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Abstract The homogeneous exciton linewidth, which captures the coherent quantum dynamics of an excitonic state, is a vital parameter in exploring light–matter interactions in 2D transition metal dichalcogenides (TMDs). An efficient control of the exciton linewidth is of great significance, and in particular of its intrinsic linewidth, which determines the minimum timescale for the coherent manipulation of excitons. However, such a control is rarely achieved in TMDs at room temperature (RT). While the intrinsic A exciton linewidth is down to 7 meV in monolayer WS2, the reported RT linewidth is typically a few tens of meV due to inevitable homogeneous and inhomogeneous broadening effects. Here, it is shown that a 7.18 meV near‐intrinsic linewidth can be observed at RT when monolayer WS2is coupled with a moderate‐refractive‐index hydrogenated silicon nanosphere in water. By boosting the dynamic competition between exciton and trion decay channels in WS2through the nanosphere‐supported Mie resonances, the coherent linewidth can be tuned from 35 down to 7.18 meV. Such modulation of exciton linewidth and its associated mechanism are robust even in presence of defects, easing the sample quality requirement and providing new opportunities for TMD‐based nanophotonics and optoelectronics.
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Contributions to the optical linewidth of shallow donor-bound excitonic transition in ZnO
Neutral shallow donors in zinc oxide (ZnO) are spin qubits with optical access via the donor-bound exciton. This spin–photon interface enables applications in quantum networking, memories, and transduction. Essential optical parameters which impact the spin–photon interface include radiative lifetime, optical inhomogeneous and homogeneous linewidth, and optical depth. We study the donor-bound exciton optical linewidth properties of Al, Ga, and In donors in single-crystal ZnO. The ensemble photoluminescence linewidth ranges from 4 to 11 GHz, less than two orders of magnitude larger than the expected lifetime-limited linewidth. The ensemble linewidth remains narrow in absorption through samples with an estimated optical depth up to several hundred. The primary thermal relaxation mechanism is identified and found to have a negligible contribution to the total linewidth at 2 K. We find that inhomogeneous broadening due to the disordered isotopic environment in natural ZnO is significant, contributing 2 GHz. Two-laser spectral hole burning measurements indicate that the dominant mechanism, however, is homogeneous. Despite this broadening, the high homogeneity, large optical depth, and potential for isotope purification indicate that the optical properties of the ZnO donor-bound exciton are promising for a wide range of quantum technologies, and motivate a need to improve the isotope and chemical purity of ZnO for quantum technologies.
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- Award ID(s):
- 2212017
- PAR ID:
- 10484893
- Publisher / Repository:
- Optical Society of America
- Date Published:
- Journal Name:
- Optica Quantum
- Volume:
- 2
- Issue:
- 1
- ISSN:
- 2837-6714
- Format(s):
- Medium: X Size: Article No. 7
- Size(s):
- Article No. 7
- Sponsoring Org:
- National Science Foundation
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