Enhancement of Spontaneous Photon Emission in Inverse Photoemission Transitions in Semiconductor Quantum Dots

Nicole Spanedda, Chandler Martin, Kevin Mesta, Arindam Chakraborty

Research output: Contribution to journalArticlepeer-review

Abstract

Inverse photoemission (IPE) is a radiative electron capture process where an electron is transiently captured in the conduction band (CB) followed by intraband de-excitation and spontaneous photon emission. IPE in quantum dots (QDs) bypasses optical selection rules for populating the CB and provides insights into the capacity for electron capture in the CB, the propensity for spontaneous photon emission, intraband transition energies where both initial and final states are in the CB, and the generation of photons with frequencies lower than the bandgap. Here, we demonstrate using time-dependent perturbation theory that judicious application of electric fields can significantly enhance the IPE transition in QDs. For a series of CdSe, CdS, PbSe, and PbS QDs, we present evidence of field-induced enhancement of IPE intensities (188% for Cd54Se54), field-dependent control of emitted photon frequencies (Δω = 0.73 eV for Cd54Se54), and enhancement of light-matter interaction using directed Stark fields (103% for Cd54Se54).

Original languageEnglish (US)
Pages (from-to)364-370
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume15
Issue number2
DOIs
StatePublished - Jan 18 2024

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry

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