title: Comparison of carrier multiplication yields in PbS and PbSe nanocrystals: the role of competing energy-loss processes.
abstract: Infrared band gap semiconductor nanocrystals are promising materials for exploring generation III photovoltaic concepts that rely on carrier multiplication or multiple exciton generation, the process in which a single high-energy photon generates more than one electron-hole pair. In this work, we present measurements of carrier multiplication yields and biexciton lifetimes for a large selection of PbS nanocrystals and compare these results to the well-studied PbSe nanocrystals. The similar bulk properties of PbS and PbSe make this an important comparison for discerning the pertinent properties that determine efficient carrier multiplication. We observe that PbS and PbSe have very similar biexciton lifetimes as a function of confinement energy. Together with the similar bulk properties, this suggests that the rates of multiexciton generation, which is the inverse of Auger recombination, are also similar. The carrier multiplication yields in PbS nanocrystals, however, are strikingly lower than those observed for PbSe nanocrystals. We suggest that this implies the rate of competing processes, such as phonon emission, is higher in PbS nanocrystals than in PbSe nanocrystals. Indeed, our estimations for phonon emission mediated by the polar Fröhlich-type interaction indicate that the corresponding energy-loss rate is approximately twice as large in PbS than in PbSe.
authors.affiliation: Center for Advanced Solar Photophysics, C-PCS, Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA. jstewart@lanl.gov
authors.forename: John T
authors.initials: JT
authors.lastname: Stewart
authors.forename: Lazaro A
authors.initials: LA
authors.lastname: Padilha
authors.forename: M Mumtaz
authors.initials: MM
authors.lastname: Qazilbash
authors.forename: Jeffrey M
authors.initials: JM
authors.lastname: Pietryga
authors.forename: Aaron G
authors.initials: AG
authors.lastname: Midgett
authors.forename: Joseph M
authors.initials: JM
authors.lastname: Luther
authors.forename: Matthew C
authors.initials: MC
authors.lastname: Beard
authors.forename: Arthur J
authors.initials: AJ
authors.lastname: Nozik
authors.forename: Victor I
authors.initials: VI
authors.lastname: Klimov
mesh_terms: D004736:Energy-Generating Resources; D007854:Lead / Q000737:chemistry*; D010316:Particle Size; D045663:Quantum Dots; D018036:Selenium Compounds / Q000737:chemistry*; D013440:Sulfides / Q000737:chemistry*; D013499:Surface Properties
chemical_list: D018036:Selenium Compounds; D013440:Sulfides; C088065:lead selenide; C018391:lead sulfide; D007854:Lead