Review
Chemistry, Physical
Neepa T. Maitra
Summary: Time-dependent density functional theory is a preferred method for calculating spectra and response properties in physics, chemistry, and biology. Its ability to scale to larger systems has made computations possible that were not previously achievable. While simple functional approximations have been successful in handling increasingly complex and interesting systems, there is a growing awareness that these approximations may fail for certain classes of problems. This review discusses the challenges and progress in describing double excitations and charge-transfer excitations, two common obstacles to the theory's application.
ANNUAL REVIEW OF PHYSICAL CHEMISTRY
(2022)
Article
Materials Science, Multidisciplinary
F. Aryasetiawan
Summary: It is found that the equation of motion for the one-particle Green function in an interacting many-electron system is determined by a time-dependent exchange-correlation potential, which is the Coulomb potential of a time-varying exchange-correlation hole. This exchange-correlation hole satisfies a sum rule, extending the well-known sum rule of the static exchange-correlation hole. It is suggested that this proposed formalism may offer an alternative approach for calculating the Green function by approximating the exchange-correlation hole or potential using techniques such as the local-density approximation.
Article
Chemistry, Physical
Jared R. Williams, Nicolas Tancogne-Dejean, Carsten A. Ullrich
Summary: Time-dependent density-functional theory (TDDFT) is an efficient method for calculating optical spectra, providing insight into exciton dynamics by obtaining exciton wave functions and understanding the formation and dissociation of excitons in real time.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Physical
Julien Paquier, Julien Toulouse
Summary: In this study, a complementary short-range correlation relativistic local-density-approximation functional was constructed for use in relativistic range-separated density-functional theory. By performing relativistic random-phase-approximation calculations of the correlation energy of the relativistic homogeneous electron gas, the behavior at high densities was studied and the results were fitted to a parametrized expression. The obtained functional is expected to be useful for electronic-structure calculations of strongly correlated systems containing heavy elements.
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY
(2021)
Article
Materials Science, Multidisciplinary
K. Karlsson, F. Aryasetiawan
Summary: This study investigates the exchange-correlation hole and potential of the homogeneous electron gas using the random-phase approximation and the plasmon-pole approximation. It shows the angular and time dependence of the exchange-correlation hole for a Wigner-Seitz radius rs = 4. The study reveals a substantial cancellation between exchange and correlation potentials in space and time, similar to the cancellation of exchange and correlation self-energies. Analysis of the sum rule explains the advantage of using a noninteracting Green function in calculating the response function and self-energy within the random-phase approximation and the GW approximation. This research provides a starting point for more accurate calculations of the exchange-correlation hole and potential, aiming to construct a model based on the local density approximation in density functional theory.
Article
Materials Science, Multidisciplinary
N. D. Woods, M. T. Entwistle, R. W. Godby
Summary: In the context of inhomogeneous one-dimensional finite systems, recent numerical advances have enabled the computation of the exact coupling-constant dependent exchange-correlation kernel within linear response time-dependent density-functional theory, leading to an improved understanding of ground-state total energies derived from ACFDT. Neglecting frequency dependence in the exact functional while considering both one-shot and self-consistent ACFDT calculations has shown to reliably preserve chemical accuracy, with the spatial structure in the exact functional largely remedying self-interaction issues. The implicit orbitals within a self-consistent ACFDT calculation utilizing the adiabatic exact kernel are remarkably similar to the exact Kohn-Sham orbitals, indicating that the spatial dependence of the functional at zero frequency captures the majority of physics for ground-state total energy.
