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Electronic Supplementary Information : Photo-sensitizing thin-film
ferroelectric oxides using materials databases and high-throughput
calculations
Jose J. Plata,1 Javier Amaya Suárez,1 Santiago
Cuesta-López,2 Antonio M. Márquez,1 and Javier Fdez Sanz1
1Departamento de Qúımica F́ısica, Universidad de Sevilla, Seville, Spain∗2International Center in Advanced Materials and raw materials of Castilla y Leon, León, Spain
(Dated: November 20, 2019)
AbstractConventional solar cell efficiency is usually limited by the Shockley-Queisser limit. This is not the case,
however, for ferroelectric materials, which present a spontaneous electric polarization that is responsible
for their bulk photovoltaic effect. Even so, most ferroelectric oxides exhibit large band gaps, reducing the
amount of solar energy that can be harvested. In this work, a high-throughput approach to tune the electronic
properties of thin-film ferroelectric oxides is presented. Materials databases were systematically used to find
substrates for the epitaxial growth of KNbO3 thin-films, using topological and stability filters. Interface
models were built and their electronic and optical properties were predicted. Strain and substrate-thin-film
band interaction effects were examined in detail, in order to understand the interaction between both materi-
als. We found substrates that significantly reduce the KNbO3 band gap, maintain KNbO3 polarization, and
potentially present the right band alignment, favoring the electron injection in the substrate/electrode. This
methodology can be easily applied to other ferroelectric oxides, optimizing their band gaps and accelerating
the development of new ferroelectric-based solar cells.
S1
Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A.This journal is © The Royal Society of Chemistry 2019
mailto:[email protected]
S1. SUPERLATTICE CONSTRUCTION
In order to build all the surfaces with an area nA, the primitive surface vectors, a and b, aretransformed in the superlattice surface vectors, u and v, using transformation matrices [1],(
u
v
)=
(i j
0 m
)(a
b
), (1)
where i, j and m are integers, and
i ·m = n, (2)
i,m > 0, (3)
0 ≤ j ≤ m− 1. (4)
S2. KNBO3 BULK BENCHMARK
TABLE S1. Lattice parameters a and c, ratio c/a, and indirect (M → Γ) band gap, Eg, for tetragonalKNbO3.
LDA PBEsol PBE+U HSE06-30 HSE06 exp.
a 3.945 [2] 3.969 [2] 3.998 - - 3.997 [3]
c 3.989 [2] 4.058 [2] 4.022 - - 4.063 [3]
c/a 1.011 [2] 1.022 [2] 1.006 - - 1.017 [3]
Eg 1.40,1.50 [4, 5] - 1.75 3.23 [2] 2.66 [4] 3.08,3.30 [6, 7]
S3. KNBO3 BAND STRUCTURE
−4
−2
0
2
4
y
−4
−2
0
2
4
G X M G Z R
y
G X M G Z R G X M G Z R G X M G Z R G X M G Z R
FIG. S1. Band structure for KNbO3 bulk (top panels) and thin-film (bottom panels) applying compressive
(negative) and tensile (positive) strain.
S2
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dx2�y2AAAB8nicbVBNS8NAEN34WetX1aOXYBG8WJIo6LHoxWMF+wFpWjabTbt0sxt2J2IJ/RlePCji1V/jzX/jts1BWx8MPN6bYWZemHKmwXG+rZXVtfWNzdJWeXtnd2+/cnDY0jJThDaJ5FJ1QqwpZ4I2gQGnnVRRnISctsPR7dRvP1KlmRQPME5pkOCBYDEjGIzkR/38qeedj3vepF+pOjVnBnuZuAWpogKNfuWrG0mSJVQA4Vhr33VSCHKsgBFOJ+VupmmKyQgPqG+owAnVQT47eWKfGiWyY6lMCbBn6u+JHCdaj5PQdCYYhnrRm4r/eX4G8XWQM5FmQAWZL4ozboO0p//bEVOUAB8bgoli5labDLHCBExKZROCu/jyMml5Nfei5t1fVus3RRwldIxO0Bly0RWqozvUQE1EkETP6BW9WWC9WO/Wx7x1xSpmjtAfWJ8/vVCQ5Q==
FIG. S2. Upper panel: schematic representation of Nb 4d orbitals splitting on a cubic (left), tetragonal
(center) and tensile strained tetragonal perovskite. Bottom panel: partial electron density of the first 5
unoccupied states at Γ.
