相关论文: Fantastical Excited State Optimized Structures and…
State-specific electronic structure theory provides a route towards balanced excited-state wave functions by exploiting higher-energy stationary points of the electronic energy. Multiconfigurational wave function approximations can describe…
We study the structure of the eigenstates and the dynamics of a system that undergoes an excited state quantum phase transition (ESQPT). The analysis is performed for two-level pairing models characterized by a U(n+1) algebraic structure.…
State-specific approximations can provide an accurate representation of challenging electronic excitations by enabling relaxation of the electron density. While state-specific wave functions are known to be local minima or saddle points of…
We report a set of adiabatic potential energy surfaces (PESs) for diiodomethane, including the ground electronic state and all excited states accessible via single-photon absorption near 260 nm. Although constrained to four dimensions,…
We demonstrate that, rather than resorting to high-cost dynamic correlation methods, qualitative failures in excited-state potential energy surface predictions can often be remedied at no additional cost by ensuring that optimal molecular…
Exceptional points (EPs) are distinct characteristics of non-Hermitian Hamiltonians that have no counterparts in Hermitian systems. In this study, we focus on EPs in continuous systems rather than discrete non-Hermitian systems, which are…
This paper presents two new adiabatic, global potential energy surfaces (PESs) for the two lowest $^3A'$ and $^3A''$ electronic states of the O($^3P$)+H$_2$ system. For each of these states, ab initio electronic energies were calculated for…
State-specific complete active space self-consistent field (SS-CASSCF) theory has emerged as a promising route to accurately predict electronically excited energy surfaces away from molecular equilibria. However, its accuracy and…
Determining quantum excited states is crucial across physics and chemistry but presents significant challenges for variational methods, primarily due to the need to enforce orthogonality to lower-energy states, often requiring…
The accurate quantum chemical calculation of excited states is a challenging task, often requiring computationally demanding methods. When entire ground and excited potential energy surfaces (PESs) are desired, e.g., to predict the…
A main distinguishing feature of non-Hermitian quantum mechanics is the presence of exceptional points (EPs). They correspond to the coalescence of two energy levels and their respective eigenvectors. Here, we use the Lipkin-Meshkov-Glick…
This work is concerned with the excited state quantum phase transitions (ESQPTs) defined in Ann.Phys. 323, 1106 (2008). In many-body models that exhibit such transitions, the ground state quantum phase transition (QPT) occurs in parallel…
Recent experimental advances have made it possible to study excited structure in superheavy nuclei. The observed states have often been interpreted as quasi-particle excitations. We show that in superheavy nuclei collective vibrations…
Full-dimensional reactive potential energy surfaces (PESs) for the OCS$^+$ cation are constructed to describe S$^+$ loss in the electronic ground state and seven low-lying electronically excited states. High-level \textit{ab initio}…
Quantum phase transitions universally exist in the ground and excited states of quantum many-body systems, and they have a close relationship with the nonequilibrium dynamical phase transitions, which however are challenging to identify. In…
We study the connection between exceptional points (EPs) and optimal parameter estimation, in a simple system consisting of two counter-propagating traveling wave modes in a microring resonator. The unknown parameter to be estimated is the…
The fragmentation dynamics of predissociative SO2(C1B2) is investigated on an accurate adiabatic potential energy surface (PES) determined from high level ab initio data. This singlet PES features non-C2v equilibrium geometries for SO2,…
Two-dimensional Projected Entangled Pair States (PEPS) provide a unique framework giving access to detailed entanglement features of correlated (spin or electronic) systems. For a bi-partitioned quantum system, it has been argued that the…
The nature of electronic excited states has a deep impact on the dynamics of molecular spins, but remains poorly understood and characterized. Here we carry out a thorough multiconfigurational investigation for two prototypical molecular…
We report a detailed study of the stationary points (zero-force points) of the potential energy surface (PES) of a model structural glassformer. We compare stationary points found with two different algorithms (eigenvector following and…