Electronic Structure - IOPscience

Electronic Structure - IOPscience
Electronic Structure
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is a coalition of three not-for-profit publishers in the field of physical sciences: AIP Publishing, the American Physical Society and IOP Publishing.
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Electronic Structure
is a new multidisciplinary journal covering all theoretical and experimental aspects of electronic structure research, including the development of new methods. It is dedicated to the entirety of electronic structure research and its community, spanning materials science, physics, chemistry and biology.
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The following article is
Open access
The physical significance of imaginary phonon modes in crystals
Ioanna Pallikara
et al
2022
Electron. Struct.
033002
View article
, The physical significance of imaginary phonon modes in crystals
PDF
, The physical significance of imaginary phonon modes in crystals
The lattice vibrations (phonon modes) of crystals underpin a large number of material properties. The harmonic phonon spectrum of a solid is the simplest description of its structural dynamics and can be straightforwardly derived from the Hellman–Feynman forces obtained in a ground-state electronic structure calculation. The presence of imaginary harmonic modes in the spectrum indicates that a structure is not a local minimum on the structural potential-energy surface and is instead a saddle point or a hilltop, for example. This can in turn yield important insight into the fundamental nature and physical properties of a material. In this review article, we discuss the physical significance of imaginary harmonic modes and distinguish between cases where imaginary modes are indicative of such phenomena, and those where they reflect technical problems in the calculations. We outline basic approaches for exploring and renormalising imaginary modes, and demonstrate their utility through a set of three case studies in the materials sciences.
The following article is
Open access
Roadmap on Machine learning in electronic structure
H J Kulik
et al
2022
Electron. Struct.
023004
View article
, Roadmap on Machine learning in electronic structure
PDF
, Roadmap on Machine learning in electronic structure
In recent years, we have been witnessing a paradigm shift in computational materials science. In fact, traditional methods, mostly developed in the second half of the XXth century, are being complemented, extended, and sometimes even completely replaced by faster, simpler, and often more accurate approaches. The new approaches, that we collectively label by machine learning, have their origins in the fields of informatics and artificial intelligence, but are making rapid inroads in all other branches of science. With this in mind, this Roadmap article, consisting of multiple contributions from experts across the field, discusses the use of machine learning in materials science, and share perspectives on current and future challenges in problems as diverse as the prediction of materials properties, the construction of force-fields, the development of exchange correlation functionals for density-functional theory, the solution of the many-body problem, and more. In spite of the already numerous and exciting success stories, we are just at the beginning of a long path that will reshape materials science for the many challenges of the XXIth century.
The following article is
Open access
Roadmap on methods and software for electronic structure based simulations in chemistry and materials
Volker Blum
et al
2024
Electron. Struct.
042501
View article
, Roadmap on methods and software for electronic structure based simulations in chemistry and materials
PDF
, Roadmap on methods and software for electronic structure based simulations in chemistry and materials
This Roadmap article provides a succinct, comprehensive overview of the state of electronic structure (ES) methods and software for molecular and materials simulations. Seventeen distinct sections collect insights by 51 leading scientists in the field. Each contribution addresses the status of a particular area, as well as current challenges and anticipated future advances, with a particular eye towards software related aspects and providing key references for further reading. Foundational sections cover density functional theory and its implementation in real-world simulation frameworks, Green’s function based many-body perturbation theory, wave-function based and stochastic ES approaches, relativistic effects and semiempirical ES theory approaches. Subsequent sections cover nuclear quantum effects, real-time propagation of the ES, challenges for computational spectroscopy simulations, and exploration of complex potential energy surfaces. The final sections summarize practical aspects, including computational workflows for complex simulation tasks, the impact of current and future high-performance computing architectures, software engineering practices, education and training to maintain and broaden the community, as well as the status of and needs for ES based modeling from the vantage point of industry environments. Overall, the field of ES software and method development continues to unlock immense opportunities for future scientific discovery, based on the growing ability of computations to reveal complex phenomena, processes and properties that are determined by the make-up of matter at the atomic scale, with high precision.
The following article is
Open access
High-throughput design of magnetic materials
Hongbin Zhang 2021
Electron. Struct.
033001
View article
, High-throughput design of magnetic materials
PDF
, High-throughput design of magnetic materials
Materials design based on density functional theory (DFT) calculations is an emergent field of great potential to accelerate the development and employment of novel materials. Magnetic materials play an essential role in green energy applications as they provide efficient ways of harvesting, converting, and utilizing energy. In this review, after a brief introduction to the major functionalities of magnetic materials, we demonstrated how the fundamental properties can be tackled via high-throughput DFT calculations, with a particular focus on the current challenges and feasible solutions. Successful case studies are summarized on several classes of magnetic materials, followed by bird-view perspectives.
The following article is
Open access
High-resolution angle-resolved photoemission spectroscopy and microscopy
Hideaki Iwasawa 2020
Electron. Struct.
043001
View article
, High-resolution angle-resolved photoemission spectroscopy and microscopy
PDF
, High-resolution angle-resolved photoemission spectroscopy and microscopy
This review outlines fundamental principles, instrumentation, and capabilities of angle-resolved photoemission spectroscopy (ARPES) and microscopy. We will present how high-resolution ARPES enables to investigate fine structures of electronic band dispersions, Fermi surfaces, gap structures, and many-body interactions, and how angle-resolved photoemission microscopy (spatially-resolved ARPES) utilizing micro/nano-focused light allows to extract spatially localized electronic information at small dimensions. This work is focused on specific results obtained by the author from strongly correlated copper and ruthenium oxides, to help readers to understand consistently how these techniques can provide essential electronic information of materials, which can, in principle, apply to a wide variety of systems.
The following article is
Open access
Benchmarking ANO-R basis set for multiconfigurational calculations
E D Larsson
et al
2022
Electron. Struct.
014009
View article
, Benchmarking ANO-R basis set for multiconfigurational calculations
PDF
, Benchmarking ANO-R basis set for multiconfigurational calculations
The selection of basis sets is very important for multiconfigurational wave function calculation, due to a balance between a desired accuracy and computational costs. Recently, the atomic natural orbital-relativistic (ANO-R) basis set was published as a suggested replacement for the ANO-RCC basis set for scalar-relativistic correlated calculations Zobel
et al
(2021
J. Chem. Theory Comput.
16
278–294). Benchmarking ANO-R basis set against ANO-RCC for atoms (from H to Rn) and their compounds is the goal of this study. Many of these compounds (for instance, diatomic molecules containing transition metals) have open shells, for which reason a multiconfigurational approach is necessary and was primarily used throughout this project. Performance of the ANO-R basis set in multiconfigurational calculations is similar to the ANO-RCC basis set for the ionisation potential of atoms, and the bond distance in diatomic molecules. Deficiencies are noted for atomic electron affinities and dissociation energies of fluoride diatomic molecules. ANO-R basis sets are more compact in comparison to the corresponding ANO-RCC basis sets leading to smaller computational costs, which was demonstrated by chloroiron corrole molecule as an example.
