Optical identification of sulfur vacancies: Bound excitons at the edges of monolayer tungsten disulfide

Science Advances
Victor CarozoMauricio Terrones

Abstract

Defects play a significant role in tailoring the optical properties of two-dimensional materials. Optical signatures of defect-bound excitons are important tools to probe defective regions and thus interrogate the optical quality of as-grown semiconducting monolayer materials. We have performed a systematic study of defect-bound excitons using photoluminescence (PL) spectroscopy combined with atomically resolved scanning electron microscopy and first-principles calculations. Spatially resolved PL spectroscopy at low temperatures revealed bound excitons that were present only on the edges of monolayer tungsten disulfide and not in the interior. Optical pumping of the bound excitons was sublinear, confirming their bound nature. Atomic-resolution images reveal that the areal density of monosulfur vacancies is much larger near the edges (0.92 ± 0.45 nm-2) than in the interior (0.33 ± 0.11 nm-2). Temperature-dependent PL measurements found a thermal activation energy of ~36 meV; surprisingly, this is much smaller than the bound-exciton binding energy of ~300 meV. We show that this apparent inconsistency is related to a thermal dissociation of the bound exciton that liberates the neutral excitons from negatively charged point defects...Continue Reading

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Citations

Jul 1, 2017·The Journal of Physical Chemistry Letters·Long YuanLibai Huang
Aug 22, 2018·Nanoscale·Pawan KumarViswanath Balakrishnan
Oct 16, 2018·Advanced Materials·Jichen DongFeng Ding
Mar 13, 2020·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Durgesh Kumar SharmaSushil Auluck
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Jul 8, 2020·Journal of Computational Chemistry·Adriana PecoraroMichele Pavone
May 30, 2019·Science Advances·Fu ZhangMauricio Terrones
Dec 5, 2020·Advanced Materials·Matthias WurdackElena A Ostrovskaya
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Mar 17, 2020·ACS Applied Materials & Interfaces·Yusuf Koçak, Emre Gür

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Methods Mentioned

BETA
atomic force microscopy
transmission electron microscopy
scanning electron microscopy
AFM

Software Mentioned

BerkeleyGW
Quantum ESPRESSO package
QSTEM
QUANTIFOIL
ImageJ
Vienna Ab initio Simulation Package

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