arXiv subjects

Salvatore Gatto

Publications and source records attributed to Salvatore Gatto.

4 recordsLinked to original sources

arXiv2026

Full Quantum and Mixed Quantum--Classical Dynamics of Hot Exciton Cooling in Semiconductor Nanocrystals

Hot-exciton relaxation in semiconductor nanocrystals (NCs) is often described using perturbative theories, but their accuracy is difficult to assess for realistic exciton--phonon Hamiltonians. Here, we benchmark the perturbative quantum master equation (QME) and several mixed quantum--classical (MQC) methods against fully quantum mechanical dynamics. Using atomistically parameterized models for CdSe core and CdSe/CdS core--shell NCs, we find that bare CdSe exhibits an ultrafast initial decay followed by slower cooling, whereas the core--shell system is dominated by the slower component. Analysis of reduced models shows that the ultrafast component arises from rapid diabatic state mixing driven by thermal fluctuations of low-frequency phonons, rather than from nuclear-assisted energy relaxation. The QME captures the initial fast decay but can fail for the slower relaxation in the diabatic representation, while the mapping approach to surface hopping (MASH) gives the most consistent agreement with both benchmark dynamics and equilibrium populations. These results establish a benchmark for exciton-cooling dynamics in NCs and clarify the physical regimes in which widely used approximate methods are reliable.

physics.chem-ph↗

arXiv2026

Quantum Otto cycle in the Anderson impurity model

We study the thermodynamic performance of a periodic quantum Otto cycle operating on the single-impurity Anderson model. Using a decomposition of the time-evolution generator based on the principle of minimal dissipation, combined with the numerically exact hierarchical equations of motion (HEOM) method, we analyze the operating regimes of the quantum thermal machine and investigate effects of Coulomb interactions, strong system-reservoir coupling, and energy level alignments. Our results show that Coulomb interaction can change the operating regimes and may lead to an enhancement of the efficiency.

cond-mat.mes-hall↗

arXiv2025

Unraveling Exciton Trap Dynamics and Nonradiative Loss Pathways in Quantum Dots via Atomistic Simulations

Surface defects in colloidal quantum dots are a major source of nonradiative losses, yet the microscopic mechanisms underlying exciton trapping and recombination remain elusive. Here, we develop a model Hamiltonian based on atomistic electronic calculations to investigate exciton dynamics in CdSe/CdS core/shell QDs containing a single hole trap introduced by an unpassivated sulfur atom. By systematically varying the defect depth and reorganization energy, we uncover how defect-induced excitonic states mediate energy relaxation pathways. Our simulations reveal that a single localized defect can induce a rich spectrum of excitonic states, leading to multiple dynamical regimes, from slow, energetically off-resonant trapping to fast, cascaded relaxation through in-gap defect states. Crucially, we quantify how defect-induced polaron shifts and exciton-phonon couplings govern the balance between efficient radiative emission and rapid nonradiative decay. These insights clarify the microscopic origin of defect-assisted loss channels and suggest pathways for tailoring QD optoelectronic properties via surface and defect engineering.

physics.chem-ph↗

arXiv2024

Quantum thermodynamics of the spin-boson model using the principle of minimal dissipation

A recently developed approach to the thermodynamics of open quantum systems, on the basis of the principle of minimal dissipation, is applied to the spin-boson model. Employing a numerically exact quantum dynamical treatment based on the hierarchical equations of motion (HEOM) method, we investigate the influence of the environment on quantities such as work, heat and entropy production in a range of parameters which go beyond the weak-coupling limit and include both the non-adiabatic and the adiabatic regimes. The results reveal significant differences to the weak-coupling forms of work, heat and entropy production, which are analyzed in some detail.

quant-ph↗