Carbene Functionalization of Monolayer Tungsten Disulfide for Enhanced Quantum Emission

Dasgupta, Anushka; López-Arteaga, Rafael; Park, Hong Youl; Kerwin, Brendan P.; Utama, M. Iqbal Bakti; Sadhukhan, Tumpa; Gavin, S. Carin; Wan, Xi; Kachman, Dana E.; Wang, Wei; Ananth, Riddhi; Vong, Albert F.; Stern, Nathaniel P.; Schatz, George C.; Ma, Xuedan; Marks, Tobin J.; Weiss, Emily A.; Hersam, Mark C.

doi:10.1021/acsnano.5c06400

Carbene Functionalization of Monolayer Tungsten Disulfide for Enhanced Quantum Emission

Journal Article · Tue Jun 03 00:00:00 EDT 2025 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5c06400· OSTI ID:2588399

^[1]; ^[1]; Park, Hong Youl ^[1]; Kerwin, Brendan P. ^[1]; ^[1]; Sadhukhan, Tumpa ^[1]; Gavin, S. Carin ^[1]; Wan, Xi ^[1]; ^[1]; ^[2]; Ananth, Riddhi ^[1]; Vong, Albert F. ^[1]; ^[1]; ^[1]; Ma, Xuedan ^[2]; ^[1]; ^[1]; ^[1]

Northwestern Univ., Evanston, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Semiconducting two-dimensional (2D) transition metal dichalcogenides (TMDs) are promising materials for an array of applications, ranging from conventional field-effect transistors, photodetectors, and light-emitting diodes to their more recent use in quantum photonic technologies. Chemical functionalization of 2D TMDs with organic ligands and adlayers provides an additional means for customizing their electronic and optical properties. While many pathways have been reported for the chemical functionalization of 2D TMDs, their frequent reliance on solution-based methods results in limited control over adlayer thickness and coverage, thus hindering utility in high-performance applications. Here, in this study, we describe the vapor-phase functionalization of a 2D TMD with carbene ligands, specifically tungsten disulfide (WS₂) with N-heterocyclic carbenes (NHCs), resulting in molecularly smooth, thin, and uniform adlayers. Reacting NHCs with monolayer WS₂ reduces the broad photoluminescence background observed at cryogenic temperatures by 58%, which facilitates the detection of single-photon emitters from strained monolayer WS₂, as indicated by second order correlation values (g⁽²⁾) as low as 0.17 ± 0.07. Chemical characterization coupled with density functional theory calculations suggests that the NHC adlayer has a dual defect-passivation and doping effect on monolayer WS₂ that results in enhanced single-photon emission. Overall, this study establishes vapor-phase carbene functionalization as a homogeneous surface modification scheme for tailoring the quantum emission properties of semiconducting 2D TMDs.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Department of Commerce; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

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

OSTI ID:: 2588399

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 23 Vol. 19; ISSN 1936-0851; ISSN 1936-086X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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