The GW approximation represents the state-of-the-art ab-initio method for computing excited-state properties.Its execution requires control over a larger number of parameters,and therefore,its application in high-thro...The GW approximation represents the state-of-the-art ab-initio method for computing excited-state properties.Its execution requires control over a larger number of parameters,and therefore,its application in high-throughput studies is hindered by the complex and time-consuming convergence process across a multidimensional parameter space.To address these challenges,we develop a fullyautomated open-source workflow for G0W0 calculations within the AiiDA framework and the projector augmented wave(PAW)method.The workflow is based on an efficient estimation of the errors in the quasi-particle(QP)energies due to basis-set truncation and ultra-soft PAWpotentials norm violation,which allows a reduction in the dimensionality of the parameter space and avoids the need for multidimensional convergence searches.Protocol validation is conducted through a systematic comparison against established experimental and state-of-the-art GW data.To demonstrate the effectiveness of the approach,we construct a database of QP energies for a dataset of over 320 bulk structures.展开更多
We introduce an automated,flexible framework(aiida-hubbard)to self-consistently calculate Hubbard U and V parameters from first-principles.By leveraging density-functional perturbation theory,the computation of the Hu...We introduce an automated,flexible framework(aiida-hubbard)to self-consistently calculate Hubbard U and V parameters from first-principles.By leveraging density-functional perturbation theory,the computation of the Hubbard parameters is efficiently parallelized using multiple concurrent and inexpensive primitive cell calculations.Furthermore,the intersite V parameters are defined on-the-fly during the iterative procedure to account for atomic relaxations and diverse coordination environments.We devise a novel,code-agnostic data structure to store Hubbard related information together with the atomistic structure,to enhance the reproducibility of Hubbard-corrected calculations.We demonstrate the scalability and reliability of the framework by computing in high-throughput fashion the self-consistent onsite U and intersite V parameters for 115 Li-containing bulk solids with up to 32 atoms in the unit cell.Our analysis of the Hubbard parameters calculated reveals a significant correlation of the onsite U values on the oxidation state and coordination environment of the atom on which the Hubbard manifold is centered,while intersite V values exhibit a general decay with increasing interatomic distance.We find,e.g.,that the numerical values of U for the 3d orbitals of Fe and Mn can vary up to 3 eV and 6 eV,respectively;their distribution is characterized by typical shifts of about 0.5 eV and 1.0 eV upon change in oxidation state,or local coordination environment.For the intersite V a narrower spread is found,with values ranging between 0.2 eV and 1.6 eV when considering transition metal and oxygen interactions.This framework paves the way for the exploration of redox materials chemistry and high-throughput screening of d and f compounds across diverse research areas,including the discovery and design of novel energy storage materials,as well as other technologically-relevant applications.展开更多
基金funded by the European Union—Next Generation EU—“PNRR - M4C2, investimento 1.1—Fondo PRIN 2022”—“Superlattices of relativistic oxides” (ID 2022L28H97, CUP D53D23002260006)The authors acknowledge the CINECA award under the ISCRA initiative, for the availability of high-performance computing resources and support, as well as computing time granted by the Vienna Scientific Cluster. Open Access funding is provided by University of Vienna.
文摘The GW approximation represents the state-of-the-art ab-initio method for computing excited-state properties.Its execution requires control over a larger number of parameters,and therefore,its application in high-throughput studies is hindered by the complex and time-consuming convergence process across a multidimensional parameter space.To address these challenges,we develop a fullyautomated open-source workflow for G0W0 calculations within the AiiDA framework and the projector augmented wave(PAW)method.The workflow is based on an efficient estimation of the errors in the quasi-particle(QP)energies due to basis-set truncation and ultra-soft PAWpotentials norm violation,which allows a reduction in the dimensionality of the parameter space and avoids the need for multidimensional convergence searches.Protocol validation is conducted through a systematic comparison against established experimental and state-of-the-art GW data.To demonstrate the effectiveness of the approach,we construct a database of QP energies for a dataset of over 320 bulk structures.
基金support from the Deutsche Forschungsgemeinschaft(DFG)under Germany’s Excellence Strategy(EXC 2077,No.390741603,University Allowance,University of Bremen),Lucio Colombi Ciacchi,the host of the“U Bremen Excellence Chair Program”C.M.and E.M acknowledge funding by MaX“Materials Design at the Exascale”,a Center of Excellence co-funded by the European High Performance Computing Joint Undertaking(JU)and participating countries under grant agreement No.101093374+4 种基金M.B.acknowledges funding by the European Centre of Excellence MaX“Materials design at the Exascale”(grant no.824143)and by the SwissTwins project,funded by the Swiss State Secretariat for Education,Research and Innovation(SERI)I.T.acknowledges funding by the Swiss National Science Foundation(grant no.200021-227641)We acknowledge support by the NCCR MARVEL,a National Centre of Competence in Research,funded by the Swiss National Science Foundation(Grant number 205602)This work was supported by a grant from the Swiss National Supercomputing Centre(CSCS)under project ID 465000416(LUMI-G).We thank Julian Geiger,Gabriel Joalland,Austin Zadoks and Timo Reents for useful discussions and feedbacks.
文摘We introduce an automated,flexible framework(aiida-hubbard)to self-consistently calculate Hubbard U and V parameters from first-principles.By leveraging density-functional perturbation theory,the computation of the Hubbard parameters is efficiently parallelized using multiple concurrent and inexpensive primitive cell calculations.Furthermore,the intersite V parameters are defined on-the-fly during the iterative procedure to account for atomic relaxations and diverse coordination environments.We devise a novel,code-agnostic data structure to store Hubbard related information together with the atomistic structure,to enhance the reproducibility of Hubbard-corrected calculations.We demonstrate the scalability and reliability of the framework by computing in high-throughput fashion the self-consistent onsite U and intersite V parameters for 115 Li-containing bulk solids with up to 32 atoms in the unit cell.Our analysis of the Hubbard parameters calculated reveals a significant correlation of the onsite U values on the oxidation state and coordination environment of the atom on which the Hubbard manifold is centered,while intersite V values exhibit a general decay with increasing interatomic distance.We find,e.g.,that the numerical values of U for the 3d orbitals of Fe and Mn can vary up to 3 eV and 6 eV,respectively;their distribution is characterized by typical shifts of about 0.5 eV and 1.0 eV upon change in oxidation state,or local coordination environment.For the intersite V a narrower spread is found,with values ranging between 0.2 eV and 1.6 eV when considering transition metal and oxygen interactions.This framework paves the way for the exploration of redox materials chemistry and high-throughput screening of d and f compounds across diverse research areas,including the discovery and design of novel energy storage materials,as well as other technologically-relevant applications.
