Substrates modulate charge-reorganization allosteric effects in protein-protein association

Banerjee-Ghosh, Koyel; Ghosh, Shirsendu; Levy, Dorit; Riven, Inbal; Naaman, Ron; Haran, Gilad

doi:10.1101/2021.02.11.430712

Cited by 3 publications

(4 citation statements)

References 20 publications

(24 reference statements)

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“…The findings here, combined with previous studies (10, 11), point to a new role of charge reorganization, or of polarizability, in modulating protein activities. Surprisingly, not much is known about the involvement of polarizability in protein function, though the development of polarizable force fields for molecular dynamics simulations of biomolecules in recent years may change this situation(19).…”

Section: Discussionsupporting

confidence: 80%

“…Due to their internal conformational dynamics, as well as the presence of titratable side chains, proteins may possess significant polarizability values. Recent computational work from Takano and coworkers [6][7] , and experimental work from our labs [8][9] has indeed hinted at a role for charge reorganization as an allosteric signal in proteins. Here we decisively establish this role by studying the effect of phototriggered charge injection on both protein-protein association kinetics and enzyme kinetics.…”

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confidence: 93%

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Control of protein activity by photoinduced spin polarized charge reorganization

Ghosh

Banerjee-Ghosh

Levy

et al. 2021

Preprint

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Biomolecules within the living cell are subject to extensive electrical fields, particularly next to membranes. Indeed, a role for bioelectricity has been well established at the organismal level. While the importance of electrostatics in protein functions such as protein-protein association and enzymatic activity has been well documented, very little is known on how biomolecules respond to external electric fields, or in other words, what may be the potential contribution of polarizability to protein function. Here we use phototriggered charge injection from a site-specifically attached ruthenium photosensitizer to directly demonstrate the effects of charge redistribution within a protein. We find that binding of an antibody to phosphoglycerate kinase (PGK) is increased two folds under illumination. Remarkably, illumination is found to suppress the enzymatic activity of PGK by a factor as large as three. These responses are sensitive to the photosensitizer position on the protein. Surprisingly, left (but not right) circularly polarized light elicits these responses, indicating that the electrons involved in the observed dynamics are spin polarized, due to spin filtration by protein chiral structures. Our results directly establish the contribution of electrical polarization and the importance of the spin-dependent charge reorganization in the function of proteins. Future experiments with phototriggered charge injection will allow delineation of charge rearrangement pathways within proteins and will further depict their effects on protein function.

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Section: Discussionsupporting

confidence: 80%

mentioning

confidence: 93%

Control of protein activity by photoinduced spin polarized charge reorganization

Ghosh

Banerjee-Ghosh

Levy

et al. 2021

Preprint

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“…Ghosh et al further reported that the degree of binding modulation may be tuned through control of the dipole moment across the binding antigen. 68 The unmodified antigen used in the experiments described thus far binds to the surfacetethered antibody at its positively charged C-terminus. However, upon binding a negatively charged substrate molecule, the dipole moment across the antigen was found to decrease, thus reducing the induced charge redistribution across the antibody.…”

Section: Chiral-induced Spin Selectivity: Recent Advancesmentioning

confidence: 98%

A Chirality-Based Quantum Leap

Aiello¹,

Abbas²,

Abendroth³

et al. 2022

ACS Nano

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There is increasing interest in the study of chiral degrees of freedom occurring in matter and in electromagnetic fields. Opportunities in quantum sciences will likely exploit two main areas that are the focus of this Review: (1) recent observations of the chiral-induced spin selectivity (CISS) effect in chiral molecules and engineered nanomaterials and (2) rapidly evolving nanophotonic strategies designed to amplify chiral light–matter interactions. On the one hand, the CISS effect underpins the observation that charge transport through nanoscopic chiral structures favors a particular electronic spin orientation, resulting in large room-temperature spin polarizations. Observations of the CISS effect suggest opportunities for spin control and for the design and fabrication of room-temperature quantum devices from the bottom up, with atomic-scale precision and molecular modularity. On the other hand, chiral–optical effects that depend on both spin- and orbital-angular momentum of photons could offer key advantages in all-optical and quantum information technologies. In particular, amplification of these chiral light–matter interactions using rationally designed plasmonic and dielectric nanomaterials provide approaches to manipulate light intensity, polarization, and phase in confined nanoscale geometries. Any technology that relies on optimal charge transport, or optical control and readout, including quantum devices for logic, sensing, and storage, may benefit from chiral quantum properties. These properties can be theoretically and experimentally investigated from a quantum information perspective, which has not yet been fully developed. There are uncharted implications for the quantum sciences once chiral couplings can be engineered to control the storage, transduction, and manipulation of quantum information. This forward-looking Review provides a survey of the experimental and theoretical fundamentals of chiral-influenced quantum effects and presents a vision for their possible future roles in enabling room-temperature quantum technologies.

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“…Due to the CISS effect, the spin polarization of a chiral molecule, such as a protein, can be influenced by interacting or binding it to a magnetized surface. 23,24 Spin distribution in a protein can be altered by controlling the magnetization of the surface to which it is adsorbed, owing to a compensational response to spin exchange interactions between the protein and the surface. 21 Moreover, chiral molecules themselves can orient paramagnetic surface magnetization according to their preferred spin direction.…”

Section: Introductionmentioning

confidence: 99%