Critical Role of Methylammonium Librational Motion in Methylammonium Lead Iodide (CH3NH3PbI3) Perovskite Photochemistry

Myeongkee Park, Nikolay Kornienko, Sebastian E. Reyes-Lillo, Minliang Lai, Jeffrey B. Neaton, Peidong Yang, Richard A. Mathies

Resultado de la investigación: Article

16 Citas (Scopus)

Resumen

Raman and photoluminescence (PL) spectroscopy are used to investigate dynamic structure-function relationships in methylammonium lead iodide (MAPbI3) perovskite. The intensity of the 150 cm-1 methylammonium (MA) librational Raman mode is found to be correlated with PL intensities in microstructures of MAPbI3. Because of the strong hydrogen bond between hydrogens in MA and iodine in the PbI6 perovskite octahedra, the Raman activity of MA is very sensitive to structural distortions of the inorganic framework. The structural distortions directly influence PL intensities, which in turn have been correlated with microstructure quality. Our measurements, supported with first-principles calculations, indicate how excited-state MA librational displacements mechanistically control PL efficiency and lifetime in MAPbI3 - material parameters that are likely important for efficient photovoltaic devices.

Idioma originalEnglish
Páginas (desde-hasta)4151-4157
Número de páginas7
PublicaciónNano Letters
Volumen17
N.º7
DOI
EstadoPublished - 12 jul 2017

Huella dactilar

librational motion
Photochemical reactions
Iodides
photochemical reactions
Perovskite
iodides
Photoluminescence
Lead
photoluminescence
Displacement control
Microstructure
Photoluminescence spectroscopy
Iodine
Excited states
microstructure
Raman spectroscopy
Hydrogen bonds
iodine
Hydrogen
hydrogen bonds

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

Citar esto

Park, Myeongkee ; Kornienko, Nikolay ; Reyes-Lillo, Sebastian E. ; Lai, Minliang ; Neaton, Jeffrey B. ; Yang, Peidong ; Mathies, Richard A. / Critical Role of Methylammonium Librational Motion in Methylammonium Lead Iodide (CH3NH3PbI3) Perovskite Photochemistry. En: Nano Letters. 2017 ; Vol. 17, N.º 7. pp. 4151-4157.
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title = "Critical Role of Methylammonium Librational Motion in Methylammonium Lead Iodide (CH3NH3PbI3) Perovskite Photochemistry",
abstract = "Raman and photoluminescence (PL) spectroscopy are used to investigate dynamic structure-function relationships in methylammonium lead iodide (MAPbI3) perovskite. The intensity of the 150 cm-1 methylammonium (MA) librational Raman mode is found to be correlated with PL intensities in microstructures of MAPbI3. Because of the strong hydrogen bond between hydrogens in MA and iodine in the PbI6 perovskite octahedra, the Raman activity of MA is very sensitive to structural distortions of the inorganic framework. The structural distortions directly influence PL intensities, which in turn have been correlated with microstructure quality. Our measurements, supported with first-principles calculations, indicate how excited-state MA librational displacements mechanistically control PL efficiency and lifetime in MAPbI3 - material parameters that are likely important for efficient photovoltaic devices.",
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Critical Role of Methylammonium Librational Motion in Methylammonium Lead Iodide (CH3NH3PbI3) Perovskite Photochemistry. / Park, Myeongkee; Kornienko, Nikolay; Reyes-Lillo, Sebastian E.; Lai, Minliang; Neaton, Jeffrey B.; Yang, Peidong; Mathies, Richard A.

En: Nano Letters, Vol. 17, N.º 7, 12.07.2017, p. 4151-4157.

Resultado de la investigación: Article

TY - JOUR

T1 - Critical Role of Methylammonium Librational Motion in Methylammonium Lead Iodide (CH3NH3PbI3) Perovskite Photochemistry

AU - Park, Myeongkee

AU - Kornienko, Nikolay

AU - Reyes-Lillo, Sebastian E.

AU - Lai, Minliang

AU - Neaton, Jeffrey B.

AU - Yang, Peidong

AU - Mathies, Richard A.

PY - 2017/7/12

Y1 - 2017/7/12

N2 - Raman and photoluminescence (PL) spectroscopy are used to investigate dynamic structure-function relationships in methylammonium lead iodide (MAPbI3) perovskite. The intensity of the 150 cm-1 methylammonium (MA) librational Raman mode is found to be correlated with PL intensities in microstructures of MAPbI3. Because of the strong hydrogen bond between hydrogens in MA and iodine in the PbI6 perovskite octahedra, the Raman activity of MA is very sensitive to structural distortions of the inorganic framework. The structural distortions directly influence PL intensities, which in turn have been correlated with microstructure quality. Our measurements, supported with first-principles calculations, indicate how excited-state MA librational displacements mechanistically control PL efficiency and lifetime in MAPbI3 - material parameters that are likely important for efficient photovoltaic devices.

AB - Raman and photoluminescence (PL) spectroscopy are used to investigate dynamic structure-function relationships in methylammonium lead iodide (MAPbI3) perovskite. The intensity of the 150 cm-1 methylammonium (MA) librational Raman mode is found to be correlated with PL intensities in microstructures of MAPbI3. Because of the strong hydrogen bond between hydrogens in MA and iodine in the PbI6 perovskite octahedra, the Raman activity of MA is very sensitive to structural distortions of the inorganic framework. The structural distortions directly influence PL intensities, which in turn have been correlated with microstructure quality. Our measurements, supported with first-principles calculations, indicate how excited-state MA librational displacements mechanistically control PL efficiency and lifetime in MAPbI3 - material parameters that are likely important for efficient photovoltaic devices.

KW - DFT

KW - MAPbI

KW - Methylammonium lead iodide perovskite

KW - photoluminescence microscopy

KW - photovoltaics

KW - Raman microscopy

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U2 - 10.1021/acs.nanolett.7b00919

DO - 10.1021/acs.nanolett.7b00919

M3 - Article

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SP - 4151

EP - 4157

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

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