S4. SUBSTRATES LIST
TABLE S2: Substrate list for KNbO3 including Pearson sym-
bol, space group number, lattice misfits, supercell generator
matrices, interface band gap (Eg) in eV and junction type.
Formula Pearson S.G.# Plane �a �b �α Msubs MKNO Eg junction type
SnO2 tI12 141 (0 0 1) 0.83 0.83 0.00
1 00 1
1 00 1
0 IIINbO2 tI12 141 (0 0 1) 1.22 1.22 0.00
1 00 1
1 00 1
0 IIIGe cF8 227 (1 1 0) 1.27 -4.52 0.00
1 00 2
1 00 3
0 III
S3
Formula Pearson S.G.# Plane �a �b �α Msubs MKNO Eg junction type
CdF2 cF12 225 (1 0 0) -3.48 -3.48 0.00
1 00 1
1 00 1
0 IIICaF2 cF12 225 (1 0 0) -3.07 -3.07 0.00
1 00 1
1 00 1
1.85 ItfCu2S cF12 225 (1 0 0) -2.42 -2.42 0.00
1 00 1
1 00 1
0 IIINa2O cF12 225 (1 0 0) -1.68 -1.68 0.00
1 00 1
1 00 1
0 IIIHgF2 cF12 225 (1 0 0) -0.67 -0.67 0.00
1 00 1
1 00 1
0 IIILi2S cF12 225 (1 0 0) 0.54 0.54 0.00
1 00 1
1 00 1
0 IIISrF2 cF12 225 (1 0 0) 3.08 3.08 0.00
1 00 1
1 00 1
2.50 ItfKF cF8 225 (0 0 1) -4.69 -4.69 0.00
1 00 1
1 00 1
1.27 ItfMgSe cF8 225 (0 0 1) -3.16 -3.16 0.00
1 00 1
1 00 1
1.67 IItfLiBr cF8 225 (0 0 1) -3.12 -3.12 0.00
1 00 1
1 00 1
1.81 IItfBaO cF8 225 (0 0 1) -1.33 -1.33 0.00
1 00 1
1 00 1
1.24 IItfAgCl cF8 225 (0 0 1) -1.20 -1.20 0.00
1 00 1
1 00 1
1.61 ItfGeSe cF8 225 (0 0 1) -0.44 -0.44 0.00
1 00 1
1 00 1
0.71 IsubTlF cF8 225 (0 0 1) -0.17 -0.17 0.00
1 00 1
1 00 1
1.89 ItfNaCl cF8 225 (0 0 1) 0.02 0.02 0.00
1 00 1
1 00 1
1.83 ItfKH cF8 225 (0 0 1) 0.10 0.10 0.00
1 00 1
1 00 1
1.63 IItf
S4
Formula Pearson S.G.# Plane �a �b �α Msubs MKNO Eg junction type
CaS cF8 225 (0 0 1) 0.45 0.45 0.00
1 00 1
1 00 1
0.60 IItfRbF cF8 225 (0 0 1) 0.85 0.85 0.00
1 00 1
1 00 1
1.79 ItfYSe cF8 225 (0 0 1) 1.61 1.61 0.00
1 00 1
1 00 1
0 IIISnAs cF8 225 (0 0 1) 2.08 2.08 0.00
1 00 1
1 00 1
0 IIIYAs cF8 225 (0 0 1) 2.56 2.56 0.00
1 00 1
1 00 1
0 IIIAgBr cF8 225 (0 0 1) 2.83 2.83 0.00
1 00 1
1 00 1
1.68 IItfSnS cF8 225 (0 0 1) 2.83 2.83 0.00
1 00 1
1 00 1
0.25 IItfLaS cF8 225 (0 0 1) 3.30 3.30 0.00
1 00 1
