Description
Magnetic field effects (MFEs) and magnetic isotope effects (MIEs) have been proposed as potential modulator of adenosine triphosphate (ATP) synthesis via a transient spin dependent intermediate due to coupling between adenosine diphosphate (ADP) and a free ion. The hypothesis originally advanced by Buchachenko et al.[1] has motivated significant theoretical and experimental interest; however, independent confirmation of these phenomena is limited and is a subject of ongoing debate[2,3]. Here, we investigate the microscopic conditions under which magnetic sensitivity may emerge in spin-sensitive chemistry in the ATP synthesis model[4]. Using a quantum dynamical framework motivated by phonon-assisted quantum chemistry, we examine the role of spin-orbit-mediated and hyperfine-mediated spin mixing. Our results indicate that phonon-mediated contributions dominate spin evolution under biologically relevant parameter regimes, leading to field-dependent modulation of spin populations. In particular, we identify regimes of orientation-independent (5 mT) and orientation-dependent (50 mT) field strengths which facilitate enhanced spin evolution. This does not result in any significant MFE, but a clear MIE is observed when incorporating vibronic contributions, increasing ATP synthesis yields by up to 45% with respect to downstream radical pair population kinetics. These findings define microscopic constraints under which magnetic sensitivity may arise in ATP synthesis and provide a mechanistic framework that refines the previously proposed model, offering testable signatures of magnetosensitvity in enzymatic systems.
[1] Buchachenko, Kuznetsov, & Arkhangel’sky; Doklady Biochemistry
and Biophysics, 2004; 396, 1-6, 197–199.
[2] Crotty, Silkstone, Poddar, Ranson, Prina-Mello, Wilson, & Coey;
Proceedings of the National Academy of Sciences, 2011; 109, 5,
1437-1442.
[3] Hore; Proceedings of the National Academy of Sciences, 2012; 109, 5,
1357–1358.
[4] Manian, Paz, Raza, & Yu; ChemRXIV:10.26434/chemrxiv.15000458/v1.
| I am the presenting author | Yes |
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