Transient reshaping of intraband transitions by hot electrons

Diroll, Benjamin T.; Banerjee, Tathagata

doi:10.1039/d1nr06203d

Title: Transient reshaping of intraband transitions by hot electrons

Journal Article · 10 January 2022 · Nanoscale

DOI: https://doi.org/10.1039/d1nr06203d · OSTI ID:1886383

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Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Illinois at Urbana-Champaign, IL (United States)

Hot electrons, far above the lattice temperature of a material, present opportunities for enhanced solar energy harvesting or performance of otherwise unfavorable chemistry. The spectroscopic signatures and dynamics of hot carrier absorption and emission have been extensively studied in bulk and nanoscopic semiconductors, but the effects on intraband transitions are largely unexplored. In this work, the effect of hot electrons on the properties of colloidal quantum wells made of cadmium selenide is examined using ultrafast spectroscopy. Similar to expitaxial quantum wells, these atomically precise materials support intersubband transitions (a class of intraband transitions in 1D and 2D materials) in the near-infrared spectral window. Using energy-dependent photoexcitation, it is shown that electrons reach effective temperatures of 2000 K or greater. This results in a substantial transient shift in the oscillator strength of the instersubband transition to lower energies on a sub-picosecond time-scale. Similar heating of electrons is achieved under mid-infrared re-excitation, which permits ultrafast transmittance modulation throughout the near-infrared.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials; Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1886383

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 4 Vol. 14; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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