The following article is
Open access
Superconductivity in bcc high-entropy alloys: a comparative review of experimental data and DFT predictions
Piotr Sobota
et al
2025
Electron. Struct.
023002
View article
, Superconductivity in bcc high-entropy alloys: a comparative review of experimental data and DFT predictions
PDF
, Superconductivity in bcc high-entropy alloys: a comparative review of experimental data and DFT predictions
High-entropy alloys (HEAs) with body-centred cubic (bcc) structures possess one of the highest critical parameters among HEA superconductors, making them one of the most promising candidates for practical applications in their field. This review systematically compares experimental data and theoretical predictions from density functional theory (DFT) for superconducting bcc HEAs, focusing on critical parameters such as the superconducting critical temperature, the Debye temperature, and the electron-phonon coupling constant. Although DFT provides valuable information on electronic structures, lattice dynamics, and thermodynamic stability, significant discrepancies persist between the computed and measured parameters. Possible reasons for this are discussed.
The following article is
Open access
Phonons from density-functional perturbation theory using the all-electron full-potential linearized augmented plane-wave method
FLEUR
Christian-Roman Gerhorst
et al
2024
Electron. Struct.
017001
View article
, Phonons from density-functional perturbation theory using the all-electron full-potential linearized augmented plane-wave method FLEUR
PDF
, Phonons from density-functional perturbation theory using the all-electron full-potential linearized augmented plane-wave method FLEUR
Phonons are quantized vibrations of a crystal lattice that play a crucial role in understanding many properties of solids. Density functional theory provides a state-of-the-art computational approach to lattice vibrations from first-principles. We present a successful software implementation for calculating phonons in the harmonic approximation, employing density-functional perturbation theory within the framework of the full-potential linearized augmented plane-wave method as implemented in the electronic structure package
FLEUR
. The implementation, which involves the Sternheimer equation for the linear response of the wave function, charge density, and potential with respect to infinitesimal atomic displacements, as well as the setup of the dynamical matrix, is presented and the specifics due to the muffin-tin sphere centered linearized augmented plane-wave basis-set and the all-electron nature are discussed. As a test, we calculate the phonon dispersion of several solids including an insulator, a semiconductor as well as several metals. The latter are comprised of magnetic, simple, and transition metals. The results are validated on the basis of phonon dispersions calculated using the finite displacement approach in conjunction with the
FLEUR
code and the
phonopy
package, as well as by some experimental results. An excellent agreement is obtained.
The following article is
Open access
Electronic structure of cesium-based photocathode materials from density functional theory: performance of PBE, SCAN, and HSE06 functionals
Holger-Dietrich Saßnick and Caterina Cocchi 2021
Electron. Struct.
027001
View article
, Electronic structure of cesium-based photocathode materials from density functional theory: performance of PBE, SCAN, and HSE06 functionals
PDF
, Electronic structure of cesium-based photocathode materials from density functional theory: performance of PBE, SCAN, and HSE06 functionals
The development of novel materials for vacuum electron sources in particle accelerators is an active field of research that can greatly benefit from the results of
ab initio
calculations for the characterization of the electronic structure of target systems. As state-of-the-art many-body perturbation theory calculations are too expensive for large-scale material screening, density functional theory offers the best compromise between accuracy and computational feasibility. The quality of the obtained results, however, crucially depends on the choice of the exchange–correlation potential,
xc
. To address this essential point, we systematically analyze the performance of three popular approximations of
xc
[PBE, strongly constrained and appropriately normed (SCAN), and HSE06] on the structural and electronic properties of bulk Cs
Sb and Cs
Te as representative materials of Cs-based semiconductors employed in photocathode applications. Among the adopted approximations, PBE shows expectedly the largest discrepancies from the target: the unit cell volume is overestimated compared to the experimental value, while the band gap is severely underestimated. On the other hand, both SCAN and HSE06 perform remarkably well in reproducing both structural and electronic properties. Spin–orbit coupling, which mainly impacts the valence region of both materials inducing a band splitting and, consequently, a band-gap reduction of the order of 0.2 eV, is equally captured by all functionals. Our results indicate SCAN as the best trade-off between accuracy and computational costs, outperforming the considerably more expensive HSE06.
The following article is
Open access
Perspective on Moreau–Yosida regularization in density-functional theory
Markus Penz
et al
2026
Electron. Struct.
022001
View article
, Perspective on Moreau–Yosida regularization in density-functional theory
PDF
, Perspective on Moreau–Yosida regularization in density-functional theory
Within density-functional theory (DFT), Moreau–Yosida regularization enables both a reformulation of the theory and a mathematically well-defined definition of the Kohn–Sham approach. It is further employed in density–potential inversion schemes and, through the choice of topology for the density and potential space, can be directly linked to classical field theories. This perspective collects various appearances of the regularization technique within DFT alongside possibilities for their future development.
The following article is
Open access
Perspective on Moreau–Yosida regularization in density-functional theory
Markus Penz
et al
2026
Electron. Struct.
022001
View article
, Perspective on Moreau–Yosida regularization in density-functional theory
PDF
, Perspective on Moreau–Yosida regularization in density-functional theory
Within density-functional theory (DFT), Moreau–Yosida regularization enables both a reformulation of the theory and a mathematically well-defined definition of the Kohn–Sham approach. It is further employed in density–potential inversion schemes and, through the choice of topology for the density and potential space, can be directly linked to classical field theories. This perspective collects various appearances of the regularization technique within DFT alongside possibilities for their future development.
Energetics, structural magic numbers, and vibrational modes of small carbon clusters
= 3–8): a comparative study of different
ab initio
methods and basis sets
Angelo A Redoblado and Darwin B Putungan 2026
Electron. Struct.
