Intersubband Relaxation in CdSe Colloidal Quantum Wells

Diroll, Benjamin T.; Schaller, Richard D.

doi:10.1021/acsnano.0c05459

Intersubband Relaxation in CdSe Colloidal Quantum Wells

Journal Article · Mon Aug 31 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c05459· OSTI ID:1798707

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Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, iL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

The dynamics of intersubband relaxation are critical to quantum well technologies such as quantum cascade lasers and quantum well infrared photodetectors. In this work, intersubband relaxation in CdSe colloidal quantum wells, or nanoplatelets, is studied via pump-push-probe transient spectroscopy. An initial interband pump pulse is followed by a secondary infrared push excitation, resonant with intersubband absorption, which promotes electrons from the first conduction band of the quantum well to the second conduction band. A probe pulse monitors subsequent electron cooling to the band edge of the quantum well. Using this technique, intersubband relaxation is studied as a function of critical variables such as colloidal quantum well size and thickness, surface ligand chemistry, temperature, and excitation pulse intensity. Larger quantum well sizes, judicious selection of surface ligand chemistry (e.g., thiolates), low temperatures, and elevated push pulse fluences slow intersubband relaxation. However, compared to resonant intraband relaxation in colloidal quantum dots (up to hundreds of picoseconds), intersubband relaxation in colloidal quantum wells is rapid (<1 ps) under all examined conditions. These experiments indicate that rapid relaxation is driven by both LO phonon and surface scattering. The short time scale of relaxation observed in these materials may hinder intersubband technologies such as mid-infrared detectors, although such rapid relaxation may prove valuable in optical switching.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1798707

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 9 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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