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arXiv:2603.02735

Geometric mechanisms enabling spin- and enantio-sensitive observables in one photon ionization of chiral molecules

Philip Caesar M. Flores, Stefanos Carlström, Serguei Patchkovskii, Misha Ivanov, Andres F. Ordonez, Olga Smirnova

physics.atom-phquant-phSubmitted Mar 3, 2026• Announced Mar 4, 2026• Revised Mar 13, 2026 (v2)

v1 · Mar 3, 2026 v2 · Mar 13, 2026 v3 · Jun 11, 2026

Abstract

We examine spin-resolved photoionization of randomly oriented chiral molecules via circularly polarized light, and revisit earlier predictions of Cherepkov (J. Phys. B: Atom. Mol. Phys. 16, 1543, 1983). We will show that the dynamical origin of spin- and enantio-sensitive observables arise from two intrinsic mechanisms that are quantified by two pseudovectors stemming from the geometric properties of the photoionization dipoles in spin space and in real space, and an extrinsic mechanism which is a directional bias introduced by the well-defined direction of light polarization. These mechanisms arise solely from electric dipole interactions. Consequently, this means that the ten independent parameters that was earlier predicted by Cherepkov to fully describe spin-resolved photoionization of chiral molecules can be reduced as moments of these three pseudovectors. We also find that the molecular pseudoscalars describing the spin- and enantio-sensitive components of the yield can be described by the flux of these pseudovectors through the energy shell, which changes sign upon switching enantiomers. Our results provide compact expressions for these observables which provide an intuitive picture on what determines the strength of these spin- and enantio-sensitive observables. The approach can be readily generalized to photoexcitation, multiphoton processes, and arbitrary field polarizations. Regardless of the specific driving conditions, the resulting spin- and enantio-sensitive observables are still controlled by the same three pseudovectors, underscoring their universal role as the primary generators of chirality-induced spin asymmetries, emphasizing their fundamental geometric origin and the universality of the mechanism identified here.

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We examine spin-resolved photoionization of randomly oriented chiral molecules via circularly polarized light, and revisit earlier predictions of Cherepkov (J. Phys. B: Atom. Mol. Phys. 16, 1543, 1983). We will show that the dynamical origin of spin- and enantio-sensitive observables arise from two intrinsic mechanisms that are quantified by two pseudovectors stemming from the geometric properties of the photoionization dipoles in spin space and in real space, and an extrinsic mechanism which is a directional bias introduced by the well-defined direction of light polarization. These mechanisms arise solely from electric dipole interactions. Consequently, this means that the ten independent parameters that was earlier predicted by Cherepkov to fully describe spin-resolved photoionization of chiral molecules can be reduced as moments of these three pseudovectors. We also find that the molecular pseudoscalars describing the spin- and enantio-sensitive components of the yield can be described by the flux of these pseudovectors through the energy shell, which changes sign upon switching enantiomers. Our results provide compact expressions for these observables which provide an intuitive picture on what determines the strength of these spin- and enantio-sensitive observables. The approach can be readily generalized to photoexcitation, multiphoton processes, and arbitrary field polarizations. Regardless of the specific driving conditions, the resulting spin- and enantio-sensitive observables are still controlled by the same three pseudovectors, underscoring their universal role as the primary generators of chirality-induced spin asymmetries, emphasizing their fundamental geometric origin and the universality of the mechanism identified here.

The chirality-induced spin selectivity (CISS) effect has been invoked to explain recent reports of differences in the time-resolved EPR signals between chiral and achiral molecules. However, the microscopic origin of these differences and their connection to CISS remains contested, particularly since these systems lack a metal interface. Here we introduce an intramolecular spinterface-like mechanism that naturally arises within donor-chiral bridge-acceptor (D--

χ

B--A) complexes and quantitatively reproduces experimentally reported observed spin polarization in time-resolved EPR studies. In our two-electron Lindblad model, the photoexcited charge-transfer electron traversing the chiral bridge exchanges with the residual donor electron, which acts as a localized magnetic moment analogous to an induced magnetic moment on an electrode surface. The resulting through-bridge charge current produces an effective solenoidal field at the donor--bridge interface, breaking spin degeneracy and directional symmetry, thus enabling spin-selective transport without invoking intrinsic spin-orbit coupling on the bridge. We show that the interplay between this current-induced field, donor thermalization (which breaks time-reversal symmetry), and bridge spin mixing yields tens-of-percent polarization over realistic experimental conditions and charge-transfer time scales, matching reported CISS signatures in triads and DNA hairpins. By explicitly resolving the dependence on solenoidal coupling strength, temperature, and spin-mixing rates, the model identifies the regime in which internal spinterfaces can generate robust CISS-like spin filtering. These findings demonstrate that CISS-like signals in isolated D--

χ

B--A complexes are fully compatible with a spinterface mechanism, providing a unified conceptual framework for interpreting both device-based and molecule-internal CISS platforms.

