arXiv subjects

Yang-Cheng Ye

Publications and source records attributed to Yang-Cheng Ye.

3 recordsLinked to original sources

arXiv2026

Quantum Dynamics of Enantiomers in Chiral Optical Cavities

Chirality, the absence of mirror symmetry, is a fundamental molecular property with far-reaching consequences from chemistry to biology. Yet enantiosensitive optical responses are very weak. Here, we introduce a theoretical framework in which a chiral optical cavity under strong coupling directly lifts the degeneracy of opposite enantiomers at the electronic-dipole level. The cavity's parity-breaking field inside the cavity induces distinct site-energy shifts for left- versus right-handed molecules, producing robust enantioselective polariton states that overcome the weakness of traditional chiroptical effects. Using cavity quantum electrodynamics simulations, we show that strong light-matter coupling reshapes the polaritonic energy landscape and leads to enantiomer-specific coherence lifetimes and relaxation pathways. To reveal these dynamics, we propose ultrafast two-dimensional electronic spectroscopy (2DES) as a probe, capable of resolving polaritonic splittings on femtosecond timescales. Simulated 2DES spectra exhibit unambiguous enantioselective signatures of the cavity-induced asymmetry. These findings establish that chiral cavities provide a powerful platform for detecting and controlling molecular handedness beyond the limits of conventional optical methods.

physics.optics↗

arXiv2025

Controlling Nonadiabatic Transitions Through Engineered Ultrafast Laser Fields at Conical Intersections

In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes.

quant-ph↗

arXiv2025

Unraveling Geometric-phase at Conical Intersection by Cavity-enhanced Two-dimensional Electronic Spectroscopy

The geometric phase is a fundamental quantum mechanical phenomenon uniquely associated with conical intersections (CI) between potential energy surfaces and serves as a definitive signature of their presence. In this study, we propose a novel spectroscopic approach to directly detect the geometric phase using two-dimensional electronic spectroscopy (2DES) enhanced by strong light-matter interactions within an optical cavity. Focusing on a prototypical pentacene dimer undergoing singlet fission, we model the nonadiabatic wave packet dynamics as it evolves through a CI between electronically excited states. The optical cavity enables dynamic modulation of the coupling between the optical field and molecular vibrational modes, allowing precise control over the wave packet pathways. Importantly, we identify a cancellation in the spectral amplitude, arising from phase differences accumulated along different trajectories, which serves as a clear spectroscopic manifestation of the geometric phase (GP). This cavity-enhanced 2DES framework not only enables direct observation of GP effects but also offers a versatile platform for probing ultrafast nonadiabatic processes. Our results provide fundamental insights into topological effects in molecular dynamics and pave the way for experimental strategies in quantum control, photochemistry, and the design of advanced optoelectronic materials.

physics.optics↗