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Title: Mechanistic Investigation of Molybdenum Disulfide Defect Photoluminescence Quenching by Adsorbed Metallophthalocyanines

Journal Article · · Journal of the American Chemical Society
 [1];  [1];  [2]; ORCiD logo [2];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1];  [4];  [4]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; Northwestern Univ., Evanston, IL (United States)
  3. Northwestern Univ., Evanston, IL (United States). Nanoscale Characterization Experimental (NUANCE) Center
  4. Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials; Northwestern Argonne Institute of Science and Engineering, Evanston, IL (United States)

Lattice defects play an important role in determining the optical and electrical properties of monolayer semiconductors such as MoS2. Although the structures of various defects in monolayer MoS2 are well studied, little is known about the nature of the fluorescent defect species and their interaction with molecular adsorbates. In this study, the quenching of the low-temperature defect photoluminescence (PL) in MoS2 is investigated following the deposition of metallophthalocyanines (MPcs). The quenching is found to significantly depend on the identity of the phthalocyanine metal, with the quenching efficiency decreasing in the order CoPc > CuPc > ZnPc, and almost no quenching by metal-free H2Pc is observed. Futher, time-correlated single photon counting (TCSPC) measurements corroborate the observed trend, indicating a decrease in the defect PL lifetime upon MPc adsorption, and the gate voltage-dependent PL reveals the suppression of the defect emission even at large Fermi level shifts. Density functional theory modeling argues that the MPc complexes stabilize dark negatively charged defects over luminescent neutral defects through an electrostatic local gating effect. These results demonstrate the control of defectbased excited-state decay pathways via molecular electronic structure tuning, which has broad implications for the design of mixeddimensional optoelectronic devices.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM) and Laboratory Computing Resource Center (LCRC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1846383
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 41 Vol. 143; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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