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Quantum Dynamics of Enantiomers in Chiral Optical Cavities

Yang-Cheng Ye, Panpan Zhang, Ajay Jha, Fulu Zheng, Hong-Guang Duan

Abstract

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.

Quantum Dynamics of Enantiomers in Chiral Optical Cavities

Abstract

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.
Paper Structure (5 equations, 4 figures)

This paper contains 5 equations, 4 figures.

Figures (4)

  • Figure 1: Chiral cavity (left and right circularly polarized light) with 1-Fluoroethanamine molecule inside.
  • Figure 2: The 2DES with left- (a, d and g) and right-handed (b, e and h) chiral cavity at waiting time of T = 0 fs. The differential signal of subtracting from left- to the right-handed cavities, the resulted data is shown in (c), (f) and (i), respectively.
  • Figure 3: (a, c and e)Time-resolved traces and residuals of peaks A, B and C. The fitting curves are plotted as red and blue dashed lines. The time-resolved residuals are plotted as blue and red solid lines in (b), (d) and (f).
  • Figure 4: Results after wavelet analysis of peak A in (a) and (b). The wavelet resulted data of cross peak B are in (c) and (d). (c and f) show the wavelet resulted data with resolved vibrational coherences.