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Title: Ultrahigh-Purity Single-Photon Emission from 2D WSe 2 via Effective Suppression of Classical Emission
Award ID(s):
2246564 1943895 2235276 2326628 2503230 1753054 2103842 2443684 2326837
PAR ID:
10612870
Author(s) / Creator(s):
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Publisher / Repository:
ACS
Date Published:
Journal Name:
Nano Letters
ISSN:
1530-6984
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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  1. Realizing stimulated emission from defects in 2D layered semiconductors has the potential to enhance the sensitivity of characterizing their defects. However, stimulated emission from defects in layered materials presents a different set of challenges in carrier lifetime and energy level design and has not been achieved so far. Here, we combine photoluminescence (PL) spectroscopy, Raman spectroscopy, and first-principles theory to reveal an anomalous PL intensity-temperature relation and strong polarization effects at a defect emission peak in annealed multilayer MoS2, suggesting defect-based stimulated emission. The emergence of stimulated emission behavior is also controllable (by temperature) and reversible. The observed stimulated emission behavior is supported by a three-level system involving two defect levels from chalcogen vacancies and a pump level from the conduction band edge. First-principles calculations show that the special indirect gap that enables stimulated emission is not native to pristine bulk MoS2 and only emerges under thermal strain. 
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