The efficiencies of solar cells based on kesterite Cu2ZnSnS4 (CZTS) and Cu2ZnSnSe4 (CZTSe) are limited by a low open-circuit voltage due to high rates of non-radiative electron-hole recombination. To probe the origin of this bottleneck, we calculate the band offset of CZTS(Se) with CdS, confirming a weak spike of 0.1 eV for CZTS/wurtzite-CdS and a strong spike of 0.4 eV for CZTSe/wurtzite-CdS. We also consider the effects of temperature on the band alignment, finding that increasing temperature significantly enhances the spike-type offset. We further resolve an outstanding discrepancy between the measured and calculated phonon frequencies for the kesterites, and use these to estimate the upper limit of electron and hole mobilities based on optic phonon Fröhlich scattering, which uncovers an intrinsic asymmetry with faster (minority carrier) electron mobility.
References
1.
A.
Walsh
, S.
Chen
, S.-H.
Wei
, and X.-G.
Gong
, Adv. Energy Mater.
2
, 400
(2012
).2.
A.
Polizzotti
, I. L.
Repins
, R.
Noufi
, S.-H.
Wei
, and D. B.
Mitzi
, Energy Environ. Sci.
6
, 3171
(2013
).3.
S. K.
Wallace
, D. B.
Mitzi
, and A.
Walsh
, ACS Energy Lett.
2
, 776
(2017
).4.
W.
Wang
, M. T.
Winkler
, O.
Gunawan
, T.
Gokmen
, T. K.
Todorov
, Y.
Zhu
, and D. B.
Mitzi
, Adv. Energy Mater.
4
, 1301465
(2014
).5.
K.-J.
Yang
, D.-H.
Son
, S.-J.
Sung
, J.-H.
Sim
, Y.-I.
Kim
, S.-N.
Park
, D.-H.
Jeon
, J.
Kim
, D.-K.
Hwang
, C.-W.
Jeon
, D.
Nam
, H.
Cheong
, J.-K.
Kang
, and D.-H.
Kim
, J. Mater. Chem. A
4
, 10151
(2016
).6.
S.
Chen
, X. G.
Gong
, A.
Walsh
, and S.-H.
Wei
, Appl. Phys. Lett.
94
, 041903
(2009
).7.
H.
Zhao
and C.
Persson
, Thin Solid Films
519
, 7508
(2011
).8.
W.
Shockley
and H. J.
Queisser
, J. Appl. Phys.
32
, 510
(1961
).9.
J.
Kim
and B.
Shin
, Electron. Mater. Lett.
13
, 373
(2017
).10.
M.
Gloeckler
and J.
Sites
, Thin Solid Films
480
, 241
(2005
).11.
A.
Crovetto
and O.
Hansen
, Sol. Energy Mater Sol. Cells
169
, 177
(2017
).12.
P. E.
Blöchl
, Phys. Rev. B
50
, 17953
(1994
).13.
G.
Kresse
and D.
Joubert
, Phys. Rev. B
59
, 1758
(1999
).14.
G.
Kresse
and J.
Hafner
, Phys. Rev. B
47
, 558
(1993
).15.
G.
Kresse
and J.
Hafner
, Phys. Rev. B
49
, 14251
(1994
).16.
G.
Kresse
and J.
Furthmüller
, Comput. Mater. Sci.
6
, 15
(1996
).17.
G.
Kresse
and J.
Furthmüller
, Phys. Rev. B
54
, 11169
(1996
).18.
J. P.
Perdew
, K.
Burke
, and M.
Ernzerhof
, Phys. Rev. Lett.
77
, 3865
(1996
).19.
J. P.
Perdew
, A.
Ruzsinszky
, G. I.
Csonka
, O. A.
Vydrov
, G. E.
Scuseria
, L. A.
Constantin
, X.
Zhou
, and K.
Burke
, Phys. Rev. Lett.
100
, 136406
(2008
).20.
J.
Heyd
, G. E.
Scuseria
, and M.
Ernzerhof
, J. Chem. Phys.
118
, 8207
(2003
).21.
J.
Paier
, M.
Marsman
, K.
Hummer
, G.
Kresse
, I. C.
Gerber
, and J. G.
Ángyán
, J. Chem. Phys.
124
, 154709
(2006
).22.
J.
Paier
, M.
Marsman
, K.
Hummer
, G.
Kresse
, I. C.
Gerber
, and J. G.
Ángyán
, J. Chem. Phys.
125
, 249901
(2006
).23.
K.
Kunc
and R. M.
Martin
, Phys. Rev. Lett.
48
, 406
(1982
).24.
J. H.
Lloyd-Williams
and B.
Monserrat
, Phys. Rev. B
92
, 184301
(2015
).25.
B.
Monserrat
, J. Phys. Condens. Matter
30
, 083001
(2018
).26.
M. T.
Dove
, Introduction to Lattice Dynamics
(Cambridge University Press
, 1993
).27.
P. B.
Allen
and V.
Heine
, J. Phys. C
9
, 2305
(1976
).28.
F.
Giustino
, S. G.
Louie
, and M. L.
Cohen
, Phys. Rev. Lett.
105
, 265501
(2010
).29.
B.
Monserrat
and R. J.
Needs
, Phys. Rev. B
89
, 214304
(2014
).30.
S.
Poncé
, G.
Antonius
, P.
Boulanger
, E.
Cannuccia
, A.
Marini
, M.
Côté
, and X.
Gonze
, Comput. Mater. Sci.
