2026
|
Desmarais, Jacques K; Bencheikh, Kamel; Vignale, Giovanni; Pittalis, Stefano Physical Spin Torques from Exactly Constrained Exchange-Correlation
Torques PHYSICAL REVIEW LETTERS, 136 (1), 2026, DOI: 10.1103/lt1f-8pz2. Abstract | BibTeX | Endnote @article{WOS:001681866100003,
title = {Physical Spin Torques from Exactly Constrained Exchange-Correlation
Torques},
author = {Jacques K Desmarais and Kamel Bencheikh and Giovanni Vignale and Stefano Pittalis},
doi = {10.1103/lt1f-8pz2},
times_cited = {1},
issn = {0031-9007},
year = {2026},
date = {2026-01-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {136},
number = {1},
publisher = {AMER PHYSICAL SOC},
address = {ONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA},
abstract = {The problem of capturing physical spin torques in noncollinear magnetic
systems has dominated the scene of spin-density functional theory (SDFT)
in the last two decades. Progress has been hindered by the fact that the
spin torque is directly connected to the divergence of the spin current,
a quantity that is extraneous to SDFT-thus leading to spurious
exchange-correlation (xc) torques in the spin dynamics. Moreover, SDFT
cannot rigorously include vector potentials and spin-orbit couplings.
Here, we propose a solution that exploits the U & eth;1 & THORN; x SU
& eth;2 & THORN; invariance of the xc energy of Spin-current DFT-an
exact constraint that is not accessible to SDFT. Nonvanishing xc torques
obtained on noncollinear solutions are constrained by the aforementioned
exact internal symmetry and do not enter the propagation of the spin
magnetization-i.e., the spin dynamics involve only the physical currents
and physical spin torques.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The problem of capturing physical spin torques in noncollinear magnetic
systems has dominated the scene of spin-density functional theory (SDFT)
in the last two decades. Progress has been hindered by the fact that the
spin torque is directly connected to the divergence of the spin current,
a quantity that is extraneous to SDFT-thus leading to spurious
exchange-correlation (xc) torques in the spin dynamics. Moreover, SDFT
cannot rigorously include vector potentials and spin-orbit couplings.
Here, we propose a solution that exploits the U & eth;1 & THORN; x SU
& eth;2 & THORN; invariance of the xc energy of Spin-current DFT-an
exact constraint that is not accessible to SDFT. Nonvanishing xc torques
obtained on noncollinear solutions are constrained by the aforementioned
exact internal symmetry and do not enter the propagation of the spin
magnetization-i.e., the spin dynamics involve only the physical currents
and physical spin torques. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFJacques K Desmarais
Kamel Bencheikh
Giovanni Vignale
Stefano Pittalis
- TIPhysical Spin Torques from Exactly Constrained Exchange-Correlation
Torques - SOPHYSICAL REVIEW LETTERS
- DTArticle
- ABThe problem of capturing physical spin torques in noncollinear magnetic
systems has dominated the scene of spin-density functional theory (SDFT)
in the last two decades. Progress has been hindered by the fact that the
spin torque is directly connected to the divergence of the spin current,
a quantity that is extraneous to SDFT-thus leading to spurious
exchange-correlation (xc) torques in the spin dynamics. Moreover, SDFT
cannot rigorously include vector potentials and spin-orbit couplings.
Here, we propose a solution that exploits the U & eth;1 & THORN; x SU
& eth;2 & THORN; invariance of the xc energy of Spin-current DFT-an
exact constraint that is not accessible to SDFT. Nonvanishing xc torques
obtained on noncollinear solutions are constrained by the aforementioned
exact internal symmetry and do not enter the propagation of the spin
magnetization-i.e., the spin dynamics involve only the physical currents
and physical spin torques. - Z91
- PUAMER PHYSICAL SOC
- PAONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA
- SN0031-9007
- VL136
- DI10.1103/lt1f-8pz2
- UTWOS:001681866100003
- ER
- EF
|
2025
|
Peng, Liangtao; Vignale, Giovanni; Adam, Shaffique Many-body perturbation theory for moiré systems PHYSICAL REVIEW B, 112 (7), 2025, DOI: 10.1103/5qws-l9ny. Abstract | BibTeX | Endnote @article{WOS:001556600200001,
title = {Many-body perturbation theory for moiré systems},
author = {Liangtao Peng and Giovanni Vignale and Shaffique Adam},
doi = {10.1103/5qws-l9ny},
times_cited = {2},
issn = {2469-9950},
year = {2025},
date = {2025-08-01},
journal = {PHYSICAL REVIEW B},
volume = {112},
number = {7},
publisher = {AMER PHYSICAL SOC},
address = {ONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA},
abstract = {Moir & eacute; systems such as magic-angle twisted bilayer graphene
have attracted significant attention due to their ability to host
correlated phenomena including superconductivity and strongly correlated
insulating states. By defining the single-particle Green's function in
the band basis, we systematically develop a many-body perturbation
theory framework to address correlations beyond the usual mean-field
Hartree-Fock approaches. As a specific example, we first analyze twisted
bilayer graphene within the Hartree-Fock approximation. We derive
analytical solutions for symmetry-breaking states at integer fillings
and the finite-temperature metal-insulator transition that closely match
previously known numerical results in the literature. Moving beyond
Hartree-Fock, we incorporate self-consistent GW corrections
demonstrating that first-order diagrams significantly overestimate the
filling-dependent fluctuations in the electronic compressibility. This
framework provides a comprehensive pathway for exploring strong
electronic correlations in moir & eacute; systems beyond the mean-field
theory, giving new insights into the interplay of symmetry breaking and
electron correlations.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Moir & eacute; systems such as magic-angle twisted bilayer graphene
have attracted significant attention due to their ability to host
correlated phenomena including superconductivity and strongly correlated
insulating states. By defining the single-particle Green's function in
the band basis, we systematically develop a many-body perturbation
theory framework to address correlations beyond the usual mean-field
Hartree-Fock approaches. As a specific example, we first analyze twisted
bilayer graphene within the Hartree-Fock approximation. We derive
analytical solutions for symmetry-breaking states at integer fillings
and the finite-temperature metal-insulator transition that closely match
previously known numerical results in the literature. Moving beyond
Hartree-Fock, we incorporate self-consistent GW corrections
demonstrating that first-order diagrams significantly overestimate the
filling-dependent fluctuations in the electronic compressibility. This
framework provides a comprehensive pathway for exploring strong
electronic correlations in moir & eacute; systems beyond the mean-field
theory, giving new insights into the interplay of symmetry breaking and
electron correlations. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFLiangtao Peng
Giovanni Vignale
Shaffique Adam
- TIMany-body perturbation theory for moiré systems
- SOPHYSICAL REVIEW B
- DTArticle
- ABMoir & eacute; systems such as magic-angle twisted bilayer graphene
have attracted significant attention due to their ability to host
correlated phenomena including superconductivity and strongly correlated
insulating states. By defining the single-particle Green's function in
the band basis, we systematically develop a many-body perturbation
theory framework to address correlations beyond the usual mean-field
Hartree-Fock approaches. As a specific example, we first analyze twisted
bilayer graphene within the Hartree-Fock approximation. We derive
analytical solutions for symmetry-breaking states at integer fillings
and the finite-temperature metal-insulator transition that closely match
previously known numerical results in the literature. Moving beyond
Hartree-Fock, we incorporate self-consistent GW corrections
demonstrating that first-order diagrams significantly overestimate the
filling-dependent fluctuations in the electronic compressibility. This
framework provides a comprehensive pathway for exploring strong
electronic correlations in moir & eacute; systems beyond the mean-field
theory, giving new insights into the interplay of symmetry breaking and
electron correlations. - Z92
- PUAMER PHYSICAL SOC
- PAONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA
- SN2469-9950
- VL112
- DI10.1103/5qws-l9ny
- UTWOS:001556600200001
- ER
- EF
|
Majumdar, Sangita; Shi, Zekun; Vignale, Giovanni Orbital-Free Density Functional Theory for Periodic Solids: Construction
of the Pauli Potential JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 21 (12), pp. 6007-6022, 2025, DOI: 10.1021/acs.jctc.5c00442. Abstract | BibTeX | Endnote @article{WOS:001500033200001,
title = {Orbital-Free Density Functional Theory for Periodic Solids: Construction
of the Pauli Potential},
author = {Sangita Majumdar and Zekun Shi and Giovanni Vignale},
doi = {10.1021/acs.jctc.5c00442},
times_cited = {1},
issn = {1549-9618},
year = {2025},
date = {2025-05-01},
journal = {JOURNAL OF CHEMICAL THEORY AND COMPUTATION},
volume = {21},
number = {12},
pages = {6007-6022},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {The practical success of density functional theory (DFT) is largely
credited to the Kohn-Sham approach, which enables the exact calculation
of the noninteracting electron kinetic energy via an auxiliary
noninteracting system. Yet, the realization of DFT's full potential
awaits the discovery of a direct link between the electron density, n,
and the noninteracting kinetic energy, T S [n]. In this work, we
address two key challenges toward this objective. First, we introduce a
new algorithm for directly solving the constrained minimization problem
yielding T S [n] for periodic densities-a class of densities that, in
spite of its central importance for materials science, has received
limited attention in the literature. Second, we present a numerical
procedure that allows us to calculate the functional derivative of T S
[n] with respect to the density at a constant electron number, also
known as the Kohn-Sham potential V S [n](r). Lastly, the algorithm is
augmented with a subroutine that computes the ``derivative
discontinuity'', i.e., the spatially uniform jump in V S [n](r)
which occurs upon increasing or decreasing the total number of
electrons. This feature allows us to distinguish between
``insulating'' and ``conducting'' densities for noninteracting
electrons. The code integrates key methodological innovations such as
the use of an adaptive basis set (''equidensity orbitals'') for wave
function expansion and the QR decomposition to accelerate the
implementation of the orthogonality constraint. Notably, we derive a
closed-form expression for the Pauli potential in one dimension,
expressed solely in terms of the input density without relying on
Kohn-Sham eigenvalues and eigenfunctions. We validate this method on
one-dimensional periodic densities, achieving results within ``chemical
accuracy''.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The practical success of density functional theory (DFT) is largely
credited to the Kohn-Sham approach, which enables the exact calculation
of the noninteracting electron kinetic energy via an auxiliary
noninteracting system. Yet, the realization of DFT's full potential
awaits the discovery of a direct link between the electron density, n,
and the noninteracting kinetic energy, T S [n]. In this work, we
address two key challenges toward this objective. First, we introduce a
new algorithm for directly solving the constrained minimization problem
yielding T S [n] for periodic densities-a class of densities that, in
spite of its central importance for materials science, has received
limited attention in the literature. Second, we present a numerical
procedure that allows us to calculate the functional derivative of T S
[n] with respect to the density at a constant electron number, also
known as the Kohn-Sham potential V S [n](r). Lastly, the algorithm is
augmented with a subroutine that computes the ``derivative
discontinuity'', i.e., the spatially uniform jump in V S [n](r)
which occurs upon increasing or decreasing the total number of
electrons. This feature allows us to distinguish between
``insulating'' and ``conducting'' densities for noninteracting
electrons. The code integrates key methodological innovations such as
the use of an adaptive basis set (''equidensity orbitals'') for wave
function expansion and the QR decomposition to accelerate the
implementation of the orthogonality constraint. Notably, we derive a
closed-form expression for the Pauli potential in one dimension,
expressed solely in terms of the input density without relying on
Kohn-Sham eigenvalues and eigenfunctions. We validate this method on
one-dimensional periodic densities, achieving results within ``chemical
accuracy''. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFSangita Majumdar
Zekun Shi
Giovanni Vignale
- TIOrbital-Free Density Functional Theory for Periodic Solids: Construction
of the Pauli Potential - SOJOURNAL OF CHEMICAL THEORY AND COMPUTATION
- DTArticle
- ABThe practical success of density functional theory (DFT) is largely
credited to the Kohn-Sham approach, which enables the exact calculation
of the noninteracting electron kinetic energy via an auxiliary
noninteracting system. Yet, the realization of DFT's full potential
awaits the discovery of a direct link between the electron density, n,
and the noninteracting kinetic energy, T S [n]. In this work, we
address two key challenges toward this objective. First, we introduce a
new algorithm for directly solving the constrained minimization problem
yielding T S [n] for periodic densities-a class of densities that, in
spite of its central importance for materials science, has received
limited attention in the literature. Second, we present a numerical
procedure that allows us to calculate the functional derivative of T S
[n] with respect to the density at a constant electron number, also
known as the Kohn-Sham potential V S [n](r). Lastly, the algorithm is
augmented with a subroutine that computes the ``derivative
discontinuity'', i.e., the spatially uniform jump in V S [n](r)
which occurs upon increasing or decreasing the total number of
electrons. This feature allows us to distinguish between
``insulating'' and ``conducting'' densities for noninteracting
electrons. The code integrates key methodological innovations such as
the use of an adaptive basis set (''equidensity orbitals'') for wave
function expansion and the QR decomposition to accelerate the
implementation of the orthogonality constraint. Notably, we derive a
closed-form expression for the Pauli potential in one dimension,
expressed solely in terms of the input density without relying on
Kohn-Sham eigenvalues and eigenfunctions. We validate this method on
one-dimensional periodic densities, achieving results within ``chemical
accuracy''. - Z91
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1549-9618
- VL21
- BP6007
- EP6022
- DI10.1021/acs.jctc.5c00442
- UTWOS:001500033200001
- ER
- EF
|
Sun, Hao; Vignale, Giovanni Orbital magnetic moment dynamics and Hanle magnetoresistance in
multilayered two-dimensional materials PHYSICAL REVIEW B, 111 (18), 2025, DOI: 10.1103/PhysRevB.111.L180408. Abstract | BibTeX | Endnote @article{WOS:001501130000006,
title = {Orbital magnetic moment dynamics and Hanle magnetoresistance in
multilayered two-dimensional materials},
author = {Hao Sun and Giovanni Vignale},
doi = {10.1103/PhysRevB.111.L180408},
times_cited = {0},
issn = {2469-9950},
year = {2025},
date = {2025-05-01},
journal = {PHYSICAL REVIEW B},
volume = {111},
number = {18},
publisher = {AMER PHYSICAL SOC},
address = {ONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA},
abstract = {The orbital Hall effect (OHE) has several potential advantages over the
spin Hall effect (SHE), the latter being well known for its many
applications in spintronics. Like the spin Hall effect, the OHE occurs
in nonmagnetic materials without stringent symmetry requirements, but
unlike the SHE it does not rely on relatively weak spinorbit
interaction. In two-dimensional (2D) materials these advantages risk
being nullified by the difficulty of turning the orbital moment away
from the out-of-plane direction. Multilayered 2D materials offer a way
out of this difficulty because the fluctuating in-plane component of the
orbital moment, due to motion of electrons between the layers, can latch
to a magnetic field. To describe this effect we have derived a
semiphenomenological equation of motion for the density of orbital
magnetic moment in stacked 2D materials subjected to a magnetic field.
