期刊
NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-022-30016-0
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资金
- Swiss Innovation Agency (Innosuisse) [32908.1 IP-EE]
- European Union through Horizon 2020 research and innovation program [819740]
- Netherlands Organization of Scientific Research (NWO) [723.013.002]
- NWO [722.017.011]
- Swiss National Supercomputing Centre (CSCS) [s1003]
- Swiss National Science Foundation through the Quantum Sciences and Technology NCCR
- Air Force Office of Scientific Research
- Office of Naval Research [FA8655-21-1-7013]
- European Union [899141]
- Swiss National Science Foundation [188404]
Semiconductor quantum dots, considered as artificial atoms, have broader emission spectrum than atomic emission lines. By simulating the interactions between excitons and surface phonons, the emission line-broadening in quantum dots can be controlled.
Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr3 quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35-65 meV (vs. initial values of 70-120 meV), which are on par with the best values known for structurally rigid, colloidal II-VI quantum dots (20-60 meV). Ultra-narrow emission at room-temperature is desired for conventional light-emitting devices and paramount for emerging quantum light sources. Narrow emission is desired for light-emitting devices. Here, Kovalenko et al. demonstrate that the emission line-broadening in perovskite quantum dots is dominated by the coupling between excitons and surface phonon modes which can be controlled by minimal surface modifications.
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