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Title: Defect creation in WSe2 with a microsecond photoluminescence lifetime by focused ion beam irradiation

Abstract

Defect engineering is important for tailoring the electronic and optical properties of two-dimensional materials, and the capability of generating defects of certain types at specific locations is meaningful for potential applications such as optoelectronics and quantum photonics. Herein, atomic defects are created in single-layer WSe2 using focused ion beam (FIB) irradiation, with defect densities spanning many orders of magnitude. The influences of defects are systematically characterized. Raman spectroscopy can only discern defects in WSe2 for a FIB dose higher than 1 × 1013 cm–2, which causes blue shifts of both A'1 and E' modes. Photoluminescence (PL) of WSe2 is more sensitive to defects. At cryogenic temperature, the low-energy PL induced by defects can be revealed, which shows redshifts and broadenings with increased FIB doses. Similar Raman shifts and PL spectrum changes are observed for the WSe2 film grown by chemical vapor deposition (CVD). A four microsecond-long lifetime is observed in the PL dynamics and is three orders of magnitude longer than the often observed delocalized exciton lifetime and becomes more dominant for WSe2 with increasing FIB doses. The ultra-long lifetime of PL in single-layer WSe2 is consistent with first-principles calculation results considering the creation of both chalcogen and metal vacanciesmore » by FIB, and can be valuable for photo-catalytic reactions, valleytronics and quantum light emissions owing to the longer carrier separation/manipulation time.« less

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
  1. Pennsylvania State Univ., University Park, PA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1660954
Alternate Identifier(s):
OSTI ID: 1581664
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 12; Journal Issue: 3; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Qian, Qingkai, Peng, Lintao, Perea-Lopez, Nestor, Fujisawa, Kazunori, Zhang, Kunyan, Zhang, Xiaotian, Choudhury, Tanushree H., Redwing, Joan M., Terrones, Mauricio, Ma, Xuedan, and Huang, Shengxi. Defect creation in WSe2 with a microsecond photoluminescence lifetime by focused ion beam irradiation. United States: N. p., 2019. Web. doi:10.1039/c9nr08390a.
Qian, Qingkai, Peng, Lintao, Perea-Lopez, Nestor, Fujisawa, Kazunori, Zhang, Kunyan, Zhang, Xiaotian, Choudhury, Tanushree H., Redwing, Joan M., Terrones, Mauricio, Ma, Xuedan, & Huang, Shengxi. Defect creation in WSe2 with a microsecond photoluminescence lifetime by focused ion beam irradiation. United States. https://doi.org/10.1039/c9nr08390a
Qian, Qingkai, Peng, Lintao, Perea-Lopez, Nestor, Fujisawa, Kazunori, Zhang, Kunyan, Zhang, Xiaotian, Choudhury, Tanushree H., Redwing, Joan M., Terrones, Mauricio, Ma, Xuedan, and Huang, Shengxi. Tue . "Defect creation in WSe2 with a microsecond photoluminescence lifetime by focused ion beam irradiation". United States. https://doi.org/10.1039/c9nr08390a. https://www.osti.gov/servlets/purl/1660954.
@article{osti_1660954,
title = {Defect creation in WSe2 with a microsecond photoluminescence lifetime by focused ion beam irradiation},
author = {Qian, Qingkai and Peng, Lintao and Perea-Lopez, Nestor and Fujisawa, Kazunori and Zhang, Kunyan and Zhang, Xiaotian and Choudhury, Tanushree H. and Redwing, Joan M. and Terrones, Mauricio and Ma, Xuedan and Huang, Shengxi},
abstractNote = {Defect engineering is important for tailoring the electronic and optical properties of two-dimensional materials, and the capability of generating defects of certain types at specific locations is meaningful for potential applications such as optoelectronics and quantum photonics. Herein, atomic defects are created in single-layer WSe2 using focused ion beam (FIB) irradiation, with defect densities spanning many orders of magnitude. The influences of defects are systematically characterized. Raman spectroscopy can only discern defects in WSe2 for a FIB dose higher than 1 × 1013 cm–2, which causes blue shifts of both A'1 and E' modes. Photoluminescence (PL) of WSe2 is more sensitive to defects. At cryogenic temperature, the low-energy PL induced by defects can be revealed, which shows redshifts and broadenings with increased FIB doses. Similar Raman shifts and PL spectrum changes are observed for the WSe2 film grown by chemical vapor deposition (CVD). A four microsecond-long lifetime is observed in the PL dynamics and is three orders of magnitude longer than the often observed delocalized exciton lifetime and becomes more dominant for WSe2 with increasing FIB doses. The ultra-long lifetime of PL in single-layer WSe2 is consistent with first-principles calculation results considering the creation of both chalcogen and metal vacancies by FIB, and can be valuable for photo-catalytic reactions, valleytronics and quantum light emissions owing to the longer carrier separation/manipulation time.},
doi = {10.1039/c9nr08390a},
journal = {Nanoscale},
number = 3,
volume = 12,
place = {United States},
year = {Tue Dec 10 00:00:00 EST 2019},
month = {Tue Dec 10 00:00:00 EST 2019}
}

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