1 00 1
0 IIICaSe cF8 225 (0 0 1) 4.81 4.81 0.00
1 00 1
1 00 1
0.17 IItfTlF cF8 225 (1 1 0) -0.16 -0.16 0.00
1 00 1
1 00 1
1.89 ItfRbF cF8 225 (1 1 0) 0.85 -4.92 0.00
1 00 2
1 00 3
2.12 ItfRbF cF8 225 (1 1 0) 0.85 -4.92 0.00
4 00 1
3 00 1
2.12 ItfLiF cF8 225 (1 1 0) 1.48 -4.33 0.00
4 00 1
1 00 3
1.97 ItfYSe cF8 225 (1 1 0) 1.61 -4.20 0.00
1 00 2
1 00 3
0 IIIYSe cF8 225 (1 1 0) 1.61 -4.20 0.00
1 00 2
3 00 1
0 IIISnAs cF8 225 (1 1 0) 2.08 -3.75 0.00
1 00 2
3 00 1
0 III
S5
Formula Pearson S.G.# Plane �a �b �α Msubs MKNO Eg junction type
YAs cF8 225 (1 1 0) 2.56 -3.31 0.00
1 00 2
1 00 3
0 IIIAgBr cF8 225 (1 1 0) 2.83 -3.05 0.00
1 00 2
3 00 1
1.65 IsubSnS cF8 225 (1 1 0) 2.83 -3.05 0.00
1 00 2
3 00 1
1.07 IItfLaS cF8 225 (1 1 0) 3.30 -2.61 0.00
1 00 2
1 00 3
0 IIIZnS hP4 186 (1 1 0) -4.37 4.66 0.00
3 00 1
1 00 2
1.91 IIsubLaN hP4 186 (1 1 0) 2.71 -1.26 0.00
1 00 3
2 00 1
0.41 IItfBeO hP4 186 (1 1 0) -4.97 0.80 0.00
3 00 1
2 00 1
2.55 IItfZnSe hP4 186 (1 1 0) 0.91 -4.86 0.00
1 00 2
3 00 1
1.65 ItfGaAs hP4 186 (1 1 0) 1.04 -4.73 0.00
1 00 2
1 00 3
0.87 IsubCdS hP4 186 (1 1 0) 4.39 -1.57 0.00
1 00 2
3 00 1
1.35 IIsub
S6
a(null)(null)(null)(null)
b(null)(null)(null)(null)
cAAAB6HicbVA9SwNBEJ2LXzF+RS1tFoNgFe5ioWXQxjIB8wHJEfY2c8mavb1jd08IR36BjYUitv4kO/+Nm+QKTXww8Hhvhpl5QSK4Nq777RQ2Nre2d4q7pb39g8Oj8vFJW8epYthisYhVN6AaBZfYMtwI7CYKaRQI7ASTu7nfeUKleSwfzDRBP6IjyUPOqLFSkw3KFbfqLkDWiZeTCuRoDMpf/WHM0gilYYJq3fPcxPgZVYYzgbNSP9WYUDahI+xZKmmE2s8Wh87IhVWGJIyVLWnIQv09kdFI62kU2M6ImrFe9ebif14vNeGNn3GZpAYlWy4KU0FMTOZfkyFXyIyYWkKZ4vZWwsZUUWZsNiUbgrf68jpp16reVdVt1ir12zyOIpzBOVyCB9dQh3toQAsYIDzDK7w5j86L8+58LFsLTj5zCn/gfP4Axm+M5w==
FIG. S3. Top, side and bottom view of interfaces models for the epitaxial growth of KNbO3 thin-films with
different prototypes: a) anatase, b) diamond, c) zincblende, d) wurtzite and e) fluorite. Colors: K, purple;
Nb, cyan; O, red; Sn, gray; Ge, tan ; Zn, silver; S, yellow; Ga, orange; As, light green; Ca, white; F, green.