025001
View article
, Energetics, structural magic numbers, and vibrational modes of small carbon clusters Cn (n = 3–8): a comparative study of different ab initio methods and basis sets
PDF
, Energetics, structural magic numbers, and vibrational modes of small carbon clusters Cn (n = 3–8): a comparative study of different ab initio methods and basis sets
Carbon clusters are fundamental building blocks of nanostructured carbon materials with applications in materials science, biomaterials, and energy technologies. In this work, the structural stability, electronic properties, and vibrational characteristics of small carbon clusters
= 3–8) were investigated using
ab initio
methods, including Hartree–Fock (HF), density functional theory (DFT) with the B3LYP functional with and without Grimme’s dispersion correction, and coupled-cluster singles and doubles (CCSD). Calculations employed the 6–31+G(d), 6–311+G(d,p), and cc-pVTZ basis sets. Linear isomers were identified as the most stable structures for all cluster sizes, indicating that linear geometries can already be captured at the HF level. Binding energies increase with cluster size, while DFT and CCSD accurately reproduce stability trends and identify
and
as magic-number clusters. Vibrational analyses reveal dominant asymmetric stretching modes in the mid-infrared (IR) region and bending modes in the far-IR region, consistent with available experimental data.
Kinetic energy density functional: advances, challenges, and future directions
Fahhad H Alharbi 2026
Electron. Struct.
023001
View article
, Kinetic energy density functional: advances, challenges, and future directions
PDF
, Kinetic energy density functional: advances, challenges, and future directions
Density functional theory (DFT) is widely used for electronic structure calculations, primarily utilizing the Kohn–Sham scheme. However, this approach reintroduces orbitals, resulting in a high computational cost. In contrast, the original orbital-free Hohenberg–Kohn DFT (OF-DFT) offers the potential for linear-scaling computations suitable for large systems. The advancement of OF-DFT relies on the development of an accurate and universal kinetic energy density functional (KEDF). This review surveys the progress, challenges, and prospects in KEDF development. It presents the essential physical and mathematical constraints that any KEDF must comply with, tracing the evolution from early models like Thomas–Fermi and von Weizsäcker to contemporary semi-local, nonlocal, and machine-learned approaches. While the developed KEDFs have improved the treatment of metals and some semiconductors, achieving transferable accuracy for molecules and systems with considerable density inhomogeneities remains a critical challenge. We highlight two emerging paradigms; the use of physics-guided machine learning to identify accurate KEDFs and information-theoretic approaches that provide deep insights. The path forward requires a renewed focus on fundamental physical constraints, steering the field away from purely empirical fitting toward a universal, computationally efficient KEDF that maximizes the advantages of OF-DFT. The main KEDFs are listed, including gradient expansions, enhancement-factor strategies, density-decomposition methods, and nonlocal KEDFs guided by linear-response theory.
Electronic structure and charge transition levels in oxygen deficient monoclinic zirconia
Sanat Kumar Gogoi and Manish Jain 2026
Electron. Struct.
015009
View article
, Electronic structure and charge transition levels in oxygen deficient monoclinic zirconia
PDF
, Electronic structure and charge transition levels in oxygen deficient monoclinic zirconia
We present the modification of electronic structure properties due to the presence of oxygen vacancies in monoclinic-zirconia (m-ZrO
). Using a combined density functional theory (DFT) and GW formalism, we study the electronic structure and charge transition levels (CTLs) of oxygen vacancy (OV) defects in m-ZrO
. The CTLs are calculated using two paths and employing electrostatic corrections due to localized charge at the defect site. We find +1/0 CTL is at 3.48 eV (2.50 eV) and +2/+1 CTL is at 1.92 eV (0.98 eV) for 3-fold (4-fold) OV in m-ZrO
. We also describe a relaxation mechanism of atoms near an OV site. Finally, we compare the calculated CTLs using only DFT and the combined approach of both DFT and GW method with appropriate electrostatic corrections. Our results agree well with the experimental findings of electronic trap level in m-
, as reported by Mondal
et al
(2020
IEEE Electron. Dev. Lett.
41
717–20), Li
et al
(2010
Thin Solid Films
518
6382–4), Cong
et al
(2009
J. Phys. Chem. C
113
13974–8)
Defect-induced spin-split localized states with strong out-of-plane spin polarization in monolayer 1H-WSe
: DFT and
analysis
Muhammad Oktavian Dharma Setyawan
et al
2026
Electron. Struct.
015008
View article
, Defect-induced spin-split localized states with strong out-of-plane spin polarization in monolayer 1H-WSe2: DFT and analysis
PDF
, Defect-induced spin-split localized states with strong out-of-plane spin polarization in monolayer 1H-WSe2: DFT and analysis
This study presents a comprehensive density functional theory analysis of the structural and electronic modifications induced by point defects and spin–orbit coupling in monolayer 1H-WSe
. Among intrinsic point defects, the selenium vacancy is identified as the most energetically favorable and is shown to generate well-localized in-gap states predominantly originating from the
orbitals of neighboring W atoms. Spin–orbit coupling lifts the spin degeneracy of these defect states, giving rise to pronounced spin splitting with a dominant out-of-plane spin component as a consequence of broken local in-plane mirror symmetry and the strong atomic spin–orbit interaction of tungsten. Spin-resolved band structure calculations further reveal valley-dependent spin polarization with a dominant out-of-plane spin component at the
and
′ points, indicating a nontrivial coupling between defect states and the spin and valley degrees of freedom. The essential features of the defect-induced spin splitting and spin texture are captured by a minimal
Hamiltonian, providing analytical insight into the underlying symmetry and spin–orbit mechanisms. Our results establish defect engineering as an effective route to realize localized spin-polarized states in two-dimensional transition metal dichalcogenides, offering promising prospects for spintronic and valleytronic quantum device applications.
Kinetic energy density functional: advances, challenges, and future directions
Fahhad H Alharbi 2026
Electron. Struct.
023001
View article
, Kinetic energy density functional: advances, challenges, and future directions
PDF
, Kinetic energy density functional: advances, challenges, and future directions
Density functional theory (DFT) is widely used for electronic structure calculations, primarily utilizing the Kohn–Sham scheme. However, this approach reintroduces orbitals, resulting in a high computational cost. In contrast, the original orbital-free Hohenberg–Kohn DFT (OF-DFT) offers the potential for linear-scaling computations suitable for large systems. The advancement of OF-DFT relies on the development of an accurate and universal kinetic energy density functional (KEDF). This review surveys the progress, challenges, and prospects in KEDF development. It presents the essential physical and mathematical constraints that any KEDF must comply with, tracing the evolution from early models like Thomas–Fermi and von Weizsäcker to contemporary semi-local, nonlocal, and machine-learned approaches. While the developed KEDFs have improved the treatment of metals and some semiconductors, achieving transferable accuracy for molecules and systems with considerable density inhomogeneities remains a critical challenge. We highlight two emerging paradigms; the use of physics-guided machine learning to identify accurate KEDFs and information-theoretic approaches that provide deep insights. The path forward requires a renewed focus on fundamental physical constraints, steering the field away from purely empirical fitting toward a universal, computationally efficient KEDF that maximizes the advantages of OF-DFT. The main KEDFs are listed, including gradient expansions, enhancement-factor strategies, density-decomposition methods, and nonlocal KEDFs guided by linear-response theory.
