Condensed-matter emitters offer enriched cavity quantum electrodynamical effects due to the coupling to external degrees of freedom. In the case of carbon nanotubes, a very peculiar coupling between localized excitons and the one-dimensional acoustic phonon modes can be achieved, which gives rise to pronounced phonon wings in the luminescence spectrum. By coupling an individual nanotube to a tunable optical microcavity, we show that this peculiar exciton-phonon coupling is a valuable resource to enlarge the tuning range of the single-photon source while keeping an excellent exciton-photon coupling efficiency and spectral purity. Using the unique flexibility of our scanning fiber cavity, we are able to measure the efficiency spectrum of the very same nanotube in the Purcell regime for several mode volumes. Whereas this efficiency spectrum looks very much like the free-space luminescence spectrum when the Purcell factor is small (large mode volume), we show that the deformation of this spectrum at lower mode volumes can be traced back to the strength of the exciton-photon coupling. It shows an enhanced efficiency on the red wing that arises from the asymmetry of the incoherent energy exchange processes between the exciton and the cavity. This allows us to obtain a tuning range up to several hundred times the spectral width of the source.
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http://dx.doi.org/10.1021/acs.nanolett.7b00973 | DOI Listing |
Nano Lett
January 2025
Department of Chemistry, University of Rochester, Rochester, New York 14627, United States.
Recent experiments have shown that exciton transport can be significantly enhanced through hybridization with confined photonic modes in a cavity. The light-matter hybridization generates exciton-polariton (EP) bands, whose group velocity is significantly larger than the excitons. Dissipative mechanisms that affect the constituent states of EPs, such as exciton-phonon coupling and cavity loss, have been observed to reduce the group velocities in experiments.
View Article and Find Full Text PDFACS Mater Au
January 2025
Beijing National Laboratory for Molecular Science, State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
Two-dimensional lead iodide perovskites have attracted significant attention for their potential applications in optoelectronic and photonic devices due to their tunable excitonic properties. The choice of organic spacer cations significantly influences the light emission and exciton transport properties of these materials, which are vital for their device performance. In this Perspective, we discuss the impact of spacer cations on lattice dynamics and exciton-phonon coupling, focusing on three representative 2D lead iodide perovskites that exhibit distinct types of structural distortions.
View Article and Find Full Text PDFJ Phys Chem Lett
December 2024
School of Physics and Astronomy, Applied Optics Beijing Area Major Laboratory, Center for Advanced Quantum Studies, Beijing Normal University, Beijing 100875, China.
2D hybrid organic-inorganic perovskites (HOIPs) have great prospects in new-generation photovoltaic and luminescence applications. The complex interaction between exciton and lattice motions plays an important role in determining the exciton properties of 2D HOIPs. However, the exploration of the regulation mechanism of phonons and the exciton-phonon (ex-ph) interaction is still very limited, especially for Dion-Jacobson (DJ) type 2D HOIPs.
View Article and Find Full Text PDFNanoscale
January 2025
Departments of Chemistry and Physics, Universität Hamburg, Luruper Chaussee 149, D-22761 Hamburg, Germany.
We used a computational method based on (constrained) density functional theory to obtain the photoluminescence spectrum of graphene quantum dots with up to 240 carbon atoms, including the effect of multiphonons. We found that only a few phonon modes couple effectively to the excitons, namely one size- and shape-dependent global mode and two high frequency local modes. The exciton-phonon coupling decreases with increasing size for all structures and has a magnitude in the mid-range, leading to only relatively small multiphonon effects.
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