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
Ener
gy(null)(null)(null)(null)
Substrate(null)(null)(null)(null)
Eg(null)(null)(null)(null)
EF(null)(null)(null)(null)
0
10
20
30
40
50
−10 −5 0 5 10
DOS
(sta
tes/
eV)
E−EF (eV)
TotalKNbO3NaCl
−10
−8
−6
−4
−2
20 10 8 6 4 3
Ener
gy (e
V)
Distance (Å)
KNbO3 NaCl
a(null)(null)(null)(null)
b(null)(null)(null)(null)
cAAAB6HicbVA9SwNBEJ2LXzF+RS1tFoNgFe5ioWXQxjIB8wHJEfY2c8mavb1jd08IR36BjYUitv4kO/+Nm+QKTXww8Hhvhpl5QSK4Nq777RQ2Nre2d4q7pb39g8Oj8vFJW8epYthisYhVN6AaBZfYMtwI7CYKaRQI7ASTu7nfeUKleSwfzDRBP6IjyUPOqLFSkw3KFbfqLkDWiZeTCuRoDMpf/WHM0gilYYJq3fPcxPgZVYYzgbNSP9WYUDahI+xZKmmE2s8Wh87IhVWGJIyVLWnIQv09kdFI62kU2M6ImrFe9ebif14vNeGNn3GZpAYlWy4KU0FMTOZfkyFXyIyYWkKZ4vZWwsZUUWZsNiUbgrf68jpp16reVdVt1ir12zyOIpzBOVyCB9dQh3toQAsYIDzDK7w5j86L8+58LFsLTj5zCn/gfP4Axm+M5w==
FIG. S4. Density of states, DOS, for the KNbO3/NaCl interface. Total DOS is shown with solid black line
and KNbO3 and NaCl DOS projections are coloured on orange and blue areas respectively.
S7
S5. Itf JUNCTIONS
1
2
3
2 3 4 5 6
Eg
inte
rfase
(eV)
Eg sustrato (eV)
FIG. S5. Correlation between KNbO3/substrate band gaps, EKNO/subsg , and substrate band gaps, Esubsg , for
Itf heterojuntions.
S6. KNBO3 RECONSTRUCTION
DOS
(u.a
.)
E-EF (eV)
TotalKNOCdS
-4 -2 0 2 4
FIG. S6. a) Density of states, DOS, for the reconstructed KNbO3/CdS interface. b) Side and c) top view of
interfaces models for epitaxial growth of reconstructed KNbO3 (001) thin-films on top of CdS.
S8
S7. KNBO3 SPECTRA
0 1 2 3 4 5
e 2(w
)
hn (eV)
PBE+UHSE
h⌫ (eV)AAAB83icbVDLSgNBEJyNrxhfUY9eBhMhXsJuPOgx6MVjBPOA7BJmJ73JkNnZZR5CWPIbXjwo4tWf8ebfOEn2oIkFDUVVN91dYcqZ0q777RQ2Nre2d4q7pb39g8Oj8vFJRyVGUmjThCeyFxIFnAloa6Y59FIJJA45dMPJ3dzvPoFULBGPeppCEJORYBGjRFvJH1d9Yaq4Bp1LPChX3Lq7AF4nXk4qKEdrUP7yhwk1MQhNOVGq77mpDjIiNaMcZiXfKEgJnZAR9C0VJAYVZIubZ/jCKkMcJdKW0Hih/p7ISKzUNA5tZ0z0WK16c/E/r290dBNkTKRGg6DLRZHhWCd4HgAeMglU86klhEpmb8V0TCSh2sZUsiF4qy+vk06j7l3V3YdGpXmbx1FEZ+gc1ZCHrlET3aMWaiOKUvSMXtGbY5wX5935WLYWnHzmFP2B8/kDwD6QLQ==
✏ 2(!
