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Many-body processes in the photophysics of colloidal semiconductor nanocrystals

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dc.contributor.advisor Moungi G. Bawendi. en_US Nair, Gautham Padmanabhan en_US
dc.contributor.other Massachusetts Institute of Technology. Dept. of Chemistry. en_US 2010-04-26T19:19:53Z 2010-04-26T19:19:53Z 2009 en_US 2009 en_US
dc.description Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2009. en_US
dc.description This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections. en_US
dc.description Vita. Cataloged from student submitted PDF version of thesis. en_US
dc.description Includes bibliographical references (p. 135-143). en_US
dc.description.abstract In this work we have experimentally studied several aspects of two Coulomb processes that change the number of electrons and holes in colloidal semiconductor nanocrystals (NCs). Carrier Multiplication (CM) is the production of additional electron-hole pairs by collision of a highly excited carrier with valence electrons. Efficient CM would improve the performance of solar energy conversion devices, but it is weak in the bulk. Recent reports by several groups suggested highly efficient CM in semi-conductor NCs. We describe here our assessment of CM using transient photoluminescence in CdSe and lead chalcogenide NCs. Biexciton radiative and nonradiative rates were determined. In our study, no detectable CM was found in CdSe NCs photoexcited at a photon energy of up to 5.9 eV, and the CM yields observed for PbSe NCs at 3.1 eV were found consistent with bulk values. Reasons for the strong disagreement with prior measurements are discussed, and the low yields are theoretically accounted for. The second part of the thesis describes two studies of the "Auger" nonradiative recombination process whereby an electron-hole pair recombines while transferring its energy to a third particle. This mechanism is responsible for the short multiexciton lifetimes in NCs. In one study, we demonstrate a direct method for determining biexciton quantum yields in single nanocrystals by photon cross-correlation (antibunching) measurements. We find significant inhomogeneity in these values, indicating a previously obscured variation in Auger recombination rates. en_US
dc.description.abstract (cont.) Another set of experiments tests the conventional charging model of NC fluorescence intermittency ("blinking") which attributes off-state quenching to Auger decay, by studying single NCs with relatively long multiexciton Auger lifetimes. We find that off-state exciton quantum yields are significantly lower than the quantum yield of a biexciton and we demonstrate that multiexciton emission also shows strong intermittency. Both of these findings contradict the standard charging model. Alternatives are discussed. en_US
dc.description.statementofresponsibility by Gautham Padmanabhan Nair. en_US
dc.format.extent 145 p. en_US
dc.language.iso eng en_US
dc.publisher Massachusetts Institute of Technology en_US
dc.rights M.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission. en_US
dc.rights.uri en_US
dc.subject Chemistry. en_US
dc.title Many-body processes in the photophysics of colloidal semiconductor nanocrystals en_US
dc.type Thesis en_US Ph.D. en_US
dc.contributor.department Massachusetts Institute of Technology. Dept. of Chemistry. en_US
dc.identifier.oclc 588972266 en_US

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