Assessment of the LFAs-PBE exchange–correlation potential for high-order harmonic generation of aligned H2+ molecules

Sun, Hsiao-Ling; Peng, Wei-Tao; Chai, Jeng-Da

doi:10.1039/c6ra03713e

Cited by 6 publications

(8 citation statements)

References 108 publications

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“…Consequently, most semilocal density functionals can yield erroneous results for the highest occupied molecular orbital (HOMO) energies [33][34][35][36][37][38] and high-lying Rydberg excitation energies [11,[39][40][41]. Even if the asymptote problems can be properly resolved by the recently developed semilocal density functionals with correct asymptotic behavior [42][43][44][45][46] and asymptotically corrected model XC potentials [47][48][49][50][51], the SIE problems may remain unresolved [52]. Besides, semilocal density functionals are inaccurate for charge-transfer (CT) excitation energies [41,42,[52][53][54][55][56][57][58][59][60][61], due to the lack of a space-and frequency-dependent discontinuity in the adiabatic XC kernel adopted in TDDFT [62].…”

Section: Introductionmentioning

confidence: 99%

Short- and long-range corrected hybrid density functionals with the D3 dispersion corrections

Wang

Hui

Chai

2016

The Journal of Chemical Physics

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We propose a short-and long-range corrected (SLC) hybrid scheme employing 100% HartreeFock (HF) exchange at both zero and infinite interelectronic distances, wherein three SLC hybrid density functionals with the D3 dispersion corrections (SLC-LDA-D3, SLC-PBE-D3, and SLC-B97-D3) are developed. SLC-PBE-D3 and SLC-B97-D3 are shown to be accurate for a very diverse range of applications, such as core ionization and excitation energies, thermochemistry, kinetics, noncovalent interactions, dissociation of symmetric radical cations, vertical ionization potentials, vertical electron affinities, fundamental gaps, and valence, Rydberg, and long-range charge-transfer excitation energies. Relative to ωB97X-D, SLC-B97-D3 provides significant improvement for core ionization and excitation energies and noticeable improvement for the self-interaction, asymptote, energy-gap, and charge-transfer problems, while performing similarly for thermochemistry, kinetics, and noncovalent interactions.

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Section: Introductionmentioning

confidence: 99%

Short- and long-range corrected hybrid density functionals with the D3 dispersion corrections

Wang

Hui

Chai

2016

The Journal of Chemical Physics

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“…Sun et al 81 studied the molecular ion H + 2 . Their work focused on the numerical analysis of the self-interaction error in RT-TDDFT for H + 2 which has just one electron.…”

Section: Discussionmentioning

confidence: 99%

Role of exchange and correlation in high-harmonic generation spectra of H2, N2, and CO2: Real-time time-dependent electronic-structure approaches

Pauletti

Coccia²,

Luppi

2021

The Journal of Chemical Physics

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This study arises from the attempt to answer the following question: how different descriptions of electronic exchange and correlation affect the high-harmonic generation (HHG) spectroscopy of H 2 , N 2 , and CO 2 molecules? We compare HHG spectra for H 2 , N 2 , and CO 2 with different ab initio electronic structure methods: real-time time-dependent configuration interaction and real-time time-dependent density functional theory (RT-TDDFT) using truncated basis sets composed of correlated wave functions expanded on Gaussian basis sets. In the framework of RT-TDDFT, we employ Perdew-Burke-Ernzerhof (PBE) and long-range corrected Perdew-Burke-Ernzerhof (LC-ωPBE) functionals. We study HHG spectroscopy by disentangling the effect of electronic exchange and correlation. We first analyze the electronic exchange alone, and in the case of RT-TDDFT with LC-ωPBE, we use ω = 0.3 and ω = 0.4 to tune the percentage of long-range Hartree-Fock exchange and short-range exchange PBE. Then, we added the correlation as described by the PBE functional. All the methods give very similar HHG spectra, and they seem not to be particularly sensitive to the different description of exchange and correlation or to the correct asymptotic behavior of the Coulomb potential. Despite this general trend, some differences are found in the region connecting the cutoff and the background. Here, the harmonics can be resolved with different accuracy depending on the theoretical schemes used. We believe that the investigation of the molecular continuum and its coupling with strong fields merits further theoretical investigations in the near future.

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“…They also studied the performance of the LB94 and of the Fermi-Amaldi scheme plus PBE (LFAsPBE) which have the correct asymptotic behaviour of the Coulomb potential. [80]. They found that LB94 and LFAsPBE are in better agreement with exact TDSE, i.e.…”

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confidence: 93%

Role of Exchange and Correlation in High-Harmonic Generation Spectra of H2, N2 and CO2: Real-Time Time-Dependent Electronic-Structure Approaches

Coccia

Luppi²,

Pauletti³

2020

Preprint

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This study arises from the attempt to answer the following question: how different descriptions of electronic exchange and correlation affect the high-harmonic generation (HHG) spectroscopy of H2, N2 and CO2 molecules? We compare HHG spectra for H2, N2 and CO2 with different ab initio electronic structures methods: real-time time-dependent configuration interaction (RT-TDCIS) and real-time time-dependent density functional theory (RT-TDDFT) using truncated basis sets composed of correlated wave functions expanded on Gaussian basis sets. In the framework of RT-TDDFT, we employ PBE and LC-ωPBE functionals. We study HHG spectroscopy by disentangling the effect of electronic exchange and correlation. We first analyse the electronic exchange alone and in the case of RT-TDDFT with LC-ωPBE, we use ω = 0.3 and ω = 0.4 to tune the percentage of long-range Hartree-Fock exchange and of short-range exchange PBE. Then, we added the correlation as described by PBE functional. All the methods give very similar HHG spectra and they seem not to be particularly sensitive to the different description of exchange and correlation or to the correct asymptotic behaviour of the Coulomb potential. Despite this general trend, some differences are found in the region connecting the cutoff and the background. Here, the harmonics can be resolved with different accuracy depending on the theoretical schemes used. We believe that the investigation of the molecular continuum and its coupling with strong fields merits further theoretical investigations in the next future.

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Assessment of the LFAs-PBE exchange–correlation potential for high-order harmonic generation of aligned H₂⁺ molecules

Cited by 6 publications

References 108 publications

Short- and long-range corrected hybrid density functionals with the D3 dispersion corrections

Short- and long-range corrected hybrid density functionals with the D3 dispersion corrections

Role of exchange and correlation in high-harmonic generation spectra of H2, N2, and CO2: Real-time time-dependent electronic-structure approaches

Role of Exchange and Correlation in High-Harmonic Generation Spectra of H2, N2 and CO2: Real-Time Time-Dependent Electronic-Structure Approaches

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