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
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
Nanoscience & Nanotechnology
Mohamed A. Abdelati, Mohamed M. Fadlallah, Yosr E. E-D Gamal, Ahmed A. Maarouf
Summary: This study investigated the structural stabilities and optical properties of graphene quantum dots (GQDs) and holey GQDs with different sizes, edge terminations, and pore passivations using density functional theory (DFT) and time dependent DFT. Results showed that the optical spectra of GQDs primarily depend on their size, while pore passivation has the biggest effect on the absorption spectra of holey GQDs. These findings can be applied in the development of promising materials for various applications, such as biological sensors and optoelectronic devices.
PHYSICA E-LOW-DIMENSIONAL SYSTEMS & NANOSTRUCTURES
(2021)
Article
Chemistry, Physical
Yevhen Horbatenko, Saima Sadiq, Seunghoon Lee, Michael Filatov, Cheol Ho Choi
Summary: The MRSF-TDDFT method demonstrates high accuracy in describing the multiconfigurational electronic states of diradicals and diradicaloids, avoiding spin-contamination pitfalls. It accurately predicts adiabatic singlet-triplet gaps and various effects in different systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Multidisciplinary
William Livernois, M. P. Anantram
Summary: The electrical properties of conductive heme-based nanowires in Geobacter sulfurreducens bacteria were investigated using spin-dependent density functional theory (DFT). Charge transport simulations at different length scales revealed that tunneling rates between heme sites depend on oxidation state and transport pathway modeled. The study demonstrates the importance of spin dependence for electron hopping, oxidation state, and decoherence transport in cytochromes.
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
Chemistry, Physical
Jie Liu, Wei Hu, Jinlong Yang
Summary: A two-level iterative solver for linear response time-dependent density functional theory has been proposed and successfully implemented, showing significantly reduced computational cost and storage requirement for calculating excited-state properties of molecules and low-dimensional semiconductors compared to standard iterative algorithms.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Mathematics, Applied
Francois Mauger, Cristel Chandre, Mette B. Gaarde, Kenneth Lopata, Kenneth J. Schafer
Summary: This study revisits the equations of Kohn-Sham time-dependent density-functional theory (TDDFT) and demonstrates their derivation from a canonical Hamiltonian formalism. By using a geometric description, families of symplectic split-operator schemes are defined to accurately and efficiently simulate the time propagation for specific classes of DFT functionals. Numerical simulations are conducted to illustrate the approach, focusing on the far-from-equilibrium electronic dynamics of a one-dimensional carbon chain. The optimized 4th order scheme is found to provide a good compromise between numerical complexity and accuracy of the simulation.
COMMUNICATIONS IN NONLINEAR SCIENCE AND NUMERICAL SIMULATION
(2024)
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
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
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, Multidisciplinary
Yin-Pai Lin, Inta Isakovica, Aleksejs Gopejenko, Anna Ivanova, Aleksandrs Zacinskis, Roberts I. Eglitis, Pavel N. D'yachkov, Sergei Piskunov
Summary: Based on time-dependent density functional theory (TD-DFT), first-principle calculations were performed to predict optical properties and transition states of pristine, N- and S-doped, and N+S-codoped anatase TiO2 nanotubes of 1 nm-diameter. The study shows that dopants can enhance the visible-light-driven photoresponse in TiO2 nanotubes, potentially improving the efficiency of hydrogen production in water-splitting applications.
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
Physics, Condensed Matter
Daniel Vieira
Summary: The emergence of Wigner oscillations is obtained by employing a time-dependent density-functional theory formalism to simulate a real time cooling process in one-dimensional quantum dots.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2023)
Article
Multidisciplinary Sciences
Mark Kamper Svendsen, Yaniv Kurman, Peter Schmidt, Frank Koppens, Ido Kaminer, Kristian S. Thygesen
Summary: The authors have developed a framework by combining density functional theory with macroscopic quantum electrodynamics to quantify the Purcell effect in van der Waals heterostructures.
NATURE COMMUNICATIONS
(2021)