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Kamyar Rashidi

Publications and source records attributed to Kamyar Rashidi.

4 recordsLinked to original sources

Optical Modulation Due to Energy Exchange Between Photonic and Exciton Modes in the Intermediate Coupling Regime

Actively tunable photonic devices are vital for next-generation optoelectronics requiring rapid switching and high bandwidth. Although organic optoelectronic devices have found wide application, their use as optical modulators has been limited by low absorption in the critical near-infrared (NIR) region, slow response time, and weak nonlinearities. To address these limitations, we developed a scheme based on intermediate exciton-photon coupling in a NIR absorbing squaraine-dye based photonic structure. Using energy-momentum resolved pump-probe spectroscopy, we show that the sign and magnitude of the optical response of our system depends strongly on the energy detuning between the excitonic and photonic modes. These data are analyzed using temporal coupled-mode theory to show that near resonance, a distinct energy exchange process emerges in the cross-over regime between strong and weak light-matter coupling. This effect enables dynamical control over the photoinduced response, providing a pathway for broadband optical signal modulation extending into the NIR spectral region.

physics.optics

Modified Transfer Matrix Method for the Extraction of Material Properties via Terahertz Time-Domain Spectroscopy

Terahertz Time-Domain Spectroscopy is a powerful technique for extracting the low-frequency optical properties of materials. However, the optical constants are difficult to determine directly from the experimental transfer function, such that various numerical approximations must be implemented to describe specific conditions. Here, we introduce a modified Transfer Matrix Method that uses a genetic algorithm for optimization to determine the refractive index of materials in the THz regime. We show that this approach is generally applicable across a wide range of refractive indices, structures, and frequency ranges. Our method is intuitive and yields accurate results compared to leading methods across a wide spectral range (0.1 - 15 THz).

physics.optics

Efficient and Tunable Photochemical Charge Transfer via Long-Lived Bloch Surface Wave Polaritons

Achieving precise control of photoinduced molecular charge transfer reactions underpins key emerging technologies. As such, the use of hybrid light-matter molecular exciton-polariton states has been proposed as a scheme to directly modify the efficiency and rate of such reactions. However, the efficacy of polariton-driven photochemistry remains an open question. Here, we demonstrate conditions under which photoinduced polaritonic charge transfer can be achieved and directly visualized using momentum resolved ultrafast spectroscopy. Key conditions for charge transfer are satisfied using Bloch surface wave polaritons, which exhibit favorable dispersion characteristics that permit the selective pumping of hybrid states with long lifetimes (100-400 fs) that permit vibrationally assisted molecular charge transfer. Using this approach, we tune the energetic driving force for charge separation, reducing it by as much as 0.5 eV compared to the bare exciton. These results establish that tunable and efficient polariton-driven molecular charge transfer is indeed possible using carefully considered photonic systems.

physics.optics

Addressing the Dark State Problem in Strongly Coupled Organic Exciton-Polariton Systems

The manipulation of molecular excited state processes through strong coupling has attracted significant interest for its potential to provide precise control of photochemical phenomena. However, the key limiting factor for achieving this control has been the dark state problem, in which photoexcitation populates long-lived reservoir states with similar energies and dynamics to bare excitons. Here, we use a sensitive ultrafast transient reflection method with momentum and spectral resolution to achieve the selective excitation of organic exciton-polaritons in open photonic cavities. We show that the energy dispersions of these systems allow us to avoid the parasitic effect of reservoir states. Under phase-matching conditions, we observe the direct population and decay of polaritons on time scales of less than 100 fs and find that momentum scattering processes occur on even faster timescales. We establish that it is possible to overcome the dark state problem through careful design of strongly coupled systems.

physics.optics