Breaking the phonon bottleneck in semiconductor nanocrystals via multiphonon emission induced by intrinsic nonadiabatic interactions |
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Authors: | Schaller Richard D Pietryga Jeffrey M Goupalov Serguei V Petruska Melissa A Ivanov Sergei A Klimov Victor I |
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Institution: | Chemistry Division, C-PCS, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA. |
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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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