Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite

Myeongkee Park, Amanda J. Neukirch, Sebastian E. Reyes-Lillo, Minliang Lai, Scott R. Ellis, Daniel Dietze, Jeffrey B. Neaton, Peidong Yang, Sergei Tretiak, Richard A. Mathies

Resultado de la investigación: Article

25 Citas (Scopus)

Resumen

Hybrid organic-inorganic perovskites have attractive optoelectronic properties including exceptional solar cell performance. The improved properties of perovskites have been attributed to polaronic effects involving stabilization of localized charge character by structural deformations and polarizations. Here we examine the Pb-I structural dynamics leading to polaron formation in methylammonium lead iodide perovskite by transient absorption, time-domain Raman spectroscopy, and density functional theory. Methylammonium lead iodide perovskite exhibits excited-state coherent nuclear wave packets oscillating at ~20, 43, and 75 cm-1 which involve skeletal bending, in-plane bending, and c-axis stretching of the I-Pb-I bonds, respectively. The amplitudes of these wave packet motions report on the magnitude of the excited-state structural changes, in particular, the formation of a bent and elongated octahedral PbI6 4- geometry. We have predicted the excited-state geometry and structural changes between the neutral and polaron states using a normal-mode projection method, which supports and rationalizes the experimental results. This study reveals the polaron formation via nuclear dynamics that may be important for efficient charge separation.

Idioma originalEnglish
Número de artículo2525
PublicaciónNature Communications
Volumen9
N.º1
DOI
EstadoPublished - 1 dic 2018

Huella dactilar

Gene Conversion
Iodides
Excited states
iodides
Wave packets
perovskites
wave packets
excitation
dynamic structural analysis
Geometry
Raman Spectrum Analysis
Structural dynamics
polarization (charge separation)
geometry
Optoelectronic devices
Stretching
Density functional theory
Raman spectroscopy
Solar cells
Stabilization

ASJC Scopus subject areas

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

Citar esto

Park, Myeongkee ; Neukirch, Amanda J. ; Reyes-Lillo, Sebastian E. ; Lai, Minliang ; Ellis, Scott R. ; Dietze, Daniel ; Neaton, Jeffrey B. ; Yang, Peidong ; Tretiak, Sergei ; Mathies, Richard A. / Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite. En: Nature Communications. 2018 ; Vol. 9, N.º 1.
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abstract = "Hybrid organic-inorganic perovskites have attractive optoelectronic properties including exceptional solar cell performance. The improved properties of perovskites have been attributed to polaronic effects involving stabilization of localized charge character by structural deformations and polarizations. Here we examine the Pb-I structural dynamics leading to polaron formation in methylammonium lead iodide perovskite by transient absorption, time-domain Raman spectroscopy, and density functional theory. Methylammonium lead iodide perovskite exhibits excited-state coherent nuclear wave packets oscillating at ~20, 43, and 75 cm-1 which involve skeletal bending, in-plane bending, and c-axis stretching of the I-Pb-I bonds, respectively. The amplitudes of these wave packet motions report on the magnitude of the excited-state structural changes, in particular, the formation of a bent and elongated octahedral PbI6 4- geometry. We have predicted the excited-state geometry and structural changes between the neutral and polaron states using a normal-mode projection method, which supports and rationalizes the experimental results. This study reveals the polaron formation via nuclear dynamics that may be important for efficient charge separation.",
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Park, M, Neukirch, AJ, Reyes-Lillo, SE, Lai, M, Ellis, SR, Dietze, D, Neaton, JB, Yang, P, Tretiak, S & Mathies, RA 2018, 'Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite', Nature Communications, vol. 9, n.º 1, 2525. https://doi.org/10.1038/s41467-018-04946-7

Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite. / Park, Myeongkee; Neukirch, Amanda J.; Reyes-Lillo, Sebastian E.; Lai, Minliang; Ellis, Scott R.; Dietze, Daniel; Neaton, Jeffrey B.; Yang, Peidong; Tretiak, Sergei; Mathies, Richard A.

En: Nature Communications, Vol. 9, N.º 1, 2525, 01.12.2018.

Resultado de la investigación: Article

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AU - Park, Myeongkee

AU - Neukirch, Amanda J.

AU - Reyes-Lillo, Sebastian E.

AU - Lai, Minliang

AU - Ellis, Scott R.

AU - Dietze, Daniel

AU - Neaton, Jeffrey B.

AU - Yang, Peidong

AU - Tretiak, Sergei

AU - Mathies, Richard A.

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Hybrid organic-inorganic perovskites have attractive optoelectronic properties including exceptional solar cell performance. The improved properties of perovskites have been attributed to polaronic effects involving stabilization of localized charge character by structural deformations and polarizations. Here we examine the Pb-I structural dynamics leading to polaron formation in methylammonium lead iodide perovskite by transient absorption, time-domain Raman spectroscopy, and density functional theory. Methylammonium lead iodide perovskite exhibits excited-state coherent nuclear wave packets oscillating at ~20, 43, and 75 cm-1 which involve skeletal bending, in-plane bending, and c-axis stretching of the I-Pb-I bonds, respectively. The amplitudes of these wave packet motions report on the magnitude of the excited-state structural changes, in particular, the formation of a bent and elongated octahedral PbI6 4- geometry. We have predicted the excited-state geometry and structural changes between the neutral and polaron states using a normal-mode projection method, which supports and rationalizes the experimental results. This study reveals the polaron formation via nuclear dynamics that may be important for efficient charge separation.

AB - Hybrid organic-inorganic perovskites have attractive optoelectronic properties including exceptional solar cell performance. The improved properties of perovskites have been attributed to polaronic effects involving stabilization of localized charge character by structural deformations and polarizations. Here we examine the Pb-I structural dynamics leading to polaron formation in methylammonium lead iodide perovskite by transient absorption, time-domain Raman spectroscopy, and density functional theory. Methylammonium lead iodide perovskite exhibits excited-state coherent nuclear wave packets oscillating at ~20, 43, and 75 cm-1 which involve skeletal bending, in-plane bending, and c-axis stretching of the I-Pb-I bonds, respectively. The amplitudes of these wave packet motions report on the magnitude of the excited-state structural changes, in particular, the formation of a bent and elongated octahedral PbI6 4- geometry. We have predicted the excited-state geometry and structural changes between the neutral and polaron states using a normal-mode projection method, which supports and rationalizes the experimental results. This study reveals the polaron formation via nuclear dynamics that may be important for efficient charge separation.

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