Paramagnetic Nuclear Magnetic Resonance Shifts for Triplet Systems and Beyond with Modern Relativistic Density Functional Methods

Franzke, Yannick J.; Bruder, Florian; Gillhuber, Sebastian; Holzer, Christof; Weigend, Florian

doi:10.1021/acs.jpca.3c07093

Cited by 5 publications

(1 citation statement)

References 202 publications

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“…In the course of the present work, this low-scaling DLU scheme was implemented for all X2C modules in TURBOMOLE. [91,[106][107][108][109][110][111][112][113][114][115][116][117][118][119]…”

Section: Exact Two-component Transformation For Fermionsmentioning

confidence: 99%

Beyond Electrons: Correlation and Self‐Energy in Multicomponent Density Functional Theory

Holzer,

Franzke

2024

ChemPhysChem

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Post‐Kohn‐‐Sham methods are used to evaluate the ground‐state correlation energy and the orbital self‐energy of systems consisting of multiple flavors of different fermions. Starting from multicomponent density functional theory, suitable ways to arrive at the corresponding multicomponent random‐phase approximation and the multicomponent Green's function GW approximation, including relativistic effects, are outlined. Given the importance of both of this methods in the development of modern Kohn‐‐Sham density functional approximations, this work will provide a foundation to design advanced multicomponent density functional approximations. Additionally, the GW quasiparticle energies are needed to study light‐matter interactions with the Bethe‐‐Salpeter equation.

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“…In the course of the present work, this low-scaling DLU scheme was implemented for all X2C modules in TURBOMOLE. [91,[106][107][108][109][110][111][112][113][114][115][116][117][118][119]…”

Section: Exact Two-component Transformation For Fermionsmentioning

confidence: 99%

Beyond Electrons: Correlation and Self‐Energy in Multicomponent Density Functional Theory

Holzer,

Franzke

2024

ChemPhysChem

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A General and Transferable Local Hybrid Functional for Electronic Structure Theory and Many-Fermion Approaches

Holzer,

Franzke

2024

J. Chem. Theory Comput.

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Density functional theory has become the workhorse of quantum physics, chemistry, and materials science. Within these fields, a broad range of applications needs to be covered. These applications range from solids to molecular systems, from organic to inorganic chemistry, or even from electrons to other Fermions, such as protons or muons. This is emphasized by the plethora of density functional approximations that have been developed for various cases. In this work, two new local hybrid exchange−correlation density functionals are constructed from first-principles, promoting generality and transferability. We show that constraint satisfaction can be achieved even for admixtures with full exact exchange, without sacrificing accuracy. The performance of the new functionals CHYF-PBE and CHYF-B95 is assessed for thermochemical properties, excitation energies, Mossbauer isomer shifts, NMR spin−spin coupling constants, NMR shieldings and shifts, magnetizabilities, and EPR hyperfine coupling constants. Here, the new density functional shows excellent performance throughout all tests and is numerically robust only requiring small grids for converged results. Additionally, both functionals can easily be generalized to arbitrary Fermions as shown for electron−proton correlation energies. Therefore, we outline that density functionals generated in this way are general purpose tools for quantum mechanical studies.

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Application of the Adiabatic Connection Random Phase Approximation to Electron–Nucleus Hyperfine Coupling Constants

Bruder,

Weigend,

Franzke

2024

J. Phys. Chem. A

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The electron−nucleus hyperfine coupling constant is a challenging property for density functional methods. For accurate results, hybrid functionals with a large amount of exact exchange are often needed and there is no clear "one-for-all" functional which describes the hyperfine coupling interaction for a large set of nuclei. To alleviate this unfavorable situation, we apply the adiabatic connection random phase approximation (RPA) in its post-Kohn−Sham fashion to this property as a first test. For simplicity, only the Fermi-contact and spin−dipole terms are calculated within the nonrelativistic and the scalar-relativistic exact two-component framework. This requires to solve a single coupled-perturbed Kohn−Sham equation to evaluate the relaxed density matrix, which comes with a modest increase in computational demands. RPA performs remarkably well and substantially improves upon its Kohn−Sham (KS) starting point while also reducing the dependence on the KS reference. For main-group systems, RPA outperforms global, range-separated, and local hybrid functionals�at similar computational costs. For transition-metal compounds and lanthanide complexes, a similar performance as for hybrid functionals is observed. In contrast, related post-Hartree− Fock methods such as Møller−Plesset perturbation theory or CC2 perform worse than semilocal density functionals.

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Paramagnetic Nuclear Magnetic Resonance Shifts for Triplet Systems and Beyond with Modern Relativistic Density Functional Methods

Cited by 5 publications

References 202 publications

Beyond Electrons: Correlation and Self‐Energy in Multicomponent Density Functional Theory

Beyond Electrons: Correlation and Self‐Energy in Multicomponent Density Functional Theory

A General and Transferable Local Hybrid Functional for Electronic Structure Theory and Many-Fermion Approaches

Application of the Adiabatic Connection Random Phase Approximation to Electron–Nucleus Hyperfine Coupling Constants

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