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 »
- Authors:
-
- Pennsylvania State Univ., University Park, PA (United States)
- 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}
}
Web of Science
Works referenced in this record:
Coupled Spin and Valley Physics in Monolayers of and Other Group-VI Dichalcogenides
journal, May 2012
- Xiao, Di; Liu, Gui-Bin; Feng, Wanxiang
- Physical Review Letters, Vol. 108, Issue 19
High-Gain Phototransistors Based on a CVD MoS 2 Monolayer
journal, May 2013
- Zhang, Wenjing; Huang, Jing-Kai; Chen, Chang-Hsiao
- Advanced Materials, Vol. 25, Issue 25
Valley dynamics probed through charged and neutral exciton emission in monolayer
journal, August 2014
- Wang, G.; Bouet, L.; Lagarde, D.
- Physical Review B, Vol. 90, Issue 7
Carrier and Polarization Dynamics in Monolayer
journal, January 2014
- Lagarde, D.; Bouet, L.; Marie, X.
- Physical Review Letters, Vol. 112, Issue 4
High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity
journal, April 2015
- Kang, Kibum; Xie, Saien; Huang, Lujie
- Nature, Vol. 520, Issue 7549
Robust valley polarization of helium ion modified atomically thin MoS 2
journal, November 2017
- Klein, J.; Kuc, A.; Nolinder, A.
- 2D Materials, Vol. 5, Issue 1
Theory and Ab Initio Calculation of Radiative Lifetime of Excitons in Semiconducting Carbon Nanotubes
journal, December 2005
- Spataru, Catalin D.; Ismail-Beigi, Sohrab; Capaz, Rodrigo B.
- Physical Review Letters, Vol. 95, Issue 24
Exciton Radiative Lifetimes in Two-Dimensional Transition Metal Dichalcogenides
journal, March 2015
- Palummo, Maurizia; Bernardi, Marco; Grossman, Jeffrey C.
- Nano Letters, Vol. 15, Issue 5
Radiative Enhancement of Single Quantum Emitters in WSe 2 Monolayers Using Site-Controlled Metallic Nanopillars
journal, August 2018
- Cai, Tao; Kim, Je-Hyung; Yang, Zhili
- ACS Photonics, Vol. 5, Issue 9
Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material
journal, January 2015
- Zhang, Xin; Qiao, Xiao-Fen; Shi, Wei
- Chemical Society Reviews, Vol. 44, Issue 9
Excitonic resonances in thin films of WSe 2 : from monolayer to bulk material
journal, January 2015
- Arora, Ashish; Koperski, Maciej; Nogajewski, Karol
- Nanoscale, Vol. 7, Issue 23
Strain-Induced Spatial and Spectral Isolation of Quantum Emitters in Mono- and Bilayer WSe 2
journal, October 2015
- Kumar, S.; Kaczmarczyk, A.; Gerardot, B. D.
- Nano Letters, Vol. 15, Issue 11
Single-photon emission from localized excitons in an atomically thin semiconductor
journal, January 2015
- Tonndorf, Philipp; Schmidt, Robert; Schneider, Robert
- Optica, Vol. 2, Issue 4
Direct measurement of exciton valley coherence in monolayer WSe2
journal, February 2016
- Hao, Kai; Moody, Galan; Wu, Fengcheng
- Nature Physics, Vol. 12, Issue 7
Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides
journal, October 2018
- Refaely-Abramson, Sivan; Qiu, Diana Y.; Louie, Steven G.
- Physical Review Letters, Vol. 121, Issue 16
Large-scale quantum-emitter arrays in atomically thin semiconductors
journal, May 2017
- Palacios-Berraquero, Carmen; Kara, Dhiren M.; Montblanch, Alejandro R. -P.
- Nature Communications, Vol. 8, Issue 1
Atomically Thin A New Direct-Gap Semiconductor
journal, September 2010
- Mak, Kin Fai; Lee, Changgu; Hone, James
- Physical Review Letters, Vol. 105, Issue 13, Article No.136805
Deterministic strain-induced arrays of quantum emitters in a two-dimensional semiconductor
journal, May 2017
- Branny, Artur; Kumar, Santosh; Proux, Raphaël
- Nature Communications, Vol. 8, Issue 1
Uncovering electron scattering mechanisms in NiFeCoCrMn derived concentrated solid solution and high entropy alloys
journal, January 2019
- Mu, Sai; Samolyuk, German D.; Wimmer, Sebastian
- npj Computational Materials, Vol. 5, Issue 1
Defect engineering of two-dimensional transition metal dichalcogenides
journal, April 2016
- Lin, Zhong; Carvalho, Bruno R.; Kahn, Ethan
- 2D Materials, Vol. 3, Issue 2
Single photon emitters in exfoliated WSe2 structures
journal, May 2015
- Koperski, M.; Nogajewski, K.; Arora, A.
