Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices

Peijun Guo, Arun Mannodi-Kanakkithodi, Jue Gong, Yi Xia, Constantinos C. Stoumpos, Duyen H. Cao, Benjamin T. Diroll, John B. Ketterson, Gary P. Wiederrecht, Tao Xu, Maria K. Y. Chan, Mercouri G. Kanatzidis and Richard D. Schaller ()
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Peijun Guo: Argonne National Laboratory
Arun Mannodi-Kanakkithodi: Argonne National Laboratory
Jue Gong: Northern Illinois University
Yi Xia: Argonne National Laboratory
Constantinos C. Stoumpos: Northwestern University
Duyen H. Cao: Argonne National Laboratory
Benjamin T. Diroll: Argonne National Laboratory
John B. Ketterson: Northwestern University
Gary P. Wiederrecht: Argonne National Laboratory
Tao Xu: Northern Illinois University
Maria K. Y. Chan: Argonne National Laboratory
Mercouri G. Kanatzidis: Northwestern University
Richard D. Schaller: Argonne National Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Organic-inorganic hybrid perovskites such as methylammonium lead iodide (CH3NH3PbI3) are game-changing semiconductors for solar cells and light-emitting devices owing to their defect tolerance and exceptionally long carrier lifetimes and diffusion lengths. Determining whether the dynamically disordered organic cations with large dipole moment benefit the optoelectronic properties of CH3NH3PbI3 has been an outstanding challenge. Herein, via transient absorption measurements employing an infrared pump pulse tuned to a methylammonium vibration, we observe slow, nanosecond-long thermal dissipation from the selectively excited organic mode to the inorganic sublattice. The resulting transient electronic signatures, during the period of thermal-nonequilibrium when the induced thermal motions are mostly concentrated on the organic sublattice, reveal that the induced atomic motions of the organic cations do not alter the absorption or the photoluminescence response of CH3NH3PbI3, beyond thermal effects. Our results suggest that the attractive optoelectronic properties of CH3NH3PbI3 mainly derive from the inorganic lead-halide framework.

Date: 2019
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DOI: 10.1038/s41467-019-08363-2

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