Chemical Reaction Rates for Systems with Spin–Orbit Coupling and an Odd Number of Electrons: Does Berry’s Phase Lead to Meaningful Spin-Dependent Nuclear Dynamics for a Two State Crossing?

Wu, Yanze; Miao, Gaohan; Subotnik, Joseph E.

doi:10.1021/acs.jpca.0c04562

Cited by 27 publications

(20 citation statements)

References 102 publications

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“…As previous work on a first-principles description of CISS, 36,37 our results clearly point out the need for including further mechanisms, such as electron-phonon coupling 138 or other terms resulting in leakage 35 or dephasing, 25,29 spin polarization at the interfaces, 50 and an explicit description of electron correlation and nonequilibrium effects on the electronic structure 52 (note that our electronic structures are obtained from a self-consistent field algorithm on finite systems in equilibrium). Yet, for these studies, our findings suggest that a careful study of the dependence on computational and structural parameters is crucial to prevent seemingly correct results due to error compensation.…”

Section: Discussionsupporting

confidence: 70%

The Influence of Electronic Structure Modelling and Junction Structure on First-Principles Chiral Induced Spin Selectivity

Zöllner¹,

Mújica²,

Herrmann³

2020

Preprint

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<br>We have carried out a comprehensive study of the influence of electronic structure modeling and junction structure description on the first-principles calculation of the spin polarization in molecular junctions caused by the chiral induced spin selectivity (CISS) effect. We explore the limits and the sensitivity to modelling decisions of a Landauer / Green’s function / density functional theory approach to CISS. We find that although the CISS effect is entirely attributed in the literature to molecular spin filtering, spin-orbit coupling being partially inherited from the metal electrodes plays an important role in our calculations, even though this effect cannot explain the experi- mental conductance results. Also, an important dependence on the specific description of exchange interaction and spin–orbit coupling is manifest in our approach. This is important because the interplay between exchange effects and spin-orbit coupling may play an important role in the description of the junction magnetic response. Our calculations are relevant for the whole field of spin-polarized electron transport and electron transfer because there is still an open discussion in the literature about the detailed underlying mechanism and the magnitude of relevant physical parameters that need to be included to achieve a consistent description of the CISS effect<br>

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Section: Discussionsupporting

confidence: 70%

The Influence of Electronic Structure Modelling and Junction Structure on First-Principles Chiral Induced Spin Selectivity

Zöllner¹,

Mújica²,

Herrmann³

2020

Preprint

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show abstract

“…This clearly suggests a need for including further mechanisms, such as electron–phonon coupling , or other terms resulting in leakage or dephasing, , spin polarization at the interfaces, and an explicit description of electron correlation and nonequilibrium effects on the electronic structure , (note that our electronic structures are obtained from a self-consistent field algorithm on finite systems in equilibrium). For these studies, our findings suggest that a careful study of the dependence on computational and structural parameters is crucial to prevent seemingly correct results due to error compensation.…”

Section: Discussionmentioning

confidence: 99%

Influence of Electronic Structure Modeling and Junction Structure on First-Principles Chiral Induced Spin Selectivity

Zöllner

Saghatchi

Mújica

et al. 2020

J. Chem. Theory Comput.

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We have carried out a comprehensive study of the influence of electronic structure modeling and junction structure description on the first-principles calculation of the spin polarization in molecular junctions caused by the chiral induced spin selectivity (CISS) effect. We explore the limits and the sensitivity to modeling decisions of a Landauer/Green's function/two-component density functional theory approach to CISS. We find that although the CISS effect is entirely attributed in the literature to molecular spin filtering, spin−orbit coupling being partially inherited from the metal electrodes plays an important role in our calculations on ideal carbon helices, even though this effect cannot explain the experimental conductance results. Its magnitude depends considerably on the shape, size, and material of the metal clusters modeling the electrodes. Also, a pronounced dependence on the specific description of exchange interaction and spin−orbit coupling is manifest in our approach. This is important because the interplay between exchange effects and spin−orbit coupling may play an important role in the description of the junction magnetic response. Our calculations are relevant for the whole field of spinpolarized electron transport and electron transfer, because there is still an open discussion in the literature about the detailed underlying mechanism and the magnitude of physical parameters that need to be included to achieve a consistent description of the CISS effect: seemingly good quantitative agreement between simulation and the experiment can be caused by error compensation, because spin polarization as contained in a Landauer/Green's function/two-component density functional theory approach depends strongly on computational and structural parameters.

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“… 96 Beyond the description of exchange/electronic interactions, intermolecular and interface effects, it may be important to consider nuclear dynamics as well as electronic dynamics. 97 , 98 …”

Section: Chiral-induced Spin Selectivity: Recent Advancesmentioning

confidence: 99%

A Chirality-Based Quantum Leap

Aiello¹,

Abbas²,

Abendroth³

et al. 2022

ACS Nano

110

126

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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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Chemical Reaction Rates for Systems with Spin–Orbit Coupling and an Odd Number of Electrons: Does Berry’s Phase Lead to Meaningful Spin-Dependent Nuclear Dynamics for a Two State Crossing?

Cited by 27 publications

References 102 publications

The Influence of Electronic Structure Modelling and Junction Structure on First-Principles Chiral Induced Spin Selectivity

The Influence of Electronic Structure Modelling and Junction Structure on First-Principles Chiral Induced Spin Selectivity

Influence of Electronic Structure Modeling and Junction Structure on First-Principles Chiral Induced Spin Selectivity

A Chirality-Based Quantum Leap

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