High‐Temperature Single‐Photon Emission From Covalently Functionalized van der Waals Heterostructures

Gavin, S. Carin; Chuang, Hsun‐Jen; Dasgupta, Anushka; Kar, Moumita; McCreary, Kathleen M.; Lee, Sung‐Joon; Utama, M. Iqbal Bakti; Zhou, Chunxi; Li, Xiangzhi; Schatz, George C.; Marks, Tobin J.; Hersam, Mark C.; Jonker, Berend T.; Stern, Nathaniel P.

doi:10.1002/advs.202511319

High‐Temperature Single‐Photon Emission From Covalently Functionalized van der Waals Heterostructures

Journal Article · Tue Oct 07 00:00:00 EDT 2025 · Advanced Science

DOI:https://doi.org/10.1002/advs.202511319· OSTI ID:3029256

^[1]; Chuang, Hsun‐Jen ^[2]; Dasgupta, Anushka ^[1]; Kar, Moumita ^[1]; McCreary, Kathleen M. ^[2]; Lee, Sung‐Joon ^[2]; Utama, M. Iqbal Bakti ^[1]; Zhou, Chunxi ^[1]; Li, Xiangzhi ^[3]; Schatz, George C. ^[1]; Marks, Tobin J. ^[1]; Hersam, Mark C. ^[1]; Jonker, Berend T. ^[2]; ^[1]

Northwestern University, Evanston, IL (United States)
United States Naval Research Laboratory, Washington D.C. (United States)
Stevens Institute of Technology Hoboken, NJ (United States)

Two-dimensional (2D) transition metal dichalcogenides (TMDs) such as tungsten diselenide (WSe₂) are attractive nanomaterials for quantum information applications due to single-photon emission (SPE) from intrinsic atomic defects. Defect and strain engineering techniques have been developed to produce high purity, deterministically placed SPE in WSe₂. However, a major challenge in the application of these techniques is the low temperature required to observe defect-bound TMD exciton emission, typically limiting SPE to T < 30 K. SPE at higher temperatures either loses purity or requires integration into complex devices such as optical cavities. Here, 2D heterostructure engineering and molecular functionalization are combined to achieve high purity (>90%) SPE in strained WSe₂ persisting to over T = 90 K. Covalent diazonium functionalization of graphite in layered WSe₂/graphite heterostructures maintains high purity up to T = 90 K and single-photon source integrity up to T = 115 K. This method preserves the best qualities of SPE from WSe₂ while increasing working temperature to more than three times the typical range. This work demonstrates the versatility of surface functionalization and heterostructure design to synergistically improve the properties of quantum emission and offers new insights into the phenomenon of SPE from 2D materials.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern University, Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021314

Other Award/Contract Number:: DMR‐2308691

OSTI ID:: 3029256

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 48 Vol. 12; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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High‐Temperature Single‐Photon Emission From Covalently Functionalized van der Waals Heterostructures

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