83
, 341
(2014
).31.
C. E.
Patrick
and F.
Giustino
, Nat. Commun.
4
, 2006
(2013
).32.
B.
Monserrat
, E. A.
Engel
, and R. J.
Needs
, Phys. Rev. B
92
, 140302
(2015
).33.
Y.-H.
Li
, A.
Walsh
, S.
Chen
, W.-J.
Yin
, J.-H.
Yang
, J.
Li
, J. L.
Da Silva
, X.
Gong
, and S.-H.
Wei
, Appl. Phys. Lett.
94
, 212109
(2009
).34.
S.-H.
Wei
and S.
Zhang
, Phys. Rev. B
62
, 6944
(2000
).35.
A.
Khare
, B.
Himmetoglu
, M.
Johnson
, D. J.
Norris
, M.
Cococcioni
, and E. S.
Aydil
, J. Appl. Phys.
111
, 083707
(2012
).36.
N. B.
Mortazavi Amiri
and A.
Postnikov
, Phys. Rev. B
82
, 205204
(2010
).37.
T.
Gürel
, C.
Sevik
, and T.
Çağin
, Phys. Rev. B
84
, 205201
(2011
).38.
A. J.
Jackson
and A.
Walsh
, J. Mater. Chem. A
2
, 7829
(2014
).39.
J. M.
Skelton
, A. J.
Jackson
, M.
Dimitrievska
, S. K.
Wallace
, and A.
Walsh
, APL Mater.
3
, 041102
(2015
).40.
S. P.
Ramkumar
, Y.
Gillet
, A.
Miglio
, M. J.
van Setten
, X.
Gonze
, and G.-M.
Rignanese
, Phys. Rev. B
94
, 224302
(2016
).41.
M.
Dimitrievska
, A.
Fairbrother
, X.
Fontané
, T.
Jawhari
, V.
Izquierdo-Roca
, E.
Saucedo
, and A.
Pérez-Rodríguez
, Appl. Phys. Lett.
104
, 021901
(2014
).42.
C. V.
Caillie
and R. D.
Amos
, Chem. Phys. Lett.
328
, 446
(2000
).43.
H.
Fröhlich
and N. F.
Mott
, Proc. R. Soc. London. Ser. A
171
, 496
(1939
).44.
J. M.
Frost
, Phys. Rev. B
96
, 195202
(2017
).45.
R. P.
Feynman
, Phys. Rev.
97
, 660
(1955
).46.
O.
Gunawan
, S. R.
Pae
, D. M.
Bishop
, Y. S.
Lee
, Y.
Virgus
, N. J.
Jeon
, J. H.
Noh
, X.
Shao
, T.
Todorov
, D. B.
Mitzi
, and B.
Shin
, preprint arXiv:1802.07910 (2018
).47.
M.
Yuan
, X.
Zhang
, J.
Kong
, W.
Zhou
, Z.
Zhou
, Q.
Tian
, Y.
Meng
, S.
Wu
, and D.
Kou
, Electrochim. Acta
215
, 374
(2016
).48.
S.
Chen
, J.-H.
Yang
, X.-G.
Gong
, A.
Walsh
, and S.-H.
Wei
, Phys. Rev. B
81
, 245204
(2010
).49.
A.
Nagoya
, R.
Asahi
, and G.
Kresse
, J. Phys. Condens. Matter
23
, 404203
(2011
).50.
Z.-Y.
Dong
, Y.-F.
Li
, B.
Yao
, Z.-H.
Ding
, G.
Yang
, R.
Deng
, X.
Fang
, Z.-P.
Wei
, and L.
Liu
, J. Phys. D
47
, 075304
(2014
).51.
S.
Tajima
, K.
Kataoka
, N.
Takahashi
, Y.
Kimoto
, T.
Fukano
, M.
Hasegawa
, and H.
Hazama
, Appl. Phys. Lett.
103
, 243906
(2013
).52.
N.
Terada
, S.
Yoshimoto
, K.
Chochi
, T.
Fukuyama
, M.
Mitsunaga
, H.
Tampo
, H.
Shibata
, K.
Matsubara
, S.
Niki
, N.
Sakai
, T.
Katou
, and H.
Sugimoto
, Thin Solid Films
582
, 166
(2015
).53.
K.
Kataoka
, S.
Tajima
, M.
Umehara
, N.
Takahashi
, N.
Isomura
, K.
Kitazumi
, and Y.
Kimoto
, Appl. Phys. Lett.
109
, 203902
(2016
).54.
S.
Chen
, A.
Walsh
, J.-H.
Yang
, X.-G.
Gong
, L.
Sun
, P.-X.
Yang
, J.-H.
Chu
, and S.-H.
Wei
, Phys. Rev. B
83
, 125201
(2011
).55.
M. L.
Palsgaard
, A.
Crovetto
, T.
Gunst
, T.
Markussen
, O.
Hansen
, K.
Stokbro
, and M.
Brandbyge
, in 2016 International Conference on Simulation of Semiconductor Processes and Devices (SISPAD)
(IEEE, 2016
), pp. 377
–380
.56.
J.-S.
Park
, S.
Kim
, and A.
Walsh
, Phys. Rev. Mater.
2
, 014602
(2018
).57.
Y.-H.
Li
, X.
Gong
, and S.-H.
Wei
, Phys. Rev. B
73
, 245206
(2006
).© 2018 Author(s).
2018
Author(s)
You do not currently have access to this content.
