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arXiv:2605.08307

Chiral-Induced Spin Selectivity Regulates Triplet formation in Heliobacterial Photosynthesis

Parul Raghuvanshi, Vishvendra Singh Poonia

physics.bio-phquant-phSubmitted May 8, 2026• Announced May 11, 2026• Revised Jul 5, 2026 (v2)
v1 · May 8, 2026v2 · Jul 5, 2026
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Abstract

Triplet formation and its regulation have always been of central interest in understanding the photophysical behavior of living systems. In organic systems, excessive triplet formation poses significant challenges, as it can promote photochemical damage and reduce the efficiency of charge separation processes, making its regulation critically important.Here, we present a theoretical investigation of the intrinsic quantum spin dynamics governing triplet formation in the heliobacterial reaction center, a system that operates without any internal magnetic field. Using an open quantum systems approach based on the Lindblad formalism, we simulate the spin-correlated radical pair dynamics occurring during charge separation in the heliobacterial reaction center. The study systematically examines how triplet formation is regulated by variations in two key parameters, hyperfine coupling strengths and recombination rates, and how this regulation is further influenced by the inclusion of chirality-induced spin selectivity (CISS) in conjunction with the radical pair mechanism (RPM). Our results demonstrate that the CISS effect significantly suppresses triplet formation across the parameter space relevant to the heliobacterial molecular environment, revealing an intrinsic quantum protective mechanism operating through spin control in heliobacterial photosynthesis.

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Triplet formation and its regulation have always been of central interest in understanding the photophysical behavior of living systems. In organic systems, excessive triplet formation poses significant challenges, as it can promote photochemical damage and reduce the efficiency of charge separation processes, making its regulation critically important.Here, we present a theoretical investigation of the intrinsic quantum spin dynamics governing triplet formation in the heliobacterial reaction center, a system that operates without any internal magnetic field. Using an open quantum systems approach based on the Lindblad formalism, we simulate the spin-correlated radical pair dynamics occurring during charge separation in the heliobacterial reaction center. The study systematically examines how triplet formation is regulated by variations in two key parameters, hyperfine coupling strengths and recombination rates, and how this regulation is further influenced by the inclusion of chirality-induced spin selectivity (CISS) in conjunction with the radical pair mechanism (RPM). Our results demonstrate that the CISS effect significantly suppresses triplet formation across the parameter space relevant to the heliobacterial molecular environment, revealing an intrinsic quantum protective mechanism operating through spin control in heliobacterial photosynthesis.
This work investigates the effect of chirality-induced spin selectivity (CISS) on quantum coherence in the radical-pair (RP) mechanism of avian magnetoreception. Additionally, we examine the correlation of global and local coherence measures with the yield of the signaling state in the RP model. We find that both relative entropy of global coherence and local coherence in the radical pair increase with CISS. However, only global coherence shows a strong correlation with the signaling state yield and thus indicates a plausible utilitarian role for the avian compass. We also analyze the interplay of dipolar and exchange interaction with the CISS and their effect on the coherence of the radical-pair spin. Further, we analyze the effect of environmental decoherence along with CISS. We conclude that a high CISS results in a high correlation of global coherence with signaling state yield. We propose that CISS might play an important role in developing quantum technologies by sustaining coherence in radical-pair-like quantum systems.
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--χχχB--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--χχχB--A complexes are fully compatible with a spinterface mechanism, providing a unified conceptual framework for interpreting both device-based and molecule-internal CISS platforms.
Radical-ion pairs, fundamental for understanding photosynthesis and the avian magnetic compass, were recently shown to be biological open quantum systems. We here show that the coupling of the radical-pair's spin degrees of freedom to its decohering vibrational reservoir leads to a shift of the radical-pair's magnetic energy levels. The Lamb shift Hamiltonian is diagonal in the singlet-triplet basis, and results in a singlet-triplet energy splitting physically indistinguishable from an exchange interaction. This could have profound implications for understanding photosynthetic reaction centers.
Chiral-induced spin selectivity (CISS) enables spin selectivity of charge carriers in chiral molecular systems without magnetic materials. While spin selectivity has been widely investigated, its quantum coherence has not yet been explored. Here, we investigate spin-dependent photoluminescence (PL) dynamics in multilayer quantum-dot (QD) assemblies coupled by chiral linkers. Using circularly polarized excitation in the presence of an external magnetic field, we observe a pronounced modulation of the PL lifetime that depends on the magnetic field magnitude and geometry. The lifetime difference between left- and right-circularly polarized excitations exhibits a field-angle dependence, consistent with spin precession driven by the transverse magnetic-field component relative to the chiral axis. A model incorporating coupled spin precession and decay processes reproduces the experimental trends. These results establish chiral QD assemblies as a room-temperature platform for probing quantum coherent manifestations of the CISS effect, with implications for spintronic and quantum technologies.
Identification of the external electromagnetic fields and internal hyperfine parameters which optimize the quantum singlet-triplet yield of simplified radical pairs modeled by Schrödinger system with spin Hamiltonians given by the sum of Zeeman interaction and hyperfine coupling interaction terms are analyzed. A method that combines sensitivity analysis with Tikhonov regularization is implemented. Numerical results demonstrate that the quantum singlet-triplet yield of the radical pair system can be significantly reduced if optimization is pursued simultaneously for both external magnetic fields and internal hyperfine parameters. The results may contribute towards understanding the structure-function relationship of a putative magnetoreceptor to manipulate and enhance quantum coherences at room temperature and leveraging biofidelic function to inspire novel quantum devices.
We provide a theoretical analysis of spin-selective recombination processes in clusters of n ≥ 3 radicals. Specifically, we discuss how spin correlation can ensue from random encounters of n radicals, i.e., "F-clusters" as a generalization of radical F-pairs, acting as precursors of spin-driven magnetic field effects. Survival probabilities and the spin correlation of the surviving radical population, as well as transients, are evaluated by expanding the spin density operator in an operator basis that is closed under application of the Haberkorn recombination operator and singlet-triplet dephasing. For the primary spin cluster, the steady-state density operator is found to be independent of the details of the recombination network, provided that it is irreducible; pairs of surviving radicals are triplet-polarized independent of whether they are actually reacting with each other. The steady state is independent of the singlet-triplet dephasing, but the kinetics and the population of sister clusters of smaller size can depend on the degree of dephasing. We also analyze reaction-induced singlet-triplet interconversion in radical pairs due to radical scavenging by initially uncorrelated radicals ("chemical Zeno effect"). We generalize previous treatments for radical triads by discussing the effect of spin-selective recombination in the original pair and extending the analysis to four radicals, i.e., radical pairs interacting with two radical scavengers.