vides energy relaxation channels, which reduce the mean action [66], it is possible to approximate an energy and
electronic energy and prevent the electron gas from over- momentum relaxation time utilizing Fermi’s golden rule.
heating. We describe the electron gas as thermalised at Following Conwell [67], the probability per unit time of a
a certain electronic temperature Te . In the following we carrier scattering out of state with momentum ~k = [k, k]
calculate closed relationships between the applied field, with exchanged momentum ~q = [q, q] is given by
1 2π X ~ ~ 2 ~ ~ 2
= |hk + ~q, NL − 1|ĤFrö |k, NL i| δ ε~k+~q − ε~k − ~ωL + |hk − ~q, NL + 1|ĤFrö |k, NL i| δ ε~k−~q − ε~k + ~ωL ,
τ~k (Tl ) ~
q
~
(C5)
in which the first term is the transition probability from where EF is the bulk Fröhlich matrix element
phonon absorption, the second is from phonon emission.
Here NL (Tl ) is the equilibrium phonon population in
m∗ e2 ~ωL 1 1
the LO phonon modes which are assumed to be non- eEF = − , (C7)
4π~2 0 ∞ st
dispersive. If we assume spherical bands we can compute
the inverse scattering time directly as
in which ∞ (st ) is the high-frequency (static) dielectric
constant of the lattice and 0 is the permittivity of free-
r
1 2eEF −1 ε~k space.
=p ∗ NL (Tl ) sinh The inverse scattering time τ~−1 (Tl ) is not a relaxation
τ~k (Tl ) 2m ε~k ~ωL k
r time, and as discussed above one cannot be strictly de-
−1 ε~k fined for the polar interaction. We can however define the
+ (NL (Tl ) + 1) sinh − 1 , (C6)
~ωL rate of energy change for an electron with momentum ~k
13
8π 3 e−ε~k /kB Te
f~k (Te ) = , (C9)
dε~k ~ωL LA Nc (Te )
= , (C8)
dt PI τ~k (Tl ) h ∗ i3/2
where Nc (Te ) = 2η m2π~ k B Te
2 is the density of states
in the conduction band, ne is the electronic density and
Pseudo-relaxation times can then be calculated by taking η is the degeneracy factor in the conduction band. Inte-
the distributional average of this rate of energy change. grating over the distribution we find the energy pseudo-
Assuming the electron gas is described by a Maxwell- relaxation time
r
1 1 dε~k 2 eg(Tl )−g(Te )/2 − eg(Te )/2 p g (Te )
≈ =− eEF g (Te )K0 , (C10)
τε (Te , Tl ) ~ωL dt PI πm∗ ~ωL eg(Tl ) − 1 2
where the angular brackets are an average calculated over the distribution in Eq. C9, the Ki are modified Bessel
functions, and we defined the dimensionless quantity g (T ) = ~ωL /kB T .
To find the momentum pseudo-relaxation time we start instead by calculating the change of electronic wavevector in
the transport direction ~z for a carrier with momentum ~k = [k, k], given by
dk 2π X
= k|h~k + ~q, NL − 1|HFrö |~k, NL i|2 δ ε~k+~q − ε~k − ~ωL − k|h~k − ~q, NL + 1|HFrö |~k, NL i|2 δ ε~k−~q − ε~k + ~ωL .
dt ~
q
~
(C11)
As for the previous case we can integrate analytically, yielding the result
s r s s !
dk eEF k ~ωL ~ωL −1 ε~k ~ωL ~ωL ~ωL
=− NL 1+ − sinh +(NL +1) 1− + sinh−1 1− .
dt ~ |~k| ε~k ε~k ~ωL ε~k ε~k ε~k
(C12)
Analogously to the energy relaxation rate we can find the pseudo-relaxation time by integrating over the electronic
distribution. To do this we need to assume the distribution function is drifted, as the gas propagates at drift velocity ν
along ~z. The zero-order spherically symmetric term does not contribute, the first-order perturbation of the distribution
is
(1) ~ν 8π 3 e−ε~k /kB Te
f~ (Te ) = k , (C13)
k kB Te LA Nc (Te )
and integrating over the distribution yields the momentum pseudo-relaxation time
3/2
1 1 d (~k) 2eEF NL (Tl ) g (Te )
≈ ∗ =− √ √ ∗ eg(Te )/2
τm (Te , Tl ) m ν dt PI 3 π 2m ~ωL
g(Tl )−g(Te ) g (Te ) g(Tl )−g(Te ) g (Te )
× e + 1 K1 + e − 1 K0 . (C14)
2 2
We thus arrive at our results for the drift velocity and the field intensity
g(T )−g(T )
g(Te )
~ωL τm (Te , Tl ) 3~ωL e l e
− 1 K 0 2
ν2 = ∗ =√ ,
m τε (Te , Tl ) ∗
2m g (Te ) g(Te ) g(Te )
e g(Tl )−g(Te ) + 1 K1 + e g(T l )−g(T e ) − 1 K0
2 2
(C15a)
2 ∗ 2 2 h i
E (Te , Tl ) m ~ωL 2NL (Tl ) g (Te ) g(Te ) g(Tl )−g(Te ) g (Te )
= 2 2 = e e − 1 K0
EF e EF τm (Te , Tl ) τε (Te , Tl ) 3π 2
g (Te ) g (Te )
× eg(Tl )−g(Te ) + 1 K1 + eg(Tl )−g(Te ) − 1 K0 . (C15b)
2 2
Appendix D: Calculation of Electrical Injection by the distribution in Eq. C9. As described in Ap-
pendix C this electronic temperature can be related to LTP of in-plane wavevector q in branch j, while exchang-
the electronic drift velocity. ing out-of-plane momentum k 0 is given by
The rate at which electrons with wavevector ~k emit an
where the ∓ refers to emission (+) and absorption (−) of a LTP respectively. Integrating over the incident electronic
wavevector ~k we derive the total rate at which all electrons emit LTPs in branch j with in-plane wavevector q
X Z Z Z Z Z Z
∓ ∓ AL2 0 2 ∓ 2 ne 0
Γq,j = Γ ~ 0 = dk dk d k Γ ~ 0 = ~AL dk dk d2 k|κq,k,k0 ,j |2
q,k,k ,j (2π)4 q,k,k ,j Nc
k0 ,~
k
ε~
−k k
LTP
×e B Te δ(εk,k − εk∓q,k0 ∓ ~ωq,j ). (D2)
We account for linewidth broadening of the LTP modes by using, instead of the Dirac’s delta, the Lorentzian density
of states from Eq. A18.
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