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Slow thermal equilibration in methylammonium lead iodide revealed by transient mid-infrared spectroscopy

Journal Article · · Nature Communications
 [1];  [2];  [3];  [3];  [4];  [3];  [4];  [4];  [4];  [3];  [3];  [5];  [6]
  1. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; DOE/OSTI
  2. Northern Illinois Univ., DeKalb, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
  4. Northwestern Univ., Evanston, IL (United States)
  5. Northern Illinois Univ., DeKalb, IL (United States); Northwestern Univ., Evanston, IL (United States)
  6. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States)
Hybrid organic–inorganic perovskites are emerging semiconductors for cheap and efficient photovoltaics and light-emitting devices. Different from conventional inorganic semiconductors, hybrid perovskites consist of coexisting organic and inorganic sub-lattices, which present disparate atomic masses and bond strengths. The nanoscopic interpenetration of these disparate components, which lack strong electronic and vibrational coupling, presents fundamental challenges to the understanding of charge and heat dissipation. Here we study phonon population and equilibration processes in methylammonium lead iodide (MAPbI3) by transiently probing the vibrational modes of the organic sub-lattice following above-bandgap optical excitation. We observe inter-sub-lattice thermal equilibration on timescales ranging from hundreds of pico seconds to a couple of nanoseconds. As supported by a two temperature model based on first-principles calculations, the slow thermal equilibration is attributable to the sequential phonon populations of the inorganic and organic sub-lattices, respectively. The observed long-lasting thermal non-equilibrium offers insights into thermal transport and heat management of the emergent hybrid material class.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Univ. of California, Santa Barbara, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; SC0012541
OSTI ID:
1624106
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (6)

Photoinduced, reversible phase transitions in all-inorganic perovskite nanocrystals journal January 2019
Thermal equilibration in infinite harmonic crystals journal March 2019
Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices journal January 2019
Hot carrier solar cells and the potential of perovskites for breaking the Shockley–Queisser limit journal January 2019
Thermochromism of bromotellurates( iv ): experimental insights journal January 2019
Structural origins of the electronic properties of materials via time-resolved infrared spectroscopy journal January 2019

Figures / Tables (5)


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