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Theory of Photoluminescence Spectral Line Shapes of Semiconductor Nanocrystals.
Lin, Kailai; Jasrasaria, Dipti; Yoo, Jason J; Bawendi, Moungi; Utzat, Hendrik; Rabani, Eran.
Afiliação
  • Lin K; Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States.
  • Jasrasaria D; Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States.
  • Yoo JJ; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02143, United States.
  • Bawendi M; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02143, United States.
  • Utzat H; Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States.
  • Rabani E; Department of Chemistry, University of California, Berkeley, Berkeley, California 94720, United States.
J Phys Chem Lett ; 14(32): 7241-7248, 2023 Aug 17.
Article em En | MEDLINE | ID: mdl-37552653
ABSTRACT
Single-molecule photoluminescence (PL) spectroscopy of semiconductor nanocrystals (NCs) reveals the nature of exciton-phonon interactions in NCs. Understanding the homogeneous spectral line shapes and their temperature dependence remains an open problem. Here, we develop an atomistic model to describe the PL spectrum of NCs, accounting for excitonic effects, phonon dispersion relations, and exciton-phonon couplings. We validate our model using single-NC measurements on CdSe/CdS NCs from T = 4 to 290 K, and we find that the slightly asymmetric main peak at low temperatures is comprised of a narrow zero-phonon line (ZPL) and acoustic phonon sidebands. Furthermore, we identify the specific phonon modes that give rise to the optical phonon sidebands. At temperatures above 200 K, the spectral line width shows a stronger dependence upon the temperature, which we demonstrate to be correlated with higher order exciton-phonon couplings. We also identify the line width dependence upon reorganization energy, NC core sizes, and shell thicknesses.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Phys Chem Lett Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Phys Chem Lett Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos