Related papers: Spin-vibronic dynamics in open-shell systems beyon…
In the construction of diabatic vibronic Hamiltonians for quantum dynamics in the excited-state manifold of molecules, the coupling constants are often extracted solely from information on the excited-state energies. Here, a new protocol is…
An effective Hamiltonian without symmetry restriction has been developed to model the rotational and fine structure of two nearly degenerate electronic states of an open-shell molecule. In addition to the rotational Hamiltonian for an…
The interaction of electronic spin and molecular vibrations mediated by spin-orbit coupling governs spin relaxation in molecular qubits. I derive an extended molecular spin Hamiltonian that includes both adiabatic and non-adiabatic…
Molecular vibrations play a key role in magnetic relaxation processes of molecular spin qubits as they couple to spin states, leading to the loss of quantum information. Direct experimental determination of vibronic coupling is crucial to…
We consider a fully quadratic vibronic model Hamiltonian for studying photoinduced electronic transitions through conical intersections. Using a second order perturbative approximation for diabatic couplings we derive an analytical…
Molecular and lattice vibrations are able to couple to the spin of electrons and lead to their relaxation and decoherence. Ab initio simulations have played a fundamental role in shaping our understanding of this process but further…
Open-shell non-rigid molecular systems exhibiting an internal rotation are likely candidates for a coupling between the spin angular momentum of the unpaired electron and the torsional motion. This electron spin-torsion coupling lacked both…
In computational chemistry of molecular materials, strong static correlation effects appear when electronic states, often involving the ground state, become quasi-degenerate, as occurs, for example, in bond-breaking processes. Such…
Spin-lattice relaxation is a key open problem to understand the spin dynamics of single-molecule magnets and molecular spin qubits. While modelling the coupling between spin states and local vibrations allows to determine the more relevant…
We derive an electron-vibration model Hamiltonian in a quantum chemical framework, and explore the extent to which such a Hamiltonian can capture key effects of nonadiabatic dynamics. The model Hamiltonian is a simple two-body operator, and…
Magnetic resonance is a prime method for the study of chemical and biological structures and their dynamical processes. The interpretation of these experiments relies on considering the spin of electrons as the sole relevant degree of…
The coupling between electronic spins and lattice vibrations is fundamental for driving relaxation in magnetic materials. The debate over the nature of spin-phonon coupling dates back to the 40's, but the role of spin-spin, spin-orbit and…
We present a qualitative model for a fundamental process in molecular electronics: the change in conductance upon bond breaking. In our model a diatomic molecule is attached to spin-polarized contacts. Employing a Hubbard Hamiltonian,…
Spin-orbit coupling in crystals is known to lead to unusual direction dependent exchange interactions, however understanding of the consequeces of such effects in molecular crystals is incomplete. Here we perform four component relativistic…
Here we present theoretical studies of the effect of vibronic coupling on nonlinear transport characteristics (current-voltage and conductance-voltage) in molecular electronic devices. Considered device is composed of molecular quantum dot…
Quantum computing has the potential to reduce the computational cost required for quantum dynamics simulations. However, existing quantum algorithms for coupled electron-nuclear dynamics simulation either require fault-tolerant devices, or…
The realisation of quantum computers based on molecular electronic spins requires the design of qubits with very long coherence times, T2. Dephasing can proceed over several different microscopic pathways, active at the same time and in…
We developed a method which performs the coupled adiabatic spin and lattice dynamics based on the tight-binding electronic structure model, where the intrinsic magnetic field and ionic forces are calculated from the converged…
Paramagnetic molecules can show long spin-coherence times, which make them good candidates as quantum bits. Reducing the efficiency of the spin-phonon interaction is the primary challenge towards achieving long coherence times over a wide…
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,…