TY - JOUR
T1 - Simulations of nonradiative processes in semiconductor nanocrystals
AU - Jasrasaria, Dipti
AU - Weinberg, Daniel
AU - Philbin, John P.
AU - Rabani, Eran
N1 - Publisher Copyright:
© 2022 Author(s).
PY - 2022/7/14
Y1 - 2022/7/14
N2 - The description of carrier dynamics in spatially confined semiconductor nanocrystals (NCs), which have enhanced electron-hole and exciton-phonon interactions, is a great challenge for modern computational science. These NCs typically contain thousands of atoms and tens of thousands of valence electrons with discrete spectra at low excitation energies, similar to atoms and molecules, that converge to the continuum bulk limit at higher energies. Computational methods developed for molecules are limited to very small nanoclusters, and methods for bulk systems with periodic boundary conditions are not suitable due to the lack of translational symmetry in NCs. This perspective focuses on our recent efforts in developing a unified atomistic model based on the semiempirical pseudopotential approach, which is parameterized by first-principle calculations and validated against experimental measurements, to describe two of the main nonradiative relaxation processes of quantum confined excitons: exciton cooling and Auger recombination. We focus on the description of both electron-hole and exciton-phonon interactions in our approach and discuss the role of size, shape, and interfacing on the electronic properties and dynamics for II-VI and III-V semiconductor NCs.
AB - The description of carrier dynamics in spatially confined semiconductor nanocrystals (NCs), which have enhanced electron-hole and exciton-phonon interactions, is a great challenge for modern computational science. These NCs typically contain thousands of atoms and tens of thousands of valence electrons with discrete spectra at low excitation energies, similar to atoms and molecules, that converge to the continuum bulk limit at higher energies. Computational methods developed for molecules are limited to very small nanoclusters, and methods for bulk systems with periodic boundary conditions are not suitable due to the lack of translational symmetry in NCs. This perspective focuses on our recent efforts in developing a unified atomistic model based on the semiempirical pseudopotential approach, which is parameterized by first-principle calculations and validated against experimental measurements, to describe two of the main nonradiative relaxation processes of quantum confined excitons: exciton cooling and Auger recombination. We focus on the description of both electron-hole and exciton-phonon interactions in our approach and discuss the role of size, shape, and interfacing on the electronic properties and dynamics for II-VI and III-V semiconductor NCs.
UR - http://www.scopus.com/inward/record.url?scp=85133972408&partnerID=8YFLogxK
U2 - 10.1063/5.0095897
DO - 10.1063/5.0095897
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C2 - 35840368
AN - SCOPUS:85133972408
SN - 0021-9606
VL - 157
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 2
M1 - 020901
ER -