TY - JOUR
T1 - Enhancement of Spontaneous Photon Emission in Inverse Photoemission Transitions in Semiconductor Quantum Dots
AU - Spanedda, Nicole
AU - Martin, Chandler
AU - Mesta, Kevin
AU - Chakraborty, Arindam
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society.
PY - 2024/1/18
Y1 - 2024/1/18
N2 - 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).
AB - 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).
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U2 - 10.1021/acs.jpclett.3c02934
DO - 10.1021/acs.jpclett.3c02934
M3 - Article
C2 - 38175542
AN - SCOPUS:85182001420
SN - 1948-7185
VL - 15
SP - 364
EP - 370
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 2
ER -