Theory and Ab Initio Computation of the Anisotropic Light Emission in Monolayer Transition Metal Dichalcogenides

Chen, Hsiao-Yi; Palummo, Maurizia; Sangalli, Davide; Bernardi, Marco

doi:10.1021/acs.nanolett.8b01114

Title: Theory and Ab Initio Computation of the Anisotropic Light Emission in Monolayer Transition Metal Dichalcogenides

Journal Article · Mon May 07 00:00:00 EDT 2018 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.8b01114· OSTI ID:1543682

Chen, Hsiao-Yi ^[1];

^[2];

^[3];

^[4]

California Inst. of Technology (CalTech), Pasadena, CA (United States). Dept. of Applied Physics and Materials Science, Dept. of Physics
Dipartimento di Fisica and INFN, Università di Roma Tor Vergata, Via della Ricerca Scientifica 1, 00133 Roma, Italy
Consiglio Nazionale delle Ricerche (CNR), Monterotondo Scalo (Italy). Division of Ultrafast Processes in Materials (FLASHit)
California Inst. of Technology (CalTech), Pasadena, CA (United States). Dept. of Applied Physics and Materials Science

Monolayer transition metal dichalcogenides (TMDCs) are direct gap semiconductors with a unique potential for use in ultrathin light emitters. However, their photoluminescence (PL) is not completely understood. We develop an approach to compute the radiative recombination rate in monolayer TMDCs as a function of photon emission direction and polarization. Using exciton wavefunctions and energies obtained with the ab initio Bethe-Salpeter equation, we obtain polar plots of the PL for different scenarios. Our results can explain the PL anisotropy and polarization dependence measured in recent experiments and predict that light is emitted with a peak intensity normal to the exciton dipole in monolayer TMDCs. We show that excitons emit light anisotropically upon recombination when they are in any quantum superposition state of the K and K' inequivalent valleys. When averaged over the emission angle and exciton momentum, our new treatment recovers the temperature-dependent radiative lifetimes that we previously derived. Our work demonstrates a generally applicable first-principles approach to studying anisotropic light emission in two-dimensional materials.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1543682

Journal Information:: Nano Letters, Vol. 18, Issue 6; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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