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Ab Initio Calculations of Exciton Radiative Lifetimes in Bulk Crystals, Nanostructures and Molecules

Chen, Hsiao-Yi and Jhalani, Vatsal A. and Palummo, Maurizia and Bernardi, Marco (2019) Ab Initio Calculations of Exciton Radiative Lifetimes in Bulk Crystals, Nanostructures and Molecules. Physical Review B, 100 (7). Art. No. 075135. ISSN 2469-9950. http://resolver.caltech.edu/CaltechAUTHORS:20190429-081350448

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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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1103/PhysRevB.100.075135DOIArticle
https://journals.aps.org/prb/abstract/10.1103/PhysRevB.100.075135PublisherArticle
https://arxiv.org/abs/1901.08747arXivDiscussion Paper
ORCID:
AuthorORCID
Jhalani, Vatsal A.0000-0003-0866-0858
Palummo, Maurizia0000-0002-3097-8523
Bernardi, Marco0000-0001-7289-9666
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.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0019166
NSFACI-1642443
Tor Vergata University2DUTOPI
Department of Energy (DOE)DE-AC02-05CH11231
Issue or Number:7
Record Number:CaltechAUTHORS:20190429-081350448
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20190429-081350448
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:95063
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:29 Apr 2019 15:53
Last Modified:16 Aug 2019 16:42

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