Visualizing Orbital Content of Electronic Bands in Anisotropic 2D Semiconducting ReSe2

Choi, Byoung Ki; Ulstrup, Søren; Gunasekera, Surani M.; Kim, Jiho; Lim, Soo Yeon; Moreschini, Luca; Oh, Ji Seop; Chun, Seung-Hyun; Jozwiak, Chris; Bostwick, Aaron; Rotenberg, Eli; Cheong, Hyeonsik; Lyo, In-Whan; Mucha-Kruczynski, Marcin; Chang, Young Jun

doi:10.1021/acsnano.0c01054

Title: Visualizing Orbital Content of Electronic Bands in Anisotropic 2D Semiconducting ReSe₂

Journal Article · Thu May 28 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c01054· OSTI ID:1783099

^[1]; Ulstrup, Søren ^[2]; Gunasekera, Surani M. ^[3]; Kim, Jiho ^[4]; Lim, Soo Yeon ^[5]; Moreschini, Luca ^[6]; Oh, Ji Seop ^[7];

^[8]; Jozwiak, Chris ^[6]; Bostwick, Aaron ^[6];

^[6];

^[5]; Lyo, In-Whan ^[4]; Mucha-Kruczynski, Marcin ^[3];

^[1]

Univ. of Seoul (South Korea)
Aarhus Univ. (Denmark); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Univ. of Bath (United Kingdom). Centre for Nanoscience and Nanotechnology
Yonsei Univ., Seoul (South Korea)
Sogang Univ., Seoul (South Korea)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Inst. for Basic Science (IBS), Seoul (South Korea). Center for Correlated Electron Systems
Sejong Univ., Seoul (South Korea)

Many properties of layered materials change as they are thinned from their bulk forms down to single layers, with examples including indirect-to-direct band gap transition in 2H semiconducting transition metal dichalcogenides as well as thickness-dependent changes in the valence band structure in post-transition-metal monochalcogenides and black phosphorus. Here, we use angle-resolved photoemission spectroscopy to study the electronic band structure of monolayer ReSe₂, a semiconductor with a distorted 1T structure and in-plane anisotropy. By changing the polarization of incoming photons, we demonstrate that for ReSe₂, in contrast to the 2H materials, the out-of-plane transition metal dz2 and chalcogen pz orbitals do not contribute significantly to the top of the valence band, which explains the reported weak changes in the electronic structure of this compound as a function of layer number. We estimate a band gap of 1.7 eV in pristine ReSe₂ using scanning tunneling spectroscopy and explore the implications on the gap following surface doping with potassium. Additionally, a lower bound of 1.4 eV is estimated for the gap in the fully doped case, suggesting that doping-dependent many-body effects significantly affect the electronic properties of ReSe₂. Our results, supported by density functional theory calculations, provide insight into the mechanisms behind polarization-dependent optical properties of rhenium dichalcogenides and highlight their place among two-dimensional crystals.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF); Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC02-05CH11231; 2020R1A2C200373211; 2019K1A3A7A09033389; 2019R1A2C3006189; EP/L015544/1EPSRC

OSTI ID:: 1783099

Journal Information:: ACS Nano, Vol. 14, Issue 7; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
anisotropic 2D semiconductor
rhenium diselenide
orbital-selective electronic structure
transition metal dichalcogenides
potassium
band structure
layers
energy
electrical conductivity

Title: Visualizing Orbital Content of Electronic Bands in Anisotropic 2D Semiconducting ReSe2

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Title: Visualizing Orbital Content of Electronic Bands in Anisotropic 2D Semiconducting ReSe₂