This work presents an E(3)equivariant graph neural network called HamGNN,which can fit the electronic Hamiltonian matrix of molecules and solids by a complete data-driven method.Unlike invariant models that achieve eq...This work presents an E(3)equivariant graph neural network called HamGNN,which can fit the electronic Hamiltonian matrix of molecules and solids by a complete data-driven method.Unlike invariant models that achieve equivariance approximately through data augmentation,HamGNN employs E(3)equivariant convolutions to construct the Hamiltonian matrix,ensuring strict adherence to all equivariant constraints inherent in the physical system.In contrast to previous models with limited transferability,HamGNN demonstrates exceptional accuracy on various datasets,including QM9 molecular datasets,carbon allotropes,silicon allotropes,SiO_(2) isomers,and BixSey compounds.The trained HamGNN models exhibit accurate predictions of electronic structures for large crystals beyond the training set,including the Moirétwisted bilayer MoS2 and silicon supercells with dislocation defects,showcasing remarkable transferability and generalization capabilities.The HamGNN model,trained on small systems,can serve as an efficient alternative to density functional theory(DFT)for accurately computing the electronic structures of large systems.展开更多
The Poisson–Boltzmann(PB)theory is one of the most important theoretical models describing charged systems continuously.However,it suffers from neglecting ion correlations,which hinders its applicability to more gene...The Poisson–Boltzmann(PB)theory is one of the most important theoretical models describing charged systems continuously.However,it suffers from neglecting ion correlations,which hinders its applicability to more general charged systems other than extremely dilute ones.Therefore,some modified versions of the PB theory are developed to effectively include ion correlations.Focused on their applications to ionic solutions,the original PB theory and its variances,including the field-theoretic approach,the correlation-enhanced PB model,the Outhwaite–Bhuiyan modified PB theory and the mean field theories,are briefly reviewed in this paper with the diagnosis of their advantages and limitations.展开更多
基金We thank Dr.Hongli Guo for providing the structure of the Moirésuperlattice of bilayer MoS2.We acknowledge financial support from the Ministry of Science and Technology of the People´s Republic of China(No.2022YFA1402901)NSFC(grants No.11825403,11991061,12188101)the Guangdong Major Project of the Basic and Applied Basic Research(Future functional materials under extreme conditions-2021B0301030005).
文摘This work presents an E(3)equivariant graph neural network called HamGNN,which can fit the electronic Hamiltonian matrix of molecules and solids by a complete data-driven method.Unlike invariant models that achieve equivariance approximately through data augmentation,HamGNN employs E(3)equivariant convolutions to construct the Hamiltonian matrix,ensuring strict adherence to all equivariant constraints inherent in the physical system.In contrast to previous models with limited transferability,HamGNN demonstrates exceptional accuracy on various datasets,including QM9 molecular datasets,carbon allotropes,silicon allotropes,SiO_(2) isomers,and BixSey compounds.The trained HamGNN models exhibit accurate predictions of electronic structures for large crystals beyond the training set,including the Moirétwisted bilayer MoS2 and silicon supercells with dislocation defects,showcasing remarkable transferability and generalization capabilities.The HamGNN model,trained on small systems,can serve as an efficient alternative to density functional theory(DFT)for accurately computing the electronic structures of large systems.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDA17010504)the National Natural Science Foundation of China(Nos.11774357 and 11947302)the CAS Biophysics Interdisciplinary Innovation Team Project(No.2060299)。
文摘The Poisson–Boltzmann(PB)theory is one of the most important theoretical models describing charged systems continuously.However,it suffers from neglecting ion correlations,which hinders its applicability to more general charged systems other than extremely dilute ones.Therefore,some modified versions of the PB theory are developed to effectively include ion correlations.Focused on their applications to ionic solutions,the original PB theory and its variances,including the field-theoretic approach,the correlation-enhanced PB model,the Outhwaite–Bhuiyan modified PB theory and the mean field theories,are briefly reviewed in this paper with the diagnosis of their advantages and limitations.
