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, Richard D Schaller

Research output: Contribution to journalArticle

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.

Original languageEnglish
Article number482
JournalNature Communications
Volume10
Issue number1
DOIs
Publication statusPublished - Dec 1 2019

Fingerprint

Iodides
iodides
sublattices
Hot Temperature
Pumps
pumps
Infrared radiation
cations
Optoelectronic devices
Cations
probes
games
perovskites
carrier lifetime
diffusion length
electronics
halides
temperature effects
dipole moments
Carrier lifetime

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices. / Guo, Peijun; Mannodi-Kanakkithodi, Arun; Gong, Jue; Xia, Yi; Stoumpos, Constantinos C.; Cao, Duyen H.; Diroll, Benjamin T.; Ketterson, John B.; Wiederrecht, Gary P.; Xu, Tao; Chan, Maria K.Y.; Kanatzidis, Mercouri G; Schaller, Richard D.

In: Nature Communications, Vol. 10, No. 1, 482, 01.12.2019.

Research output: Contribution to journalArticle

Guo, P, Mannodi-Kanakkithodi, A, Gong, J, Xia, Y, Stoumpos, CC, Cao, DH, Diroll, BT, Ketterson, JB, Wiederrecht, GP, Xu, T, Chan, MKY, Kanatzidis, MG & Schaller, RD 2019, 'Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices', Nature Communications, vol. 10, no. 1, 482. https://doi.org/10.1038/s41467-019-08363-2
Guo, Peijun ; Mannodi-Kanakkithodi, Arun ; Gong, Jue ; Xia, Yi ; Stoumpos, Constantinos C. ; Cao, Duyen H. ; Diroll, Benjamin T. ; Ketterson, John B. ; Wiederrecht, Gary P. ; Xu, Tao ; Chan, Maria K.Y. ; Kanatzidis, Mercouri G ; Schaller, Richard D. / Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices. In: Nature Communications. 2019 ; Vol. 10, No. 1.
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