Interfaces between the absorbing perovskite and transporting layers are gaining attention as the key locus that governs solar cell operation and long term performance. The interplay of ionic and electronic processes, along with the asymmetrical architecture of any solar cell, makes the interpretation of electrical measurements always inconclusive. A strategy to progress in relating electric responses, operating mechanisms, and device architecture relies upon simplifying the probing structure. Macroscopic CH3NH3PbBr3 single crystals with symmetrical contacts are tested by means of long-time current transient and impedance spectroscopy. It is observed that interfaces govern carrier injection to (and extraction from) perovskite layers through an inductive (negative capacitance) mechanism with a response time in the range of ∼1100 s under dark conditions and inert atmosphere. Current transient exhibits a slow recovering after the occurrence of an undershoot, signaling a complex carrier dynamics which involves changes in surface state occupancy.

1.
J. M.
Azpiroz
,
E.
Mosconi
,
J.
Bisquert
, and
F.
De Angelis
,
Energy Environ. Sci.
8
,
2118
(
2015
).
2.
T.-Y.
Yang
,
G.
Gregori
,
N.
Pellet
,
M.
Grätzel
, and
J.
Maier
,
Angew. Chem. Int. Ed.
54
,
7905
(
2015
).
3.
C.
Eames
,
J. M.
Frost
,
P. R.
Barnes
,
B. C.
O'Regan
,
A.
Walsh
, and
M. S.
Islam
,
Nat. Commun.
6
,
7497
(
2015
).
4.
N.
Vicente
and
G.
Garcia-Belmonte
,
Adv. Energy Mater.
7
,
1700710
(
2017
).
5.
Z.
Li
,
C.
Xiao
,
Y.
Yang
,
S.
Harvey
,
D. H.
Kim
,
J. A.
Christians
,
M.
Yang
,
P.
Schulz
,
S. U.
Nanayakkara
,
C.-S.
Jiang
,
J. M.
Luther
,
J.
Berry
,
M. C.
Beard
,
M. M.
Al-Jassim
, and
K.
Zhu
,
Energy Environ. Sci.
10
,
1234
(
2017
).
6.
J.
Carrillo
,
A.
Guerrero
,
S.
Rahimnejad
,
O.
Almora
,
I.
Zarazua
,
E.
Mas-Marza
,
J.
Bisquert
, and
G.
Garcia-Belmonte
,
Adv. Energy Mater.
6
,
1502246
(
2016
).
7.
S.
Cacovich
,
L.
Ciná
,
F.
Matteocci
,
G.
Divitini
,
P. A.
Midgley
,
A. D.
Carlob
, and
C.
Ducati
,
Nanoscale
9
,
4700
(
2017
).
8.
K.
Domanski
,
J.-P.
Correa-Baena
,
N.
Mine
,
M. K.
Nazeeruddin
,
A.
Abate
,
M.
Saliba
,
W.
Tress
,
A.
Hagfeldt
, and
M.
Grätzel
,
ACS Nano
10
,
6306
6314
(
2016
).
9.
C.
Li
,
S.
Tscheuschner
,
F.
Paulus
,
P. E.
Hopkinson
,
J.
Kießling
,
A.
Köhler
,
Y.
Vaynzof
, and
S.
Huettner
,
Adv. Mater.
28
,
2446
(
2016
).
10.
B.
Chen
,
M.
Yang
,
X.
Zheng
,
C.
Wu
,
W.
Li
,
Y.
Yan
,
J.
Bisquert
,
G.
Garcia-Belmonte
,
K.
Zhu
, and
S.
Priya
,
J. Phys. Chem. Lett.
6
,
4693
4700
(
2015
).
11.
P.
Lopez-Varo
,
J. A.
Jime´nez-Tejada
,
M.
García-Rosell
,
J. A.
Anta
,
S.
Ravishankar
,
A.
Bou
, and
J.
Bisquert
,
ACS Energy Lett.
2
,
1450
1453
(
2017
).
12.
E. L.
Unger
,
E. T.
Hoke
,
C. D.
Bailie
,
W. H.
Nguyen
,
A. R.
Bowring
,
T.
Heumuller
,
M. G.
Christoforo
, and
M. D.
McGehee
,
Energy Environ. Sci.
7
,
3690
(
2014
).
13.
W.
Tress
,
N.
Marinova
,
T.
Moehl
,
S. M.
Zakeeruddin
,
M. K.
Nazeeruddin
, and
M.
Gratzel
,
Energy Environ. Sci.
8
,
995
(
2015
).
14.
G.
Garcia-Belmonte
and
J.
Bisquert
,
ACS Energy Lett.
1
,
683
688
(
2016
).
15.
S.
Meloni
,
T.
Moehl
,
W.
Tress
,
M.
Franckevičius
,
M.
Saliba
,
Y. H.
Lee
,
P.
