Basis set effects on the hyperpolarizability of CHCl3: Gaussian-type orbitals, numerical basis sets and real-space grids

Vila, Fernando D.; Strubbe, David A.; Takimoto, Y.; Andrade, Xavier; Rubio, Ángel; Louie, Steven G.; Rehr, J. J.

doi:10.1063/1.3457362

Cited by 48 publications

(45 citation statements)

References 44 publications

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“…Such methods are advantageous for density response, as they are often semiquantitative, yet require little computational effort beyond ground state DFT. RT-TDDFT has been successfully applied both to linear and non-linear optical response [26][27][28][29] as well as core level x-ray absorption spectra ignoring satellites [30]. However, to our knowledge, neither its application to the cumulant method nor to CT excitations has previously been carried out.…”

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confidence: 99%

Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra

et al. 2015

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X-ray photoemission spectra generally exhibit satellite features in addition to the quasi-particle peaks due to many-body excitations, which have been of considerable theoretical and experimental interest. However, the satellites attributed to charge-transfer (CT) excitations in correlated materials have proved difficult to calculate from first principles. Here we report a real-time, real-space approach for such calculations based on a cumulant representation of the core-hole Green's function and time-dependent density functional theory. This approach also yields an interpretation of CT satellites in terms of a complex oscillatory, transient response to a suddenly created core hole. Illustrative results for TiO2 and NiO are in good agreement with experiment.

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Section: Fig 1: (Color Online)mentioning

confidence: 99%

Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra

et al. 2015

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“…It can perform Ehrenfest-TDDFT non-adiabatic molecular dynamics [14,31] and adiabatic molecular dynamics based on the modified Ehrenfest scheme [32,33], which inherits the scalability properties of real-time TDDFT, or the standard Born-Oppenheimer and Car-Parrinello [34] schemes. Different response properties in TDDFT [35] can also be obtained using linearresponse formalisms like Casida [36], or the density-functional perturbation theory/Sternheimer approach [37][38][39][40][41][42][43]. Octopus can also do quantum optimal-control calculations [44][45][46] and realtime quantum transport calculations [47].…”

Section: Octopus Features 21 Theorymentioning

confidence: 99%

Time-dependent density-functional theory in massively parallel computer architectures: the octopus project

Andrade¹,

Alberdi-Rodríguez²,

Strubbe³

et al. 2012

J. Phys.: Condens. Matter

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Octopus is a general-purpose density-functional theory (DFT) code, with a particular emphasis on the time-dependent version of DFT (TDDFT). In this article we present the ongoing efforts for the parallelisation of octopus. We focus on the real-time variant of TDDFT, where the time-dependent Kohn-Sham equations are directly propagated in time. This approach has a great potential for execution in massively parallel systems such as modern supercomputers with thousands of processors and graphics processing units (GPUs).For harvesting the potential of conventional supercomputers, the main strategy is a multilevel parallelisation scheme that combines the inherent scalability of real-time TDDFT with a real-space grid domain-partitioning approach. A scalable Poisson solver is critical for the efficiency of this scheme. For GPUs, we show how using blocks of Kohn-Sham states * xavier@tddft.org 60 provides the required level of data-parallelism and that this strategy is also applicable for code-optimisation on standard processors. Our results show that real-time TDDFT, as implemented in octopus, can be the method of choice to study the excited states of large molecular systems in modern parallel architectures.

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“…Its variables are represented on grids in real space b (not using a basis of given functions), which feature allows for systematic control of the discretisation error, of particular importance for excited-state properties. 77 Furthermore, OCTOPUS uses a multi-level parallelisation scheme where the data is distributed following a tree-based approach. This scheme uses the message passing interface (MPI) library and was shown to be quite efficient in modern parallel computers.…”

Section: Methodsmentioning

confidence: 99%

A survey of the parallel performance and accuracy of Poisson solvers for electronic structure calculations

et al. 2013

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We present an analysis of different methods to calculate the classical electrostatic Hartree potential created by charge distributions. Our goal is to provide the reader with an estimation * To whom correspondence should be addressed † on the performance -in terms of both numerical complexity and accuracy-of popular Poisson solvers, and to give an intuitive idea on the way these solvers operate. Highly parallelisable routines have been implemented in the first-principle simulation code OCTOPUS to be used in our tests, so that reliable conclusions about the capability of methods to tackle large systems in cluster computing can be obtained from our work.

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Basis set effects on the hyperpolarizability of CHCl3: Gaussian-type orbitals, numerical basis sets and real-space grids

Cited by 48 publications

References 44 publications

Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra

Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra

Time-dependent density-functional theory in massively parallel computer architectures: the octopus project

A survey of the parallel performance and accuracy of Poisson solvers for electronic structure calculations

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