Strong light-matter coupling generates hybrid states that inherit properties of both light and matter, effectively allowing the modification of the molecular potential energy landscape. This phenomenon opens up a plethora of options for manipulating the properties of molecules, with a broad range of applications in photochemistry and photophysics. In this article, we use strong light-matter coupling to transform an endothermic triplet-triplet annihilation process into an exothermic one. The resulting gradual on-off photon upconversion experiment demonstrates a direct conversion between molecular states and hybrid light-matter states. Our study provides a direct evidence that energy can relax from nonresonant low energy molecular states directly into hybrid light-matter states and lays the groundwork for tunable photon upconversion systems that modify molecular properties in situ by optical cavities rather than with chemical modifications.
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http://dx.doi.org/10.1021/jacs.1c02306 | 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 PDFSci Rep
January 2025
Terahertz Research Center, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 610054, China.
Strong light-matter coupling occurs when the rate of energy exchange between the electromagnetic mode and the molecular ensemble exceeds the competitive dissipation process. Coupled photon molecules with near-field light-matter interactions may produce new hybridized states when they reach the strong coupling region. Tunable Terahertz (THz) meta materials can be used to design sensors, optical modulators, etc.
View Article and Find Full Text PDFACS Nano
January 2025
Instituto de Física de São Carlos, Universidade de São Paulo, São Carlos 13566-590, Brazil.
Monolayers of transition-metal dichalcogenides, such as MoS, have attracted significant attention for their exceptional electronic and optical properties, positioning them as ideal candidates for advanced optoelectronic applications. Despite their strong excitonic effects, the atomic-scale thickness of these materials limits their light absorption efficiency, necessitating innovative strategies to enhance light-matter interactions. Plasmonic nanostructures offer a promising solution to overcome those challenges by amplifying the electromagnetic field and also introducing other mechanisms, such as hot electron injection.
View Article and Find Full Text PDFJ Chem Phys
January 2025
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People's Republic of China.
Vibro-polaritons are hybrid light-matter states that arise from the strong coupling between the molecular vibrational transitions and the photons in an optical cavity. Developing theoretical and computational methods to describe and predict the unique properties of vibro-polaritons is of great significance for guiding the design of new materials and experiments. Here, we present the ab initio cavity Born-Oppenheimer density functional theory (CBO-DFT) and formulate the analytic energy gradient and Hessian as well as the nuclear and photonic derivatives of dipole and polarizability within the framework of CBO-DFT to efficiently calculate the harmonic vibrational frequencies, infrared absorption, and Raman scattering spectra of vibro-polaritons as well as to explore the critical points on the cavity potential energy surface.
View Article and Find Full Text PDFAdv Mater
January 2025
Center for Hybrid Organic-Inorganic Semiconductors for Energy, Golden, Colorado, 80401, USA.
Recent activity in the area of chiroptical phenomena has been focused on the connection between structural asymmetry, electron spin configuration and light/matter interactions in chiral semiconductors. In these systems, spin-splitting phenomena emerge due to inversion symmetry breaking and the presence of extended electronic states, yet the connection to chiroptical phenomena is lacking. Here, we develop an analytical effective mass model of chiral excitons, parameterized by density functional theory.
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