Light-induced electron spin qubit coherences in the purple bacteria reaction center protein.

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Photosynthetic reaction center proteins (RCs) provide ideal model systems for studying quantum entanglement between multiple spins, a quantum mechanical phenomenon wherein the properties of the entangled particles become inherently correlated. Following light-generated sequential electron transfer, RCs generate spin-correlated radical pairs (SCRPs), also referred to as entangled spin qubit (radical) pairs (SQPs). Understanding and controlling coherence mechanisms in SCRP/SQPs is important for realizing practical uses of electron spin qubits in quantum sensing applications. The bacterial RC (bRC) provides an experimental system for exploring quantum effects in the SCRP P865+ QA-, where P865, a special pair of bacteriochlorophylls, is the primary donor, and QA is the primary quinone acceptor. In this study, we focus on understanding how local molecular environments and isotopic substitution, particularly deuteration, influence spin coherence times (TM). Using high-frequency electron paramagnetic resonance (EPR) spectroscopy, we observed that the local environment surrounding P865 and QA plays a significant role in determining TM. Our findings show that while deuteration led to a modest increase in TM, particularly at low temperatures, but the effect was substantially smaller than predicted by classical nuclear spin diffusion alone. This result is in contrast to our previous study of the photosystem I (PSI) RC, where no increase in TM was observed upon deuteration. Theoretical modeling identified several methyl groups at key distances from the spin centers of both bRC and PSI, and methyl group tunneling at low temperatures has been previously suggested as a mechanism for enhanced spin decoherence. Additionally, our study revealed a strong dependence of spin coherence on the orientation of the external magnetic field, highlighting the influence of the protein microenvironment on spin dynamics. These results offer new insights for optimizing coherence times in quantum system design for quantum information science and sensing applications.