Ab Initio Calculations of Exciton Radiative Lifetimes in Bulk Crystals, Nanostructures and Molecules
Abstract
Excitons are bound electron-hole pairs that dominate the optical response of semiconductors and insulators, especially in materials where the Coulomb interaction is weakly screened. Light absorption (including excitonic effects) has been studied extensively using first-principles calculations, but methods for computing radiative recombination and light emission are still being developed. Here we show a unified ab initio approach to compute exciton radiative recombination in materials ranging from bulk crystals to nanostructures and molecules. We derive the rate of exciton radiative recombination in bulk crystals, isolated systems, and in one- and two-dimensional materials, using Fermi's golden rule within the Bethe-Salpeter equation approach. We present benchmark calculations of radiative lifetimes in a GaAs crystal and in gas-phase organic molecules. Our work provides a general method for studying exciton recombination and light emission in bulk, nanostructured, and molecular materials from first principles.
Additional Information
© 2019 American Physical Society. Received 25 January 2019; revised manuscript received 26 July 2019; published 16 August 2019. The authors thank Davide Sangalli for fruitful discussions. This work was partially supported by the Department of Energy under Grant No. DE-SC0019166, which provided for theory and method development, and by the National Science Foundation under Grant No. ACI-1642443, which provided for code development. M.P. acknowledges the Tor Vergata University for financial support through the mission sustainability project 2DUTOPI. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231.Attached Files
Published - PhysRevB.100.075135.pdf
Submitted - 1901.08747.pdf
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Additional details
- Eprint ID
- 95063
- Resolver ID
- CaltechAUTHORS:20190429-081350448
- DE-SC0019166
- Department of Energy (DOE)
- ACI-1642443
- NSF
- 2DUTOPI
- Tor Vergata University
- DE-AC02-05CH11231
- Department of Energy (DOE)
- Created
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2019-04-29Created from EPrint's datestamp field
- Updated
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2021-11-16Created from EPrint's last_modified field