Evidence for nitrogen binding to surface defects for topological insulator Bi2Se3

Gottschalk, Michael; Lee, Mal-Soon; Goodwin, Eric; Mikolas, Camille; Chasapis, Thomas; Chung, Duck Young; Kanatzidis, Mercouri G.; Mahanti, Subhendra D.; Tessmer, Stuart

doi:10.1016/j.ssc.2022.115012

Evidence for nitrogen binding to surface defects for topological insulator Bi₂Se₃

Journal Article · Thu Nov 10 00:00:00 UTC 2022 · Solid State Communications

DOI:https://doi.org/10.1016/j.ssc.2022.115012· OSTI ID:1960004

^[1]; Lee, Mal-Soon ^[2]; Goodwin, Eric ^[3]; ^[3]; Chasapis, Thomas ^[4]; Chung, Duck Young ^[5]; Kanatzidis, Mercouri G. ^[4]; ^[3]; ^[3]

Michigan State Univ., East Lansing, MI (United States); Michigan State University
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Michigan State Univ., East Lansing, MI (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Using scanning tunneling spectroscopy and theoretical simulations we have studied the effects of nitrogen gas exposure on the electronic density of states of Bi₂Se₃, a well-studied topological insulator. In carefully controlled measurements, Bi₂Se₃ crystals were initially cleaved in a helium gas environment and then exposed to a 22 SCFH flow of ultra-high purity N₂ gas. We observe a resulting change in the spectral curves, with the exposure effect saturating after approximately 50 min, ultimately bringing the Dirac point about 50 meV closer to the Fermi level. Furthermore, these results are compared to density functional theory calculations, which support a picture of N₂ molecules physisorbing near Se vacancies. Furthermore, ab initio molecular dynamics simulations aided by a Blue Moon ensemble method reveal the dissociative adsorption of N₂ molecules which then bind strongly to Se vacancies at the surface. In this scenario, the binding of the N atom to a Se vacancy site removes the surface defect state created by the vacancy and changes the position of the Fermi energy with respect to the Dirac point.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Michigan State Univ., East Lansing, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0017888

OSTI ID:: 1960004

Alternate ID(s):: OSTI ID: 2340753
OSTI ID: 1899807

Journal Information:: Solid State Communications, Journal Name: Solid State Communications Vol. 359; ISSN 0038-1098

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
Chemisorption
Density functional theory
Dissociative adsorption
Physisorption
Scanning tunneling microscopy
Topological insulator
ab initio molecular dynamics