2D materials beyond MXenes: recent progress, exotic properties, and future perspectives of alkaline earth metal based structures and their isoelectronic analogues
Krishnanshu Basak
et al
2026
Electron. Struct.
013001
View article
, 2D materials beyond MXenes: recent progress, exotic properties, and future perspectives of alkaline earth metal based structures and their isoelectronic analogues
PDF
, 2D materials beyond MXenes: recent progress, exotic properties, and future perspectives of alkaline earth metal based structures and their isoelectronic analogues
The advent of computational and experimental approaches of novel two-dimensional (2D) metal carbides and nitrides, encompassing a variety of metal species of group IIA, IIB, IIIA and various transition metals (collectively known as MXenes) has unveiled significant advances in materials science and technology. Among them, alkaline-earth metal nitrides and carbides (AEXenes) have attracted enormous attention particularly following the experimental realization of few AEXenes as a 2D electride. Herein we have systematically reviewed the structural, electronic, thermal, mechanical, magnetic and optical properties of the 2D AEXenes, reported in recent literature. Leveraging these intriguing features, we have assigned their prospective applications across diverse domains including energy storage, energy harvesting, catalytic and spintronic devices. For instance, BeN monolayers possess significantly high storage capacity (3489 mAh gm
−1
) with low diffusion barrier and placing them on par with functionalized MXenes. However, Mg
C and Mg
display remarkably low lattice thermal conductivity of 20.26 Wm
−1
−1
and 1.5 Wm
−1
−1
, attributed to distinctive structural complexity, elevated scattering rate and ultimately result better energy conversion efficiency. We have further outlined viable approaches i.e. external carrier doping, adsorption, various defect engineering to modulate their electronic and magnetic properties to facilitate themselves for different applications. In this topical review, we aim to explore recent advancement of these functionalized materials and their isoelectronic analogues to harness their exceptional properties from both theoretical and experimental perspectives.
The following article is
Open access
Introduction to the fifth-rung density functional approximations: concept, formulation, and applications
Igor Ying Zhang
et al
2025
Electron. Struct.
043002
View article
, Introduction to the fifth-rung density functional approximations: concept, formulation, and applications
PDF
, Introduction to the fifth-rung density functional approximations: concept, formulation, and applications
The widespread use of (generalized) Kohn–Sham (KS) density functional theory lies in the fact that hierarchical sets of approximations of the exchange-correlation (XC) energy functional can be designed, offering versatile choices to satisfy different levels of accuracy needs. The XC functionals standing on the fifth (top) rung of Jacob’s ladder incorporate the information of unoccupied KS orbitals, and by doing so can describe seamlessly non-local electron correlations that the lower-rung functionals fail to capture. The doubly hybrid approximations (DHAs) and random phase approximation (RPA) based methods are two representative classes of fifth-rung functionals that have been under active development over the past two decades. In this review, we recapitulate the basic concepts of DHAs and RPA, derive their underlying theoretical formulation from the perspective of adiabatic-connection fluctuation-dissipation theory, and describe the implementation algorithms based on the resolution-of-identity technique within an atomic-orbital basis-set framework. Illustrating examples of practical applications of DHAs and RPA are presented, highlighting the usefulness of these functionals in resolving challenging problems in computational materials science. The most recent advances in the realms of these two types of functionals are briefly discussed.
High-entropy electrocatalysts toward high-performance oxygen evolution reaction: a perspective from atomic-scale electronic structure modulation
Xiaoliang Zhang
et al
2025
Electron. Struct.
043001
View article
, High-entropy electrocatalysts toward high-performance oxygen evolution reaction: a perspective from atomic-scale electronic structure modulation
PDF
, High-entropy electrocatalysts toward high-performance oxygen evolution reaction: a perspective from atomic-scale electronic structure modulation
Water electrolysis represents a critical pathway towards sustainable hydrogen production within the global green energy landscape. The oxygen evolution reaction (OER), the kinetically limiting anodic process, necessitates the development of highly active and durable electrocatalysts. High-entropy materials, offering unparalleled compositional diversity and inherent multi-component synergistic effects, have emerged as promising candidates to address the OER bottleneck. While recent reviews have explored various aspects of high-entropy electrocatalysts (HECs), a comprehensive understanding of the atomic-level design and modulation strategies that govern their exceptional OER performance remains a critical gap. This review aims to bridge this gap by focusing on the atomic-level insights crucial for designing and optimizing HECs. We first examine advancements in machine learning-assisted atomic-level design strategies for OER HECs. Subsequently, we delve into five key atomic-level modulation approaches: tailoring local atomic coordination environments, engineering atomic interface architectures, manipulating intrinsic lattice strain, controlled introduction of atomic-scale defects, and exploiting synergistic multi-site atomic interactions. Finally, we delineate future research directions to accelerate the rational design and practical implementation of efficient and robust HECs under demanding operating conditions.
The following article is
Open access
Superconductivity in bcc high-entropy alloys: a comparative review of experimental data and DFT predictions
Piotr Sobota
et al
2025
Electron. Struct.
023002
View article
, Superconductivity in bcc high-entropy alloys: a comparative review of experimental data and DFT predictions
PDF
, Superconductivity in bcc high-entropy alloys: a comparative review of experimental data and DFT predictions
High-entropy alloys (HEAs) with body-centred cubic (bcc) structures possess one of the highest critical parameters among HEA superconductors, making them one of the most promising candidates for practical applications in their field. This review systematically compares experimental data and theoretical predictions from density functional theory (DFT) for superconducting bcc HEAs, focusing on critical parameters such as the superconducting critical temperature, the Debye temperature, and the electron-phonon coupling constant. Although DFT provides valuable information on electronic structures, lattice dynamics, and thermodynamic stability, significant discrepancies persist between the computed and measured parameters. Possible reasons for this are discussed.
