Related papers: Molecular g-Tensors From Spin-Orbit Quasidegenerat…
We present a formulation and implementation of second-order quasidegenerate N-electron valence perturbation theory (QDNEVPT2) that provides a balanced and accurate description of spin-orbit coupling and dynamic correlation effects in…
We present the first implementation of spin-orbit coupling effects in fully internally contracted second-order quasidegenerate N-electron valence perturbation theory (SO-QDNEVPT2). The SO-QDNEVPT2 approach enables the computations of…
The control of spins and spin to charge conversion in organics requires understanding the molecular spin-orbit coupling (SOC), and a means to tune its strength. However, quantifying SOC strengths indirectly through spin relaxation effects…
Qubits encoded in the spin state of heavy holes confined in Si- and Ge-based semiconductor quantum dots are currently leading the efforts toward spin-based quantum information processing. The virtual absence of spinful nuclei in purified…
The variational inclusion of spin-orbit coupling in self-consistent field (SCF) calculations requires a generalised two-component framework, which permits the single-determinant wave function to completely break spin symmetry. The…
We present a measurement-cost efficient implementation of Strongly-Contracted $N$-Electron Valence Perturbation Theory (SC-NEVPT2) for use on near-term quantum devices. At the heart of our algorithm we exploit the properties of adaptive…
We consider an electron confined in a gated nanowire quantum dot (NQD) with arbitrarily strong spin-orbit coupling (SOC) and weak static magnetic field, and treat the latter as a perturbation to seek the maximal spin-motion entangled states…
An analytical gradient theory for single-state N-electron valence state perturbation theory (NEVPT2), using both strongly contracted (SC) and partially contracted (PC) internal contraction schemes, is developed. We demonstrate the utility…
We present a theoretical study of the mesoscopic fluctuations of $g$-tensors in a metal nanoparticle. The calculations were performed using a semi-realistic tight-binding model, which contains both spin and orbital contributions to the…
We introduce QRDM-NEVPT2: a hybrid quantum-classical implementation of strongly-contracted N-electron Valence State $2^{nd}$-order Perturbation Theory (SC-NEVPT2), in which the Complete Active Space Configuration Interaction (CASCI) step,…
The tunability of high-mobility organic semi-conductors (OSCs) holds great promise for molecular spintronics. In this study, we show this extreme variability - and therefore potential tunability - of the molecular gyromagnetic coupling…
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…
We present a second-order N-electron valence state perturbation theory (NEVPT2) based on a density matrix renormalization group (DMRG) reference wave function that exploits a Cholesky decomposition of the two-electron repulsion integrals…
We present a perturbative method for ab initio calculations of rotational and rovibrational effective Hamiltonians of both rigid and non-rigid molecules. Our approach is based on a curvilinear implementation of second order vibrational…
Understanding and controlling spin relaxation in molecular qubits is essential for developing chemically tunable quantum information platforms. We present a fully first-principles framework for computing the spin relaxation tensor in a…
We calculate the proton and neutron spin contributions for nuclei using semi-empirical methods, as well as a novel hybrid \emph{ab initio}/semi-empirical method, for interpretation of experimental data. We demonstrate that core-polarisation…
Once the periodic properties of elements were unveiled, chemical bonds could be understood in terms of the valence of atoms. Ideally, this rationale would extend to quantum dots, often termed artificial atoms, and quantum computation could…
The magnetization of semiconductor quantum dots in the presence of spin-orbit coupling and interactions is investigated numerically. When the dot is occupied by two electrons we find that a level crossing between the two lowest many-body…
We present a stochastic approach to perform strongly contracted n-electron valence state perturbation theory (SC-NEVPT), which only requires one- and two-body reduced density matrices, without introducing approximations. We use this method…
Solid-state molecular qubits with open-shell ground states have great potential for addressability, scalability, and tunability, but understanding the fundamental limits of quantum coherence in these systems is challenging due to the…