A substitutional quantum defect in WS2 discovered by high-throughput computational screening and fabricated by site-selective STM manipulation

John C Thomas; Wei Chen; Yihuang Xiong; Bradford A Barker; Junze Zhou; Weiru Chen; Antonio Rossi; Nolan Kelly; Zhuohang Yu; Da Zhou; Shalini Kumari; Edward S Barnard; Joshua A Robinson; Mauricio Terrones; Adam Schwartzberg; D Frank Ogletree; Eli Rotenberg; Marcus M Noack; Sinéad Griffin; Archana Raja; David A Strubbe; Gian-Marco Rignanese; Alexander Weber-Bargioni; Geoffroy Hautier

doi:10.1038/s41467-024-47876-3

A substitutional quantum defect in WS₂ discovered by high-throughput computational screening and fabricated by site-selective STM manipulation

Nat Commun. 2024 Apr 26;15(1):3556. doi: 10.1038/s41467-024-47876-3.

Authors

John C Thomas^#^{1

2

3}, Wei Chen^#⁴, Yihuang Xiong^#⁵, Bradford A Barker⁶, Junze Zhou⁷, Weiru Chen⁵, Antonio Rossi^{7

8

9}, Nolan Kelly⁶, Zhuohang Yu^{10

11}, Da Zhou¹², Shalini Kumari^{10

11}, Edward S Barnard⁷, Joshua A Robinson^{10

11

12

13}, Mauricio Terrones^{10

11

12

13}, Adam Schwartzberg⁷, D Frank Ogletree⁷, Eli Rotenberg⁹, Marcus M Noack¹⁴, Sinéad Griffin^{7

8}, Archana Raja^{7

8}, David A Strubbe⁶, Gian-Marco Rignanese⁴, Alexander Weber-Bargioni^{15

16}, Geoffroy Hautier¹⁷

Affiliations

¹ Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. jthomas@lbl.gov.
² Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. jthomas@lbl.gov.
³ Thayer School of Engineering, Dartmouth College, Hanover, NH, 03755, USA. jthomas@lbl.gov.
⁴ Institute of Condensed Matter and Nanoscicence, Université Catholique de Louvain, Louvain-la-Neuve, 1348, Belgium.
⁵ Thayer School of Engineering, Dartmouth College, Hanover, NH, 03755, USA.
⁶ Department of Physics, University of California, Merced, Merced, CA, 95343, USA.
⁷ Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁸ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
⁹ Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
¹⁰ Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, 16082, USA.
¹¹ Center for Two-Dimensional and Layered Materials, The Pennsylvania State University, University Park, PA, 16802, USA.
¹² Department of Physics, The Pennsylvania State University, University Park, PA, 16802, USA.
¹³ Department of Chemistry, The Pennsylvania State University, University Park, PA, 16802, USA.
¹⁴ Applied Mathematics and Computational Research Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
¹⁵ Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. afweber-bargioni@lbl.gov.
¹⁶ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. afweber-bargioni@lbl.gov.
¹⁷ Thayer School of Engineering, Dartmouth College, Hanover, NH, 03755, USA. geoffroy.hautier@dartmouth.edu.

^# Contributed equally.

Abstract

Point defects in two-dimensional materials are of key interest for quantum information science. However, the parameter space of possible defects is immense, making the identification of high-performance quantum defects very challenging. Here, we perform high-throughput (HT) first-principles computational screening to search for promising quantum defects within WS₂, which present localized levels in the band gap that can lead to bright optical transitions in the visible or telecom regime. Our computed database spans more than 700 charged defects formed through substitution on the tungsten or sulfur site. We found that sulfur substitutions enable the most promising quantum defects. We computationally identify the neutral cobalt substitution to sulfur (Co $_{S}^{0}$ ) and fabricate it with scanning tunneling microscopy (STM). The Co $_{S}^{0}$ electronic structure measured by STM agrees with first principles and showcases an attractive quantum defect. Our work shows how HT computational screening and nanoscale synthesis routes can be combined to design promising quantum defects.

Grants and funding

DE-SC0022289/U.S. Department of Energy (DOE)