arXiv subjects

Ivo Neefjes

Publications and source records attributed to Ivo Neefjes.

2 recordsLinked to original sources

arXiv2022

Multipolar exchange interaction and complex order in insulating lanthanides

In insulating lanthanides, unquenched orbital momentum and weak crystal-field (CF) splitting of the atomic $J$ multiplet at lanthanide ions result in a highly ranked (multipolar) exchange interaction between them and a complex low-temperature magnetic order not fully uncovered by experiment. Explicitly correlated {\it ab initio } methods proved to be highly efficient for an accurate description of CF multiplets and magnetism of individual lanthanide ions in such materials. Here we extend this {\it ab initio } methodology and develop a first-principles microscopic theory of multipolar exchange interaction between $J$-multiplets in $f$ metal compounds. The key point of the approach is a complete account of Goodenough's exchange mechanism along with traditional Anderson's superexchange and other contributions, the former being dominant in many lanthanide materials. Application of this methodology to the description of the ground-state order in the neodymium nitride with rocksalt structure reveals the multipolar nature of its ferromagnetic order. We found that the primary and secondary order parameters (of $T_{1u}$ and $E_g$ symmetry, respectively) contain non-negligible $J$-tensorial contributions up to the ninth order. The calculated spin-wave dispersion and magnetic and thermodynamic properties show that they cannot be simulated quantitatively by confining to the ground CF multiplet on the Nd sites. Our results demonstrate that the {\it ab initio } approach to the low-energy Hamiltonian represents a powerful tool for the study of materials with complex magnetic order.

cond-mat.str-el↗

arXiv2021

Collision-sticking kinetics of acid-base clusters and its influence on atmospheric new particle formation

Kinetics of collision-sticking processes between vapor molecules and molecular clusters of low volatile compounds facilitates the initial steps of atmospheric clustering. Conventional theoretical models are quite inaccurate due to the neglection of long-range interactions that essentially govern the kinetics of these microscopic phenomena. Here, we present a consistent and generic theoretical model for evaluating collision rates between molecules and molecular clusters with intermolecular potentials properly incorporated. The model requires solely the elementary molecule-molecule potential as a-priori information but predicts collision rates of molecular clusters at arbitrary sizes, with an accuracy comparable to all-atom molecular dynamics simulations we performed for sulfuric acid-dimethylamine clusters, a typical example of acid-base induced clustering. The carefully devised simulations validate the theoretical model and elucidate the kinetics of the molecular collision-sticking process. It is found that the vibrational coupling after the collision between a sulfuric acid molecule and a sulfuric acid cluster can be occasionally unsuccessful, i.e., no stable bond is formed after the collision. However, introducing dimethylamine molecules to the sulfuric acid cluster can notably increase the probability of forming stable bonds and hence stable product clusters. The results offer fundamental insights into the initial steps of molecular clustering and will facilitate the development of efficient kinetic approach-based nucleation models.

physics.chem-ph↗