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State-resolved manipulations of optical gain in semiconductor quantum dots: Size universality, gain tailoring, and surface effects

J. Chem. Phys. 131, 164706 (2009); doi:10.1063/1.3254199

Published 30 October 2009

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Ryan R. Cooney, Samuel L. Sewall, D. M. Sagar, and Patanjali Kambhampati
Department of Chemistry, McGill University, Montreal, Quebec H3A 2K6, Canada
Optical gain in strongly confined colloidal semiconductor quantum dots is measured using state resolved pump/probe spectroscopy. Though size tunable optical amplification has been previously reported for these materials, the influence of confinement enhanced multiexcitonic interactions has limited prior demonstrations to specific particle sizes or host media. Here we show that the influence of the interfering multiexcitonic interactions, and hence the development of optical gain, is dependent on the identity of the initially prescribed excitonic state. By maintaining a constant excitonic state in the size tunable electronic structure of these materials, we recover the predicted universal development of optical gain, reflected by size-independent occupation thresholds, and differential gains. In addition, we explicitly compare the influence of surface passivation on the development and lifetime of the optical gain. Furthermore, we introduce a general, state-resolved pumping scheme which enables control over the optical gain spectrum. The capacity to manipulate the optical gain spectra of these spherically confined systems is evident in both the measured stimulated emission and amplified spontaneous emission. We anticipate that state-resolved optical excitation will be a useful method of enabling the development and manipulation of optical gain in any quantized nanostructure. ©2009 American Institute of Physics
History: Received 6 July 2009; accepted 6 October 2009; published 30 October 2009
Permalink: http://link.aip.org/link/?JCPSA6/131/164706/1
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KEYWORDS and PACS

Keywords
PACS
  • 78.67.Hc
    Optical properties of quantum dots
  • 78.55.Et
    Photoluminescence in II-VI semiconductors
  • 78.40.Fy
    Visible and ultraviolet spectra of semiconductors
  • 78.45.+h
    Stimulated emission (condensed matter)
  • 73.21.La
    Quantum dots (electron states/collective excitations)
  • 81.65.Rv
    Surface passivation
  • YEAR: 2009

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PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
Publisher:
AIP is a member of CrossRef AIP

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