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SUPPLEMENTARY INFORMATION

DOI: 10.1038/NMAT4493

Supplementary Materials for


Correlated metals as transparent conductors
Correlated metals as transparent conductors

Lei Zhang1,2, Yuanjun Zhou3, Lu Guo1,2,†, Weiwei Zhao4, Anna Barnes5,6, Hai-Tian Zhang1,2,
Craig Eaton1,2, Yuanxia Zheng1,2, Matthew Brahlek1,2, Hamna F. Haneef5,6, Nikolas J. Podraza5,6,
Moses H. W. Chan4, Venkatraman Gopalan1, Karin M. Rabe3, Roman Engel-Herbert1,2,*

Affiliations:
1
Department of Materials Science and Engineering, The Pennsylvania State University,
University Park, Pennsylvania 16802, USA.
2
Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania
16802, USA.
3
Department of Physics and Astronomy, Rutgers University, Rutgers, New Jersey 08854 USA.
4
Department of Physics, The Pennsylvania State University, University Park, Pennsylvania
16802, USA.
5
Department of Physics and Astronomy, University of Toledo, Toledo, Ohio 43606 USA.
6
Wright Center for Photovoltaics Innovation and Commercialization, University of Toledo,
Toledo, Ohio 43606 USA.


now at the Department of Materials Science and Engineering, University of Wisconsin-
Madison, Madison, Wisconsin 53706, USA.
*To whom correspondence should be addressed, E-mail: rue2@psu.edu.

This file includes:


Figures S1-S9
Tables S1-S5
References 1-39

1
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A. Film characterization

A1. X-ray diffraction. On-axis 2θ-ω scans were performed for all films. X-ray intensity

of SrVO3 (CaVO3) recorded in the 2θ interval from 45-49° (42-51°) is shown in Fig. S1a (Fig.

S1c). Pronounced thickness fringes evidenced the high quality of the thin films. The XRD data

were fitted using a simple model by taking into account film thickness as well as film and

substrate lattice parameters1. The results are summarized in Table S1 (Table S2), the

comparisons of experimental data and fit is shown for the 45 nm SrVO3 film (38nm CaVO3 film)

in Fig. S1b (Fig. S1d).

A2. Atomic force microscopy: All surfaces of thin films were atomically smooth,

exhibiting a terrace structure, see Fig. S2. The root mean square (RMS) roughness of 4, 10, 12,

15, 20 and 45 nm thick SrVO3 films were determined to 6.5, 1.8, 1.8, 2.5, 1.5, and 2.0 Å,

respectively. RMS roughness of 4, 9, 14, 18, and 38 nm thick CaVO3 films were determined to

2.2, 5.2, 2.1, 2.2 and 2.3Å, respectively.

A3. Spectroscopic ellipsometry of SrVO3 films: Three SrVO3 films, nominally 10, 20,

and 45 nm thick, were grown on single-side polished LSAT substrates and studied using ex-situ

spectroscopic ellipsometry. Room temperature ellipsometric spectra (in  ,  ) were collected at

 i =70° angle of incidence using single rotating-compensator spectroscopic ellipsometers


2, 3

over the IR to UV (0.74 to 5.89 eV; M-2000 J. A. Woollam Co.) and IR (0.049 to 0.75 eV,

FTIR-VASE J. A. Woollam Co.) spectral ranges. The complex dielectric function spectra

(=+i) and microstructural parameters (film layer thickness df, surface roughness thickness

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ds) were first extracted using a least squares regression analysis and an unweighted error function
4
to fit the experimental ellipsometric spectra collected over the near IR to UV range to an optical

model consisting of a semi-infinite LSAT substrate / SrVO3 film / SrVO3 surface roughness layer

/ air ambient. Free parameters corresponded to the thicknesses of the SrVO3 film and the surface

roughness layer and a parameterization of  for SrVO3. The parameterization of  utilized

combinations of Sellmeier, Lorentz, and Tauc-Lorentz oscillators, as well as a constant additive

term to 1 represented by ∞. Each Sellmeier oscillator is represented as 5:

A
 , (A)
E  E 02
2

where A and E0 are the amplitude and resonance energy, respectively, and E0 must be

outside the spectral range. Each Lorentz oscillator is represented by 5:

