Energy Landscape of Molecular Motion in Cubic Methylammonium Lead Iodide from First-Principles

被引：54

作者：

Bechtel, Jonathon S. ^{[1
]}

Seshadri, Ram ^{[1
,2
,3
]}

Van der Ven, Anton ^{[1
]}

机构：

[1] Univ Calif Santa Barbara, Dept Mat, Santa Barbara, CA 93106 USA

[2] Univ Calif Santa Barbara, Dept Chem & Biochem, Santa Barbara, CA 93106 USA

[3] Univ Calif Santa Barbara, Mat Res Lab, Santa Barbara, CA 93106 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2016年 / 120卷 / 23期

基金：

美国国家科学基金会;

关键词：

HYBRID HALIDE PEROVSKITE; PHASE-TRANSITIONS; ORGANIC CATIONS; SOLAR-CELL; CH3NH3PBI3; DYNAMICS; POLARIZATION; OCTAHEDRA; TRANSPORT; INTERPLAY;

D O I：

10.1021/acs.jpcc.6b03570

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Molecular A-cation dynamics are known to play a role in the electronic properties and structure Of hybrid organic-inorganic ABX(3) perovskites such as CH3NH3PbI3. We calculate the full energy landscape for rigid-body rotations and translations of the methylammonium cation in the cubic phase of CH3NH3PbI3. Energy barriers are calculated for combinations of molecular reorientation, on-axis rotation, and molecular translation within the unit cell. Alloying molecular. translations significantly stabilizes orientations along [100] which we attribute to strong N-H center dot center dot center dot I interactions between CH3NH3+ and the inorganic Pb-I host lattice.

引用

页码：12403 / 12410

页数：8

共 55 条

[1] Cation-Induced Band-Gap Tuning in Organohalide Perovskites: Interplay of Spin-Orbit Coupling and Octahedra Tilting [J].

Amat, Anna ;

Mosconi, Edoardo ;

Ronca, Enrico ;

Quarti, Claudio ;

Umari, Paolo ;

Nazeeruddin, Md. K. ;

Graetzel, Michael ;

De Angelis, Filippo .

NANO LETTERS, 2014, 14 (06) :3608-3616

[2] A combined single crystal neutron/X-ray diffraction and solid-state nuclear magnetic resonance study of the hybrid perovskites CH3NH3PbX3 (X = I, Br and Cl) [J].

Baikie, Tom ;

Barrow, Nathan S. ;

Fang, Yanan ;

Keenan, Philip J. ;

Slater, Peter R. ;

Piltz, Ross O. ;

Gutmann, Matthias ;

Mhaisalkar, Subodh G. ;

White, Tim J. .

JOURNAL OF MATERIALS CHEMISTRY A, 2015, 3 (17) :9298-9307

[3] Synthesis and crystal chemistry of the hybrid perovskite (CH3NH3) PbI3 for solid-state sensitised solar cell applications [J].

Baikie, Tom ;

Fang, Yanan ;

Kadro, Jeannette M. ;

Schreyer, Martin ;

Wei, Fengxia ;

Mhaisalkar, Subodh G. ;

Graetzel, Michael ;

White, Tim J. .

JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (18) :5628-5641

[4] Real-Time Observation of Organic Cation Reorientation in Methylammonium Lead Iodide Perovskites [J].

Bakulin, Artem A. ;

Selig, Oleg ;

Bakker, Huib J. ;

Rezus, Yves L. A. ;

Mueller, Christian ;

Glaser, Tobias ;

Lovrincic, Robert ;

Sun, Zhenhua ;

Chen, Zhuoying ;

Walsh, Aron ;

Frost, Jarvist M. ;

Jansen, Thomas L. C. .

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2015, 6 (18) :3663-3669

[5] Non-ferroelectric nature of the conductance hysteresis in CH3NH3PbI3 perovskite-based photovoltaic devices [J].

Beilsten-Edmands, J. ;

Eperon, G. E. ;

Johnson, R. D. ;

Snaith, H. J. ;

Radaelli, P. G. .

APPLIED PHYSICS LETTERS, 2015, 106 (17)

[6] Mechanical instabilities and structural phase transitions: The cubic to tetragonal transformation [J].

Bhattacharya, Jishnu ;

Van der Ven, Anton .

ACTA MATERIALIA, 2008, 56 (16) :4226-4232

[7] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[8] Ab Initio Calculations of Band Gaps and Absolute Band Positions of Polymorphs of RbPbI3 and CsPbI3: Implications for Main-Group Halide Perovskite Photovoltaics [J].

Brgoch, Jakoah ;

Lehner, Anna J. ;

Chabinyc, Michael ;

Seshadri, Ram .

JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (48) :27721-27727

[9] Relativistic quasiparticle self-consistent electronic structure of hybrid halide perovskite photovoltaic absorbers [J].

Brivio, Federico ;

Butler, Keith T. ;

Walsh, Aron ;

van Schilfgaarde, Mark .

PHYSICAL REVIEW B, 2014, 89 (15)

[10] Structural and electronic properties of hybrid perovskites for high-efficiency thin-film photovoltaics from first-principles [J].

Brivio, Federico ;

Walker, Alison B. ;

Walsh, Aron .

APL MATERIALS, 2013, 1 (04)

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