Article
Physics, Condensed Matter
John McFarland, Efstratios Manousakis
Summary: Imaginary-time time-dependent density functional theory (it-TDDFT) is proposed as an alternative method for obtaining the ground state within density functional theory, avoiding convergence difficulties encountered by the self-consistent-field iterative method. By modifying the Quantum ESPRESSO package, it-TDDFT propagation for periodic systems has been successfully implemented, demonstrating accurate results for different calculations using ultra-soft or norm-conserving pseudo potentials.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2021)
Article
Astronomy & Astrophysics
Niu Li, Wei-Zhou Jiang, Jing Ye, Rong-Yao Yang, Si-Na Wei
Summary: We investigate the neutron star core-crust transition density pt by considering the vacuum polarization in the dielectric function within the nonlinear relativistic Hartree approach (RHAn). It is discovered that the strong correlation between pt and the scalar meson mass ma exceeds the uncertainty in the nuclear equation of state in the RHAn models, contrary to the common belief that pt is mainly sensitive to the isovector nuclear potential and symmetry energy. Accurately determining pt through future gravitational wave measurements can impose a strong constraint on the long-standing uncertainty of ma and improve our understanding of vacuum properties. As an astrophysical implication, the correlation between pt and ma helps reconcile the difficulty in reproducing the large crustal moment of inertia for pulsar glitches with the well-constrained symmetry energy.
Article
Biochemistry & Molecular Biology
Austin Biaggne, William B. Knowlton, Bernard Yurke, Jeunghoon Lee, Lan Li
Summary: The properties of dye monomers greatly influence their aggregation ability and exciton dynamics. By engineering dyes with specific substituents, optimal key properties like hydrophobicity and dipole moments can be achieved. This study found that electron withdrawing substituents significantly affect the solvation energy of the dye, while various pairs of substituents can enhance the static dipole difference.
Article
Physics, Condensed Matter
M. Barhoumi, N. Sfina, M. Said, S. Znaidia
Summary: The lack of theoretical and experimental data on third-order elastic constants has hindered the development of new materials with targeted mechanical responses. By applying density functional theory and adiabatic-connection fluctuation-dissipation theorem, researchers in this study made significant progress in understanding the mechanical properties of aluminium and silicon carbide. The results show promising agreement with experimental data and suggest potential applications in material engineering.
SOLID STATE COMMUNICATIONS
(2021)
Article
Engineering, Environmental
Sharma S. R. K. C. Yamijala, Ravindra Shinde, Kota Hanasaki, Zulfikhar A. Ali, Bryan M. Wong
Summary: PFASs are hazardous contaminants found in drinking water sources, and recent experimental efforts have focused on photo-induced processes to accelerate their degradation. This study provides crucial insights into the mechanism of photo-induced degradation of PFASs using RT-TDDFT calculations, showing that photo-induced excitations can be highly selective in dissociating the C-F bond.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Physical
Moritz Humer, Michael E. Harding, Martin Schlipf, Amir Taheridehkordi, Zoran Sukurma, Wim Klopper, Georg Kresse
Summary: This paper uses the direct random-phase approximation (dRPA) to calculate and compare the atomization energies of ten selected molecules in the HEAT set and G2-1 set, using both plane waves and Gaussian-type orbitals. Detailed procedures are described for obtaining highly accurate and well converged results using the projector augmented-wave method and the explicitly correlated dRPA-F12 method. The results show that both approaches agree within chemical accuracy for all considered molecules.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Subrata Jana, Lucian A. Constantin, Prasanjit Samal
Summary: We propose a realistic density functional approximation based on a semilocal indicator that exhibits good screening properties. The local band model shows remarkable density scaling behaviors and is applicable to various atoms. We introduce the LDAg correlation functional, which correctly calculates the correlation energy of atoms and shows improvement in ionization potential.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Materials Science, Multidisciplinary
Tetsuro Habe, Koichi Nakamura
Summary: The research reveals the presence of excitons in the monolayer crystal and evaluates its optical property using numerical methods. Additionally, it confirms the consistency of the optical property of the bulk crystal with previous experimental results, independent of the number of layers.
Article
Chemistry, Physical
Aleksander P. Wozniak, Michal Przybytek, Maciej Lewenstein, Robert Moszynski
Summary: This paper investigates the effects of full electronic correlation on high harmonic generation in the helium atom. The results show that including dynamical electron correlation can improve the description of high harmonic generation. However, this effect can only be captured if the basis set used is sufficient to reproduce the most basic features.
JOURNAL OF CHEMICAL PHYSICS
(2022)