A  E0
 , (B)
E  E 2  i E
2
0

where A is the amplitude, Γ is the broadening, and E0 is the resonance energy. Each Tauc-

Lorentz oscillator is represented by 6, 7:

 AE 0  ( E  Eg )2 E  E
 2
 2   ( E  E02 ) 2   2 E 2
g
E , (C)
 E  Eg
 0

and

2     2  
1  P d , (D)
 Eg  2  E2

where A, , and E0 correspond to amplitude, broadening, and resonance energy, while Eg

represents an absorption onset determined by assuming a parabolic band, constant momentum

matrix element. A Drude oscillator represented by 5:

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 2
 , (E)
 0  (E 2  iE )

where  is the electrical resistivity,  is the mean free relaxation time,  0 the vacuum

permittivity and  the reduced Planck constant, is used to interpret the intraband response due to

free carrier absorption at low energies.

The optical properties of the surface roughness layer are represented using the
8
Bruggeman effective medium approximation consisting of a 0.5 SrVO3 and 0.5 void volume

fractions. This surface roughness layer was initially included in the model, however it was not

detectable during the data analysis, which is consistent with the film surface being atomically

smooth as verified by AFM. Parameters describing  as well as the optically-determined

thicknesses for the nominally 10, 20, and 45 nm films are given in Table S3. After thicknesses

were obtained using the parametric model, numerical inversion 9


was used to extract  directly

from the experimental ellipsometric spectra as shown in Fig. 3c.

Spectra in  are related to the complex optical conductivity ( = 1 + i2) by 10:

    i 0     1 . (F)

The optical conductivity as a function of frequency for SrVO3 is shown as Fig. S3a.

The plasma frequency p was calculated from the real part of  using 11, 12:

 p2 c
   1 ( ) d  . (G)
8 0

Systematic errors determining the plasma frequency arise from the choice of the upper

integration limit c, the approximation of optical conductivity contribution below the lowest

frequency measured (282 cm-1), and interband contribution to 1 from transition between the t2g

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bands. A cut-off frequency c of 3000 cm-1 was used and values of optical conductivity for

frequencies below 282 cm-1 were omitted. The choice of c is to include all contribution from

free carriers and to exclude contribution from interband transition. Doubling c to 000 cm-1

increased p by less than 10%, while the contribution from t2g to t2g interband transition

calculated by DFT contributed less than 4% of the total Drude peak. With sample-to-sample

deviations less than 3% the total error in p was estimated to 10%. The plasma frequency of

SrVO3 was estimated to be p = (2.10.2) eV. The sum-rule plasma frequency as a function of

cut-off frequency is shown in Fig. S3b.

A4. Spectroscopic ellipsometry of CaVO3 films: A CaVO3 film, nominally 38 nm

thick, was grown on single-side polished SLAO substrates and studied using ex-situ

spectroscopic ellipsometry. Room temperature ellipsometric spectra (in  ,  ) were collected at

 i =55°, 65° and 75° angle of incidence using single rotating-compensator spectroscopic

ellipsometers over the IR to UV (0.73 to 5.04 eV; M-2000U J. A. Woollam Co.). The complex

dielectric function spectra (=+i) and microstructural parameters (film layer thickness df)

were first extracted using a least squares regression analysis and an unweighted error function to

fit the experimental ellipsometric spectra collected over the near IR to UV range to an optical

model consisting of a semi-infinite SLAO substrate / CaVO3 film / air ambient. Free parameters

corresponded to the thicknesses of the CaVO3 film and a parameterization of  for CaVO3. The

parameterization of  utilized combinations of Lorentz and Tauc-Lorentz oscillators, as well as a

constant additive term to 1 represented by ∞. The Lorentz and Tauc-Lorentz oscillator are the

same, as introduced in Eqn (B)-(D). After thicknesses were obtained using the parametric model,

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numerical inversion 9 was used to extract  directly from the experimental ellipsometric spectra

as shown in Fig. S4.

A5. Discussions on the anisotropy of electrical conductance of correlated metals: In

order to verify the independence of electrical conductivity on different in-plane orientations of

SrVO3 and CaVO3, we have fabricated Hall bar devices on 45-nm SrVO3 and 38-nm CaVO3 thin

films and measured resistivity along three different directions: <100>, <110> and <010>. The

resistivity at room temperature and residual-resistance ratio (300K/5K) are almost identical and

independent of the transport directions, as shown in Fig. S5.

