Variations in the Quantum Efficiency of Multiple Exciton Generation for a Series of Chemically Treated PbSe Nanocrystal Films

Beard, Matthew C.; Midgett, Aaron G.; Law, Matt; Semonin, Octavi E.; Elligston, Randy J.; Nozik, Arthur J.

doi:10.1021/nl803600v

Title: Variations in the Quantum Efficiency of Multiple Exciton Generation for a Series of Chemically Treated PbSe Nanocrystal Films

Journal Article · Thu Jan 01 00:00:00 EST 2009 · Nano Letters

DOI:https://doi.org/10.1021/nl803600v· OSTI ID:952185

; Midgett, Aaron G.; Law, Matt; Semonin, Octavi E.; Elligston, Randy J.; Nozik, Arthur J.

We study multiple exciton generation (MEG) in two series of chemically treated PbSe nanocrystal (NC) films. We find that the average number of excitons produced per absorbed photon varies between 1.0 and 2.4 ({+-} 0.2) at a photon energy of {approx}4E{sub g} for films consisting of 3.7 nm NCs and between 1.1 and 1.6 ({+-} 0.1) at hv {approx}5E{sub g} for films consisting of 7.4 nm NCs. The variations in MEG depend upon the chemical treatment used to electronically couple the NCs in each film. The single and multiexciton lifetimes also change with the chemical treatment: biexciton lifetimes increase with stronger inter-NC electronic coupling and exciton delocalization, while single exciton lifetimes decrease after most treatments relative to the same NCs in solution. Single exciton lifetimes are particularly affected by surface treatments that dope the films n-type, which we tentatively attribute to an Auger recombination process between a single exciton and an electron produced by ionization of the dopant donor. These results imply that a better understanding of the effects of surface chemistry on film doping, NC carrier dynamics, and inter-NC interactions is necessary to build solar energy conversion devices that can harvest the multiple carriers produced by MEG. Our results show that the MEG efficiency is very sensitive to the condition of the NC surface and suggest that the wide range of MEG efficiencies reported in the recent literature may be a result of uncontrolled differences in NC surface chemistry.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science, Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences; USDOE Solar Energy Technologies Office; The Defense Advanced Research Projects Agency (DARPA)

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 952185

Report Number(s):: NREL/JA-270-44885; MainId:48264; UUID:e9c4ed4b-cfd4-e411-b769-d89d67132a6d; MainAdminId:30356; TRN: US200913%%397

Journal Information:: Nano Letters, Vol. 9, Issue 2

Country of Publication:: United States

Language:: English

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Title: Variations in the Quantum Efficiency of Multiple Exciton Generation for a Series of Chemically Treated PbSe Nanocrystal Films

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