Calculation of Gas-phase Standard Formation Enthalpy via Ring-Preserved Connectivity-Based Hierarchy and Automatic Bond Separation Reaction Platform

Liu, Jian; Wang, Runwen; Jie, Tian; Nie, Fude; Zhang, Chaoyang

doi:10.1016/j.fuel.2022.125203

Cited by 8 publications

(12 citation statements)

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“…In this context, we note that a few other groups have also taken notice of CBH's ease of automation, usually employing a graph-based algorithm in their implementation of the protocol. 41,42 Included with pyCBH is a lookup table of many of the common fragments formed with CBH-0 to CBH-3 along with a database of energies calculated at various levels of theory. If all fragments of a generated CBH reaction are present in the database, the ΔCBH correction (vide infra) can be computed automatically from the lookup table without the need for further electronic structure calculations.…”

Section: Generalized Graph-theoretic Approach For Cbh Generation and ...mentioning

confidence: 99%

“…Typically, in other fragmentation-based methods, the calculation of all two- to n -body overlaps between fragments is required in order to satisfy the inclusion–exclusion principle. − For CBH, however, the total number of fragments (including overlaps) is equal to the number of nodes and edges in the molecular graph, and no higher-order overlaps need to be calculated , making the algorithm highly efficient. In this context, we note that a few other groups have also taken notice of CBH’s ease of automation, usually employing a graph-based algorithm in their implementation of the protocol. , …”

Section: Generalized Graph-theoretic Approach For Cbh Generation and ...mentioning

confidence: 99%

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Approaching Coupled Cluster Accuracy with Density Functional Theory Using the Generalized Connectivity-Based Hierarchy

Raghavachari

Maier

Collins

et al. 2023

J. Chem. Theory Comput.

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This Perspective reviews connectivity-based hierarchy (CBH), a systematic hierarchy of error-cancellation schemes developed in our group with the goal of achieving chemical accuracy using inexpensive computational techniques (“coupled cluster accuracy with DFT”). The hierarchy is a generalization of Pople’s isodesmic bond separation scheme that is based only on the structure and connectivity and is applicable to any organic and biomolecule consisting of covalent bonds. It is formulated as a series of rungs involving increasing levels of error cancellation on progressively larger fragments of the parent molecule. The method and our implementation are discussed briefly. Examples are given for the applications of CBH involving (1) energies of complex organic rearrangement reactions, (2) bond energies of biofuel molecules, (3) redox potentials in solution, (4) pK a predictions in the aqueous medium, and (5) theoretical thermochemistry combining CBH with machine learning. They clearly show that near-chemical accuracy (1–2 kcal/mol) is achieved for a variety of applications with DFT methods irrespective of the underlying density functional used. They demonstrate conclusively that seemingly disparate results, often seen with different density functionals in many chemical applications, are due to an accumulation of systematic errors in the smaller local molecular fragments that can be easily corrected with higher-level calculations on those small units. This enables the method to achieve the accuracy of the high level of theory (e.g., coupled cluster) while the cost remains that of DFT. The advantages and limitations of the method are discussed along with areas of ongoing developments.

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Section: Generalized Graph-theoretic Approach For Cbh Generation and ...mentioning

confidence: 99%

Section: Generalized Graph-theoretic Approach For Cbh Generation and ...mentioning

confidence: 99%

Approaching Coupled Cluster Accuracy with Density Functional Theory Using the Generalized Connectivity-Based Hierarchy

Raghavachari

Maier

Collins

et al. 2023

J. Chem. Theory Comput.

View full text Add to dashboard Cite

show abstract

“…characteristics including H 298K , A tot , V m , ns 2 tot , etc., based on the Gaussian 09 calculated results. An automated BSR soware package, the Automatic Bond Separation Reaction Platform (ABSRP) 41 recently developed by us, was used to calculate D f -H q g , with corrections on H 298K using the connectivity-based hierarchy. 72 The logical layer and the interaction layer of EM-DB were developed using MongoDB and Vue.js, respectively.…”

Section: Code Availabilitymentioning

confidence: 99%

“…Therefore, reliable theoretical formulae or statistical models for property prediction, as well as high accuracy and low CPU-time cost methods, are necessary for the high-throughput design of energetic molecules. 26,41 Our team has been engaged in high-throughput design of energetic molecules since 2018 and carried out studies including performance prediction models, 13,14 high accuracy and low cost schemes for quantum chemical calculations, 41,42 tools for automated calculation and data processing, 43 platforms for workow management, 44,45 and virtual screening of energetic molecules. [46][47][48] These studies provide a solution for the high-throughput design of energetic molecules and enable us to develop a specic platform, namely EM-Studio.…”

Section: Introuductionmentioning

confidence: 99%