- Nature Nanotechnology, Vol. 10, Issue 6
In-situ visualization of hydrogen evolution sites on helium ion treated molybdenum dichalcogenides under reaction conditions
journal, July 2019
- Mitterreiter, Elmar; Liang, Yunchang; Golibrzuch, Matthias
- npj 2D Materials and Applications, Vol. 3, Issue 1
Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation
journal, June 2019
- Klein, J.; Lorke, M.; Florian, M.
- Nature Communications, Vol. 10, Issue 1
Defect Engineering in Single-Layer MoS 2 Using Heavy Ion Irradiation
journal, November 2018
- He, Zuyun; Zhao, Ran; Chen, Xiaofei
- ACS Applied Materials & Interfaces, Vol. 10, Issue 49
Optically active quantum dots in monolayer WSe2
journal, May 2015
- Srivastava, Ajit; Sidler, Meinrad; Allain, Adrien V.
- Nature Nanotechnology, Vol. 10, Issue 6
Defects as a factor limiting carrier mobility in WSe2: A spectroscopic investigation
journal, September 2016
- Wu, Zhangting; Luo, Zhongzhong; Shen, Yuting
- Nano Research, Vol. 9, Issue 12
Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride
journal, September 2017
- Grosso, Gabriele; Moon, Hyowon; Lienhard, Benjamin
- Nature Communications, Vol. 8, Issue 1
Screening and many-body effects in two-dimensional crystals: Monolayer
journal, June 2016
- Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.
- Physical Review B, Vol. 93, Issue 23
Defect Activated Photoluminescence in WSe 2 Monolayer
journal, May 2017
- Wu, Zhangting; Zhao, Weiwei; Jiang, Jie
- The Journal of Physical Chemistry C, Vol. 121, Issue 22
Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged and free excitons
journal, September 2013
- Tongay, Sefaattin; Suh, Joonki; Ataca, Can
- Scientific Reports, Vol. 3, Issue 1
Diffusion-Controlled Epitaxy of Large Area Coalesced WSe 2 Monolayers on Sapphire
journal, January 2018
- Zhang, Xiaotian; Choudhury, Tanushree H.; Chubarov, Mikhail
- Nano Letters, Vol. 18, Issue 2
Angstrom-Size Defect Creation and Ionic Transport through Pores in Single-Layer MoS 2
journal, February 2018
- Thiruraman, Jothi Priyanka; Fujisawa, Kazunori; Danda, Gopinath
- Nano Letters, Vol. 18, Issue 3
Highly Scalable, Atomically Thin WSe 2 Grown via Metal–Organic Chemical Vapor Deposition
journal, January 2015
- Eichfeld, Sarah M.; Hossain, Lorraine; Lin, Yu-Chuan
- ACS Nano, Vol. 9, Issue 2
Tuning Electronic Structure of Single Layer MoS 2 through Defect and Interface Engineering
journal, February 2018
- Chen, Yan; Huang, Shengxi; Ji, Xiang
- ACS Nano, Vol. 12, Issue 3
Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials
journal, July 2013
- Bernardi, Marco; Palummo, Maurizia; Grossman, Jeffrey C.
- Nano Letters, Vol. 13, Issue 8, p. 3664-3670
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012
- Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
- Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
Layer-dependent second-order Raman intensity of Mo S 2 and WS e 2 : Influence of intervalley scattering
journal, April 2018
- Qian, Qingkai; Zhang, Zhaofu; Chen, Kevin J.
- Physical Review B, Vol. 97, Issue 16
Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016
- Mak, Kin Fai; Shan, Jie
- Nature Photonics, Vol. 10, Issue 4
Effect of disorder on Raman scattering of single-layer
journal, May 2015
- Mignuzzi, Sandro; Pollard, Andrew J.; Bonini, Nicola
- Physical Review B, Vol. 91, Issue 19
High-Performance WSe 2 Complementary Metal Oxide Semiconductor Technology and Integrated Circuits
journal, July 2015
- Yu, Lili; Zubair, Ahmad; Santos, Elton J. G.