The deposition of polycrystalline films from correlated metals with a sizeable anisotropy

in electrical resistivity can affect the overall sheet resistance. While in cubic and pseudo-cubic

crystal structures, such as SrVO3, CaVO3, but also SrNbO3, SrMoO3, CaMoO3, SrRuO3 and

LaNiO3, the anisotropy ratio of resistivity :|| is expected to be small. However, the

anisotropies in correlated metals with layered structure, or uniaxial symmetry might be larger,

and should be taken into consideration. MgB213 :|| ~3, Sr2RuO414 :|| ~23, PdCoO215 ~:||

123 and LaFePO16 :|| ~21.”

B. Data analysis and modeling

B1. Determination of the correlation strength in SrVO3. Despite the conventional

metallic-like behavior of SrVO3, which is also typical for a simple metal described by a free non-

interacting electron gas, i.e. temperature-independent, high carrier concentration and monotonic

resistivity increase with temperature, the electron motion in a correlated metal is also affected by

many-body interactions. Alteration in the carrier dynamics from the expectation of a non-

interacting electron gas can be utilized to identify the type of interaction – such as electron-

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11, 12
phonon coupling or electron-electron interaction – or to gauge the strength of interaction .

Despite the itinerant behavior of carriers being preserved in the Fermi liquid, a strong electron

coupling causes a mass enhancement of the quasiparticle m* , which is quantified by the

renormalization constant Zk. Incorporating electron interaction using the renormalization

constant is common and independent of the model used to describe the correlation phenomena.

In this regard Zk is a hallmark for the correlation strength and a metric for the carrier mass

enhancement m *  m band
* *
/ Z k compared to the band effective mass mband of non-interacting

carriers, and thus at the heart of the new design scheme for transparent conductors. The

renormalization constant is determined by the ratio of a mass-dependent quantity with and

without correlation, e.g. the ratio of the square of the plasma frequencies Z k   pExp /  pDFT  or
2

the ratio of kinetic energies Z k  K Exp / K DFT from band structure calculation without correlation

effects KDFT and experimental values of the experimental kinetic energy KExp reduced by band

width normalization. In both cases the experimental values can be extracted from optical

conductivity measurements 11, 12.

B2. Calculation of the optical transmission of a free-standing film. A free standing

film of thickness t, situated between two dielectric media (air) and forming an abrupt upper and

lower interface was considered. The absorption coefficient  of the film is given by

4 k  
  , (H)

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with k extinction coefficient and  the wavelength in the film. For normal incidence and

monochromatic radiation the transmission coefficient T, i.e. the ratio of incident intensity at the

upper interface and the transmitted intensity at the lower interface is given by 17:

I 1  R   4 R sin 2 
2

T  t , (I)
I 0 e  R 2 e t  2 R cos 2(   )

with the reflectivity R:

R
n  1  k 2
2

, (K)
n  12  k 2

the refractive index n and

2 n t 2k
 ;   tan 1 . (L)
 n  k2 1
2

The term 2 R cos 2(   ) takes into account the interference effect arising from the upper and

lower film interface. The refractive index n and extinction coefficient k are intimately coupled to

the dielectric function

   1  i  2  n 2  k 2  i 2nk (M)

The thickness dependent transmission at 550 nm wavelength for freestanding conducting films

Ag, ITO, SrVO3 and CaVO3 were calculated and are shown in Fig. S6. Since the choice of a

specific wavelength can change  and R quite significantly, T averaged over the visible spectrum

from 400 to 800 nm:

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T  d
800nm

Tave 
400nm
, (N)
800nm

400nm
d

was calculated and is shown as well.

