Propagation of initially excited states in time-dependent density-functional theory

Elliott, Peter; Maitra, Neepa T.

doi:10.1103/physreva.85.052510

Cited by 44 publications

(46 citation statements)

References 50 publications

(75 reference statements)

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“…The mRKS technique can also be used for construction of exchange-correlation potentials of adiabatic time-dependent density-functional theory. [60][61][62] Extensions of the mRKS method to spinpolarized post-HF wave functions and to systems that are not pure-state v-representable remain the subject of future work.…”

Section: Discussionmentioning

confidence: 99%

Improved method for generating exchange-correlation potentials from electronic wave functions

Ospadov

Ryabinkin

Staroverov

2017

The Journal of Chemical Physics

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Ryabinkin, Kohut, and Staroverov (RKS) [Phys. Rev. Lett. 115, 083001 (2015)] devised an iterative method for reducing many-electron wave functions to Kohn-Sham exchange-correlation potentials, vXC(r). For a given type of wave function, the RKS method is exact (Kohn-Sham-compliant) in the basis-set limit; in a finite basis set, it produces an approximation to the corresponding basisset-limit vXC(r). The original RKS procedure works very well for large basis sets but sometimes fails for commonly used (small and medium) sets. We derive a modification of the method's working equation that makes the RKS procedure robust for all Gaussian basis sets and increases the accuracy of the resulting exchange-correlation potentials with respect to the basis-set limit.

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Section: Discussionmentioning

confidence: 99%

Improved method for generating exchange-correlation potentials from electronic wave functions

Ospadov

Ryabinkin

Staroverov

2017

The Journal of Chemical Physics

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“…Strictly speaking, to use Condition 2, one would need to know the exact density of the interacting excited states, but in practise one can often find appropriate KS excited states for a given functional approximation, whose densities are assumed to approximate the interacting ones [47]. This was done in Ref.…”

Section: Exact Conditionsmentioning

confidence: 99%

Studies of spuriously shifting resonances in time-dependent density functional theory

Luo

Fuks

Maitra

2016

The Journal of Chemical Physics

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Adiabatic approximations in time-dependent density functional theory (TDDFT) will in general yield unphysical time-dependent shifts in the resonance positions of a system driven far from its ground-state. This spurious time-dependence is explained in [J. I. Fuks, K. Luo, E. D. Sandoval and N. T. Maitra, Phys. Rev. Lett. 114, 183002 (2015)] in terms of the violation of an exact condition by the non-equilibrium exchange-correlation kernel of TDDFT. Here we give details on the derivation and discuss reformulations of the exact condition that apply in special cases. In its most general form, the condition states that when a system is left in an arbitrary state, the TDDFT resonance position for a given transition in the absence of time-dependent external fields and ionic motion, is independent of the state. Special cases include the invariance of TDDFT resonances computed with respect to any reference interacting stationary state of a fixed potential, and with respect to any choice of appropriate stationary Kohn-Sham reference state. We then present several case studies, including one that utilizes the adiabatically-exact approximation, that illustrate the conditions and the impact of their violation on the accuracy of the ensuing dynamics. In particular, charge-transfer across a long-range molecule is hampered, and we show how adjusting the frequency of a driving field to match the time-dependent shift in the charge-transfer resonance frequency, results in a larger charge transfer over time.

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“…The adsorbate forms a transient ion strongly coupled to the plasmonic particle, and the relevant potential energy surface is that of an excited state of the adsorbate-plasmonic particle complex, which must be treated together. Theoretical calculations of the excitedstate energy landscape using first-principles beyondground-state electronic structure methods are therefore essential for predicting such mechanisms and for interpreting femtochemistry experiments [119][120][121].…”

Section: Molecular Injection: Plasmon-enhanced Catalysis and Femtochementioning

confidence: 99%

Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion

2016

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Surface plasmons provide a pathway to efficiently absorb and confine light in metallic nanostructures, thereby bridging photonics to the nano scale. The decay of surface plasmons generates energetic 'hot' carriers, which can drive chemical reactions or be injected into semiconductors for nano-scale photochemical or photovoltaic energy conversion. Novel plasmonic hot carrier devices and architectures continue to be demonstrated, but the complexity of the underlying processes make a complete microscopic understanding of all the mechanisms and design considerations for such devices extremely challenging. Here, we review the theoretical and computational efforts to understand and model plasmonic hot carrier devices. We split the problem into three steps: hot carrier generation, transport and collection, and review theoretical approaches with the appropriate level of detail for each step along with their predictions. We identify the key advances necessary to complete the microscopic mechanistic picture and facilitate the design of the next generation of devices and materials for plasmonic energy conversion.

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Propagation of initially excited states in time-dependent density-functional theory

Cited by 44 publications

References 50 publications

Improved method for generating exchange-correlation potentials from electronic wave functions

Improved method for generating exchange-correlation potentials from electronic wave functions

Studies of spuriously shifting resonances in time-dependent density functional theory

Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion

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