arXiv subjects

Andrea Mattioni

Publications and source records attributed to Andrea Mattioni.

5 recordsLinked to original sources

arXiv2024

Vibronic effects on the quantum tunnelling of magnetisation in Kramers single-molecule magnets

Single-molecule magnets are among the most promising platforms for achieving molecular-scale data storage and processing. Their magnetisation dynamics are determined by the interplay between electronic and vibrational degrees of freedom, which can couple coherently, leading to complex vibronic dynamics. Building on an ab initio description of the electronic and vibrational Hamiltonians, we formulate a non-perturbative vibronic model of the low-energy magnetic degrees of freedom in monometallic single-molecule magnets. Describing their low-temperature magnetism in terms of magnetic polarons, we are able to quantify the vibronic contribution to the quantum tunnelling of the magnetisation, a process that is commonly assumed to be independent of spin-phonon coupling. We find that the formation of magnetic polarons lowers the tunnelling probability in both amorphous and crystalline systems by stabilising the low-lying spin states. This work, thus, shows that spin-phonon coupling subtly influences magnetic relaxation in single-molecule magnets even at extremely low temperatures where no vibrational excitations are present.

quant-ph↗

arXiv2022

A Lyapunov approach for the exponential stability of a damped Timoshenko beam

In this technical note, we consider the stability properties of a viscously damped Timoshenko beam equation with spatially varying parameters. With the help of the port-Hamiltonian framework, we first prove the existence of solutions and show, by an appropriate Lyapunov function, that the system is exponentially stable and has an explicit decay rate. The explicit exponential bound is computed for an illustrative example of which we provide some numerical simulations.

math.OC↗

arXiv2021

Design principles for long-range energy transfer at room temperature

Under physiological conditions, ballistic long-range transfer of electronic excitations in molecular aggregates is generally expected to be suppressed by noise and dissipative processes. Hence, quantum phenomena are not considered to be relevant for the design of efficient and controllable energy transfer over significant length and time scales. Contrary to this conventional wisdom, here we show that the robust quantum properties of small configurations of repeating clusters of molecules can be used to tune energy transfer mechanism that take place on much larger scales. With the support of an exactly solvable model, we demonstrate that coherent exciton delocalization and dark states within unit cells can be used to harness dissipative phenomena of varying nature (thermalization, fluorescence, non-radiative decay and weak inter-site correlations) to support classical propagation over macroscopic distances. In particular, we argue that coherent delocalization of electronic excitations over just a few pigments can drastically alter the relevant dissipation pathways which influence the energy transfer mechanism, and thus serve as a molecular control tool for large-scale properties of molecular materials. Building on these principles, we use extensive numerical simulations to demonstrate that they can explain currently not understood measurements of micron-scale exciton diffusion in nano-fabricated arrays of bacterial photosynthetic complexes. Based on these results we provide quantum design guidelines at the molecular scale to optimize both energy transfer speed and range over macroscopic distances in artificial light-harvesting architectures.

cond-mat.mes-hall↗

arXiv2020

A cyanine dye rotaxane porphyrin nanoring complex as a model light harvesting system

A nanoring-rotaxane supramolecular assembly, with a Cy7 cyanine dye (hexamethylindotricarbocyanine) threaded along the axis of the nanoring, has been synthesized as a model for the energy transfer between the light harvesting complex LH1 and the reaction center in purple bacteria photosynthesis. The complex displays efficient energy transfer from the central cyanine dye to the surrounding zinc porphyrin nanoring. We present a theoretical model that reproduces the absorption spectrum of the nanoring and quantifies the excitonic coupling between the nanoring and the central dye, explaining the efficient energy transfer and elucidating the similarity with structurally related natural light harvesting systems.

physics.chem-ph↗

arXiv2018

Which-way interference within biomimetic unit-cells for efficient energy transfer

We show that `which-way' interference within unit-cells enhances the propagation along linear arrays made upon these basic units. As a working example, we address the exciton transfer through linear aggregates of ring-like unit cells, the latter resembling the circular structure of the Light-Harvesting complexes of purple bacteria. After providing an analytic approximate solution of the eigenvalue problem for such aggregates, we show that the population transferred across the array is not a monotonic function of the coupling between nearest-neighbor rings, contrary to what is found from situations where this intra-unit cell interference is not displayed. The non-monotonicity depends on an interesting trade off between the exciton transfer speed and the amount of energy transferred, which is associated with the rupture of symmetry among paths within the ring-like cells, due to the inter-ring coupling strength.

quant-ph↗