B3. Calculation of enhanced surface scattering effect. The electron mean free path

(EMFP)  considered here is calculated from the Sommerfeld model 18:


3 2 n 3 ,
1
    vF  (O)
e

where  is the relaxation time, v F the Fermi velocity,  the carrier mobility, n the carrier

concentration, and e the elemental charge. Values for the EMFP of selected materials considered

here, including conventional metals, degenerately doped semiconductors, and SrVO3 and CaVO3
19 20
are given in Table S3. Fuchs and Sondheimer attributed the pronounced conductivity

decrease in ultrathin films to enhanced surface scattering, if film thickness is on the order of the

EMFP or below:

 31  p    1 1  1  e   
 FS   0 1 
 2 1



3
 
  1  pe
5  
d  ,

(P)

with  0 the bulk conductivity, = t/  the normalized length with t referring to the film

thickness and  the EMFP and p the reflection coefficient ( 0  p  1 , p=0 diffuse: random

direction and magnitude of velocity after surface scattering event, p=1 specular: elastic scattering

at the surface with reversal of the normal component). Mayadas and Shatzkes 21 have expanded

the Fuchs Sondheimer model by considering the following three main mechanisms: background

scattering, grain boundary scattering and external surface scattering.

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 3  1   R
 MS   0 1    3 2  3 3 ln 1   ,   (R)
 2    D 1 R

with  the EMFP, D the average grain size and R the reflection coefficient. The total

resistivity =1 of SrVO3, CaVO3, Ag and ITO thin films have been calculated as a function of

thickness and the resistivity increase  due to enhanced carrier scattering in the films was

calculated 22 using    FS   MS   0 and the experimental data and fitting for SrVO3, CaVO3

, Ag and ITO are shown in Fig. S7.

B4. Calculation of the figure of merit for transparent conductors. Two parameters

determine the performance of a transparent conducting film: optical transmission T, and sheet

resistance Rs. Both are connected via the film thickness t to the material specific parameters

optical absorption  and electrical conductivity . The best performance is achieved for

simultaneously high electrical conductivity and optical transmission. The figure of merit (FOM)

TC used is based on the metric proposed by Haacke 23

T 10
 TC ( t )   0   . (S)
t

Here T is the optical transmission and (0+)/t represents the sheet resistance Rs that takes into

account surface scattering effects, as described in Section C3 of the supplement. The exponent of

the transmission in Eqn. (S) balances the relative weights of T and (0+)/t contributing to TC

and determines the transmission for the thickness at maximum TC. Using an exponent of 10

stipulates a transmission close to 90% at maximum TC 23


. As discussed in Section C2 of the

supplement and shown in Fig. S6, the choice of a specific wavelength affects T, which can

10

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dramatically alter TC due to the large exponent. Therefore, rather than performing the
23
calculation at a selected wavelength (550 nm was chosen by Haacke , close to the maximum

spectral sensitivity of the human eye) the average transmission [Eqn. (N)] was used instead.

To ensure a meaningful comparison across the different material options considered,

namely conventional metals, represented by Ag, degenerately doped wide band gap

semiconductors, represented by ITO, and the proposed correlated metals, represented by SrVO3

and CaVO3, the FOM has been modified to incorporate effects of enhanced carrier scattering,

relevant for films with thicknesses smaller than the electron mean free path (see C3), and

changes in the transmission from multiple reflection at the top and bottom surface and the

interference effects arising from it for the free standing film (see C2), relevant for film

thicknesses with optical path length on the order of /4. Taking into account both effects caused

a sizable overall reduction of TC compared to the uncorrected FOM.

Figure S5 shows the impact of the different corrections to TC for the case of Ag and

ITO. In the first case, averaging the transmission over the entire visible spectrum compared to

the transmission at 550 nm resulted in a small TC increase, attributed to the strong interband

transition of Ag around 360 nm. Taking reflection into account the transmission increased from

interference and multiple reflection within the film. The effect of enhanced surface scattering of

electrons is rather strong. Although FOM only scales linearly with this effect, the electron mean

free path (EMFP) in Ag is rather large (52 nm, see Table S5) The maximum TC for a film

thickness around 4 nm is only a small fraction of the EMFP, resulting in a more than one order of

magnitude increase in the conductivity compared to the bulk value, see Fig. S8a 23, 24.

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Much more dramatic is the effect of reflection for thicker films, i.e. in the case of degenerately

doped wide band gap semiconductors, where low electrical conductivity is compensated by low

optical absorption allowing a larger film thickness. In case of ITO, averaging T over the entire

visible spectrum resulted in a reduction of the average T, which is further reduced by taking

reflection into account, showing pronounced interference effects in TC with a local minimum at

a film thickness of 60 nm. Taking surface scattering effects into consideration TC only

marginally decreased at the maximum around 150 nm, but was reduced at the second local

maxima at 10 nm, see Fig. S8b.