The following article is
Open access
Static correlation diagnostics from the grand potential of fermions
Soriano-Agueda et al
View accepted manuscript
, Static correlation diagnostics from the grand potential of fermions
PDF
, Static correlation diagnostics from the grand potential of fermions
The accurate identification of static (non-dynamical) electron correlation remains a fundamental challenge in quantum chemistry, particularly for systems that exhibit pronounced multireference character. In this work, we derive two diagnostics, R_MAX and 〖Δε〗_MAX, for quantifying the multireference nature of molecular systems. Both indices are rigorously derived from the Grand Potential of Fermions and are dependent on natural orbitals, offering complementary perspectives on the degree of static correlation in electronic species. Univocal numerical thresholds are provided to identify cases where static correlation significantly impacts the electronic structure. An evaluation was also performed using two well-established diagnostics, I_ND^MAX and D2[MP2], as benchmarks. Our results reveal excellent agreement between the proposed and reference diagnostics, with Pearson correlation coefficients exceeding 0.93 across a customized dataset of 1925 chemical systems, extracted from the GMTKN55 database. The strong correspondence between R_MAX, 〖Δε〗_MAX and I_ND^MAX, D2[MP2] confirms that the Grand Potential of Fermions provides a physically meaningful and transferable foundation for diagnosing multireference character. Their balance of interpretability, computational efficiency, and diagnostic accuracy makes them promising tools for guiding the selection of electronic structure methods and identifying cases where single-reference approaches may be insufficient
The following article is
Open access
Static correlation diagnostics from the grand potential of fermions
Luis Soriano-Agueda and Marco Franco-Pérez 2026
Electron. Struct.
View article
, Static correlation diagnostics from the grand potential of fermions
PDF
, Static correlation diagnostics from the grand potential of fermions
The accurate identification of static (non-dynamical) electron correlation remains a fundamental challenge in quantum chemistry, particularly for systems that exhibit pronounced multireference character. In this work, we derive two diagnostics, R_MAX and 〖Δε〗_MAX, for quantifying the multireference nature of molecular systems. Both indices are rigorously derived from the Grand Potential of Fermions and are dependent on natural orbitals, offering complementary perspectives on the degree of static correlation in electronic species. Univocal numerical thresholds are provided to identify cases where static correlation significantly impacts the electronic structure. An evaluation was also performed using two well-established diagnostics, I_ND^MAX and D2[MP2], as benchmarks. Our results reveal excellent agreement between the proposed and reference diagnostics, with Pearson correlation coefficients exceeding 0.93 across a customized dataset of 1925 chemical systems, extracted from the GMTKN55 database. The strong correspondence between R_MAX, 〖Δε〗_MAX and I_ND^MAX, D2[MP2] confirms that the Grand Potential of Fermions provides a physically meaningful and transferable foundation for diagnosing multireference character. Their balance of interpretability, computational efficiency, and diagnostic accuracy makes them promising tools for guiding the selection of electronic structure methods and identifying cases where single-reference approaches may be insufficient
The following article is
Open access
Perspective on Moreau–Yosida regularization in density-functional theory
Markus Penz
et al
2026
Electron. Struct.
022001
View article
, Perspective on Moreau–Yosida regularization in density-functional theory
PDF
, Perspective on Moreau–Yosida regularization in density-functional theory
Within density-functional theory (DFT), Moreau–Yosida regularization enables both a reformulation of the theory and a mathematically well-defined definition of the Kohn–Sham approach. It is further employed in density–potential inversion schemes and, through the choice of topology for the density and potential space, can be directly linked to classical field theories. This perspective collects various appearances of the regularization technique within DFT alongside possibilities for their future development.
The following article is
Open access
The origin of metallic conductivity in Pt
: a first principles study
Akhil R Peeketi
et al
2026
Electron. Struct.
015002
View article
, The origin of metallic conductivity in Pt3O4: a first principles study
PDF
, The origin of metallic conductivity in Pt3O4: a first principles study
The platinum oxide Pt
exhibits metallic conductivity even though it contains square-planar PtO
units, which in related oxides such as PtO are usually associated with insulating behavior. To identify the electronic origin of this anomalous metallicity, we performed a comprehensive first-principles study using the PBE and
SCAN functionals together with Hubbard
corrections and spin-orbit coupling (SOC). Structural benchmarks show that
SCAN with SOC and a moderate
value (
eV) reproduces the experimental lattice constants and formation enthalpy, whereas larger
values (
eV) destabilize the cubic structure. Across all functionals and
values considered in this work, Pt
remains metallic. Analyses of the projected density of states, band structures, charge-density isosurfaces, and bonding characteristics demonstrate that the dominant contribution to the metallic character originates from delocalized Pt–O–Pt hybridized antibonding states at the Fermi level. Direct Pt–Pt interactions are present but contribute less strongly to the conductivity. Bader charge analysis reveals only weak Pt charge disproportionation, consistent with mixed Pt
II
/Pt
III
character, and a small charge-transfer energy that prevents localization of the Pt 5
electrons even at elevated
. In contrast, PtO develops a Mott or charge-transfer gap under modest
despite having the same PtO
coordination environment. These findings demonstrate that persistent Pt–O–Pt covalency is the primary driver of metallicity in Pt
and support the view that this phase can remain conductive under oxygen reduction and oxygen evolution reaction conditions in fuel cell and electrolyzer environments.
The following article is
Open access
Role of electron–electron correlations and disorder in the metal-insulator transition of SrTi
thin films
J Laverock
et al
2025
Electron. Struct.
045003
View article
, Role of electron–electron correlations and disorder in the metal-insulator transition of SrTi VxO3 thin films
PDF
, Role of electron–electron correlations and disorder in the metal-insulator transition of SrTi VxO3 thin films
SrTi
(STVO) is a disordered strongly correlated oxide with potential applications in future oxide electronic devices and as a next-generation transparent conducting oxide. STVO exhibits a compositional metal–insulator transition (MIT) that lies at the heart of such applications. However, a solid framework for the MIT in real strongly correlated systems when faced with competing disorder remains in its infancy. We present site-selective x-ray spectroscopies of STVO which we compare with advanced density functional theory plus dynamical mean-field theory calculations. Together, these allow us to separate the effects of strong electron correlation (Mott behaviour) from those of disorder (Anderson localisation), providing a detailed window into the character of the MIT in STVO. We find signatures of both effects in our spectroscopic data, establishing both behaviours as essential ingredients in the collaborative Mott–Anderson transition.
The following article is
Open access
Introduction to the fifth-rung density functional approximations: concept, formulation, and applications
Igor Ying Zhang
et al
2025
Electron. Struct.
