Thin-film solar cells based on Methylammonium triiodideplumbate (CH3NH3PbI3) halide perovskites have recently shown remarkable performance. First-principle calculations show that CH3NH3PbI3 has unusual defect physics: (i) Different from common p-type thin-film solar cell absorbers, it exhibits flexible conductivity from good p-type, intrinsic to good n-type depending on the growth conditions; (ii) Dominant intrinsic defects create only shallow levels, which partially explain the long electron-hole diffusion length and high open-circuit voltage in solar cell. The unusual defect properties can be attributed to the strong Pb lone-pair s orbital and I p orbital antibonding coupling and the high ionicity of CH3NH3PbI3.

1.
A.
Kojima
,
K.
Teshima
,
Y.
Shirai
, and
T.
Miyasaka
,
J. Am. Chem. Soc.
131
,
6050
(
2009
).
2.
I.
Chung
,
B.
Lee
,
J. Q.
He
,
R. P. H.
Chang
, and
M. G.
Kanatzidis
,
Nature
485
,
486
(
2012
).
3.
M. M.
Lee
,
J.
Teuscher
,
T.
Miyasaka
,
T. N.
Murakami
, and
H. J.
Snaith
,
Science
338
,
643
(
2012
).
4.
J.
Burschka
,
N.
Pellet
,
S. J.
Moon
,
R.
Humphry-Baker
,
P.
Gao
,
M. K.
Nazeeruddin
, and
M.
Gratzel
,
Nature
499
,
316
(
2013
).
5.
M. Z.
Liu
,
M. B.
Johnston
, and
H. J.
Snaith
,
Nature
501
,
395
(
2013
).
6.
J. H.
Noh
,
S. H.
Im
,
J. H.
Heo
,
T. N.
Mandal
, and
S. I.
Seok
,
Nano Lett.
13
,
1764
(
2013
).
7.
N. G.
Park
,
J. Phys. Chem. Lett.
4
,
2423
(
2013
).
8.
G. C.
Xing
,
N.
Mathews
,
S. Y.
Sun
,
S. S.
Lim
,
Y. M.
Lam
,
M.
Gratzel
,
S.
Mhaisalkar
, and
T. C.
Sum
,
Science
342
,
344
(
2013
).
9.
S. D.
Stranks
,
G. E.
Eperon
,
G.
Grancini
,
C.
Menelaou
,
M. J. P.
Alcocer
,
T.
Leijtens
,
L. M.
Herz
,
A.
Petrozza
, and
H. J.
Snaith
,
Science
342
,
341
(
2013
).
10.
W.
Schokley
and
H. J.
Queisser
,
J. Appl. Phys.
32
,
510
(
1961
).
11.
G.
Kresse
and
J.
Furthmuller
,
Phys. Rev. B
54
,
11169
(
1996
).
12.
L. P. J.
Even
,
J.-M.
Jancu
, and
C.
Katan
,
J. Phys. Chem. Lett.
4
,
2999
(
2013
).
13.
E.
Mosconi
,
A.
Amat
,
M. K.
Nazeeruddin
,
M.
Gratzel
, and
F.
De Angelis
,
J. Phys. Chem. C
117
,
13902
(
2013
).
14.
M. A.
Pena
and
J. L. G.
Fierro
,
Chem. Rev.
101
,
1981
(
2001
).
15.
F.
Brivio
,
A. B.
Walker
, and
A.
Walsh
,
APL Materials
1
,
042111
(
2013
).
16.
Y.
Wang
,
T.
Gould
,
J.
Dobson
,
H.
Zhang
,
H.
Yang
,
X.
Yao
, and
H.
Zhao
, “
Density functional theory analysis of structural and electronic properties of orthorhombic perovskite CH3NH3PbI3
,”
Phys. Chem. Chem. Phys
16
,
1424
1429
(
2014
).
17.
S. H.
Wei
,
Computational Materials Science
30
,
337
(
2004
).
18.
S. B.
Zhang
,
S. H.
Wei
,
A.
Zunger
, and
H.
Katayama-Yoshida
,
Phys Rev B
57
,
9642
(
1998
).
19.
S. Y.
Chen
,
X. G.
Gong
,
A.
Walsh
, and
S. H.
Wei
,
Appl. Phys. Lett.
94
,
041903
(
2009
).
20.
A.
Polizzotti
,
I. L.
Repins
,
R.
Noufi
,
S. H.
Wei
, and
D. B.
Mitzi
,
Energy Environ. Sci.
6
,
3171
(
2013
).
21.
W. J.
Yin
,
S. H.
Wei
,
M. M.
Al-Jassim
, and
Y. F.
Yan
,
Appl. Phys. Lett.
99
,
142109
(
2011
).
22.
C. S.
Stoumpos
,
C. D.
Malliakas
, and
M. G.
Kanatzidis
,
Inorg. Chem.
52
,
9019
(
2013
).
23.
Y.
Zhao
and
K
Zhu
,
J. Phys. Chem. Lett.
4
,
2880
(
2013
).
24.
M. H.
Kumar
,
N.
Yantara
,
S.
Dharani
,
M.
Graetzel
,
S.
Mhaisalkar
,
P. P.
Boix
, and
N.
Mathews
,
Chem. Commun.
49
,
11089
(
2013
).
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