Breaking the phonon bottleneck in semiconductor nanocrystals via multiphonon emission induced by intrinsic nonadiabatic interactions

We observe ultrafast 1P-to-1S intraband relaxation in PbSe and CdSe nanocrystals (NCs) that have distinct energy spectra. While ultrafast dynamics in CdSe NCs has typically been interpreted in terms of electron-hole energy transfer, this mechanism is not active in PbSe NCs because of sparse densitie...

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Bibliographic Details
Published in:Physical review letters 2005-11, Vol.95 (19), p.196401.1-196401.4, Article 196401
Main Authors: SCHALLER, Richard D, PIETRYGA, Jeffrey M, GOUPALOV, Serguei V, PETRUSKA, Melissa A, IVANOV, Sergei A, KLIMOV, Victor I
Format: Article
Language:English
Subjects:
Condensed matter: electronic structure, electrical, magnetic, and optical properties
Exact sciences and technology
Nanocrystals and nanoparticles
Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation
Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures
Physics
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Summary:We observe ultrafast 1P-to-1S intraband relaxation in PbSe and CdSe nanocrystals (NCs) that have distinct energy spectra. While ultrafast dynamics in CdSe NCs has typically been interpreted in terms of electron-hole energy transfer, this mechanism is not active in PbSe NCs because of sparse densities of states in the conduction and valence bands. Our observations of temperature activation and confinement-enhanced relaxation in PbSe NCs can be explained by efficient multiphonon emission triggered by nonadiabatic electron-phonon interactions and are indicative of large, size-dependent, intraband Huang-Rhys parameters.
ISSN:0031-9007
1079-7114
DOI:10.1103/physrevlett.95.196401