Approaching the Quantum Limit of Optical Rotatory Dispersion: From First-Principles to Single-Photon Monochromators

Abstract

Optical rotatory dispersion (ORD) in chiral media, classically demonstrated as the "sweet monochromator," provides a robust mechanism for liquid-tunable spectral filtering. However, the ultimate physical boundaries governing its spectral bandwidth remain fundamentally unexplored beyond classical electromagnetic theory. Here, we present a comprehensive framework bridging macroscopic optical filtering with the quantum electrodynamic (QED) limits of chiral light-matter interaction. Using time-dependent density functional theory (TD-DFT) combined with Boltzmann conformational averaging, we accurately compute the ORD curves of representative saccharide systems, revealing that the theoretical minimum bandwidth is intrinsically tied to the anomalous dispersion (Cotton effect) near the molecular absorption band. While our macroscopic experiments demonstrate a classical bandwidth limit of ~ 20 nm due to heterogeneous broadening and instrumental constraints, our first-principles calculations predict achievable sub-nanometer bandwidths utilizing visible-absorbing chiral molecules. Furthermore, we extrapolate this framework to the strict quantum limit, proposing a single-photon QED architecture operating at ultra-low temperatures (~ 10 mK). In this regime, the spectral purity is constrained solely by the natural lifetime of the molecular excited state, governed by the Heisenberg uncertainty principle. This work establishes the ultimate theoretical criteria for chiral optical filters and pioneers the concept of the "quantum monochromator" for ultrasensitive chiral spectroscopy and quantum information processing.