Perspective: Ab initio force field methods derived from quantum mechanics The Journal of Chemical Physics 148, 090901 (2018) Time-dependent coupled-cluster method with time-varying orbital functions, called time-dependent optimized coupled-cluster (TD-OCC) method, is formulated for multielectron dynamics in an intense laser field. We have successfully derived the equations of motion for CC amplitudes and orthonormal orbital functions based on the real action functional, and implemented the method including double excitations (TD-OCCD) and double and triple excitations (TD-OCCDT) within the optimized active orbitals. The present method is size extensive and gauge invariant, a polynomial cost-scaling alternative to the time-dependent multiconfiguration self-consistent-field method. The first application of the TD-OCC method of intense-laser driven correlated electron dynamics in Ar atom is reported. Published by AIP Publishing. https://doi

We have employed both Z-vector method and the expectation value approach in the relativistic coupled-cluster framework to calculate the scalar-pseudoscalar (S-PS) P, T -odd interaction constant (Ws) and the effective electric field (E eff ) experienced by the unpaired electron in the ground electronic state of RaF. Further, the magnetic hyperfine structure constants of 223 Ra in RaF and 223 Ra + are also calculated and compared with the experimental values wherever available to judge the extent of accuracy obtained in the employed methods. The outcome of our study reveals that the Z-vector method is superior than the expectation value approach in terms of accuracy obtained for the calculation of ground state property. The Z-vector calculation shows that RaF has a high E eff (52.5 GV/cm) and Ws (141.2 kHz) which makes it a potential candidate for the eEDM experiment.

The article deals with the general implementation of 4-component spinor relativistic extended coupled cluster (ECC) method to calculate first order property of atoms and molecules in their open-shell ground state configuration. The implemented relativistic ECC is employed to calculate hyperfine structure (HFS) constant of alkali metals (Li, Na, K, Rb and Cs), singly charged alkaline earth metal atoms (Be + , Mg + , Ca + and Sr + ) and molecules (BeH, MgF and CaH). We have compared our ECC results with the calculations based on restricted active space configuration interaction (RAS-CI) method. Our results are in better agreement with the available experimental values than those of the RAS-CI values.

We report the implementation of a cost-effective approximation method within the framework of time-dependent optimized coupled-cluster (TD-OCC) method [J. Chem. Phys. 148, 051101 (2018)] for real-time simulations of intense laser-driven multielectron dynamics. The method, designated as TD-OCEPA0, is a time-dependent extension of the simplest version of the coupled-electron pair approximation with optimized orbitals [J. Chem. Phys. 139, 054104 (2013)]. It is size extensive, gauge invariant, and computationally much more efficient than the TD-OCC with double excitations (TD-OCCD). We employed this method to simulate the electron dynamics in Ne and Ar atoms exposed to intense near infrared laser pulses with various intensities. The computed results, including high-harmonic generation spectra and ionization yields, are compared with those of various other methods ranging from uncorrelated time-dependent Hartree-Fock (TDHF) to fully-correlated (within the active orbital space) time-dependent completeactive-space self-consistent-field (TD-CASSCF). The TD-OCEPA0 results show a good agreement with TD-CASSCF ones for moderate laser intensities. For higher intensities, however, TD-OCEPA0 tends to overestimate the correlation effect, as occasionally observed for CEPA0 in the ground-state correlation energy calculations.

We report successful implementation of the time-dependent second-order many-body perturbation theory using optimized orthonormal orbital functions called time-dependent optimized second-order many-body perturbation theory to reach out to relatively larger chemical systems for the study of intense-laser-driven multielectron dynamics. We apply this method to strong-field ionization and high-order harmonic generation of Ar. The calculation results are benchmarked against ab initio time-dependent complete-active-space self-consistent field, time-dependent optimized coupled-cluster double, and time-dependent Hartree–Fock methods, as well as a single active electron model to explore the role of electron correlation.

We present an N(5) scaling modification to the standard EOMEA-CCSD method, based on the matrix partitioning technique and perturbative approximations. The method has lower computational scaling and smaller storage requirements than the standard EOMEA-CCSD method and, therefore, can be used to calculate electron affinities of large molecules and clusters. The performance and capabilities of the new method have been benchmarked with the standard EOMEA-CCSD method, for a test set of 20 small molecules, and the average absolute deviation is only 0.03 eV. The method is further used to investigate electron affinities of DNA and RNA nucleobases, and the results are in excellent agreement with the experimental values.

Nowadays, companies such as Amazon, Alibaba, and even pizza chains are pushing forward to use drones, also called UAVs (Unmanned Aerial Vehicles), for service provision, such as package and food delivery. As governments intend to use these immense economic benefits that UAVs have to offer, urban planners are moving forward to incorporate so-called UAV flight zones and UAV highways in their smart city designs. However, the high-speed mobility and behavior dynamics of UAVs need to be monitored to detect and, subsequently, to deal with intruders, rogue drones, and UAVs with a malicious intent.This paper proposes a UAV defense system for the purpose of intercepting and escorting a malicious UAV outside the flight zone. The proposed UAV defense system consists of a defense UAV swarm, which is capable to self-organize its defense formation in the event of intruder detection, and chase the malicious UAV as a networked swarm.Modular design principles have been used for our fully localized approach. We developed an innovative auto-balanced clustering process to realize the intercept-and capture-formation. As it turned out, the resulting networked defense UAV swarm is resilient against communication losses. Finally, a prototype UAV simulator has been implemented. Through extensive simulations, we show the feasibility and performance of our approach.

The effective electric field experienced by the unpaired electron in the ground state of PbF, which is a potential candidate in the search of electron electric dipole moment due to some special characteristics, is calculated using Z-vector method in the coupled cluster single-and double-excitation approximation with four component Dirac spinor. This is an important quantity to set the upper bound limit of the electron electric dipole moment. Further, we have calculated molecular dipole moment and parallel magnetic hyperfine structure constant (A ) of 207 Pb in PbF to test the accuracy of the wave function obtained in the Z-vector method. The outcome of our calculations clearly suggests that the core electrons have significant contribution to the "atom in compound (AIC)" properties.