Gao
,
M. K.
Nazeeruddin
,
S. M.
Zakeeruddin
,
U.
Rothlisberger
, and
M.
Graetzel
,
Nat. Commun.
7
,
10334
(
2016
).
16.
O.
Almora
,
I.
Zarazua
,
E.
Mas-Marza
,
I.
Mora-Sero
,
J.
Bisquert
, and
G.
Garcia-Belmonte
,
J. Phys. Chem. Lett.
6
,
1645
(
2015
).
17.
O.
Almora
,
A.
Guerrero
, and
G.
Garcia-Belmonte
,
Appl. Phys. Lett.
108
,
043903
(
2016
).
18.
I.
Zarazua
,
J.
Bisquert
, and
G.
Garcia-Belmonte
,
J. Phys. Chem. Lett.
7
,
525
528
(
2016
).
19.
I.
Zarazua
,
G.
Han
,
P. P.
Boix
,
S.
Mhaisalkar
,
F.
Fabregat-Santiago
,
I.
Mora-Seró
,
J.
Bisquert
, and
G.
Garcia-Belmonte
,
J. Phys. Chem. Lett.
7
,
5105
5113
(
2016
).
20.
E.
Ghahremanirad
,
A.
Bou
,
S.
Olyaee
, and
J.
Bisquert
,
J. Phys. Chem. Lett.
8
,
1402
1406
(
2017
).
21.
Y.
Liu
,
Z.
Yang
,
D.
Cui
,
X.
Ren
,
J.
Sun
,
X.
Liu
,
J.
Zhang
,
Q.
Wei
,
H.
Fan
,
F.
Yu
,
X.
Zhang
,
C.
Zhao
, and
S. F.
Liu
,
Adv. Mater.
27
,
5176
(
2015
).
22.
W.
Peng
,
L.
Wang
,
B.
Murali
,
K.-T.
Ho
,
A.
Bera
,
N.
Cho
,
C.-F.
Kang
,
V. M.
Burlakov
,
J.
Pan
,
L.
Sinatra
,
C.
Ma
,
W.
Xu
,
D.
Shi
,
E.
Alarousu
,
A.
Goriely
,
J.-H.
He
,
O. F.
Mohammed
,
T.
Wu
, and
O. M.
Bakr
,
Adv. Mater.
28
,
3383
(
2016
).
23.
M. I.
Saidaminov
,
A. L.
Abdelhady
,
B.
Murali
,
E.
Alarousu
,
V. M.
Burlakov
,
W.
Peng
,
I.
Dursun
,
L.
Wang
,
Y.
He
,
G.
Maculan
,
A.
Goriely
,
T.
Wu
,
O. F.
Mohammed
, and
O. M.
Bakr
,
Nat. Commun.
6
,
7586
(
2015
).
24.
A.
Senocrate
,
I.
Moudrakovski
,
G. Y.
Kim
,
T.-Y.
Yang
,
G.
Gregori
,
M.
Grätzel
, and
J.
Maier
,
Angew. Chem. Int. Ed.
56
,
7755
7759
(
2017
).
25.
R. S.
Sanchez
,
V.
Gonzalez-Pedro
,
J.-W.
Lee
,
N.-G.
Park
,
Y. S.
Kang
,
I.
Mora-Sero
, and
J.
Bisquert
,
J. Phys. Chem. Lett.
5
,
2357
(
2014
).
26.
Q.
Tai
,
P.
You
,
H.
Sang
,
Z.
Liu
,
C.
Hu
,
H. L. W.
Chan
, and
F.
Yan
,
Nat. Commun.
7
,
11105
(
2016
).
27.
A.
Guerrero
,
G.
Garcia-Belmonte
,
I.
Mora-Sero
,
J.
Bisquert
,
Y. S.
Kang
,
T. J.
Jacobsson
,
J.-P.
Correa-Baena
, and
A.
Hagfeldt
,
J. Phys. Chem. C
120
,
8023
8032
(
2016
).
28.
A.
Zohar
,
N.
Kedem
,
I.
Levine
,
D.
Zohar
,
A.
Vilan
,
D.
Ehre
,
G.
Hodes
, and
D.
Cahen
,
J. Phys. Chem. Lett.
7
,
191
197
(
2016
).
29.
E.
Radvanyi
,
K. V.
Havenbergh
,
W.
Porcher
,
S.
Jouanneau
,
J.-S.
Bridel
,
S.
Put
, and
S.
Franger
,
Electrochim. Acta
137
,
751
(
2014
).
30.
J.
Bisquert
,
G.
Garcia-Belmonte
,
Á.
Pitarch
, and
H. J.
Bolink
,
Chem. Lett.
422
,
184
(
2006
).
31.
G.
Garcia-Belmonte
,
H. J.
Bolink
, and
J.
Bisquert
,
Phys. Rev. B
75
,
085316
(
2007
).

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