)AAACAHicbZC7TsMwFIadcivlFmBgYLFokMpSJWWAsYKFsUj0IjVR5binrVXHiWwHqYq68CosDCDEymOw8Ta4bQZo+SVLn/5zjo7PHyacKe2631ZhbX1jc6u4XdrZ3ds/sA+PWipOJYUmjXksOyFRwJmApmaaQyeRQKKQQzsc387q7UeQisXiQU8SCCIyFGzAKNHG6tknjg+JYtxwzcFOxY8jGJILp2eX3ao7F14FL4cyytXo2V9+P6ZpBEJTTpTqem6ig4xIzSiHaclPFSSEjskQugYFiUAF2fyAKT43Th8PYmme0Hju/p7ISKTUJApNZ0T0SC3XZuZ/tW6qB9dBxkSSahB0sWiQcqxjPEsD95kEqvnEAKGSmb9iOiKSUG0yK5kQvOWTV6FVq3qXVfe+Vq7f5HEU0Sk6QxXkoStUR3eogZqIoil6Rq/ozXqyXqx362PRWrDymWP0R9bnDzyllN4=
HSEAAAB6nicbVDLSgNBEOyNrxhfUY9eBoPgKezGgx6DIuQYiXlAsoTZSScZMju7zMwKYcknePGgiFe/yJt/4yTZgyYWNBRV3XR3BbHg2rjut5Pb2Nza3snvFvb2Dw6PiscnLR0limGTRSJSnYBqFFxi03AjsBMrpGEgsB1M7uZ++wmV5pF8NNMY/ZCOJB9yRo2VGrXGfb9YcsvuAmSdeBkpQYZ6v/jVG0QsCVEaJqjWXc+NjZ9SZTgTOCv0Eo0xZRM6wq6lkoao/XRx6oxcWGVAhpGyJQ1ZqL8nUhpqPQ0D2xlSM9ar3lz8z+smZnjjp1zGiUHJlouGiSAmIvO/yYArZEZMLaFMcXsrYWOqKDM2nYINwVt9eZ20KmXvquw+VErV2yyOPJzBOVyCB9dQhRrUoQkMRvAMr/DmCOfFeXc+lq05J5s5hT9wPn8Azp+NeA==
PBE+UAAAB7HicbVBNS8NAEJ34WetX1aOXxSIIQknqQY+lInisYNpCG8pmO2mXbjZhdyOU0t/gxYMiXv1B3vw3btsctPXBwOO9GWbmhang2rjut7O2vrG5tV3YKe7u7R8clo6OmzrJFEOfJSJR7ZBqFFyib7gR2E4V0jgU2ApHtzO/9YRK80Q+mnGKQUwHkkecUWMlv1G/u/R7pbJbcecgq8TLSRlyNHqlr24/YVmM0jBBte54bmqCCVWGM4HTYjfTmFI2ogPsWCppjDqYzI+dknOr9EmUKFvSkLn6e2JCY63HcWg7Y2qGetmbif95ncxEN8GEyzQzKNliUZQJYhIy+5z0uUJmxNgSyhS3txI2pIoyY/Mp2hC85ZdXSbNa8a4q7kO1XKvncRTgFM7gAjy4hhrcQwN8YMDhGV7hzZHOi/PufCxa15x85gT+wPn8Ac60jgM=
FIG. S7. Imaginary part of the frequency-dependent dielectric function, �2 (ω), for the KNbO3/CdS using
PBE+U (blue) and HSE (orange) functional.
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S9
Electronic Supplementary Information : Photo-sensitizing thin-film ferroelectric oxides using materials databases and high-throughput calculationsAbstractSuperlattice constructionKNbO3 bulk benchmarkKNbO3 band structureSubstrates listItf junctionsKNbO3 reconstructionKNbO3 spectraReferences