Dark-exciton energy splitting in monolayer WSe2: Insights from time-dependent density functional theory

Shi, Jia; Turkowski, Volodymyr; Rahman, Talat S.

doi:10.1103/physrevb.107.155431

Dark-exciton energy splitting in monolayer W Se2 : Insights from time-dependent density functional theory

Journal Article · Wed Apr 26 00:00:00 EDT 2023 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.107.155431· OSTI ID:2419192

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University of Science and Technology Beijing (China); Univ. of Central Florida, Orlando, FL (United States); OSTI
Univ. of Central Florida, Orlando, FL (United States)

Here, we present here a formalism based on time-dependent density functional theory to describe characteristics of both intra- and intervalley excitons in semiconductors, the latter of which had remained a challenge. Through the usage of an appropriate exchange-correlation kernel (nanoquanta), we trace the energy difference between the intra- and intervalley dark excitons in monolayer (1L) W⁢ Se₂ to the domination of the exchange part in the exchange-correlation energies of these states. Furthermore, our calculated transition contribution maps establish the momentum resolved weights of the electron-hole excitations in both bright and dark excitons thereby providing a comprehensive understanding of excitonic properties of 1L W⁢ Se₂. We find that the states consist of hybridized excitations around the corresponding valleys which leads to brightening of the dark excitons, i.e., significantly decreasing their lifetime which is reflected in the PL spectrum. Using many-body perturbation theory, we calculate the phonon contribution to the energy band gap and the linewidths of the excited electrons, holes, and (bright) exciton to find that as the temperature increases the band gap significantly decreases, while the linewidths increase. Our work paves for describing the ultrafast charge dynamics of transition metal dichalcogenide within an ab initio framework.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Central Florida, Orlando, FL (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: FG02-07ER46354

OSTI ID:: 2419192

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 15 Vol. 107; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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