Formation Mechanisms of Electronically Excited Nitrogen Molecules from N + N2 and N + N + N Collisions Revealed by Full-Dimensional Potential Energy Surfaces.

This work reports six new full-dimensional adiabatic potential energy surfaces (PESs) of the N3 system (four 4A″ states and two 2A″ states) at the MRCI + Q/AVQZ level of theory that correlated to N2(X1Σg+) + N(4S), N2(X1Σg+) + N(2D), N2(A3Σu+) + N(4S), N2(B3Πg) + N(4S), N2(W3Δu) + N(4S), and N(4S) + N(4S) + N(4S) channels. The neural networks with a proper account of the nuclear permutation invariant symmetry of N3 were employed to fit the PESs based on about 4000 ab initio points. The accuracy of the PESs was validated by excellent agreement on the equilibrium bond length, vertical excitation energy, and dissociation energy with experimental values. Two possible mechanisms of the formation of N2(A) were found. One is that the collision occurs between N2(X) and N(4S) in the 14A″ state, followed by a nonadiabatic transition through the conical intersection with the 24A″ PES, resulting in the formation of the N2(A) + N(4S) product. The other takes place in the collision among three N(4S) atoms in the adiabatic 24A″ state, and then, N2(A) + N(4S) is formed. This is the first systematical research of the N3 system focusing on the formation of the excited states of N2 via both adiabatic and nonadiabatic pathways.

Enhancement of electron-impact ionization induced by warm dense environments.

Studies have shown significant discrepancies between the recent experiment [Berg et al., Phys. Rev. Lett. 120, 055002 (2018)PRLTAO10.1103/PhysRevLett.120.055002] and current theoretical calculations on the electron-impact ionization cross section of ions in warm dense magnesium. Here, we present a systematic study the effects of the ionic correlations and free-electron screening on the electron-impact ionization of ions in warm dense matter. The ionic correlation and the free-electron screening effects yield additional Hermitian terms to the calculation of the ionic central-force-field potential, which significantly change the electronic structure compared with that of the isolated ion. In calculating the electron-impact ionization, we describe the impact and ionized electrons using a damped-distorted wave function, which considers the momentum relaxation of free electrons due to collisions with other free electrons and ions. We reproduce the electron-impact ionization process for Mg^{7+} in the solid-density plasma and increase the ionization cross section by one order of magnitude compared with that of the isolated ion, which excellently agrees with the experimental result of Berg et al.

Local field correction to ionization potential depression of ions in warm or hot dense matter.

An analytical self-consistent approach was recently established to predict the ionization potential depression (IPD) in multicomponent dense plasmas, which is achieved by considering the self-energy of ions and electrons within the quantum statistical theory. In order to explicitly account for the exchange-correlation effect of electrons, we incorporate the effective static approximation of local field correction (LFC) within our IPD framework through the connection of dynamical structure factor. The effective static approximation poses an accurate description for the asymptotic large wave number behavior with the recently developed machine learning representation of static LFC induced from the path-integral Monte Carlo data. Our calculation shows that the introduction of static LFC through dynamical structure factor brings a nontrivial influence on IPD at warm/hot dense matter conditions. The correlation effect within static LFC could provide up to 20% correction to free-electron contribution of IPD in the strong coupling and degeneracy regime. Furthermore, a new screening factor is obtained from the density distribution of free electrons calculated within the average-atom model, with which excellent agreements are observed with other methods and experiments at warm/hot dense matter conditions.

Phase diagrams and multistep condensations of spin-1 bosonic gases in optical lattices.

Motivated by recent experimental processes, we systemically investigate strongly correlated spin-1 ultracold bosons trapped in a three-dimensional optical lattice in the presence of an external magnetic field. Based on a recently developed bosonic dynamical mean-field theory (BDMFT), we map out complete phase diagrams of the system for both antiferromagnetic and ferromagnetic interactions, where various phases are found as a result of the interplay of spin-dependent interaction and quadratic Zeeman energy. For antiferromagnetic interactions, the system demonstrates competing magnetic orders, including nematic, spin-singlet and ferromagnetic insulating phase, depending on longitudinal magnetization, whereas, for ferromagnetic case, a ferromagnetic-to-nematic-insulating phase transition is observed for small quadratic Zeeman energy, and the insulating phase demonstrates the nematic order for large Zeeman energy. Interestingly, at low magnetic field and finite temperature, we find an abnormal multi-step condensation of the strongly correlated superfluid, i.e. the critical condensing temperature of the m F = -1 component with antiferromagnetic interactions demonstrates an increase with longitudinal magnetization, while, for ferromagnetic case, the Zeeman component m F = 0 demonstrates a local minimum for the critical condensing temperature, in contrast to weakly interacting cases.