Probing femtosecond lattice displacement upon photo-carrier generation in lead halide perovskite

Nature Communications
Giovanni BatignaniTullio Scopigno

Abstract

Electronic properties and lattice vibrations are expected to be strongly correlated in metal-halide perovskites, due to the soft fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultrafast photoexcitation is necessary for understanding the optoelectronic behavior of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal vibrational modes of methylammonium lead-bromide perovskite under electronically resonant and non-resonant conditions. We identify two excited state coherent phonons at 89 and 106 cm-1, whose phases reveal a shift of the potential energy minimum upon ultrafast photocarrier generation. This indicates the transition to a new geometry, reached after approximately 90 fs, and fully equilibrated within the phonons lifetime of about 1 ps. Our results unambiguously prove that these modes drive the crystalline distortion occurring upon photo-excitation, demonstrating the presence of polaronic effects.

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Citations

Aug 20, 2019·Advanced Materials·Silvia G MottiAnnamaria Petrozza
Aug 6, 2020·The Journal of Chemical Physics·Nabeel S DahodWilliam A Tisdale
Jan 16, 2019·Nature Materials·Félix ThouinAjay Ram Srimath Kandada
Apr 4, 2020·Physical Review Letters·Bernhard ThalerMarkus Koch
Feb 10, 2019·The Journal of Chemical Physics·Keisuke YanoHisao Yanagi
Jan 26, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Zi-Wu WangZhiqing Li
Apr 21, 2021·Physical Chemistry Chemical Physics : PCCP·Lei GaoZhenhua Ni
Jun 3, 2021·Journal of the American Chemical Society·Oliviero CannelliGiulia F Mancini
Jun 29, 2021·Nano Letters·Emma H MassasaYehonadav Bekenstein
Nov 26, 2019·The Journal of Physical Chemistry Letters·Giovanni BatignaniTullio Scopigno
Aug 26, 2020·The Journal of Physical Chemistry Letters·Giovanni BatignaniTullio Scopigno
Mar 20, 2020·The Journal of Physical Chemistry Letters·Ajay Ram Srimath Kandada, Carlos Silva
Dec 16, 2020·Journal of the American Chemical Society·Feifan WangX-Y Zhu
Apr 2, 2020·The Journal of Physical Chemistry Letters·Guangjun NanClaudio Quarti
Jul 9, 2020·The Journal of Physical Chemistry Letters·Hiroto OkochiHisao Yanagi
Apr 4, 2020·The Journal of Physical Chemistry Letters·Kyle T MunsonJohn B Asbury
Sep 4, 2021·The Journal of Physical Chemistry Letters·Xijia ZhengArtem A Bakulin
Sep 18, 2021·The Journal of Physical Chemistry Letters·Giovanni BatignaniTullio Scopigno
Oct 8, 2021·Nature Communications·Claudiu M IaruAndrei Yu Silov
Nov 14, 2021·Advanced Materials·Jiaying WuJames R Durrant

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