Chemomechanical modification of quantum emission in monolayer WSe2

Utama, M. Iqbal Bakti; Zeng, Hongfei; Sadhukhan, Tumpa; Dasgupta, Anushka; Gavin, S. Carin; Ananth, Riddhi; Lebedev, Dmitry; Wang, Wei; Chen, Jia-Shiang; Watanabe, Kenji; Taniguchi, Takashi; Marks, Tobin J.; Ma, Xuedan; Weiss, Emily A.; Schatz, George C.; Stern, Nathaniel P.; Hersam, Mark C.

doi:10.1038/s41467-023-37892-0

Title: Chemomechanical modification of quantum emission in monolayer WSe2

Journal Article · 17 April 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-37892-0 · OSTI ID:2325125

; Zeng, Hongfei;

;

; Gavin, S. Carin; Ananth, Riddhi; Lebedev, Dmitry;

;

Abstract Two-dimensional (2D) materials have attracted attention for quantum information science due to their ability to host single-photon emitters (SPEs). Although the properties of atomically thin materials are highly sensitive to surface modification, chemical functionalization remains unexplored in the design and control of 2D material SPEs. Here, we report a chemomechanical approach to modify SPEs in monolayer WSe ₂ through the synergistic combination of localized mechanical strain and noncovalent surface functionalization with aryl diazonium chemistry. Following the deposition of an aryl oligomer adlayer, the spectrally complex defect-related emission of strained monolayer WSe ₂ is simplified into spectrally isolated SPEs with high single-photon purity. Density functional theory calculations reveal energetic alignment between WSe ₂ defect states and adsorbed aryl oligomer energy levels, thus providing insight into the observed chemomechanically modified quantum emission. By revealing conditions under which chemical functionalization tunes SPEs, this work broadens the parameter space for controlling quantum emission in 2D materials.

View Journal Article

Cite

Export

Save

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0021314; AC02-06CH11357

OSTI ID:: 2325125

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (70)

