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Evidence for energy relaxation via a radiative cascade in surface-passivated PbS quantum dots

Mark J Fernée, Andrew Watt, Jamie Warner, Norman Heckenberg and Halina Rubinsztein-Dunlop

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Multiple emission peaks have been observed from surface passivated PbS nanocrystals displaying strong quantum confinement. The emission spectra are shown to be strongly dependent on the excited-state parity. We also find that intraband energy relaxation from initial states excited far above the band-edge is nearly three orders of magnitude slower than that found in other nanocrystal quantum dots, providing evidence of inefficient energy relaxation via phonon emission. The initial-state parity dependence of the photoluminescent emission properties suggests that energy relaxation from the higher excited states occurs via a radiative cascade, analogous to energy relaxation in atomic systems. Such radiative cascade emission is possible from ideal zero-dimensional semiconductors, where electronic transitions can be decoupled from phonon modes.


PACS

78.67.Hc Quantum dots

63.20.-e Phonons in crystal lattices

78.55.Hx Other solid inorganic materials

78.67.Bf Nanocrystals and nanoparticles

Subjects

Condensed matter: electrical, magnetic and optical

Condensed matter: structural, mechanical & thermal

Nanoscale science and low-D systems

Dates

Issue 9 (September 2004)

Received 28 May 2004

Published 13 August 2004



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