Determining the role of the underlying orbital‐dependence of PBE0‐DH and PBE‐QIDH double‐hybrid density functionals

Sancho‐García, Juan Carlos; Pérez-Jiménez, Ángel J.; Savarese, Marika; Brémond, Éric; Adamo, Carlo

doi:10.1002/jcc.24788

Cited by 4 publications

(2 citation statements)

References 46 publications

(52 reference statements)

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“…16,17 As an alternative to GHs, successive models were revealed themselves or were specifically developed to circumvent the locality problem. A nonexhaustive list of some of them counts for the self-interaction correction (SIC), 18,19 the orbital dependence, [20][21][22] the merging between density-and wavefunctionbased approaches, 23,24 or the recent multiconfiguration pair-DFT (MC-PDFT). 25,26 Thanks to a concomitant wide implementation and an excellent performance improvement, the range-separated…”

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confidence: 99%

Range-separated hybrid density functionals made simple

Brémond

Pérez-Jiménez

Sancho‐García

et al. 2019

The Journal of Chemical Physics

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In this communication, we present a new and simple route to derive range-separated exchange (RSX) hybrid and double hybrid density functionals in a nonempirical fashion. In line with our previous developments [Brémond et al., J. Chem. Theory Comput. 14, 4052 (2018)], we show that by imposing an additional physical constraint to the exchange-correlation energy, i.e., by enforcing to reproduce the total energy of the hydrogen atom, we are able to generalize the nonempirical determination of the range-separation parameter to a family of RSX hybrid density functionals. The success of the resulting models is illustrated by an accurate modeling of several molecular systems and properties, like ionization potentials, particularly prone to the one-and many-electron self-interaction errors.

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mentioning

confidence: 99%

Range-separated hybrid density functionals made simple

Brémond

Pérez-Jiménez

Sancho‐García

et al. 2019

The Journal of Chemical Physics

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126

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“…We will also employ here the nearly exact def2-QZVP basis set, to isolate as much as possible the error due to the functional itself. Note that PBE-QIDH was also tested before for this property 83 but not in such a systematic way as it is done here since: (i) the results are now compared with other members of the PBEbased family of double-hybrid functionals and (ii) the basis set is extended from cc-pVTZ to def2-QZVP compared with that previous study mentioned.…”

Section: B Adiabatic Energies For Linear Acenesmentioning

confidence: 99%

Excitation energies of polycylic aromatic hydrocarbons by double-hybrid functionals: Assessing the PBE0-DH and PBE-QIDH models and their range-separated versions

Sandoval‐Salinas

Brémond

Pérez-Jiménez

et al. 2023

The Journal of Chemical Physics

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A family of non-empirical double-hybrid (DH) density functionals, such as Perdew–Burke–Ernzerhof (PBE)0-DH, PBE-QIDH, and their range-separated exchange (RSX) versions RSX-0DH and RSX-QIDH, all using Perdew-Burke-Ernzerhof(PBE) exchange and correlationfunctionals, is applied here to calculate the excitation energies for increasingly longer linear and cyclic acenes as part of their intense benchmarking for excited states of all types. The energies for the two lowest-lying singlet 1L a and 1L b states of linear oligoacenes as well as the triplet 3L a and 3L b states, are calculated and compared with experimental results. These functionals clearly outperform the results obtained from hybrid functionals and favorably compare with other double-hybrid expressions also tested here, such as B2-PLYP, B2GP-PLYP, ωB2-PLYP, and ωB2GP-PLYP. The study is complemented by the computation of adiabatic S0– T1 singlet-triplet energy difference for linear acenes as well as the extension of the study to strained cyclic oligomers, showing how the family of non-empirical expressions robustly leads to competitive results.

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AI‐Powered Mining of Highly Customized and Superior ESIPT‐Based Fluorescent Probes

Huang,

Fang

et al. 2024

Advanced Science

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Excited‐state intramolecular proton transfer (ESIPT) has attracted great attention in fluorescent sensors and luminescent materials due to its unique photobiological and photochemical features. However, the current structures are far from meeting the specific demands for ESIPT molecules in different scenarios; the try‐and‐error development method is labor‐intensive and costly. Therefore, it is imperative to devise novel approaches for the exploration of promising ESIPT fluorophores. This research proposes an artificial intelligence approach aiming at exploring ESIPT molecules efficiently. The first high‐quality ESIPT dataset and a multi‐level prediction system are constructed that realized accurate identification of ESIPT molecules from a large number of compounds under a stepwise distinguishing from conventional molecules to fluorescent molecules and then to ESIPT molecules. Furthermore, key structural features that contributed to ESIPT are revealed by using the SHapley Additive exPlanations (SHAP) method. Then three strategies are proposed to ensure the ESIPT process while keeping good safety, pharmacokinetic properties, and novel structures. With these strategies, >700 previously unreported ESIPT molecules are screened from a large pool of 570 000 compounds. The ESIPT process and biosafety of optimal molecules are successfully validated by quantitative calculation and experiment. This novel approach is expected to bring a new paradigm for exploring ideal ESIPT molecules.

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Determining the role of the underlying orbital‐dependence of PBE0‐DH and PBE‐QIDH double‐hybrid density functionals

Cited by 4 publications

References 46 publications

Range-separated hybrid density functionals made simple

Range-separated hybrid density functionals made simple

Excitation energies of polycylic aromatic hydrocarbons by double-hybrid functionals: Assessing the PBE0-DH and PBE-QIDH models and their range-separated versions

AI‐Powered Mining of Highly Customized and Superior ESIPT‐Based Fluorescent Probes

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