Interface Characterization and Control of 2D Materials and Heterostructures Liu, Xiaolong; Hersam, Mark C. Advanced Materials, Vol. 30, Issue 39 https://doi.org/10.1002/adma.201801586	journal	July 2018
Efficient and Layer-Dependent Exciton Pumping across Atomically Thin Organic-Inorganic Type-I Heterostructures Zhang, Linglong; Sharma, Ankur; Zhu, Yi Advanced Materials, Vol. 30, Issue 40 https://doi.org/10.1002/adma.201803986	journal	August 2018
Chemically Tuned p‐ and n‐Type WSe ₂ Monolayers with High Carrier Mobility for Advanced Electronics Ji, Hyun Goo; Solís‐Fernández, Pablo; Yoshimura, Daisuke Advanced Materials, Vol. 31, Issue 42 https://doi.org/10.1002/adma.201903613	journal	September 2019
Spatially and spectrally resolved cathodoluminescence with fast electrons: A tool for background subtraction in luminescence intensity second-order correlation measurements applied to subwavelength inhomogeneous diamond nanocrystals Tizei, Luiz Henrique Galvão; Meuret, Sophie; Nagarajan, Sounderya physica status solidi (a), Vol. 210, Issue 10 https://doi.org/10.1002/pssa.201300044	journal	July 2013
VASPKIT: A user-friendly interface facilitating high-throughput computing and analysis using VASP code Wang, Vei; Xu, Nan; Liu, Jin-Cheng Computer Physics Communications, Vol. 267 https://doi.org/10.1016/j.cpc.2021.108033	journal	October 2021
Direct Covalent Chemical Functionalization of Unmodified Two-Dimensional Molybdenum Disulfide Chu, Ximo S.; Yousaf, Ahmed; Li, Duo O. Chemistry of Materials, Vol. 30, Issue 6 https://doi.org/10.1021/acs.chemmater.8b00173	journal	March 2018
Generating Bright Emissive States by Modulating the Bandgap of Monolayer Tungsten Diselenide Sadhukhan, Tumpa; Schatz, George C. The Journal of Physical Chemistry C, Vol. 126, Issue 12 https://doi.org/10.1021/acs.jpcc.1c09508	journal	March 2022
Reaction Kinetics for the Covalent Functionalization of Two-Dimensional MoS ₂ by Aryl Diazonium Salts Li, Duo O.; Chu, Ximo S.; Wang, Qing Hua Langmuir, Vol. 35, Issue 17 https://doi.org/10.1021/acs.langmuir.8b04288	journal	April 2019
Purcell-Enhanced Single Photon Source Based on a Deterministically Placed WSe₂ Monolayer Quantum Dot in a Circular Bragg Grating Cavity Iff, Oliver; Buchinger, Quirin; Moczała-Dusanowska, Magdalena Nano Letters, Vol. 21, Issue 11 https://doi.org/10.1021/acs.nanolett.1c00978	journal	May 2021
Probing Interlayer Interactions in Transition Metal Dichalcogenide Heterostructures by Optical Spectroscopy: MoS ₂ /WS ₂ and MoSe ₂ /WSe ₂ Rigosi, Albert F.; Hill, Heather M.; Li, Yilei Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b01055	journal	July 2015
Strain-Induced Spatial and Spectral Isolation of Quantum Emitters in Mono- and Bilayer WSe ₂ Kumar, S.; Kaczmarczyk, A.; Gerardot, B. D. Nano Letters, Vol. 15, Issue 11 https://doi.org/10.1021/acs.nanolett.5b03312	journal	October 2015
Deterministic Coupling of Quantum Emitters in 2D Materials to Plasmonic Nanocavity Arrays Tran, Toan Trong; Wang, Danqing; Xu, Zai-Quan Nano Letters, Vol. 17, Issue 4 https://doi.org/10.1021/acs.nanolett.7b00444	journal	March 2017
Control of Charge Carriers and Band Structure in 2D Monolayer Molybdenum Disulfide via Covalent Functionalization Jones, Leighton O.; Mosquera, Martín A.; Ratner, Mark A. ACS Applied Materials & Interfaces, Vol. 12, Issue 4 https://doi.org/10.1021/acsami.9b19639	journal	January 2020
Basal-Plane Functionalization of Chemically Exfoliated Molybdenum Disulfide by Diazonium Salts Knirsch, Kathrin C.; Berner, Nina C.; Nerl, Hannah C. ACS Nano, Vol. 9, Issue 6 https://doi.org/10.1021/acsnano.5b00965	journal	May 2015
Chemically Tailoring Semiconducting Two-Dimensional Transition Metal Dichalcogenides and Black Phosphorus Ryder, Christopher R.; Wood, Joshua D.; Wells, Spencer A. ACS Nano, Vol. 10, Issue 4 https://doi.org/10.1021/acsnano.6b01091	journal	April 2016
Quantum Calligraphy: Writing Single-Photon Emitters in a Two-Dimensional Materials Platform Rosenberger, Matthew R.; Dass, Chandriker Kavir; Chuang, Hsun-Jen ACS Nano, Vol. 13, Issue 1 https://doi.org/10.1021/acsnano.8b08730	journal	December 2018
