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

Author

Listed:
  • Giovanni Batignani

    (Università di Roma “La Sapienza”)

  • Giuseppe Fumero

    (Università di Roma “La Sapienza”
    Università di Roma “La Sapienza”)

  • Ajay Ram Srimath Kandada

    (Istituto Italiano di Tecnologia)

  • Giulio Cerullo

    (Politecnico di Milano)

  • Marina Gandini

    (Istituto Italiano di Tecnologia
    Politecnico di Milano)

  • Carino Ferrante

    (Università di Roma “La Sapienza”
    Center for Life Nano Science @Sapienza)

  • Annamaria Petrozza

    (Istituto Italiano di Tecnologia)

  • Tullio Scopigno

    (Università di Roma “La Sapienza”
    Center for Life Nano Science @Sapienza)

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.

Suggested Citation

  • Giovanni Batignani & Giuseppe Fumero & Ajay Ram Srimath Kandada & Giulio Cerullo & Marina Gandini & Carino Ferrante & Annamaria Petrozza & Tullio Scopigno, 2018. "Probing femtosecond lattice displacement upon photo-carrier generation in lead halide perovskite," Nature Communications, Nature, vol. 9(1), pages 1-5, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04367-6
    DOI: 10.1038/s41467-018-04367-6
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    Cited by:

    1. Giovanni Batignani & Emanuele Mai & Giuseppe Fumero & Shaul Mukamel & Tullio Scopigno, 2022. "Absolute excited state molecular geometries revealed by resonance Raman signals," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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