Computational Spectroscopy of Large Systems in Solution: The DFTB/PCM and TD-DFTB/PCM Approach

Barone, Vincenzo; Carnimeo, Ivan; Scalmani, Giovanni

doi:10.1021/ct301050x

Cited by 47 publications

(65 citation statements)

References 87 publications

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“…Like DFT, DFTB has been recently extended to different formulations, to treat spin polarized systems, or long‐range phenomena . Furthermore, DFTB has been derived to be incorporated into hybrid QM/MM schemes or in a time‐dependent formalism . This extreme versatility allows this computational method to be applied in various fields of chemistry, such as the description of biological systems or metal oxides surfaces …”

Section: Introductionmentioning

confidence: 99%

SCC‐DFTB parameters for simulating hybrid gold‐thiolates compounds

et al. 2015

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We present a parametrization of a self-consistent charge density functional-based tight-binding scheme (SCC-DFTB) to describe gold-organic hybrid systems by adding new Au-X (X = Au, H, C, S, N, O) parameters to a previous set designed for organic molecules. With the aim of describing gold-thiolates systems within the DFTB framework, the resulting parameters are successively compared with density functional theory (DFT) data for the description of Au bulk, Aun gold clusters (n = 2, 4, 8, 20), and Aun SCH3 (n = 3 and 25) molecular-sized models. The geometrical, energetic, and electronic parameters obtained at the SCC-DFTB level for the small Au3 SCH3 gold-thiolate compound compare very well with DFT results, and prove that the different binding situations of the sulfur atom on gold are correctly described with the current parameters. For a larger gold-thiolate model, Au25 SCH3 , the electronic density of states and the potential energy surfaces resulting from the chemisorption of the molecule on the gold aggregate obtained with the new SCC-DFTB parameters are also in good agreement with DFT results.

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Section: Introductionmentioning

confidence: 99%

SCC‐DFTB parameters for simulating hybrid gold‐thiolates compounds

et al. 2015

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“…In comparison, tight binding and other semiempirical approaches are capable of producing molecular geometries and energetics at dramatically reduced computational costs . In particular, the self‐consistent charge density functional tight binding (SCC‐DFTB) scheme, rooted within the DFTB method developed by Seifert et al as well as its most recent DFTB3 variant, provide valuable insights and have already unraveled complex problems . In the context of organic electronic materials, the novel parameterization for (bio)organic molecules (so called 3OB) is especially relevant as it restores the proper qualitative behavior for molecules involving noncovalently bound sulfur atoms that were poorly described by the previous MIO11 parameter set .…”

Section: Introductionmentioning

confidence: 99%

A fast charge‐Dependent atom‐pairwise dispersion correction for DFTB3

Petraglia

Steinmann

Corminbœuf

2015

Int J of Quantum Chemistry

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“…78,79 In particular, TB density functional theory (DFTB) 80 and its time-dependent extension (TD-DFTB) 81 is a rapidly developing, low cost alternative for describing light-molecule interactions. 82 It has been already applied for both fullerenes 83 and nanotubes. 84 Abbreviation TB is used for first-neighbor TB in this work.…”

Section: Introductionmentioning

confidence: 99%

Vibrational optical activity of chiral carbon nanoclusters treated by a generalized π-electron method

Nagy

Śurján

Szabados

2014

The Journal of Chemical Physics

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Cross sections of inelastic light scattering accompanied by vibronic excitation in large conjugated carbon structures is assessed at the π-electron level. Intensities of Raman and vibrational Raman optical activity (VROA) spectra of fullerenes are computed, relying on a single electron per atom. When considering only first neighbor terms in the Hamiltonian (a tight-binding (TB) type or Hückel-model), Raman intensities are captured remarkably well, based on comparison with frequency-dependent linear response of the self-consistent field (SCF) method. Resorting to π-electron levels when computing spectral intensities brings a beneficial reduction in computational cost as compared to linear response SCF. At difference with total intensities, the first neighbor TB model is found inadequate for giving the left and right circularly polarized components of the scattered light, especially when the molecular surface is highly curved. To step beyond first neighbor approximation, an effective π-electron Hamiltonian, including interaction of all sites is derived from the all-electron Fockian, in the spirit of the Bloch-equation. Chiroptical cross-sections computed by this novel π-electron method improve upon first-neighbor TB considerably, with no increase in computational cost. Computed VROA spectra of chiral fullerenes, such as C76 and C28, are reported for the first time, both by conventional linear response SCF and effective π-electron models.

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Computational Spectroscopy of Large Systems in Solution: The DFTB/PCM and TD-DFTB/PCM Approach

Cited by 47 publications

References 87 publications

SCC‐DFTB parameters for simulating hybrid gold‐thiolates compounds

SCC‐DFTB parameters for simulating hybrid gold‐thiolates compounds

A fast charge‐Dependent atom‐pairwise dispersion correction for DFTB3

Vibrational optical activity of chiral carbon nanoclusters treated by a generalized π-electron method

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