Spontaneous Emission Enhancement in Strain-Induced WSe ₂ Monolayer-Based Quantum Light Sources on Metallic Surfaces Tripathi, Laxmi Narayan; Iff, Oliver; Betzold, Simon ACS Photonics, Vol. 5, Issue 5 https://doi.org/10.1021/acsphotonics.7b01053	journal	April 2018
Radiative Enhancement of Single Quantum Emitters in WSe 2 Monolayers Using Site-Controlled Metallic Nanopillars Cai, Tao; Kim, Je-Hyung; Yang, Zhili ACS Photonics, Vol. 5, Issue 9 https://doi.org/10.1021/acsphotonics.8b00580	journal	August 2018
Scanning Tunneling Microscopy, Spectroscopy, and Nanolithography of Epitaxial Graphene Chemically Modified with Aryl Moieties Hossain, Md. Zakir; Walsh, Michael A.; Hersam, Mark C. Journal of the American Chemical Society, Vol. 132, Issue 43 https://doi.org/10.1021/ja107085n	journal	November 2010
Sterically Hindered Diazonium Salts for the Grafting of a Monolayer on Metals Combellas, Catherine; Kanoufi, Frederic; Pinson, Jean Journal of the American Chemical Society, Vol. 130, Issue 27 https://doi.org/10.1021/ja8018912	journal	June 2008
Molecularly Tunable Fluorescent Quantum Defects Kwon, Hyejin; Furmanchuk, Al’ona; Kim, Mijin Journal of the American Chemical Society, Vol. 138, Issue 21 https://doi.org/10.1021/jacs.6b03618	journal	May 2016
Covalent bulk functionalization of graphene Englert, Jan M.; Dotzer, Christoph; Yang, Guang Nature Chemistry, Vol. 3, Issue 4 https://doi.org/10.1038/nchem.1010	journal	March 2011
Brightening of carbon nanotube photoluminescence through the incorporation of sp3 defects Piao, Yanmei; Meany, Brendan; Powell, Lyndsey R. Nature Chemistry, Vol. 5, Issue 10 https://doi.org/10.1038/nchem.1711	journal	July 2013
Covalent functionalization of monolayered transition metal dichalcogenides by phase engineering Voiry, Damien; Goswami, Anandarup; Kappera, Rajesh Nature Chemistry, Vol. 7, Issue 1 https://doi.org/10.1038/nchem.2108	journal	November 2014
Covalent functionalization and passivation of exfoliated black phosphorus via aryl diazonium chemistry Ryder, Christopher R.; Wood, Joshua D.; Wells, Spencer A. Nature Chemistry, Vol. 8, Issue 6 https://doi.org/10.1038/nchem.2505	journal	May 2016
Deterministic strain-induced arrays of quantum emitters in a two-dimensional semiconductor Branny, Artur; Kumar, Santosh; Proux, Raphaël Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15053	journal	May 2017
Large-scale quantum-emitter arrays in atomically thin semiconductors Palacios-Berraquero, Carmen; Kara, Dhiren M.; Montblanch, Alejandro R. -P. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15093	journal	May 2017
Isolated electron spins in silicon carbide with millisecond coherence times Christle, David J.; Falk, Abram L.; Andrich, Paolo Nature Materials, Vol. 14, Issue 2 https://doi.org/10.1038/nmat4144	journal	December 2014
Mixed-dimensional van der Waals heterostructures Jariwala, Deep; Marks, Tobin J.; Hersam, Mark C. Nature Materials, Vol. 16, Issue 2 https://doi.org/10.1038/nmat4703	journal	August 2016
Optical generation of excitonic valley coherence in monolayer WSe2 Jones, Aaron M.; Yu, Hongyi; Ghimire, Nirmal J. Nature Nanotechnology, Vol. 8, Issue 9 https://doi.org/10.1038/nnano.2013.151	journal	August 2013
Quantum emission from hexagonal boron nitride monolayers Tran, Toan Trong; Bray, Kerem; Ford, Michael J. Nature Nanotechnology, Vol. 11, Issue 1 https://doi.org/10.1038/nnano.2015.242	journal	October 2015
Optically active quantum dots in monolayer WSe2 Srivastava, Ajit; Sidler, Meinrad; Allain, Adrien V. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.60	journal	May 2015
Single photon emitters in exfoliated WSe2 structures Koperski, M.; Nogajewski, K.; Arora, A. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.67	journal	May 2015
Single quantum emitters in monolayer semiconductors He, Yu-Ming; Clark, Genevieve; Schaibley, John R. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.75	journal	May 2015
Voltage-controlled quantum light from an atomically thin semiconductor Chakraborty, Chitraleema; Kinnischtzke, Laura; Goodfellow, Kenneth M. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.79	journal	May 2015
Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons Zhou, You; Scuri, Giovanni; Wild, Dominik S. Nature Nanotechnology, Vol. 12, Issue 9 https://doi.org/10.1038/nnano.2017.106	journal	June 2017
Tunable room-temperature single-photon emission at telecom wavelengths from sp3 defects in carbon nanotubes He, Xiaowei; Hartmann, Nicolai F.; Ma, Xuedan Nature Photonics, Vol. 11, Issue 9 https://doi.org/10.1038/nphoton.2017.119	journal	July 2017
Spin and pseudospins in layered transition metal dichalcogenides Xu, Xiaodong; Yao, Wang; Xiao, Di Nature Physics, Vol. 10, Issue 5 https://doi.org/10.1038/nphys2942	journal	April 2014
Revealing the biexciton and trion-exciton complexes in BN encapsulated WSe2 Li, Zhipeng; Wang, Tianmeng; Lu, Zhengguang Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05863-5	journal	September 2018
A monolithic immersion metalens for imaging solid-state quantum emitters Huang, Tzu-Yung; Grote, Richard R.; Mann, Sander A. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10238-5	journal	June 2019
Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation Klein, J.; Lorke, M.; Florian, M. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10632-z	journal	June 2019
Integration of single photon emitters in 2D layered materials with a silicon nitride photonic chip Peyskens, Frédéric; Chakraborty, Chitraleema; Muneeb, Muhammad Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12421-0	journal	September 2019
Defect and strain engineering of monolayer WSe2 enables site-controlled single-photon emission up to 150 K Parto, Kamyar; Azzam, Shaimaa I.; Banerjee, Kaustav Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23709-5	journal	June 2021
The role of chalcogen vacancies for atomic defect emission in MoS2 Mitterreiter, Elmar; Schuler, Bruno; Micevic, Ana Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-24102-y	journal	June 2021
Bright single photon emitters with enhanced quantum efficiency in a two-dimensional semiconductor coupled with dielectric nano-antennas Sortino, Luca; Zotev, Panaiot G.; Phillips, Catherine L. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-26262-3	journal	October 2021
Narrow-band single-photon emission through selective aryl functionalization of zigzag carbon nanotubes Saha, Avishek; Gifford, Brendan J.; He, Xiaowei Nature Chemistry, Vol. 10, Issue 11 https://doi.org/10.1038/s41557-018-0126-4	journal	September 2018
Carbon nanotubes as emerging quantum-light sources He, X.; Htoon, H.; Doorn, S. K. Nature Materials, Vol. 17, Issue 8 https://doi.org/10.1038/s41563-018-0109-2	journal	June 2018
Disorder in van der Waals heterostructures of 2D materials Rhodes, Daniel; Chae, Sang Hoon; Ribeiro-Palau, Rebeca Nature Materials, Vol. 18, Issue 6 https://doi.org/10.1038/s41563-019-0366-8	journal	May 2019
Deterministic coupling of site-controlled quantum emitters in monolayer WSe2 to plasmonic nanocavities Luo, Yue; Shepard, Gabriella D.; Ardelean, Jenny V. Nature Nanotechnology, Vol. 13, Issue 12 https://doi.org/10.1038/s41565-018-0275-z	journal	October 2018
Optical initialization of a single spin-valley in charged WSe2 quantum dots Lu, Xin; Chen, Xiaotong; Dubey, Sudipta Nature Nanotechnology, Vol. 14, Issue 5 https://doi.org/10.1038/s41565-019-0394-1	journal	March 2019
2D materials for quantum information science Liu, Xiaolong; Hersam, Mark C. Nature Reviews Materials, Vol. 4, Issue 10 https://doi.org/10.1038/s41578-019-0136-x	journal	August 2019
Identifying defect-related quantum emitters in monolayer WSe2 Dang, Jianchen; Sun, Sibai; Xie, Xin npj 2D Materials and Applications, Vol. 4, Issue 1 https://doi.org/10.1038/s41699-020-0136-0	journal	February 2020
Evidence of monolayer formation via diazonium grafting with a radical scavenger: electrochemical, AFM and XPS monitoring Menanteau, T.; Levillain, E.; Downard, A. J. Physical Chemistry Chemical Physics, Vol. 17, Issue 19 https://doi.org/10.1039/C5CP01401H	journal	January 2015
Covalent chemical functionalization of semiconducting layered chalcogenide nanosheets Li, Duo O.; Gilliam, Matthew S.; Chu, Ximo S. Molecular Systems Design & Engineering, Vol. 4, Issue 4 https://doi.org/10.1039/C9ME00045C	journal	January 2019
