Electronic Supplementary Information : Photo-sensitizing thin ...Electronic Supplementary Information : Photo-sensitizing thin- lm ferroelectric oxides using materials databases and

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.

∗ [email protected]

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

t2gAAAB7XicbVBNS8NAEJ3Ur1q/qh69LBbBU0mqoMeiF48V7Ae0oWy2m3btZhN2J0IJ/Q9ePCji1f/jzX/jts1BWx8MPN6bYWZekEhh0HW/ncLa+sbmVnG7tLO7t39QPjxqmTjVjDdZLGPdCajhUijeRIGSdxLNaRRI3g7GtzO//cS1EbF6wEnC/YgOlQgFo2ilFvaz2nDaL1fcqjsHWSVeTiqQo9Evf/UGMUsjrpBJakzXcxP0M6pRMMmnpV5qeELZmA5511JFI278bH7tlJxZZUDCWNtSSObq74mMRsZMosB2RhRHZtmbif953RTDaz8TKkmRK7ZYFKaSYExmr5OB0JyhnFhCmRb2VsJGVFOGNqCSDcFbfnmVtGpV76Jau7+s1G/yOIpwAqdwDh5cQR3uoAFNYPAIz/AKb07svDjvzseiteDkM8fwB87nD4/3jx4=

egAAAB7HicbVBNS8NAEJ34WetX1aOXxSJ4KkkV9Fj04rGCaQttKJvtpF262YTdjVBCf4MXD4p49Qd589+4bXPQ1gcDj/dmmJkXpoJr47rfztr6xubWdmmnvLu3f3BYOTpu6SRTDH2WiER1QqpRcIm+4UZgJ1VI41BgOxzfzfz2EyrNE/loJikGMR1KHnFGjZV87OfDab9SdWvuHGSVeAWpQoFmv/LVGyQsi1EaJqjWXc9NTZBTZTgTOC33Mo0pZWM6xK6lksaog3x+7JScW2VAokTZkobM1d8TOY21nsSh7YypGellbyb+53UzE90EOZdpZlCyxaIoE8QkZPY5GXCFzIiJJZQpbm8lbEQVZcbmU7YheMsvr5JWveZd1uoPV9XGbRFHCU7hDC7Ag2towD00wQcGHJ7hFd4c6bw4787HonXNKWZO4A+czx8GmY7T

dxyAAAB7XicbVBNS8NAEJ34WetX1aOXxSJ4KkkV9Fj04rGC/YA2lM1m067d7IbdjRhC/4MXD4p49f9489+4bXPQ1gcDj/dmmJkXJJxp47rfzsrq2vrGZmmrvL2zu7dfOThsa5kqQltEcqm6AdaUM0FbhhlOu4miOA447QTjm6nfeaRKMynuTZZQP8ZDwSJGsLFSOxzkT9lkUKm6NXcGtEy8glShQHNQ+eqHkqQxFYZwrHXPcxPj51gZRjidlPuppgkmYzykPUsFjqn289m1E3RqlRBFUtkSBs3U3xM5jrXO4sB2xtiM9KI3Ff/zeqmJrvyciSQ1VJD5oijlyEg0fR2FTFFieGYJJorZWxEZYYWJsQGVbQje4svLpF2veee1+t1FtXFdxFGCYziBM/DgEhpwC01oAYEHeIZXeHOk8+K8Ox/z1hWnmDmCP3A+fwD9ZY9m

dxzAAAB7XicbVBNSwMxEJ2tX7V+VT16CRbBU9mtgh6LXjxWsB/QLiWbzbax2WRJsmJd+h+8eFDEq//Hm//GtN2Dtj4YeLw3w8y8IOFMG9f9dgorq2vrG8XN0tb2zu5eef+gpWWqCG0SyaXqBFhTzgRtGmY47SSK4jjgtB2Mrqd++4EqzaS4M+OE+jEeCBYxgo2VWmE/e3ya9MsVt+rOgJaJl5MK5Gj0y1+9UJI0psIQjrXuem5i/Awrwwink1Iv1TTBZIQHtGupwDHVfja7doJOrBKiSCpbwqCZ+nsiw7HW4ziwnTE2Q73oTcX/vG5qoks/YyJJDRVkvihKOTISTV9HIVOUGD62BBPF7K2IDLHCxNiASjYEb/HlZdKqVb2zau32vFK/yuMowhEcwyl4cAF1uIEGNIHAPTzDK7w50nlx3p2PeWvByWcO4Q+czx/+6o9n

dyzAAAB7XicbVBNS8NAEJ34WetX1aOXxSJ4KkkV9Fj04rGC/YA2lM1m067d7IbdjRBD/4MXD4p49f9489+4bXPQ1gcDj/dmmJkXJJxp47rfzsrq2vrGZmmrvL2zu7dfOThsa5kqQltEcqm6AdaUM0FbhhlOu4miOA447QTjm6nfeaRKMynuTZZQP8ZDwSJGsLFSOxzk2dNkUKm6NXcGtEy8glShQHNQ+eqHkqQxFYZwrHXPcxPj51gZRjidlPuppgkmYzykPUsFjqn289m1E3RqlRBFUtkSBs3U3xM5jrXO4sB2xtiM9KI3Ff/zeqmJrvyciSQ1VJD5oijlyEg0fR2FTFFieGYJJorZWxEZYYWJsQGVbQje4svLpF2veee1+t1FtXFdxFGCYziBM/DgEhpwC01oAYEHeIZXeHOk8+K8Ox/z1hWnmDmCP3A+fwAAf49o

dz2AAAB7nicbVBNS8NAEJ34WetX1aOXxSJ4KkkV9Fj04rGC/YA2ls1m2i7dbMLuRqihP8KLB0W8+nu8+W/ctjlo64OBx3szzMwLEsG1cd1vZ2V1bX1js7BV3N7Z3dsvHRw2dZwqhg0Wi1i1A6pRcIkNw43AdqKQRoHAVjC6mfqtR1Sax/LejBP0IzqQvM8ZNVZqhb3s6aE66ZXKbsWdgSwTLydlyFHvlb66YczSCKVhgmrd8dzE+BlVhjOBk2I31ZhQNqID7FgqaYTaz2bnTsipVULSj5UtachM/T2R0UjrcRTYzoiaoV70puJ/Xic1/Ss/4zJJDUo2X9RPBTExmf5OQq6QGTG2hDLF7a2EDamizNiEijYEb/HlZdKsVrzzSvXuoly7zuMowDGcwBl4cAk1uIU6NIDBCJ7hFd6cxHlx3p2PeeuKk88cwR84nz9Kd4+J

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


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


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


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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successive ferroelectric phase transitions, J. Phys. C: Solid State Phys 17, 483–514 (1984).

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KNbO3 and polarization rotation, Phys. Rev. B 89, 235105 (2014).

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Adv. M. 3, 100–107 (2007).

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hydrogen generation on cubic, orthorhombic, and tetragonal KNbO3 microcubes, Nanoscale 5, 8375–8383

(2013).

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S9

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