It is noted that simplifying assumptions in either the transmission of a free standing

conducting film, or limiting the model to only one wavelength, or ignoring the thickness

dependence of conductivity, can result in significant overestimation of TC with dramatic

implications using it as a metric to benchmark the performance of transparent conductors.

Careful consideration of all relevant effects and using a complete set of experimental data, i.e.

the  in the entire range of wavelengths considered and thickness dependent electrical

conductivity for the material to benchmark, are mandatory for a meaningful comparison.

C. First principles density functional theory calculations. First principle calculations

of SrVO3 were performed using the generalized gradient approximation (GGA) with the Perdew-

Becke-Erzenhof parameterization 25 as implemented in the Vienna Ab initio Simulation Package

(VASP-5.2.12) 26, 27. The projector augmented wave (PAW) potentials used contained 10 valence

electrons for Sr (4s24p65s2), 13 for V (2s22p63d34s2) and 6 for O (2s22p4) 28, 29. We used 500 eV

as the energy cutoff. An 8x8x8 Monkhorst-Pack k-point mesh was used for the structural

relaxation, and a 31x31x31 Γ centered k-mesh was used for the interband transition calculation.

12

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Extensive testing with the GGA+U method with nonzero U and ferromagnetic, G-type

antiferromagnetic and nonmagnetic configurations showed that the relevant features of the band

structures and interband transitions are not sensitive to U or the magnetic ordering. For U=0, the

ground state was found to be non-magnetic. Since SrVO3 is paramagnetic at room temperature 30,
31, 32
, we performed the analysis for the nonmagnetic state with U=0. The c lattice parameter of

the tetragonal five-atom unit cell was relaxed with in-plane lattice constant fixed to the

experimental value 3.868Å, preserving P4/mmm symmetry, yielding a c/a ratio of 0.979.

The unscreened plasma frequency was calculated from the band structure using11, 33

4e 2 f ( Enk ) Enk Enk


 2 , 
V 2
 n ,k 2gk
E
(e
k
)(e 
k
), (T)

where denote the direction, V denotes the volume of the unit cell, f is the occupancy,

E is the band energy, e is the unit vector, and g is the weight of k point. For SrVO3, the plasma

frequency is determined by the t2g bands that cross the Fermi level. Since the t2g band structure is

relatively simple, the uncertainty in the plasma frequency is determined by the uncertainty in the

t2g bandwidth. We have computed band structures for different U and k-meshes, and the t2g

bandwidth is found to vary by less than 2%. The uncertainty in  p can thus be estimated to be
2

about 4% of the computed value.

The intraband contribution to the dielectric function was obtained empirically from the

Drude model

 2  2 ne 2 
 int ra    1  2
1 
,  intra    3 2 
, and   ; (U)
 2    2 me

using measured values  =2×10-5 Ω×cm, n=2×1022 cm-3, to estimate  =0.1eV and

me  4.5m0 . The interband contribution  int(1)er ,  int( 2 )er to the dielectric function was calculated using

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the VASP implementation, in the approximation that the local field effects are neglected 34. The

imaginary part was determined by

4 2 e 2
er ,     2 w  E  E vk     u ck  e  q u vk u v k u ck  e  q ,
1
 int
( 2)
lim 2 k ck (V)
V q 0 q c , v ,k

where V is the volume of the unit cell, the index c and v refer to conduction and valence

bands, respectively, and u ck is the cell periodic part of the wavefunction at k-point k. e  and e 

denote unit vector in Cartesian directions. lim u ck e q u vk gives the α component of the dipole
q 0

matrix element between two bands.

The real part of the dielectric function was obtained using the Kramers-Kronig

transformation,

 int er ,  ' '


 ( 2)

(1)
int er ,    1  2
P d ' (W)
 0
 ' 2  2  i

where the P means the principal value, and η is a tiny shift.