043002
View article
, Introduction to the fifth-rung density functional approximations: concept, formulation, and applications
PDF
, Introduction to the fifth-rung density functional approximations: concept, formulation, and applications
The widespread use of (generalized) Kohn–Sham (KS) density functional theory lies in the fact that hierarchical sets of approximations of the exchange-correlation (XC) energy functional can be designed, offering versatile choices to satisfy different levels of accuracy needs. The XC functionals standing on the fifth (top) rung of Jacob’s ladder incorporate the information of unoccupied KS orbitals, and by doing so can describe seamlessly non-local electron correlations that the lower-rung functionals fail to capture. The doubly hybrid approximations (DHAs) and random phase approximation (RPA) based methods are two representative classes of fifth-rung functionals that have been under active development over the past two decades. In this review, we recapitulate the basic concepts of DHAs and RPA, derive their underlying theoretical formulation from the perspective of adiabatic-connection fluctuation-dissipation theory, and describe the implementation algorithms based on the resolution-of-identity technique within an atomic-orbital basis-set framework. Illustrating examples of practical applications of DHAs and RPA are presented, highlighting the usefulness of these functionals in resolving challenging problems in computational materials science. The most recent advances in the realms of these two types of functionals are briefly discussed.
The following article is
Open access
Line shapes in time- and angle-resolved photoemission spectroscopy explored by machine learning
Tami C Meyer
et al
2025
Electron. Struct.
045001
View article
, Line shapes in time- and angle-resolved photoemission spectroscopy explored by machine learning
PDF
, Line shapes in time- and angle-resolved photoemission spectroscopy explored by machine learning
Time- and angle-resolved photoemission spectroscopy is a powerful technique for investigating the dynamics of excited carriers in quantum materials. Typically, data analysis proceeds via the inspection of time distribution curves (TDCs), which represent the time-dependent photoemission intensity in a region of interest—often chosen somewhat arbitrarily—in energy-momentum space. Here, we employ
-means, an unsupervised machine learning technique, to systematically investigate trends in TDC line shape for quasi-free-standing monolayer graphene and for a simple analytical model. Our analysis reveals how finite energy and time resolution can affect the TDC line shape. We discuss how this can be taken into account in a quantitative analysis, and under what conditions the time-dependent photoemission intensity after laser excitation can be approximated by a simple exponential decay.
The following article is
Open access
Optimization of
ab-initio
based tight-binding models
Henrik Dick and Thomas Dahm 2025
Electron. Struct.
047001
View article
, Optimization of ab-initio based tight-binding models
PDF
, Optimization of ab-initio based tight-binding models
The electronic structure of solids can routinely be calculated by standard methods like density functional theory. However, in complicated situations like interfaces, grain boundaries or contact geometries one needs to resort to more simplified models of the electronic structure. Tight-binding models are using a reduced set of orbitals and aim to approximate the electronic structure by short range hopping processes. For example, maximally localized Wannier functions are often used for that purpose. However, their accuracy is limited by the need to disentangle the electronic bands. Here, we develop and investigate a different procedure to obtain tight-binding models inspired by machine-learning techniques. The model parameters are optimized in such a way as to reproduce
ab-initio
band structure data as accurately as possible using an as small as possible number of model parameters. The procedure is shown to result in models with smaller ranges and fewer orbitals than maximally localized Wannier functions but same or even better accuracy. We argue that such a procedure is more useful for automated construction of tight-binding models particularly for large-scale materials calculations.
The following article is
Open access
Overcoming the challenges of accessing topological hallmarks in Sb(112)
A C Åsland
et al
2025
Electron. Struct.
035002
View article
, Overcoming the challenges of accessing topological hallmarks in Sb(112)
PDF
, Overcoming the challenges of accessing topological hallmarks in Sb(112)
Sb is topologically non-trivial and semi-metallic, but differs from many topological semi-metals because of its continuous band gap. By measuring its (112) surface using angle- and spin-resolved photoemission spectroscopy, Sb(112) was shown to have 1D spin-polarised surface states resembling those on vicinal Bi surfaces and many topological insulators and topological semi-metals. The shape and spin-polarisation of the measured features and the calculated bands agreed. However, the measured features had a slightly steeper energy dispersion and different Fermi-momenta than the calculated bands. Both theoretical and experimental methods were necessary when determining the topology of Sb(112). The presence of projected bulk states near the Fermi-level and varying surface localisation of the electronic states meant it was challenging to deduce the topology of Sb(112) from the number of bands crossing the Fermi-level or a continuous contour in the bulk band gap. Ultimately, the calculations and measurements suggest that there are topological surface states on the Sb(112) surface.
The following article is
Open access
Interacting twisted bilayer graphene with systematic modeling of structural relaxation
Tianyu Kong
et al
2025
Electron. Struct.
035001
View article
, Interacting twisted bilayer graphene with systematic modeling of structural relaxation
PDF
, Interacting twisted bilayer graphene with systematic modeling of structural relaxation
Twisted bilayer graphene (TBG) has drawn significant interest due to recent experiments which show that TBG can exhibit strongly correlated behavior such as the superconducting and correlated insulator phases. Much of the theoretical work on TBG has been based on analysis of the Bistritzer–MacDonald model which includes a phenomenological parameter to account for lattice relaxation. In this work, we use a newly developed continuum model which systematically accounts for the effects of structural relaxation. In particular, we model structural relaxation by coupling linear elasticity to a stacking energy that penalizes disregistry. We compare the impact of the two relaxation models on the corresponding many-body model by defining an interacting model projected to the flat bands. We perform tests at charge neutrality at both the Hartree–Fock and coupled cluster singles and doubles level of theory and find the systematic relaxation model gives quantitative differences from the simplified relaxation model.
The following article is
Open access
Two-dimensional to bulk crossover of the WSe
electronic band structure
Raphaël Salazar
et al
2025
Electron. Struct.
025008
View article
, Two-dimensional to bulk crossover of the WSe2 electronic band structure
PDF
, Two-dimensional to bulk crossover of the WSe2 electronic band structure
Transition metal dichalcogenides (TMDs) are layered materials obtained by stacking two-dimensional sheets weakly bonded by van der Waals interactions. In bulk TMD, band dispersions are observed in the direction normal to the sheet plane (
-direction) due to the hybridization of out-of-plane orbitals but no
-dispersion is expected at the single-layer limit. Using angle-resolved photoemission spectroscopy, we precisely address the two-dimensional to three-dimensional crossover of the electronic band structure of large area epitaxial WSe
thin films. Increasing number of discrete electronic states appears in given
-ranges while increasing the number of layers. The continuous bulk dispersion is nearly retrieved for 6-sheet films. These results are reproduced by calculations going from a relatively simple tight-binding model to a sophisticated KKR-Green’s function calculation.