Molecular chirality plays a crucial role in physics, chemistry, life sciences and pharmacology. Nowadays, the chiral discrimination and control at the single-molecule level is urgently needed to reveal the origin of the chirality-relevant phenomena by recovering the information disturbed by the ensemble averaging. The method of magnetic resonance (MR), as one of powerful tools for structure analysis, is blind to the molecular chirality in the absence of a chiral reagent. Here we propose and experimentally demonstrate a direct MR-based method for determining the chirality at the single-molecule level through constructing the symmetry-breaking dynamics of nearby nuclear spins. In principle, the mirror asymmetry of two enantiomers in real space is manifested by breaking the joint symmetry of the mirror reflection and time reversal in spin space under spin dynamics. Experimentally, two enantiomers are indistinguishable from the dynamics of strongly-coupled but unpolarized nuclear spins, but diverge evidently in the dynamical results that break the field-inversion symmetry after spins are polarized. Our method and results will benefit the study of chirality-induced properties in the fields of chemistry and biology.

The ability to engineer chiral light-matter interactions is a valuable resource for realizing quantum networks and non-reciprocal quantum optics. Here, we demonstrate chiral coupling between light and a negatively charged exciton state, i.e., a four-level system, embedded in a standard photonic-crystal waveguide. By controlling the orientation and strength of an external magnetic field, we tune the polarization of the individual optical transition dipoles relative to the fixed elliptically polarized waveguide mode. In a two-sided waveguide, an optimized oblique magnetic field allows a selected transition to decay exclusively into a single propagation direction, enabling near-unity directional emission (

0.99^{+0.01}_{-0.02}

), despite the waveguide exhibiting imperfect polarization for chiral coupling. We further observe two tunable chiral branching ratios, the directional analogue of optical cyclicity, for two

Λ

-systems, with one reaching

134_{-77}^{+\infty}

. The magnetic-field-dependent spectroscopy also allows reconstruction of the local guided-mode polarization at the emitter via the Stokes parameters relative to the emitter's dipole moments. Finally, we demonstrate that this local chirality enables coherent control of an electron spin via an optical Raman process mediated by waveguide driving. Building on the simultaneous realization of a large branching ratio, directionality and spin control achieved at the same oblique magnetic-field angle, we propose a protocol with high tolerance to photon loss for generating high-fidelity remote spin-spin entanglement. Our magnetic control opens a reconfigurable and generic route for enhancing on-chip chiral spin-photon coupling in standard nanophotonic interfaces without the need to carefully engineer the polarization of the waveguide.

Chirality, or handedness, is a geometrical property denoting a lack of mirror symmetry. Chirality is ubiquitous in nature and is associated with the nonreciprocal interactions observed in complex systems ranging from biomolecules to topological materials. Here, we demonstrate that chiral arrangements of dipole-coupled atoms or molecules can facilitate the helicity-dependent superradiant emission of light. We show that the collective modes of these systems experience an emergent spin-orbit coupling that leads to chirality-dependent photon transport and nontrivial topological properties. These phenomena are fully described within the electric dipole approximation, resulting in very strong optical responses. Our results demonstrate an intimate connection between chirality, superradiance, and photon helicity and provide a comprehensive framework for studying electron transport dynamics in chiral molecules using cold atom quantum simulators. Published by the American Physical Society 2024

We develop a family of chiral measures to quantify the chirality of a distribution and assign it a handedness. Our measures are built using the tensorial moments of the distribution, which naturally encode its spatial character, not only via its angular shape consistently with existing multipolar-moment approaches, but also its radial dependence. We combine these tensorial moments into a rotationally-invariant pseudoscalar using a newly-defined cross product and triple product for arbitrary symmetric tensors. We analyze these measures for a variety of toy-model distributions, providing intuition for the geometry and guiding the choice of chiral measure optimal for a given distribution. We also apply our measures to a physically-motivated example coming from photoionization in polychromatic chiral light. Our work provides a robust, flexible, intuitive, highly geometrical, and physically-driven framework for understanding and quantifying the chirality of a wide variety of distributions, together with an open-source software package that makes this toolbox readily applicable for the analysis of numerical or experimental data.

Dipoles in triangular optical ladders constitute a flexible platform for the study of the interplay between geometric frustration and long-range anisotropic interactions, and in particular for the observation of the spontaneous onset of chirality. Frustration magnifies the effect of the dipolar interactions in itinerant polarized dipolar bosons. As a result, the dipole-induced transition between a chiral superfluid and a nonchiral two-component superfluid may be observed for current state-of-the-art temperatures even for the weak intersite interaction characterizing magnetic atoms in standard optical lattices. On the other hand, pinned spin- 1 / 2 dipoles, which we discuss in the context of polar molecules in two rotational states, realize frustrated dipolar XXZ spin models. By controlling the external electric field strength and orientation, these systems can explore a rich ground-state landscape including chiral and nematic phases, as well as intriguing chiral dynamics.