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We investigate the performance of the range-separated hybrid (RSH) scheme, which combines long-range Hartree-Fock (HF) and a short-range density-functional approximation (DFA), for calculating photoexcitation/photoionization spectra of the…

化学物理 · 物理学 2019-07-24 Felipe Zapata , Eleonora Luppi , Julien Toulouse

We study state-of-the-art approaches for calculating x-ray Thomson scattering spectra from density functional theory molecular dynamics (DFT-MD) simulations based on a modified Chihara formula that expresses the inelastic contribution in…

The energy levels of the first few low-lying states of helium and lithium atoms in intense magnetic fields up to $\approx 10^8-10^9$~T are calculated in this study. A pseudospectral method is employed for the computational procedure. The…

量子物理 · 物理学 2014-06-11 Anand Thirumalai , Jeremy S. Heyl

The computation of strongly correlated quantum systems is challenging because of its potentially exponential scaling in the number of electron configurations. Variational calculation of the two-electron reduced density matrix (2-RDM)…

量子物理 · 物理学 2021-04-01 David A. Mazziotti

The real-time-propagation formulation of time-dependent density-functional theory (RT-TDDFT) is an efficient method for modeling the optical response of molecules and nanoparticles. Compared to the widely adopted linear-response TDDFT…

材料科学 · 物理学 2019-01-15 Tuomas P. Rossi , Mikael Kuisma , Martti J. Puska , Risto M. Nieminen , Paul Erhart

We consider the calculations of photoionization spectra and core resonances of open-shell systems using range-separated time-dependent density-functional theory. Specifically, we use the time-dependent range-separated hybrid (TDRSH) scheme,…

化学物理 · 物理学 2023-01-11 Julien Toulouse , Karno Schwinn , Felipe Zapata , Antoine Levitt , Eric Cancès , Eleonora Luppi

Correlation-driven phenomena in molecular periodic systems are challenging to predict computationally not only because such systems are periodically infinite but also because they are typically strongly correlated. Here we generalize the…

化学物理 · 物理学 2022-04-18 Simon Ewing , David A. Mazziotti

It is virtually impossible to directly solve the Schr\"odinger equation for a many-electron wave function due to the exponential growth in degrees of freedom with increasing particle number. The two-body reduced density matrix (2-RDM)…

量子物理 · 物理学 2022-04-22 Nicholas Cox

Strong field photoemission and electron recollision provide a viable route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal resolution. However, since an {\em ab-initio} treatment of even the…

原子物理 · 物理学 2016-11-02 N. Suárez , A. Chacón , M. F. Ciappina , B. Wolter , J. Biegert , M. Lewenstein

The time-dependent density functional (TDDFT) equations may be written either for the Kohn-Sham orbitals in Hilbert space or for the single electron density matrix in Liouville space. A collective-oscillator, quasiparticle, representation…

强关联电子 · 物理学 2009-11-10 Oleg Berman , Shaul Mukamel

Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…

材料科学 · 物理学 2022-09-12 Marcus Annegarn , Juhan Matthias Kahk , Johannes Lischner

In this paper we motivate, formulate and analyze the Multi-Configuration Time-Dependent Hartree-Fock (MCTDHF) equations for molecular systems under Coulomb interaction. They consist in approximating the N-particle Schrodinger wavefunction…

数学物理 · 物理学 2015-05-13 C. Bardos , I. Catto , N. Mauser , S. Trabelsi

We derive a time-dependent density functional theory appropriate for calculating the near-edge X-ray absorption spectrum in molecules and condensed matter. The basic assumption is to increase the space of many-body wave functions from one…

强关联电子 · 物理学 2015-06-16 G. F. Bertsch , A. Lee

We review different computational methods for the calculation of photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses using time-dependent density-functional theory (TDDFT) that are suitable…

化学物理 · 物理学 2017-03-28 Philipp Wopperer , Umberto De Giovannini , Angel Rubio

Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…

Owing to its numerical simplicity, a two-dimensional two-electron model atom, with each electron moving in one direction, is an ideal system to study non-perturbatively a fully correlated atom exposed to a laser field. Frequently made…

原子物理 · 物理学 2009-10-30 D. Bauer

Variational minimization of the ground-state energy as a function of the two-electron reduced density matrix (2-RDM), constrained by necessary $N$-representability conditions, provides a polynomial-scaling approach to studying strongly…

量子物理 · 物理学 2011-11-09 Kasra Naftchi-Ardebili , Nathania W. Hau , David A. Mazziotti

Two-dimensional materials (2DMs) are a promising alternative to complement and upgrade high-frequency electronics. However, in order to boost their adoption, the availability of numerical tools and physically-based models able to support…

Time-dependent density-functional theory (TDDFT) is deemed to be a formally rigorous way of dealing with the time-evolution of a many-electron system at the level of electron densities rather than the underlying wavefunctions, which in turn…

化学物理 · 物理学 2024-11-26 Jochen Schirmer

The second-order reduced density matrix method (the RDM method) has performed well in determining energies and properties of atomic and molecular systems, achieving coupled-cluster singles and doubles with perturbative triples (CC SD(T))…

强关联电子 · 物理学 2012-07-23 James S. M. Anderson , Maho Nakata , Ryo Igarashi , Katsuki Fujisawa , Makoto Yamashita