Figure S6 illustrates the steps to calculate the contribution from interband transition to the

imaginary part of the dielectric function. Figure S6a shows the band structure highlighting the 8

bands with interband transitions up to 3.6 eV: the three highest valence bands, 2p1 (highest), 2p2

(second highest) and 2p3 (third highest), the two V 3d eg bands eg1 (lowest) and eg2 (highest), and

the three V 3d t2g bands t2g1 (lowest), t2g2 (middle) and t2g3 (highest). Figures S6b-f show energy

difference E and dipole matrix element M2 of optical transitions between initial and final states

in the Brillouin zone of SrVO3 along high symmetry lines. Red symbols indicate same

occupancy of initial and final state, suppressing the transition, while blue symbols represent a

filled to empty, and thus active optical transition. Sphere, triangle and cube symbols correspond

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to the lowest t2g1, middle t2g2 and highest lying t2g3 band for interband transitions. Note that either

a transition with notable M2 in the visible spectrum is suppressed due to same occupancy of

initial and final state (red symbols) or the magnitude of M2 is small. The combination of a large

M2 and a filled to empty transition in the visible spectrum does not occur. The contribution with

both, E in the visible spectrum and sizable M2 were selected for the isosurface representation in

Figs. 4c-4e. The respective contribution of these transitions and low energy interband transition

between different t2g bands to  inter ,   are shown in Fig. S9g.
( 2)

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Figure S1:

Figure S1. High resolution 2- X-ray diffraction scans of a, SrVO3 films with varying
thicknesses grown on LSAT substrates. b, Experimental and calculated X-ray diffraction
intensities of the 45-nm-thick SrVO3. c. SrVO3 films with varying thicknesses grown on LSAT
substrates. d, Experimental and calculated X-ray diffraction intensities of the 38-nm-thick
CaVO3. Film lattice parameter and thickness given in Table S1 and Table S2 were extracted
from these fits.

16

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Figure S2:

Figure S2. Atomic force micrographs of SrVO3 and CaVO3 films.

17

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Figure S3:

Figure S3. a, Optical conductivity as a function of frequency. b, Sum-rule plasma frequency as a


function of cut-off frequency.

18

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Figure S4:

Figure S4. Complex dielectric function ( = 1 + i2) spectra of CaVO3 extracted from room
temperature spectroscopic ellipsometry measurements

19

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Figure S5:

Figure S5. a, Schematic and b, optical photograph of Hall bar devices, here for CaVO3.
Temperature dependent resistivity of c, 45-nm-thick SrVO3 and d, 38-nm-thick CaVO3 films
along the different directions. The scale bar indicates 500 µm.

20

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Figure S6:

Figure S6. Optical transmission of free standing films, accounting for reflection and
interference, at a wavelength =550nm [Eqns. (H), (I), (K), (L)], and averaged over the range of
the visible spectra [Eqn. (N)]. Data of the complex refractive index of Ag, ITO, SrVO3 and
CaVO3 were taken from Refs. 35, 36 and this work.

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Figure S7:

Figure S7. Thickness dependence of the sheet resistance Rs for a, SrVO3 a, CaVO3 c, ITO, and
d, Ag taking the thickness dependent resistivity into account. The increase in resistivity 
normalized to the bulk resistivity 0 is shown below. Data for Ag, ITO, SrVO3 and CaVO3 were
taken from Refs. 37, 38 and this work, respectively.

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Figure S8:

Figure S8. Consideration for the figure of merit (FOM) for transparent conductors. Solid black
line: FOM defined after Haacke 23, calculated for light at wavelength =550 nm. Dashed gray
line: FOM using transmission value taken as average across the visible spectrum [Eqn. (N)].
Dotted blue line: Averaged transmission incorporating multiple reflection and interference
effects from top and bottom interface of a free standing film by calculating the transmission from
Eqn. (H) and averaging over the visible range, see Fig. S4. Thick solid green line. Figure of merit
from Eqn. (S) that includes thickness dependent increase of electrical conductivity due to
enhanced surface scattering for films with thicknesses below the electron mean free path, see
Fig. S5. a, Example of Ag representing ultrathin metal films. b, Example of ITO representing
degenerately doped wide band gap semiconductors.

