Polar Rotor Scattering As Atomic-level Origin of Low Mobility and Thermal Conductivity of Perovskite CHNHPbI

Overview

Journal Nat Commun

Specialty Biology

Date 2017 Jul 1

PMID 28665407

Citations 24

Authors

Bing Li

Yukinobu Kawakita

Yucheng Liu

Mingchao Wang

Masato Matsuura

Kaoru Shibata

Seiko Ohira-Kawamura

Takeshi Yamada

Shangchao Lin

Kenji Nakajima

Shengzhong Frank Liu

Affiliations

Soon will be listed here.

Abstract

Perovskite CHNHPbI exhibits outstanding photovoltaic performances, but the understanding of the atomic motions remains inadequate even though they take a fundamental role in transport properties. Here, we present a complete atomic dynamic picture consisting of molecular jumping rotational modes and phonons, which is established by carrying out high-resolution time-of-flight quasi-elastic and inelastic neutron scattering measurements in a wide energy window ranging from 0.0036 to 54 meV on a large single crystal sample, respectively. The ultrafast orientational disorder of molecular dipoles, activated at ∼165 K, acts as an additional scattering source for optical phonons as well as for charge carriers. It is revealed that acoustic phonons dominate the thermal transport, rather than optical phonons due to sub-picosecond lifetimes. These microscopic insights provide a solid standing point, on which perovskite solar cells can be understood more accurately and their performances are perhaps further optimized.

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References

Whitfield P, Herron N, Guise W, Page K, Cheng Y, Milas I . Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide. Sci Rep. 2016; 6:35685. PMC: 5073364. DOI: 10.1038/srep35685. View

Zhu X, Podzorov V . Charge Carriers in Hybrid Organic-Inorganic Lead Halide Perovskites Might Be Protected as Large Polarons. J Phys Chem Lett. 2015; 6(23):4758-61. DOI: 10.1021/acs.jpclett.5b02462. View

Christians J, Miranda Herrera P, Kamat P . Transformation of the excited state and photovoltaic efficiency of CH3NH3PbI3 perovskite upon controlled exposure to humidified air. J Am Chem Soc. 2015; 137(4):1530-8. DOI: 10.1021/ja511132a. View

Mattoni A, Filippetti A, Saba M, Caddeo C, Delugas P . Temperature Evolution of Methylammonium Trihalide Vibrations at the Atomic Scale. J Phys Chem Lett. 2016; 7(3):529-35. DOI: 10.1021/acs.jpclett.5b02546. View

Yang J, Wen X, Xia H, Sheng R, Ma Q, Kim J . Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites. Nat Commun. 2017; 8:14120. PMC: 5263885. DOI: 10.1038/ncomms14120. View

Liu Y, Zhang Y, Yang Z, Yang D, Ren X, Pang L . Thinness- and Shape-Controlled Growth for Ultrathin Single-Crystalline Perovskite Wafers for Mass Production of Superior Photoelectronic Devices. Adv Mater. 2016; 28(41):9204-9209. DOI: 10.1002/adma.201601995. View

Ponder J, Case D . Force fields for protein simulations. Adv Protein Chem. 2003; 66:27-85. DOI: 10.1016/s0065-3233(03)66002-x. View

Yang W, Noh J, Jeon N, Kim Y, Ryu S, Seo J . SOLAR CELLS. High-performance photovoltaic perovskite layers fabricated through intramolecular exchange. Science. 2015; 348(6240):1234-7. DOI: 10.1126/science.aaa9272. View

Yu J, Wang M, Lin S . Probing the Soft and Nanoductile Mechanical Nature of Single and Polycrystalline Organic-Inorganic Hybrid Perovskites for Flexible Functional Devices. ACS Nano. 2016; 10(12):11044-11057. DOI: 10.1021/acsnano.6b05913. View

10.

Leguy A, Goni A, Frost J, Skelton J, Brivio F, Rodriguez-Martinez X . Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites. Phys Chem Chem Phys. 2016; 18(39):27051-27066. DOI: 10.1039/c6cp03474h. View

11.

Filippetti A, Mattoni A, Caddeo C, Saba M, Delugas P . Low electron-polar optical phonon scattering as a fundamental aspect of carrier mobility in methylammonium lead halide CH3NH3PbI3 perovskites. Phys Chem Chem Phys. 2016; 18(22):15352-62. DOI: 10.1039/c6cp01402j. View

12.

Karakus M, Jensen S, DAngelo F, Turchinovich D, Bonn M, Canovas E . Phonon-Electron Scattering Limits Free Charge Mobility in Methylammonium Lead Iodide Perovskites. J Phys Chem Lett. 2015; 6(24):4991-6. DOI: 10.1021/acs.jpclett.5b02485. View

13.

Shi D, Adinolfi V, Comin R, Yuan M, Alarousu E, Buin A . Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals. Science. 2015; 347(6221):519-22. DOI: 10.1126/science.aaa2725. View

14.

Mante P, Stoumpos C, Kanatzidis M, Yartsev A . Electron-acoustic phonon coupling in single crystal CHNHPbI perovskites revealed by coherent acoustic phonons. Nat Commun. 2017; 8:14398. PMC: 5309855. DOI: 10.1038/ncomms14398. View

15.

Frost J, Butler K, Brivio F, Hendon C, van Schilfgaarde M, Walsh A . Atomistic origins of high-performance in hybrid halide perovskite solar cells. Nano Lett. 2014; 14(5):2584-90. PMC: 4022647. DOI: 10.1021/nl500390f. View

16.

Kojima A, Teshima K, Shirai Y, Miyasaka T . Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. J Am Chem Soc. 2009; 131(17):6050-1. DOI: 10.1021/ja809598r. View

17.

Pisoni A, Jacimovic J, Barisic O, Spina M, Gaal R, Forro L . Ultra-Low Thermal Conductivity in Organic-Inorganic Hybrid Perovskite CH3NH3PbI3. J Phys Chem Lett. 2015; 5(14):2488-92. DOI: 10.1021/jz5012109. View

18.

Wright A, Verdi C, Milot R, Eperon G, Perez-Osorio M, Snaith H . Electron-phonon coupling in hybrid lead halide perovskites. Nat Commun. 2016; 7. PMC: 4894981. DOI: 10.1038/ncomms11755. View

19.

Lin S, Buehler M . The effect of non-covalent functionalization on the thermal conductance of graphene/organic interfaces. Nanotechnology. 2013; 24(16):165702. DOI: 10.1088/0957-4484/24/16/165702. View

20.

Dong Q, Fang Y, Shao Y, Mulligan P, Qiu J, Cao L . Solar cells. Electron-hole diffusion lengths > 175 μm in solution-grown CH3NH3PbI3 single crystals. Science. 2015; 347(6225):967-70. DOI: 10.1126/science.aaa5760. View