The desirable physical properties of hardness, high temperature stability, and conductivity make the early transition metal nitrides important materials for various technological applications. To learn more about the ...The desirable physical properties of hardness, high temperature stability, and conductivity make the early transition metal nitrides important materials for various technological applications. To learn more about the nature of these materials, the local-density approximation（LDA） and GW approximation i.e. combination of the Green function G and the screened Coulomb interaction W, have been performed. This paper investigates the bulk electronic and physical properties of early transition metal mononitridcs, ScN and YN in the rocksalt structure. In this paper, the semicore electrons are regarded as valance electrons. ScN appears to be a semimetal, and YN is semiconductor with band gap of 0.142 eV within the LDA, but are in fact semiconductors with indirect band gaps of 1.244 and 0.544 eV respectively, as revealed by calculations performed using GW approximation.展开更多
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
Electronic band structure is one of the most important intrinsic properties of a material,and is in particular crucial in electronic,photo-electronic and photo-catalytic applications.Kohn-Sham Density-functional theor...Electronic band structure is one of the most important intrinsic properties of a material,and is in particular crucial in electronic,photo-electronic and photo-catalytic applications.Kohn-Sham Density-functional theory(KS-DFT)within currently available local or semi-local approximations to the exchange-correlation energy functional is problematic for the description of electronic band structure.Many-body perturbation theory based on Green’s function(GF)provides a rigorous framework to describe excited-state properties of materials.The central ingredient of the GF-based many-body perturbation theory is the exchangecorrelation self-energy,which accounts for all nonclassical electron-electron interaction effects beyond the Hartree theory,and formally can be obtained by solving a set of complicated integro-differential equations,named Hedin’s equations.The GW approximation,in which the self-energy is simply a product of Green’s function and the screened Coulomb interaction(W),is currently the most accurate first-principles approach to describe electronic band structure properties of extended systems.Compared to KS-DFT,the computational efforts required for GW calculations are much larger.Various numerical techniques or approximations have been developed to apply GW for realistic systems.In this paper,we give an overview of the theory of first-principles Green’s function approach in the GW approximation and review the state of the art for the implementation of GW in different representations and with different treatment of the frequency dependence.It is hoped that further methodological developments will be inspired by this work so that the approach can be applied to more complicated and scientifically more interesting systems.展开更多
基金Project supported by the National Natural Science Foundation of China （Grant Nos 10274946 and 60336010）.
文摘The desirable physical properties of hardness, high temperature stability, and conductivity make the early transition metal nitrides important materials for various technological applications. To learn more about the nature of these materials, the local-density approximation（LDA） and GW approximation i.e. combination of the Green function G and the screened Coulomb interaction W, have been performed. This paper investigates the bulk electronic and physical properties of early transition metal mononitridcs, ScN and YN in the rocksalt structure. In this paper, the semicore electrons are regarded as valance electrons. ScN appears to be a semimetal, and YN is semiconductor with band gap of 0.142 eV within the LDA, but are in fact semiconductors with indirect band gaps of 1.244 and 0.544 eV respectively, as revealed by calculations performed using GW approximation.
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.
文摘Electronic band structure is one of the most important intrinsic properties of a material,and is in particular crucial in electronic,photo-electronic and photo-catalytic applications.Kohn-Sham Density-functional theory(KS-DFT)within currently available local or semi-local approximations to the exchange-correlation energy functional is problematic for the description of electronic band structure.Many-body perturbation theory based on Green’s function(GF)provides a rigorous framework to describe excited-state properties of materials.The central ingredient of the GF-based many-body perturbation theory is the exchangecorrelation self-energy,which accounts for all nonclassical electron-electron interaction effects beyond the Hartree theory,and formally can be obtained by solving a set of complicated integro-differential equations,named Hedin’s equations.The GW approximation,in which the self-energy is simply a product of Green’s function and the screened Coulomb interaction(W),is currently the most accurate first-principles approach to describe electronic band structure properties of extended systems.Compared to KS-DFT,the computational efforts required for GW calculations are much larger.Various numerical techniques or approximations have been developed to apply GW for realistic systems.In this paper,we give an overview of the theory of first-principles Green’s function approach in the GW approximation and review the state of the art for the implementation of GW in different representations and with different treatment of the frequency dependence.It is hoped that further methodological developments will be inspired by this work so that the approach can be applied to more complicated and scientifically more interesting systems.