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Figure S9:

Figure S9. a, Band structure and nomenclature of bands involved in interband transitions of
SrVO3 with energies below 3.6 eV. The superscript is introduced to distinguish the different
bands involved in the transition. b-f, Dipole matrix element M2 and energy difference E
between the lower and upper electronic state along high symmetry lines in the Brillouin zone of

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SrVO3. Red symbols indicate same occupancy of initial and final state (suppressed transition),
blue symbols represent optically active filled to empty transition. Sphere, triangle and cube
symbols correspond to the lowest t2g1, middle t2g2 and highest lying t2g3 band for interband
transitions from b, t2g bands to the lower lying eg1 band [transition (I)], c, t2g bands to the higher
lying eg2 band [transition (II)], d, third highest lying oxygen 2p band 2p3 to the t2g bands
[transition (III)], e, second highest lying oxygen 2p band 2p2 to the t2g bands [transition (IV)], f,
highest lying oxygen 2p band 2p1 to the t2g bands [transition (V)]. g, Contributions of the
individual interband transitions for 2p to t2g (blue), t2g to eg (green) and interband transitions
between different t2g bands (red) to 2.

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Table S1. Thickness series of SrVO3 grown on LSAT samples. Lattice parameter and film
thickness has been extracted from XRD spectra shown in Fig. S1 after Ref. 1. Average optical
transmittance Tfs for a free standing film was calculated from Eqns. (H), (I), (K), (L), (N) using
the dielectric function of SrVO3 given in Table S3. For comparison average transmission
Tfilm/Tsub of SrVO3 on LSAT substrates from 400 to 800 nm is given as well, taken from the
measurements shown in Fig. 3a.

Nominal
Lattice film ρ
film Rs Tfs Tfilm/Tsub
parameter thickness (300 K)
thickness
(Å) (nm) (Ω cm) (%) (%)
45 nm 3.822 ± 0.001 45.9 ± 0.2 2.90×10-5 6.3 51.0 73.3

20 nm 3.824 ± 0.001 20.1 ± 0.1 2.84×10-5 14.2 69.7 83.5

15 nm 3.825 ± 0.001 14.9 ± 0.3 3.28×10-5 22.0 75.7 87.0

12 nm 3.828 ± 0.002 12.0 ± 0.3 4.15×10-5 34.5 79.9 88.6

10 nm 3.829 ± 0.002 10.2 ± 0.3 4.45×10-5 43.8 82.9 89.3

4 nm 3.827 ± 0.003 4.0 ± 0.1 6.15×10-5 153.3 91.9 95.0

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Table S2. Thickness series of CaVO3 grown on SLAO samples. Lattice parameter and film
thickness has been extracted from XRD spectra shown in Fig. S1 after Ref. 1. Average optical
transmittance Tfs for a free standing film was calculated from Eqns. (H), (I), (K), (L), (N) using
the dielectric function of CaVO3 given in Table S4. For comparison average transmission
Tfilm/Tsub of CaVO3 on SLAO substrates from 400 to 800 nm is given as well, taken from the
measurements shown in Fig. 3a.

Nominal
Lattice film ρ
film Rs Tfs Tfilm/Tsub
parameter thickness (300 K)
thickness
(Å) (nm) (Ω cm) (%) (%)
38 nm 3.782 ± 0.002 37.44 ± 0.2 3.86×10-5 10.3 55.7 75.4

18 nm 3.784 ± 0.003 18.16 ± 0.2 4.50×10-5 24.8 72.8 85.1

14 nm 3.782 ± 0.002 14.37 ± 0.3 4.83×10-5 33.6 77.7 88.8

10 nm 3.782 ± 0.002 9.07 ± 0.3 5.66×10-5 62.4 85.7 91.7

4 nm 3.786 ± 0.003 3.79 ± 0.2 7.78×10-5 205.3 93.7 95.3

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Table S3. Parameters describing  and optically-determined thickness of nominally 10, 20, and
45 nm SrVO3 films from analysis of ellipsometric spectra from 0.74 to 5.89 eV.

