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First principles coupled cluster theory of the electronic spectrum of the transition metal dichalcogenides

Pulkin, Artem and Chan, Garnet Kin-Lic (2020) First principles coupled cluster theory of the electronic spectrum of the transition metal dichalcogenides. Physical Review B, 101 (24). Art. No. 241113. ISSN 2469-9950. doi:10.1103/PhysRevB.101.241113.

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The electronic properties of two-dimensional transition metal dichalcogenides (2D TMDs) have attracted much attention during the last decade. We show how a diagrammatic ab initio coupled cluster singles and doubles (CCSD) treatment paired with a careful thermodynamic limit extrapolation in two dimensions can be used to obtain converged band gaps for monolayer materials in the MoS₂ family. We find CCSD gaps to lie in the upper range of the spread of GW approximation based on density functional theory (DFT) simulations, and also find slightly higher effective hole masses compared to previous reports. We also investigate the ability of CCSD to describe trion states, finding a reasonable qualitative structure, but poor excitation energies due to the lack of screening of three-particle excitations in the effective Hamiltonian. Our study provides an independent high-level benchmark of the role of many-body effects in 2D TMDs and showcases the potential strengths and weaknesses of diagrammatic coupled cluster approaches for realistic materials.

Item Type:Article
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URLURL TypeDescription Paper
Chan, Garnet Kin-Lic0000-0001-8009-6038
Additional Information:© 2020 American Physical Society. Received 7 October 2019; revised manuscript received 22 May 2020; accepted 26 May 2020; published 26 June 2020. A.P. thanks Swiss NSF for the support provided through the Early Postdoc Mobility program (Project No. P2ELP2_175281). G.K.-L.C. was supported by the US Department of Energy, Office of Science via Grant No. DE-SC0018140 for this work. Secondary support for pyscf software infrastructure was provided by the U.S. National Science Foundation via Grant No. 1657286. We thank Q. Sun and J. McClain for valuable discussions.
Funding AgencyGrant Number
Swiss National Science Foundation (SNSF)P2ELP2-175281
Department of Energy (DOE)DE-SC0018140
Issue or Number:24
Record Number:CaltechAUTHORS:20200122-092308523
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100832
Deposited By: Tony Diaz
Deposited On:23 Jan 2020 00:19
Last Modified:16 Nov 2021 17:57

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