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

Giovanni Batignani, Giuseppe Fumero, Ajay Ram Srimath Kandada, Giulio Cerullo, Marina Gandini, Carino Ferrante, Annamaria Petrozza () and Tullio Scopigno ()
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Giovanni Batignani: Università di Roma “La Sapienza”
Giuseppe Fumero: Università di Roma “La Sapienza”
Ajay Ram Srimath Kandada: Istituto Italiano di Tecnologia
Giulio Cerullo: Politecnico di Milano
Marina Gandini: Istituto Italiano di Tecnologia
Carino Ferrante: Università di Roma “La Sapienza”
Annamaria Petrozza: Istituto Italiano di Tecnologia
Tullio Scopigno: Università di Roma “La Sapienza”

Nature Communications, 2018, vol. 9, issue 1, 1-5

Abstract: 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.

Date: 2018
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DOI: 10.1038/s41467-018-04367-6

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