- Nano Letters, Vol. 15, Issue 8
Single quantum emitters in monolayer semiconductors
journal, May 2015
- He, Yu-Ming; Clark, Genevieve; Schaibley, John R.
- Nature Nanotechnology, Vol. 10, Issue 6
Exploring atomic defects in molybdenum disulphide monolayers
journal, February 2015
- Hong, Jinhua; Hu, Zhixin; Probert, Matt
- Nature Communications, Vol. 6, Issue 1
Interfacing single photons and single quantum dots with photonic nanostructures
journal, May 2015
- Lodahl, Peter; Mahmoodian, Sahand; Stobbe, Søren
- Reviews of Modern Physics, Vol. 87, Issue 2
Generating Sub-nanometer Pores in Single-Layer MoS 2 by Heavy-Ion Bombardment for Gas Separation: A Theoretical Perspective
journal, July 2018
- Yin, Kedi; Huang, Shengxi; Chen, Xiaofei
- ACS Applied Materials & Interfaces, Vol. 10, Issue 34
Raman and photoluminescence spectra of two-dimensional nanocrystallites of monolayer WS 2 and WSe 2
journal, April 2016
- Shi, Wei; Lin, Miao-Ling; Tan, Qing-Hai
- 2D Materials, Vol. 3, Issue 2
Defect sizing, separation, and substrate effects in ion-irradiated monolayer two-dimensional materials
journal, October 2018
- Maguire, Pierce; Fox, Daniel S.; Zhou, Yangbo
- Physical Review B, Vol. 98, Issue 13
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer
journal, August 2014
- Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M.
- Physical Review Letters, Vol. 113, Issue 7
Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: , , , and
journal, November 2014
- Li, Yilei; Chernikov, Alexey; Zhang, Xian
- Physical Review B, Vol. 90, Issue 20
Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012
- Mak, Kin Fai; He, Keliang; Shan, Jie
- Nature Nanotechnology, Vol. 7, Issue 8
Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012
- Zeng, Hualing; Dai, Junfeng; Yao, Wang
- Nature Nanotechnology, Vol. 7, Issue 8
Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers
journal, October 2017
- Robert, C.; Amand, T.; Cadiz, F.
- Physical Review B, Vol. 96, Issue 15
Microsecond Valley Lifetime of Defect-Bound Excitons in Monolayer WSe 2
journal, August 2018
- Moody, Galan; Tran, Kha; Lu, Xiaobo
- Physical Review Letters, Vol. 121, Issue 5
Large-scale quantum-emitter arrays in atomically thin semiconductors.
text, January 2017
- Palacios-Berraquero, Carmen; Kara, Dhiren; Montblanch, Alejandro R-P
- Apollo - University of Cambridge Repository
Uncovering electron scattering mechanisms in NiFeCoCrMn derived concentrated solid solution and high entropy alloys
text, January 2019
- Mu, Sai; Samolyuk, German D.; Wimmer, Sebastian
- Universität Regensburg
Single Quantum Emitters in Monolayer Semiconductors
preprint, January 2014
- He, Yu-Ming; Clark, G.; Schaibley, J. R.
- arXiv
Excitonic resonances in thin films of WSe2: From monolayer to bulk material
preprint, January 2015
- Arora, Ashish; Koperski, Maciej; Nogajewski, Karol
- arXiv
Defects as a factor limiting carrier mobility in WSe2: a spectroscopic investigation
text, January 2016
- Wu, Zhangting; Luo, Zhongzhong; Shen, Yuting
- arXiv
Large-scale quantum-emitter arrays in atomically thin semiconductors
text, January 2016
- Palacios-Berraquero, Carmen; Kara, Dhiren M.; Montblanch, Alejandro R. -P.
- arXiv
Tunable and high purity room-temperature single photon emission from atomic defects in hexagonal boron nitride
text, January 2016
- Grosso, Gabriele; Moon, Hyowon; Lienhard, Benjamin
- arXiv
Radiative enhancement of single quantum emitters in WSe2 monolayers using site-controlled metallic nano-pillars
text, January 2018
- Cai, Tao; Kim, Je-Hyung; Yang, Zhili
- arXiv
Defect-induced modification of low-lying excitons and valley selectivity in monolayer transition metal dichalcogenides
text, January 2018
- Refaely-Abramson, Sivan; Qiu, Diana Y.; Louie, Steven G.
- arXiv
Uncovering electron scattering mechanisms in NiFeCoCrMn derived concentrated solid solution and high entropy alloys
text, January 2018
- Mu, Sai; Samolyuk, G. D.; Wimmer, S.
- arXiv