title: Multiexciton dynamics in infrared-emitting colloidal nanostructures probed by a superconducting nanowire single-photon detector.
abstract: Carrier multiplication (CM) is the process in which absorption of a single photon produces multiple electron-hole pairs. Here, we evaluate the effect of particle shape on CM efficiency by conducting a comparative study of spherical nanocrystal quantum dots (NQDs) and elongated nanorods (NRs) of PbSe using a time-resolved technique that is based on photon counting in the infrared using a superconducting nanowire single-photon photodetector (SNSPD). Due to its high sensitivity and low noise levels, this technique allows for accurate determination of CM yields, even with the small excitation intensities required for quantitative measurements, and the fairly low emission quantum yields of elongated NR samples. Our measurements indicate an up to ∼60% increase in multiexciton yields in NRs versus NQDs, which is attributed primarily to a decrease in the electron-hole pair creation energy. These findings suggest that shape control is a promising approach for enhancing the CM process. Further, our work demonstrates the effectiveness of the SNSPD technique for the rapid screening of CM performance in infrared nanomaterials.
authors.affiliation: Center for Advanced Solar Photophysics, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.
authors.forename: Richard L
authors.initials: RL
authors.lastname: Sandberg
authors.forename: Lazaro A
authors.initials: LA
authors.lastname: Padilha
authors.forename: Muhammad M
authors.initials: MM
authors.lastname: Qazilbash
authors.forename: Wan Ki
authors.initials: WK
authors.lastname: Bae
authors.forename: Richard D
authors.initials: RD
authors.lastname: Schaller
authors.forename: Jeffrey M
authors.initials: JM
authors.lastname: Pietryga
authors.forename: Martin J
authors.initials: MJ
authors.lastname: Stevens
authors.forename: Burm
authors.initials: B
authors.lastname: Baek
authors.forename: Sae Woo
authors.initials: SW
authors.lastname: Nam
authors.forename: Victor I
authors.initials: VI
authors.lastname: Klimov
mesh_terms: D003102:Colloids / Q000737:chemistry; D003217:Conductometry / Q000295:instrumentation*; D004553:Electric Conductivity; D004867:Equipment Design; D019544:Equipment Failure Analysis; D007259:Infrared Rays; D036103:Nanotechnology / Q000295:instrumentation*; D043942:Nanotubes / Q000737:chemistry* / Q000528:radiation effects; D010783:Photometry / Q000295:instrumentation*; D045663:Quantum Dots
chemical_list: D003102:Colloids