dorsal/arxiv
View SchemaFast electronic relaxation in metal nanoclusters via excitation of coherent shape deformations: Circumventing a bottleneck
| Authors | Vitaly V. Kresin, Yu. N. Ovchinnikov |
|---|---|
| Categories | |
| ArXiv ID | physics/0512222 |
| URL | https://arxiv.org/abs/physics/0512222 |
| DOI | 10.1103/PhysRevB.73.115412 |
| Journal | Phys. Rev. B 73, 115412 (2006) |
Abstract
Electron-phonon relaxation in size-quantized systems may become inhibited when the spacing of discrete electron energy levels exceeds the magnitude of the phonon frequency. We show, however, that nanoclusters can support a fast nonradiative relaxation channel which derives from their distinctive ability to undergo Jahn-Teller shape deformations. Such a deformation represents a collective and coherent vibrational excitation and enables electronic transitions to occur without a multiphonon bottleneck. We analyze this mechanism for a metal cluster within the analytical framework of a three-dimensional potential well undergoing a spheroidal distortion. An expression for the time evolution of the distortion parameter is derived, the electronic level crossing condition formulated, and the probability of electronic transition at a level crossing is evaluated. An application to electron-hole recombination in a closed-shell aluminum cluster with 40 electrons shows that the short (~250 fs) excitation lifetime observed in recent pump-probe experiments can be explained by the proposed mechanism.
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"abstract": "Electron-phonon relaxation in size-quantized systems may become inhibited\nwhen the spacing of discrete electron energy levels exceeds the magnitude of\nthe phonon frequency. We show, however, that nanoclusters can support a fast\nnonradiative relaxation channel which derives from their distinctive ability to\nundergo Jahn-Teller shape deformations. Such a deformation represents a\ncollective and coherent vibrational excitation and enables electronic\ntransitions to occur without a multiphonon bottleneck. We analyze this\nmechanism for a metal cluster within the analytical framework of a\nthree-dimensional potential well undergoing a spheroidal distortion. An\nexpression for the time evolution of the distortion parameter is derived, the\nelectronic level crossing condition formulated, and the probability of\nelectronic transition at a level crossing is evaluated. An application to\nelectron-hole recombination in a closed-shell aluminum cluster with 40\nelectrons shows that the short (~250 fs) excitation lifetime observed in recent\npump-probe experiments can be explained by the proposed mechanism.",
"arxiv_id": "physics/0512222",
"authors": [
"Vitaly V. Kresin",
"Yu. N. Ovchinnikov"
],
"categories": [
"physics.atm-clus",
"cond-mat.mes-hall"
],
"doi": "10.1103/PhysRevB.73.115412",
"journal_ref": "Phys. Rev. B 73, 115412 (2006)",
"title": "Fast electronic relaxation in metal nanoclusters via excitation of coherent shape deformations: Circumventing a bottleneck",
"url": "https://arxiv.org/abs/physics/0512222"
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