Nominal Optical  Unweighted error


Thickness Thickness function
10 nm 9.1  0.1 nm 2.29 ± 0.08 3.91 x 103
Oscillator E0 (eV)  (eV) A Eg (eV)
Sellmeier 0 - 9.67 ± 0.15 eV2 -
Lorentz 0.64 ± 0.01 0.58 ± 0.02 7.95 ± 0.27 -
Lorentz 1.69 ± 0.01 0.40 ± 0.04 0.91 ± 0.09 -
Lorentz 2.14 ± 0.01 0.93 ± 0.08 1.30 ± 0.05 -
Tauc-Lorentz 3.27 ± 0.01 0.83 ± 0.01 43.45 ± 2.77 eV 2.11 ± 0.04
Lorentz 4.47 ± 0.02 1.15 ± 0.10 1.73 ± 0.19 -
Lorentz 5.63 ± 0.02 2.16 ± 0.21 2.52 ± 0.07 -
2
Sellmeier 6.91 ± 0.25 - 13.68 ± 3.92 eV -

Nominal Optical  Unweighted error


Thickness Thickness function
20 nm 18.6  0.1 nm 2.36 ± 0.02 2.50 x 103
Oscillator E0 (eV)  (eV) A Eg (eV)
Sellmeier 0 - 10.62 ± 0.08 eV2 -
Lorentz 0.62 ± 0.01 0.24 ± 0.06 6.68 ± 0.32 -
Lorentz 0.87 ± 0.02 0.41 ± 0.05 1.11 ± 0.36 -
Lorentz 1.62 ± 0.01 0.31 ± 0.02 0.47 ± 0.04 -
Lorentz 1.90 ± 0.01 0.56 ± 0.03 0.82 ± 0.03 -
Tauc-Lorentz 3.16 ± 0.01 0.58 ± 0.01 54.29 ± 2.42 eV 2.43 ± 0.01
Lorentz 3.48 ± 0.01 0.56 ± 0.04 1.84 ± 0.25 -
Lorentz 4.43 ± 0.01 0.92 ± 0.05 1.04 ± 0.08 -
Lorentz 6.03 ± 0.04 5.29 ± 0.19 2.35 ± 0.02 -

Nominal Optical  Unweighted error


Thickness Thickness function

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45 nm 44.1  0.1 nm 2.23 ± 0.03 3.70 x 103
Oscillator E0 (eV)  (eV) A Eg (eV)
Sellmeier 0 - 9.93 ± 0.08 eV2 -
Lorentz 0.53 ± 0.01 0.32 ± 0.01 7.64 ± 0.55 -
Lorentz 1.81 ± 0.01 0.68 ± 0.02 0.84 ± 0.01 -
Tauc-Lorentz 3.04 ± 0.01 0.70 ± 0.03 36.75 ± 3.08 eV 2.32 ± 0.02
Lorentz 3.35 ± 0.01 0.35 ± 0.06 1.67 ± 0.34 -
Lorentz 3.57 ± 0.02 0.46 ± 0.04 1.51 ± 0.28 -
Lorentz 4.45 ± 0.01 1.12 ± 0.07 1.38 ± 0.11 -
Lorentz 6.75 ± 0.05 4.95 ± 0.27 2.60 ± 0.03 -

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Table S4. Parameters describing  and optically-determined thickness of nominally 38 nm
CaVO3 films from analysis of ellipsometric spectra from 0.73 to 5.04 eV.

Nominal Optical  Unweighted error


Thickness Thickness function
38 nm 39.1  0.1 nm 1.95 ± 0.02 5.07 x 103
Oscillator E0 (eV)  (eV) A Eg (eV)
Lorentz 1.59 ± 0.01 0.57 ± 0.01 0.56± 0.01 -
Tauc-Lorentz 3.28 ± 0.01 0.72 ± 0.01 75.57 ± 1.17 2.49 ± 0.01
Lorentz 6.29 ± 0.04 4.69 ± 0.06 2.97 ± 0.02 -

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Table S5. Calculation of the electron mean free path (EMPF) for selected materials at room
temperature. Data for Cu, Ag and Al were taken from Ref. 22, ITO from Ref. 39 and SrVO3 from
this work.

resistivity carrier concentration EMPF


(Ω cm) (m-3) nm
Cu 1.70×10-6 8.45×1028 39
Ag 1.61×10-6 5.85×1028 52
Al 2.74×10-6 1.81×1029 15
-4 26
ITO 2.70×10 4.50×10 8.0
SrVO3 2.83×10-5 2.26×1028 5.6
CaVO3 3.87×10-5 2.40×1028 3.9

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