Static and Dynamic Disorder in Formamidinium Lead Bromide Single Crystals

Overview

Journal J Phys Chem Lett

Publisher American Chemical Society

Specialty Chemistry

Date 2023 Feb 1

PMID 36722023

Authors

Guy Reuveni

Yael Diskin-Posner

Christian Gehrmann

Shravan Godse

Giannis G Gkikas

Isaac Buchine

Sigalit Aharon

Roman Korobko

Constantinos C Stoumpos

David A Egger

Omer Yaffe

Affiliations

Soon will be listed here.

Abstract

We show that formamidinium-based crystals are distinct from methylammonium-based halide perovskite crystals because their inorganic sublattice exhibits intrinsic local static disorder that coexists with a well-defined average crystal structure. Our study combines terahertz-range Raman scattering with single-crystal X-ray diffraction and first-principles calculations to probe the evolution of inorganic sublattice dynamics with temperature in the range of 10-300 K. The temperature evolution of the Raman spectra shows that low-temperature, local static disorder strongly affects the crystal structural dynamics and phase transitions at higher temperatures.

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References

Zeiske S, Sandberg O, Zarrabi N, Wolff C, Raoufi M, Pena-Camargo F . Static Disorder in Lead Halide Perovskites. J Phys Chem Lett. 2022; 13(31):7280-7285. PMC: 9376950. DOI: 10.1021/acs.jpclett.2c01652. View

Cahen D, Lubomirsky I . Self-Repairing Energy Materials: Sine Qua Non for a Sustainable Future. Acc Chem Res. 2017; 50(3):573-576. DOI: 10.1021/acs.accounts.6b00560. View

Cohen A, Brenner T, Klarbring J, Sharma R, Fabini D, Korobko R . Diverging Expressions of Anharmonicity in Halide Perovskites. Adv Mater. 2022; 34(14):e2107932. DOI: 10.1002/adma.202107932. View

Stokes H, Kisi E, Hatch D, Howard C . Group-theoretical analysis of octahedral tilting in ferroelectric perovskites. Acta Crystallogr B. 2002; 58(Pt 6):934-8. DOI: 10.1107/s0108768102015756. View

Wang Y, Wu T, Barbaud J, Kong W, Cui D, Chen H . Stabilizing heterostructures of soft perovskite semiconductors. Science. 2019; 365(6454):687-691. DOI: 10.1126/science.aax8018. View

Taylor V, Tiwari D, Duchi M, Donaldson P, Clark I, Fermin D . Investigating the Role of the Organic Cation in Formamidinium Lead Iodide Perovskite Using Ultrafast Spectroscopy. J Phys Chem Lett. 2018; 9(4):895-901. DOI: 10.1021/acs.jpclett.7b03296. View

Yaffe O, Guo Y, Tan L, Egger D, Hull T, Stoumpos C . Local Polar Fluctuations in Lead Halide Perovskite Crystals. Phys Rev Lett. 2017; 118(13):136001. DOI: 10.1103/PhysRevLett.118.136001. View

Dunlap-Shohl W, Zhou Y, Padture N, Mitzi D . Synthetic Approaches for Halide Perovskite Thin Films. Chem Rev. 2018; 119(5):3193-3295. DOI: 10.1021/acs.chemrev.8b00318. View

Zhou H, Chen Q, Li G, Luo S, Song T, Duan H . Photovoltaics. Interface engineering of highly efficient perovskite solar cells. Science. 2014; 345(6196):542-6. DOI: 10.1126/science.1254050. View

10.

Maheshwari S, Fridriksson M, Seal S, Meyer J, Grozema F . The Relation between Rotational Dynamics of the Organic Cation and Phase Transitions in Hybrid Halide Perovskites. J Phys Chem C Nanomater Interfaces. 2019; 123(23):14652-14661. PMC: 6591771. DOI: 10.1021/acs.jpcc.9b02736. View

11.

Zhu X, Caicedo-Davila S, Gehrmann C, Egger D . Probing the Disorder Inside the Cubic Unit Cell of Halide Perovskites from First-Principles. ACS Appl Mater Interfaces. 2022; . DOI: 10.1021/acsami.1c23099. View

12.

Menahem M, Dai Z, Aharon S, Sharma R, Asher M, Diskin-Posner Y . Strongly Anharmonic Octahedral Tilting in Two-Dimensional Hybrid Halide Perovskites. ACS Nano. 2021; 15(6):10153-10162. PMC: 8223479. DOI: 10.1021/acsnano.1c02022. View

13.

Becker M, Kluner T, Wark M . Formation of hybrid ABX perovskite compounds for solar cell application: first-principles calculations of effective ionic radii and determination of tolerance factors. Dalton Trans. 2017; 46(11):3500-3509. DOI: 10.1039/c6dt04796c. View

14.

Keshavarz M, Ottesen M, Wiedmann S, Wharmby M, Kuchler R, Yuan H . Tracking Structural Phase Transitions in Lead-Halide Perovskites by Means of Thermal Expansion. Adv Mater. 2019; 31(24):e1900521. DOI: 10.1002/adma.201900521. View

15.

Gratzel M . The light and shade of perovskite solar cells. Nat Mater. 2014; 13(9):838-42. DOI: 10.1038/nmat4065. View

16.

Klarbring J, Hellman O, Abrikosov I, Simak S . Anharmonicity and Ultralow Thermal Conductivity in Lead-Free Halide Double Perovskites. Phys Rev Lett. 2020; 125(4):045701. DOI: 10.1103/PhysRevLett.125.045701. View

17.

Ricciardulli A, Yang S, Smet J, Saliba M . Emerging perovskite monolayers. Nat Mater. 2021; 20(10):1325-1336. DOI: 10.1038/s41563-021-01029-9. View

18.

Ledinsky M, Schonfeldova T, Holovsky J, Aydin E, Hajkova Z, Landova L . Temperature Dependence of the Urbach Energy in Lead Iodide Perovskites. J Phys Chem Lett. 2019; 10(6):1368-1373. DOI: 10.1021/acs.jpclett.9b00138. View

19.

Tan Z, Saberi Moghaddam R, Lai M, Docampo P, Higler R, Deschler F . Bright light-emitting diodes based on organometal halide perovskite. Nat Nanotechnol. 2014; 9(9):687-92. DOI: 10.1038/nnano.2014.149. View

20.

Kresse , Furthmuller . Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B Condens Matter. 1996; 54(16):11169-11186. DOI: 10.1103/physrevb.54.11169. View