Multi‐coefficients correlation methods

Zhang, Wenna; Kong, Xirui; Liu, Sheng; Zhao, Yan

doi:10.1002/wcms.1474

Cited by 5 publications

(5 citation statements)

References 137 publications

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“…One aspect to consider is the extension and validation of composite models for electronic structure calculations to transition metals and heavy atoms, large systems, open-shell species, and excited electronic states. Possible routes to achieve this include explicitly-correlated coupled-cluster approaches, 105,247 localized treatments of correlation (e.g. local pair natural orbitals, LPNO…”

Section: Case Study Of Magnetic Co(ii) Tetrathiolatesmentioning

confidence: 99%

Computational molecular spectroscopy

Barone

Alessandrini

Biczysko

et al. 2021

Nat Rev Methods Primers

103

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Molecular spectroscopy techniques are unique tools to probe molecular systems non-invasively and investigate their structure, properties, and dynamics in different environments and physicochemical conditions. Different spectroscopic techniques and their combination can lead to a more comprehensive picture of investigated systems. However, the increasing sophistication of these experimental techniques makes it more and more complex and difficult to interpret the results without the help of computational chemistry. As a consequence, computational molecular spectroscopy has progressively changed from a highly specialized field to a general tool also employed by experimentally-oriented researchers. Computational spectroscopy, born as a branch of quantum chemistry for providing predictions of spectroscopic properties and features, evolved as an independent field. In this Primer, we focus on the characterization of medium-sized molecular systems by means of different spectroscopic techniques. We first provide essential information about the characteristics, accuracy and limitations of the available computational approaches, and select examples with the aim of illustrating general trends, that is outcomes of general validity that can be used for modeling spectroscopic phenomena. We emphasize the need for estimating error bars and limitations, coupling accuracy with interpretability, and discuss the results in terms of widely recognized chemical concepts.

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Section: Case Study Of Magnetic Co(ii) Tetrathiolatesmentioning

confidence: 99%

Computational molecular spectroscopy

Barone

Alessandrini

Biczysko

et al. 2021

Nat Rev Methods Primers

103

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“…Many ab initio composite methods are available. ,,− High accuracy composite thermochemistry schemes include treatments of electron correlation beyond CCSD(T). In previous work, we have found out that even for a seemingly simple main-group reaction, it could be vital to include the excitations higher than quadruples for achieving reliable accuracy .…”

Section: Methodsmentioning

confidence: 99%

Predicting Bond Dissociation Energies and Bond Lengths of Coordinatively Unsaturated Vanadium–Ligand Bonds

et al. 2020

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Understanding the electronic structure of coordinatively unsaturated transitionmetal compounds and predicting their physical properties are of great importance for catalyst design. Bond dissociation energy D e and bond length r e are two of the fundamental quantities for which good predictions are important for a successful design strategy. In the present work, recent experimentally measured bond energies and bond lengths of VX diatomic molecules (X = C, N, S) are used as a gauge to consider the utility of a number of electronic structure methods. Singlereference methods are one focus because of their efficiency and utility in practical calculations, and multireference configuration interaction (MRCISD) methods and a composite coupled cluster (CCC) method are a second focus because of their potential high accuracy. The comparison is especially challenging because of the large multireference M diagnostics of these molecules, in the range 0.15−0.19. For the single-reference methods, Kohn−Sham density functional theory (KS-DFT) has been tested with a variety of approximate exchange-correlation functionals. Of these, MOHLYP provides the bond dissociation energies in best agreement with experiments, and BLYP provides the bond lengths that are in best agreement with experiments; but by requiring good performance for both the D e and r e of the vanadium compounds, MOHLYP, MN12-L, MGGA_MS1, MGGA_MS0, O3LYP, and M06-L are the most highly recommended functionals. The CCC calculations include up to connected pentuple excitations for the valence electrons and up to connected quadruple excitations for the core−valence terms; this results in highly accurate dissociation energies and good bond lengths. Averaged over the three molecules, the mean unsigned deviation of CCC bond energies from experimental ones is only 0.4 kcal/mol, demonstrating excellent convergence of theory and experiments.

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“…WMS is a composite wave-function method developed recently by our group in an attempt to approximate results at the complete configuration interaction level [22,23]. The details of WMS are given in Supporting Information.…”

Section: Benchmark Redox Potentials From Wmsmentioning

confidence: 99%

“…The purpose of the present study is to establish a benchmark database of the redox potentials of some small solvents by using the recently developed Wuhan–Minnesota‐scaling (WMS) method [22, 23], and evaluate the accuracy of 35 popular DFT methods against the new database. From the assessment, the M08‐HX has been shown to be an optimal DFT method to calculate the redox potentials.…”

Section: Introductionmentioning

confidence: 99%

Accurate redox potentials for solvents in Li‐metal batteries and assessment of density functionals

Zhang

Yang

Zhao³

et al. 2022

Int J of Quantum Chemistry

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The practical applications of Li metal batteries (LMBs) have been limited by the anodic instability which causes fatal problems including low Coulombic efficiency and short cycling lifespan. One way of addressing this issue is to develop new solvents with suitable redox potentials for electrolytes of LMBs. By using the recently developed Wuhan–Minnesota‐scaling method, the work has developed the Redox20 benchmark database consisting of the Ox10 subset of 10 oxidation potentials and the Red10 subset of 10 reduction potentials for four conventional and six fluorinated solvents in LMBs. The performances of 35 DFT methods have been assessed against Redox20. Based on the assessments, M05‐2X, M08‐HX, M08‐SO, M06‐2X, and revM06 functionals are the most accurate for the predictions of oxidation potentials, and the N12, M06‐HF, M08‐HX, HSE06, and PW6B95‐D3 functionals are best performers for calculating reduction potentials. M08‐HX gives the lowest average mean unsigned error, and it is recommended for the calculation of redox potentials. M08‐HX has been employed to calculate the redox potentials and highest occupied molecular orbital/lowest unoccupied molecular orbital structures of 48 solvents for LMBs, which is beneficial to the selection of optimal LMBs electrolyte solvents.

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Multi‐coefficients correlation methods

Cited by 5 publications

References 137 publications

Computational molecular spectroscopy

Computational molecular spectroscopy

Predicting Bond Dissociation Energies and Bond Lengths of Coordinatively Unsaturated Vanadium–Ligand Bonds

Accurate redox potentials for solvents in Li‐metal batteries and assessment of density functionals

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