Unlike the equations of motion for the spin, these equations produce a
strongly anisotropic dynamics, which is governed by an inverse effective
mass tensor for which we provide a fully microscopic expression. As a
first application, we combine our equation of motion with
phenomenological drift-diffusion equations to formulate a theory of
orbital Hanle magnetoresistance in multilayered 2D materials. This
theoretical framework also offers a tool for exploring the microscopic
theory of the orbital Hall effect, which remains an active area of
debate.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The orbital Hall effect (OHE) has several potential advantages over the
spin Hall effect (SHE), the latter being well known for its many
applications in spintronics. Like the spin Hall effect, the OHE occurs
in nonmagnetic materials without stringent symmetry requirements, but
unlike the SHE it does not rely on relatively weak spinorbit
interaction. In two-dimensional (2D) materials these advantages risk
being nullified by the difficulty of turning the orbital moment away
from the out-of-plane direction. Multilayered 2D materials offer a way
out of this difficulty because the fluctuating in-plane component of the
orbital moment, due to motion of electrons between the layers, can latch
to a magnetic field. To describe this effect we have derived a
semiphenomenological equation of motion for the density of orbital
magnetic moment in stacked 2D materials subjected to a magnetic field.
Unlike the equations of motion for the spin, these equations produce a
strongly anisotropic dynamics, which is governed by an inverse effective
mass tensor for which we provide a fully microscopic expression. As a
first application, we combine our equation of motion with
phenomenological drift-diffusion equations to formulate a theory of
orbital Hanle magnetoresistance in multilayered 2D materials. This
theoretical framework also offers a tool for exploring the microscopic
theory of the orbital Hall effect, which remains an active area of
debate. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFHao Sun
Giovanni Vignale
- TIOrbital magnetic moment dynamics and Hanle magnetoresistance in
multilayered two-dimensional materials - SOPHYSICAL REVIEW B
- DTArticle
- ABThe orbital Hall effect (OHE) has several potential advantages over the
spin Hall effect (SHE), the latter being well known for its many
applications in spintronics. Like the spin Hall effect, the OHE occurs
in nonmagnetic materials without stringent symmetry requirements, but
unlike the SHE it does not rely on relatively weak spinorbit
interaction. In two-dimensional (2D) materials these advantages risk
being nullified by the difficulty of turning the orbital moment away
from the out-of-plane direction. Multilayered 2D materials offer a way
out of this difficulty because the fluctuating in-plane component of the
orbital moment, due to motion of electrons between the layers, can latch
to a magnetic field. To describe this effect we have derived a
semiphenomenological equation of motion for the density of orbital
magnetic moment in stacked 2D materials subjected to a magnetic field.
Unlike the equations of motion for the spin, these equations produce a
strongly anisotropic dynamics, which is governed by an inverse effective
mass tensor for which we provide a fully microscopic expression. As a
first application, we combine our equation of motion with
phenomenological drift-diffusion equations to formulate a theory of
orbital Hanle magnetoresistance in multilayered 2D materials. This
theoretical framework also offers a tool for exploring the microscopic
theory of the orbital Hall effect, which remains an active area of
debate. - Z90
- PUAMER PHYSICAL SOC
- PAONE PHYSICS ELLIPSE, COLLEGE PK, MD 20740-3844 USA
- SN2469-9950
- VL111
- DI10.1103/PhysRevB.111.L180408
- UTWOS:001501130000006
- ER
- EF
|
Li, Tianbo; Lin, Min; Dale, Stephen G; Shi, Zekun; Neto, Castro A H; Novoselov, Kostya S; Vignale, Giovanni Diagonalization without Diagonalization: A Direct Optimization Approach
for Solid-State Density Functional Theory JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 21 (9), pp. 4730-4741, 2025, DOI: 10.1021/acs.jctc.4c01551. Abstract | BibTeX | Endnote @article{WOS:001478048300001,
title = {Diagonalization without Diagonalization: A Direct Optimization Approach
for Solid-State Density Functional Theory},
