TY - JOUR
T1 - Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices
AU - Guo, Peijun
AU - Mannodi-Kanakkithodi, Arun
AU - Gong, Jue
AU - Xia, Yi
AU - Stoumpos, Constantinos C.
AU - Cao, Duyen H.
AU - Diroll, Benjamin T.
AU - Ketterson, John B.
AU - Wiederrecht, Gary P.
AU - Xu, Tao
AU - Chan, Maria K.Y.
AU - Kanatzidis, Mercouri G.
AU - Schaller, Richard D.
N1 - Publisher Copyright:
© 2019, This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply.
PY - 2019/12/1
Y1 - 2019/12/1
N2 - Organic-inorganic hybrid perovskites such as methylammonium lead iodide (CH 3 NH 3 PbI 3 ) 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 CH 3 NH 3 PbI 3 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 CH 3 NH 3 PbI 3 , beyond thermal effects. Our results suggest that the attractive optoelectronic properties of CH 3 NH 3 PbI 3 mainly derive from the inorganic lead-halide framework.
AB - Organic-inorganic hybrid perovskites such as methylammonium lead iodide (CH 3 NH 3 PbI 3 ) 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 CH 3 NH 3 PbI 3 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 CH 3 NH 3 PbI 3 , beyond thermal effects. Our results suggest that the attractive optoelectronic properties of CH 3 NH 3 PbI 3 mainly derive from the inorganic lead-halide framework.
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U2 - 10.1038/s41467-019-08363-2
DO - 10.1038/s41467-019-08363-2
M3 - Article
C2 - 30696817
AN - SCOPUS:85060749798
SN - 2041-1723
VL - 10
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 482
ER -