NAST: Nonadiabatic Statistical Theory Package for Predicting Kinetics of Spin-Dependent Processes

Dergachev, Vsevolod D.; Rooein, Mitra; Dergachev, Ilya D.; Lykhin, Aleksandr O.; Mauban, Robert C.; Varganov, Sergey A.

doi:10.1007/s41061-022-00366-w

Cited by 6 publications

(26 citation statements)

References 94 publications

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Section: Discussionmentioning

confidence: 99%

“…Future extensions of this work would also benefit by treating multielectron problems. For instance, although a great deal of work has been done treating the singlet to triplet ISC problem, , the spin polarization of product states has not yet been fully explored. , In the near term, additional work could use a similar framework as that above to investigate the dynamics of a three-or-more-state system. In particular, it will be very helpful to extend the two-level results presented here to the case of a metal surface with many electronic states, where the CISS phenomenon is often observed …”

Section: Discussionmentioning

confidence: 99%

“…We have imposed several important and deliberate constraints in the construction of eq 2. 34. First, note that the interstate coupling operator depends purely on x and y; it is wholly independent from the secondary bath modes.…”

Section: An Intuitive Model With Two Intertwinedmentioning

confidence: 99%

“…If ρ α and ρ β are the densities of states in their Shown is an example of a system that may be defined by the Hamiltonian in eq 2. 34. The parameters d, W, θ, η, and ϕ are shown in context.…”

Section: An Intuitive Model With Two Intertwinedmentioning

confidence: 99%

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Effect of Duschinskii Rotations on Spin-Dependent Electron Transfer Dynamics

Chandran

Subotnik

2022

J. Phys. Chem. A

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We investigate spin-dependent electron transfer in the presence of a Duschinskii rotation. In particular, we propagate dynamics for a two-level model system for which spin–orbit coupling introduces an interstate coupling of the form e iWx , which is both position(x)-dependent and complex-valued. We demonstrate that two-level systems coupled to Brownian oscillators with Duschinskii rotations (and thus entangled normal modes) can produce marked increases in transient spin polarization relative to two-level systems coupled to simple shifted harmonic oscillators. These conclusions should have significant relevance for modeling the effect of nuclear motion on chiral induced spin selectivity.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Section: An Intuitive Model With Two Intertwinedmentioning

confidence: 99%

Section: An Intuitive Model With Two Intertwinedmentioning

confidence: 99%

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Effect of Duschinskii Rotations on Spin-Dependent Electron Transfer Dynamics

Chandran

Subotnik

2022

J. Phys. Chem. A

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“…The MS-specific transition probabilities for the quartet-sextet crossing and the corresponding SOCMEs[2].…”

mentioning

confidence: 99%

How to calculate the rate constants for nonradiative transitions between the M _S components of spin multiplets?

Rooein

Varganov

2022

Molecular Physics

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Predicting Kinetics and Dynamics of Spin-Dependent Processes

Dergachev

Rooein

et al. 2023

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: Predicting mechanisms and rates of nonadiabatic spin-dependent processes including photoinduced intersystem crossings, thermally activated spin-forbidden reactions, and spin crossovers in metal centers is a very active field of research. These processes play critical roles in transition-metal-based and metalloenzymatic catalysis, molecular magnets, lightharvesting materials, organic light-emitting diodes, photosensitizers for photodynamic therapy, and many other applications. Therefore, accurate modeling of spin-dependent processes in complex systems and on different time scales is important for many problems in chemistry, biochemistry, and materials sciences. Nonadiabatic statistical theory (NAST) and nonadiabatic molecular dynamics (NAMD) are two complementary approaches to modeling the kinetics and dynamics of spin-dependent processes. NAST predicts the probabilities and rate constants of nonradiative transitions between electronic states with different spin multiplicities using molecular properties at only few critical points on the potential energy surfaces (PESs), including the reactant minimum and the minimum energy crossing point (MECP) between two spin states. This makes it possible to obtain molecular properties for NAST calculations using accurate but often computationally expensive electronic structure methods, which is critical for predicting the rate constants of spin-dependent processes. Alternatively, NAST can be used to study spindependent processes in very large complex molecular systems using less computationally expensive electronic structure methods.The nuclear quantum effects, such as zero-point vibrational energy, tunneling, and interference between reaction paths can be easily incorporated. However, the statistical and local nature of NAST makes it more suitable for large systems and slow kinetics. In contrast, NAMD explores entire PESs of interacting electronic states, making it ideal for modeling fast barrierless spin-dependent processes. Because the knowledge of large portions of PESs is often needed, the simulations require a very large number of electronic structure calculations, which limits the NAMD applicability to relatively small molecular systems and ultrafast kinetics.In this Account, we discuss our contribution to the development of the NAST and NAMD approaches for predicting the rates and mechanism of spin-dependent processes. First, we briefly describe our NAST and NAMD implementations. The NAST implementation is an extension of the transition state theory to the processes involving two crossing potential energy surfaces of different spin multiplicities. The NAMD approach includes the trajectory surface hopping (TSH) and ab initio multiple spawning (AIMS) methods. Second, we discuss several applications of NAST and NAMD to model spin-dependent processes in different systems. The NAST applicability to large complex systems is demonstrated by the studies of the spin-forbidden isomerization of the active sites of metal−sulfur pr...

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NAST: Nonadiabatic Statistical Theory Package for Predicting Kinetics of Spin-Dependent Processes

Cited by 6 publications

References 94 publications

Effect of Duschinskii Rotations on Spin-Dependent Electron Transfer Dynamics

Effect of Duschinskii Rotations on Spin-Dependent Electron Transfer Dynamics

How to calculate the rate constants for nonradiative transitions between the M _S components of spin multiplets?

Predicting Kinetics and Dynamics of Spin-Dependent Processes

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NAST: Nonadiabatic Statistical Theory Package for Predicting Kinetics of Spin-Dependent Processes

Cited by 6 publications

References 94 publications

Effect of Duschinskii Rotations on Spin-Dependent Electron Transfer Dynamics

Effect of Duschinskii Rotations on Spin-Dependent Electron Transfer Dynamics

How to calculate the rate constants for nonradiative transitions between the M S components of spin multiplets?

Predicting Kinetics and Dynamics of Spin-Dependent Processes

Contact Info

Product

Resources

About

How to calculate the rate constants for nonradiative transitions between the M _S components of spin multiplets?