Search arXivSearch

arXiv · 2407.17345

Targeted energy transfer dynamics and chemical reactions

Abstract

Ultrafast reaction processes take place when resonant features of nonlinear model systems are taken into account. In the targeted energy or electron transfer dimer model this is accomplished through the implementation of nonlinear oscillators with opposing types of nonlinearities, one attractive while the second repulsive. In the present work we show that this resonant behavior survives if we take into account the vibrational degrees of freedom as well. After giving a summary on the basic formalism of chemical reactions we show that resonant electron transfer can be assisted by vibrations. We find the condition for this efficient transfer and show that in the case of additional interaction with noise a distinct non-Arrhenius behavior develops that is markedly different from the usual Kramers-like activated transfer.

Explore related subjects

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

N. Almazova, S. Aubry, G. P. Tsironis. 2024-07-24. Targeted energy transfer dynamics and chemical reactions. https://arxiv.org/abs/2407.17345

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

Intrinsic Matching Frustration in Fluctuating Finite Systems

We formulate intrinsic matching frustration (IMF), a fluctuation-induced, kinetics-independent reduction in the mean capacity permitted by a prescribed matching rule. For complementary one-to-one matching, the instantaneous capacity is set by the minority population, so fluctuations produce a nonzero mean deficit even when the two populations are balanced on average. At finite size, this deficit depends on the full distribution of the population difference and is determined by its variance alone only in the Gaussian limit. Compartmentalization hides matching capacity by preventing cancellation between local imbalances of opposite sign. Fusion releases this hidden capacity monotonically under coarse graining, producing a measurable recovery of product yield following local reaction to completion.

physics.chem-ph

Phonon chirality as an additive control of CISS: a symmetry-protected law

Chirality-induced spin selectivity (CISS) is usually associated with molecular handedness. The possible contribution of chiral phonons is less established. We study a helical tight-binding model in which local phonon angular momentum modulates spin-dependent nearest-neighbor hopping. Fewest-switches surface hopping calculations give the transmitted spin polarization $\mathrm{SP}=aC+b\mathrm{PH}$. Here $C$ is the molecular chirality and $\mathrm{PH}$ is the phonon chirality. A mirror symmetry reverses $C$, $\mathrm{PH}$, and $\mathrm{SP}$ simultaneously. This symmetry excludes both a chirality-independent offset and a $C\cdot\mathrm{PH}$ term. The phonon contribution can therefore enhance, cancel, or reverse the molecular CISS signal.

physics.chem-ph

A fast physics-based matrix model for the impedance of a PEM fuel cell: Incorporating functionally graded catalyst layer and channel impedances

We extend a recent physics-based matrix model for calculating PEM fuel cell impedance (doi:10.1149/2754-2734/ad6ce8) to cases of low air flow stoichiometry and functionally graded cathode catalyst layers (CCLs). We demonstrate that the matrix model produces accurate spectra and is almost three orders of magnitude faster than a model based on the standard boundary-value problem solver. The physics-based matrix model can compete with equivalent circuit models for fitting experimental EIS spectra, particularly those measured from cells with functionally graded CCL.

physics.chem-ph