author = {Tianbo Li and Min Lin and Stephen G Dale and Zekun Shi and Castro A H Neto and Kostya S Novoselov and Giovanni Vignale},
doi = {10.1021/acs.jctc.4c01551},
times_cited = {2},
issn = {1549-9618},
year = {2025},
date = {2025-04-01},
journal = {JOURNAL OF CHEMICAL THEORY AND COMPUTATION},
volume = {21},
number = {9},
pages = {4730-4741},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {We present a novel approach to address the challenges of variable
occupation numbers in direct optimization of density functional theory
(DFT). By parametrizing both the eigenfunctions and the occupation
matrix, our method minimizes the free energy with respect to these
parameters. As the stationary conditions require the occupation matrix
and the Kohn-Sham Hamiltonian to be simultaneously diagonalizable, this
leads to the concept of ``self-diagonalization,'' where, by assuming a
diagonal occupation matrix without loss of generality, the Hamiltonian
matrix naturally becomes diagonal at stationary points. Our method
incorporates physical constraints on both the eigenfunctions and the
occupations into the parametrization, transforming the constrained
optimization into an fully differentiable unconstrained problem, which
is solvable via gradient descent. Implemented in JAX, our method was
tested on aluminum and silicon, confirming that it achieves efficient
self-diagonalization, produces the correct Fermi-Dirac distribution of
the occupation numbers and yields band structures consistent with those
obtained with SCF eigensolver methods in Quantum Espresso.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present a novel approach to address the challenges of variable
occupation numbers in direct optimization of density functional theory
(DFT). By parametrizing both the eigenfunctions and the occupation
matrix, our method minimizes the free energy with respect to these
parameters. As the stationary conditions require the occupation matrix
and the Kohn-Sham Hamiltonian to be simultaneously diagonalizable, this
leads to the concept of ``self-diagonalization,'' where, by assuming a
diagonal occupation matrix without loss of generality, the Hamiltonian
matrix naturally becomes diagonal at stationary points. Our method
incorporates physical constraints on both the eigenfunctions and the
occupations into the parametrization, transforming the constrained
optimization into an fully differentiable unconstrained problem, which
is solvable via gradient descent. Implemented in JAX, our method was
tested on aluminum and silicon, confirming that it achieves efficient
self-diagonalization, produces the correct Fermi-Dirac distribution of
the occupation numbers and yields band structures consistent with those
obtained with SCF eigensolver methods in Quantum Espresso. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AFTianbo Li
Min Lin
Stephen G Dale
Zekun Shi
Castro A H Neto
Kostya S Novoselov
Giovanni Vignale
- TIDiagonalization without Diagonalization: A Direct Optimization Approach
for Solid-State Density Functional Theory - SOJOURNAL OF CHEMICAL THEORY AND COMPUTATION
- DTArticle
- ABWe present a novel approach to address the challenges of variable
occupation numbers in direct optimization of density functional theory
(DFT). By parametrizing both the eigenfunctions and the occupation
matrix, our method minimizes the free energy with respect to these
parameters. As the stationary conditions require the occupation matrix
and the Kohn-Sham Hamiltonian to be simultaneously diagonalizable, this
leads to the concept of ``self-diagonalization,'' where, by assuming a
diagonal occupation matrix without loss of generality, the Hamiltonian
matrix naturally becomes diagonal at stationary points. Our method
incorporates physical constraints on both the eigenfunctions and the
occupations into the parametrization, transforming the constrained
optimization into an fully differentiable unconstrained problem, which
is solvable via gradient descent. Implemented in JAX, our method was
tested on aluminum and silicon, confirming that it achieves efficient
self-diagonalization, produces the correct Fermi-Dirac distribution of
the occupation numbers and yields band structures consistent with those
obtained with SCF eigensolver methods in Quantum Espresso. - Z92
- PUAMER CHEMICAL SOC
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1549-9618
- VL21
- BP4730
- EP4741
- DI10.1021/acs.jctc.4c01551
- UTWOS:001478048300001
- ER
- EF
|