Breaking the Phonon Bottleneck in Semiconductor Nanocrystals via Multiphonon Emission Induced by Intrinsic Nonadiabatic Interactions

Richard D. Schaller, Jeffrey M. Pietryga, Serguei V. Goupalov, Melissa A. Petruska, Sergei A. Ivanov, and Victor I. Klimov
Phys. Rev. Lett. 95, 196401 – Published 31 October 2005

Abstract

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.

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  • Received 26 January 2005

DOI:https://doi.org/10.1103/PhysRevLett.95.196401

©2005 American Physical Society

Authors & Affiliations

Richard D. Schaller, Jeffrey M. Pietryga, Serguei V. Goupalov, Melissa A. Petruska, Sergei A. Ivanov, and Victor I. Klimov*

  • Chemistry Division, C-PCS, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA

  • *Electronic address: klimov@lanl.gov

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Issue

Vol. 95, Iss. 19 — 4 November 2005

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