High Temperature Quantum Emission from Covalently Functionalized van der Waals Heterostructures

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Hauptverfasser: Gavin, S. Carin, Chuang, Hsun-Jen, Dasgupta, Anushka, Kar, Moumita, McCreary, Kathleen M., Lee, Sung-Joon, Utama, M. Iqbal Bakti, Li, Xiangzhi, Schatz, George C., Marks, Tobin J., Hersam, Mark C., Jonker, Berend T., Stern, Nathaniel P.
Format: Preprint
Veröffentlicht: 2025
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author Gavin, S. Carin
Chuang, Hsun-Jen
Dasgupta, Anushka
Kar, Moumita
McCreary, Kathleen M.
Lee, Sung-Joon
Utama, M. Iqbal Bakti
Li, Xiangzhi
Schatz, George C.
Marks, Tobin J.
Hersam, Mark C.
Jonker, Berend T.
Stern, Nathaniel P.
author_facet Gavin, S. Carin
Chuang, Hsun-Jen
Dasgupta, Anushka
Kar, Moumita
McCreary, Kathleen M.
Lee, Sung-Joon
Utama, M. Iqbal Bakti
Li, Xiangzhi
Schatz, George C.
Marks, Tobin J.
Hersam, Mark C.
Jonker, Berend T.
Stern, Nathaniel P.
contents Two-dimensional (2D) transition metal dichalcogenides (TMDs) are attractive nanomaterials for quantum information applications due to single photon emission (SPE) from atomic defects, primarily tungsten diselenide (WSe2) monolayers. Defect and strain engineering techniques have been developed to yield high purity, deterministically positioned SPE in WSe2. However, a major challenge in 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 a layered WSe2/graphite heterostructure 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.
format Preprint
id arxiv_https___arxiv_org_abs_2506_20847
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle High Temperature Quantum 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
Li, Xiangzhi
Schatz, George C.
Marks, Tobin J.
Hersam, Mark C.
Jonker, Berend T.
Stern, Nathaniel P.
Materials Science
Mesoscale and Nanoscale Physics
Two-dimensional (2D) transition metal dichalcogenides (TMDs) are attractive nanomaterials for quantum information applications due to single photon emission (SPE) from atomic defects, primarily tungsten diselenide (WSe2) monolayers. Defect and strain engineering techniques have been developed to yield high purity, deterministically positioned SPE in WSe2. However, a major challenge in 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 a layered WSe2/graphite heterostructure 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.
title High Temperature Quantum Emission from Covalently Functionalized van der Waals Heterostructures
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2506.20847