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Open access
The physical significance of imaginary phonon modes in crystals
Ioanna Pallikara
et al
2022
Electron. Struct.
033002
View article
, The physical significance of imaginary phonon modes in crystals
PDF
, The physical significance of imaginary phonon modes in crystals
The lattice vibrations (phonon modes) of crystals underpin a large number of material properties. The harmonic phonon spectrum of a solid is the simplest description of its structural dynamics and can be straightforwardly derived from the Hellman–Feynman forces obtained in a ground-state electronic structure calculation. The presence of imaginary harmonic modes in the spectrum indicates that a structure is not a local minimum on the structural potential-energy surface and is instead a saddle point or a hilltop, for example. This can in turn yield important insight into the fundamental nature and physical properties of a material. In this review article, we discuss the physical significance of imaginary harmonic modes and distinguish between cases where imaginary modes are indicative of such phenomena, and those where they reflect technical problems in the calculations. We outline basic approaches for exploring and renormalising imaginary modes, and demonstrate their utility through a set of three case studies in the materials sciences.
The following article is
Open access
Roadmap on Machine learning in electronic structure
H J Kulik
et al
2022
Electron. Struct.
023004
View article
, Roadmap on Machine learning in electronic structure
PDF
, Roadmap on Machine learning in electronic structure
In recent years, we have been witnessing a paradigm shift in computational materials science. In fact, traditional methods, mostly developed in the second half of the XXth century, are being complemented, extended, and sometimes even completely replaced by faster, simpler, and often more accurate approaches. The new approaches, that we collectively label by machine learning, have their origins in the fields of informatics and artificial intelligence, but are making rapid inroads in all other branches of science. With this in mind, this Roadmap article, consisting of multiple contributions from experts across the field, discusses the use of machine learning in materials science, and share perspectives on current and future challenges in problems as diverse as the prediction of materials properties, the construction of force-fields, the development of exchange correlation functionals for density-functional theory, the solution of the many-body problem, and more. In spite of the already numerous and exciting success stories, we are just at the beginning of a long path that will reshape materials science for the many challenges of the XXIth century.
Twistronics: a turning point in 2D quantum materials
Zachariah Hennighausen and Swastik Kar 2021
Electron. Struct.
014004
View article
, Twistronics: a turning point in 2D quantum materials
PDF
, Twistronics: a turning point in 2D quantum materials
Moiré superlattices—
periodic orbital overlaps and lattice-reconstruction between sites of high atomic registry in vertically-stacked
2D
layered materials
—are quantum-active interfaces where non-trivial quantum phases on novel phenomena can emerge from geometric arrangements of 2D materials, which are not intrinsic to the parent materials. Unexpected distortions in band-structure and topology lead to long-range correlations, charge-ordering, and several other fascinating quantum phenomena hidden within the physical space
between
the (similar or dissimilar) parent materials. Stacking, twisting, gate-modulating, and optically-exciting these superlattices open up a new field for seamlessly exploring physics from the
weak
to
strong
correlations limit within a many-body and topological framework. It is impossible to capture it all, and the aim of this review is to highlight some of the important recent developments in synthesis, experiments, and potential applications of these materials.
Subspace methods for electronic structure simulations on quantum computers
Mario Motta
et al
2024
Electron. Struct.
013001
View article
, Subspace methods for electronic structure simulations on quantum computers
PDF
, Subspace methods for electronic structure simulations on quantum computers
Quantum subspace methods (QSMs) are a class of quantum computing algorithms where the time-independent Schrödinger equation for a quantum system is projected onto a subspace of the underlying Hilbert space. This projection transforms the Schrödinger equation into an eigenvalue problem determined by measurements carried out on a quantum device. The eigenvalue problem is then solved on a classical computer, yielding approximations to ground- and excited-state energies and wavefunctions. QSMs are examples of hybrid quantum–classical methods, where a quantum device supported by classical computational resources is employed to tackle a problem. QSMs are rapidly gaining traction as a strategy to simulate electronic wavefunctions on quantum computers, and thus their design, development, and application is a key research field at the interface between quantum computation and electronic structure (ES). In this review, we provide a self-contained introduction to QSMs, with emphasis on their application to the ES of molecules. We present the theoretical foundations and applications of QSMs, and we discuss their implementation on quantum hardware, illustrating the impact of noise on their performance.
The following article is
Open access
High-throughput design of magnetic materials
Hongbin Zhang 2021
Electron. Struct.
033001
View article
, High-throughput design of magnetic materials
PDF
, High-throughput design of magnetic materials
Materials design based on density functional theory (DFT) calculations is an emergent field of great potential to accelerate the development and employment of novel materials. Magnetic materials play an essential role in green energy applications as they provide efficient ways of harvesting, converting, and utilizing energy. In this review, after a brief introduction to the major functionalities of magnetic materials, we demonstrated how the fundamental properties can be tackled via high-throughput DFT calculations, with a particular focus on the current challenges and feasible solutions. Successful case studies are summarized on several classes of magnetic materials, followed by bird-view perspectives.
The following article is
Open access
Electronic structure of cesium-based photocathode materials from density functional theory: performance of PBE, SCAN, and HSE06 functionals
Holger-Dietrich Saßnick and Caterina Cocchi 2021
Electron. Struct.
027001
View article
, Electronic structure of cesium-based photocathode materials from density functional theory: performance of PBE, SCAN, and HSE06 functionals
PDF
, Electronic structure of cesium-based photocathode materials from density functional theory: performance of PBE, SCAN, and HSE06 functionals
The development of novel materials for vacuum electron sources in particle accelerators is an active field of research that can greatly benefit from the results of
ab initio
calculations for the characterization of the electronic structure of target systems. As state-of-the-art many-body perturbation theory calculations are too expensive for large-scale material screening, density functional theory offers the best compromise between accuracy and computational feasibility. The quality of the obtained results, however, crucially depends on the choice of the exchange–correlation potential,
xc
. To address this essential point, we systematically analyze the performance of three popular approximations of
xc
[PBE, strongly constrained and appropriately normed (SCAN), and HSE06] on the structural and electronic properties of bulk Cs
Sb and Cs
Te as representative materials of Cs-based semiconductors employed in photocathode applications. Among the adopted approximations, PBE shows expectedly the largest discrepancies from the target: the unit cell volume is overestimated compared to the experimental value, while the band gap is severely underestimated. On the other hand, both SCAN and HSE06 perform remarkably well in reproducing both structural and electronic properties. Spin–orbit coupling, which mainly impacts the valence region of both materials inducing a band splitting and, consequently, a band-gap reduction of the order of 0.2 eV, is equally captured by all functionals. Our results indicate SCAN as the best trade-off between accuracy and computational costs, outperforming the considerably more expensive HSE06.