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
The Perdew–Burke–Ernzerhof exchange-correlation functional applied to the G2-1 test set using a plane-wave basis set Paier, Joachim; Hirschl, Robin; Marsman, Martijn The Journal of Chemical Physics, Vol. 122, Issue 23 https://doi.org/10.1063/1.1926272	journal	June 2005
Microcavity enhanced single photon emission from two-dimensional WSe ₂ Flatten, L. C.; Weng, L.; Branny, A. Applied Physics Letters, Vol. 112, Issue 19 https://doi.org/10.1063/1.5026779	journal	May 2018
Atomistic defects as single-photon emitters in atomically thin MoS ₂ Barthelmi, K.; Klein, J.; Hötger, A. Applied Physics Letters, Vol. 117, Issue 7 https://doi.org/10.1063/5.0018557	journal	August 2020
Nanoscale axial position and orientation measurement of hexagonal boron nitride quantum emitters using a tunable nanophotonic environment Jha, Pankaj K.; Akbari, Hamidreza; Kim, Yonghwi Nanotechnology, Vol. 33, Issue 1 https://doi.org/10.1088/1361-6528/ac2b71	journal	October 2021
Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping Castellanos-Gomez, Andres; Buscema, Michele; Molenaar, Rianda 2D Materials, Vol. 1, Issue 1 https://doi.org/10.1088/2053-1583/1/1/011002	journal	April 2014
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Observation of Fourier transform limited lines in hexagonal boron nitride Dietrich, A.; Bürk, M.; Steiger, E. S. Physical Review B, Vol. 98, Issue 8 https://doi.org/10.1103/PhysRevB.98.081414	journal	August 2018
Localized Intervalley Defect Excitons as Single-Photon Emitters in WSe 2 Linhart, Lukas; Paur, Matthias; Smejkal, Valerie Physical Review Letters, Vol. 123, Issue 14 https://doi.org/10.1103/PhysRevLett.123.146401	journal	September 2019
Room temperature stable single-photon source Beveratos, A.; Kühn, S.; Brouri, R. The European Physical Journal D - Atomic, Molecular and Optical Physics, Vol. 18, Issue 2 https://doi.org/10.1140/epjd/e20020023	journal	February 2002
Single Photon Sources in Atomically Thin Materials Toth, Milos; Aharonovich, Igor Annual Review of Physical Chemistry, Vol. 70, Issue 1 https://doi.org/10.1146/annurev-physchem-042018-052628	journal	June 2019
Photon antibunching in the fluorescence of individual color centers in diamond Brouri, Rosa; Beveratos, Alexios; Poizat, Jean-Philippe Optics Letters, Vol. 25, Issue 17 https://doi.org/10.1364/OL.25.001294	journal	January 2000
Single-photon emission from localized excitons in an atomically thin semiconductor Tonndorf, Philipp; Schmidt, Robert; Schneider, Robert Optica, Vol. 2, Issue 4 https://doi.org/10.1364/OPTICA.2.000347	journal	January 2015
Resonant laser spectroscopy of localized excitons in monolayer WSe_2 Kumar, Santosh; Brotóns-Gisbert, Mauro; Al-Khuzheyri, Rima Optica, Vol. 3, Issue 8 https://doi.org/10.1364/OPTICA.3.000882	journal	January 2016
Substrate engineering for high-quality emission of free and localized excitons from atomic monolayers in hybrid architectures Iff, Oliver; He, Yu-Ming; Lundt, Nils Optica, Vol. 4, Issue 6 https://doi.org/10.1364/OPTICA.4.000669	journal	January 2017
Advances in quantum light emission from 2D materials Chakraborty, Chitraleema; Vamivakas, Nick; Englund, Dirk Nanophotonics, Vol. 8, Issue 11 https://doi.org/10.1515/nanoph-2019-0140	journal	August 2019

Similar Records

Conversion of Classical Light Emission from a Nanoparticle‐Strained WSe ₂ Monolayer into Quantum Light Emission via Electron Beam Irradiation

Journal Article · 2022 · Advanced Materials · OSTI ID:1905173

Xu, David D.; Vong, Albert F.; Lebedev, Dmitry; +6 more

Carbene Functionalization of Monolayer Tungsten Disulfide for Enhanced Quantum Emission

Journal Article · 2025 · ACS Nano · OSTI ID:2588399

Dasgupta, Anushka; López-Arteaga, Rafael; Park, Hong Youl; +15 more

Sub‐Diffraction Correlation of Quantum Emitters and Local Strain Fields in Strain‐Engineered WSe ₂ Monolayers

Journal Article · 2024 · Advanced Materials · OSTI ID:2328662

Xu, David D.; Vong, Albert F.; Utama, M. Iqbal Bakti; +5 more

Title: Chemomechanical modification of quantum emission in monolayer WSe2

Citation Formats

References (70)

Similar Records

Related Subjects