Dynamics and Spin-Valley Locking Effects in Monolayer Transition Metal Dichalcogenides

Ciccarino, Christopher J.; Christensen, Thomas; Sundararaman, Ravishankar; Narang, Prineha

doi:10.1021/acs.nanolett.8b02300

Title: Dynamics and Spin-Valley Locking Effects in Monolayer Transition Metal Dichalcogenides

Journal Article · Wed Aug 01 00:00:00 EDT 2018 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.8b02300· OSTI ID:1543685

Ciccarino, Christopher J. ^[1]; Christensen, Thomas ^[2];

^[3];

^[4]

Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology, and John A. Paulson School of Engineering and Applied Sciences
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Physics
Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Materials Science and Engineering
Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences

Transition metal dichalcogenides have been the primary materials of interest in the field of valleytronics for their potential in information storage, yet the limiting factor has been achieving long valley decoherence times. We explore the dynamics of four monolayer TMDCs (MoS₂, MoSe₂, WS₂, WSe₂) using ab initio calculations to describe electron–electron and electron–phonon interactions. By comparing calculations which both omit and include relativistic effects, we isolate the impact of spin-resolved spin–orbit coupling on transport properties. In our work, we find that spin–orbit coupling increases carrier lifetimes at the valence band edge by an order of magnitude due to spin-valley locking, with a proportional increase in the hole mobility at room temperature. At temperatures of 50 K, we find intervalley scattering times on the order of 100 ps, with a maximum value of ~140 ps in WSe₂. Finally, we calculate excited-carrier generation profiles which indicate that direct transitions dominate across optical energies, even for WSe₂ which has an indirect band gap. Our results highlight the intriguing interplay between spin and valley degrees of freedom critical for valleytronic applications. Further, our work points toward interesting quantum properties on-demand in transition metal dichalcogenides that could be leveraged via driving spin, valley, and phonon degrees of freedom.

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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:: 1543685

Journal Information:: Nano Letters, Vol. 18, Issue 9; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 38 works

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