Bethe–Salpeter equation for absorption and scattering spectroscopy: implementation in the exciting code
Christian Vorwerk
et al
2019
Electron. Struct.
037001
View article
, Bethe–Salpeter equation for absorption and scattering spectroscopy: implementation in the exciting code
PDF
, Bethe–Salpeter equation for absorption and scattering spectroscopy: implementation in the exciting code
The Bethe–Salpeter equation for the electron–hole correlation function is the state-of-the-art formalism for optical and core spectroscopy in condensed matter. Solutions of this equation yield the full dielectric response, including both the absorption and the inelastic scattering spectra. Here, we present an efficient implementation within the all-electron full-potential code
exciting
, which employs the linearized augmented plane-wave (L)APW+LO basis set. Being an all-electron code,
exciting
allows the calculation of optical and core excitations on the same footing. The implementation fully includes the effects of finite momentum transfer which may occur in inelastic x-ray spectroscopy and electron energy-loss spectroscopy. Our implementation does not require the application of the Tamm–Dancoff approximation that is commonly employed in the determination of absorption spectra in condensed matter. The interface with parallel linear-algebra libraries enables the calculation for complex systems. The capability of our implementation to compute, analyze, and interpret the results of different spectroscopic techniques is demonstrated by selected examples of prototypical inorganic and organic semiconductors and insulators.
Progress in the studies of electronic and magnetic properties of layered MPX
materials (M: transition metal, X: chalcogen)
Yuriy Dedkov
et al
2023
Electron. Struct.
043001
View article
, Progress in the studies of electronic and magnetic properties of layered MPX3 materials (M: transition metal, X: chalcogen)
PDF
, Progress in the studies of electronic and magnetic properties of layered MPX3 materials (M: transition metal, X: chalcogen)
The recent progress in the studies of 2D materials placed in front many experimental and theoretical works on the interesting class of materials, the so-called transition metal phosphorus trichalcogenides with structural formula MPX
(M: transition metal, X: chalcogen). Here, the diversity in the M/X combination opens the possibility to tune the electronic and magnetic properties of these materials in a very wide range, resulting in many interesting physical phenomena followed by the promoting their use in different application areas. This review gives a timely overview of the recent progress in the fundamental studies of electronic structure and magnetic properties of MPX
materials (M: Mn, Fe, Co, Ni, X: S, Se) focusing on the results obtained by density functional theory, Raman spectroscopy and electron spectroscopy methods. We pay close attention to the large amount of theoretical and experimental data giving critical analysis of the previously obtained results. It is shown how the systematic fundamental studies of the electronic and magnetic properties of MPX
can help to understand the functionality of these interesting 2D materials in different applications, ranging from optoelectronics to catalysis.
Electronic properties of candidate type-II Weyl semimetal WTe
. A review perspective
P K Das
et al
2019
Electron. Struct.
014003
View article
, Electronic properties of candidate type-II Weyl semimetal WTe2. A review perspective
PDF
, Electronic properties of candidate type-II Weyl semimetal WTe2. A review perspective
Currently, there is a flurry of research interest on materials with an unconventional electronic structure, and we have already seen significant progress in their understanding and engineering towards real-life applications. The interest erupted with the discovery of graphene and topological insulators in the previous decade. The electrons in graphene simulate massless Dirac Fermions with a linearly dispersing Dirac cone in their band structure, while in topological insulators, the electronic bands wind non-trivially in momentum space giving rise to gapless surface states and bulk bandgap. Weyl semimetals in condensed matter systems are the latest addition to this growing family of topological materials. Weyl Fermions are known in the context of high energy physics since almost the beginning of quantum mechanics. They apparently violate charge conservation rules, displaying the ‘chiral anomaly’, with such remarkable properties recently theoretically predicted and experimentally verified to exist as low energy quasiparticle states in certain condensed matter systems. Not only are these new materials extremely important for our fundamental understanding of quantum phenomena, but also they exhibit completely different transport phenomena. For example, massless Fermions are susceptible to scattering from non-magnetic impurities. Dirac semimetals exhibit non-saturating extremely large magnetoresistance as a consequence of their robust electronic bands being protected by time reversal symmetry. These open up whole new possibilities for materials engineering and applications including quantum computing. In this review, we recapitulate some of the outstanding properties of WTe
, namely, its non-saturating titanic magnetoresistance due to perfect electron and hole carrier balance up to a very high magnetic field observed for the very first time. It also indicative of hosting Lorentz violating type-II Weyl Fermions in its bandstructure, again first predicted candidate material to host such a remarkable phase. We primarily focus on the findings of our ARPES, spin-ARPES, and time-resolved ARPES studies complemented by first-principles calculations.
The following article is
Open access
Halide perovskites from first principles: from fundamental optoelectronic properties to the impact of structural and chemical heterogeneity
Marina R Filip and Linn Leppert 2024
Electron. Struct.
033002
View article
, Halide perovskites from first principles: from fundamental optoelectronic properties to the impact of structural and chemical heterogeneity
PDF
, Halide perovskites from first principles: from fundamental optoelectronic properties to the impact of structural and chemical heterogeneity
Organic-inorganic metal-halide perovskite semiconductors have outstanding and widely tunable optoelectronic properties suited for a broad variety of applications. First-principles numerical modelling techniques are playing a key role in unravelling structure-property relationships of this structurally and chemically diverse family of materials, and for predicting new materials and properties. Herein we review first-principles calculations of the photophysics of halide perovskites with a focus on the band structures, optical absorption spectra and excitons, and the effects of electron- and exciton-phonon coupling and temperature on these properties. We focus on first-principles approaches based on density functional theory and Green’s function-based many-body perturbation theory and provide an overview of these approaches. While a large proportion of first-principles studies have been focusing on the prototypical ABX
single perovskites based on Pb and Sn, recent years have witnessed significant efforts to further functionalize halide perovskites, broadening this family of materials to include double perovskites, quasi-low-dimensional structures, and other organic-inorganic materials, interfaces and heterostructures. While this enormous chemical space of perovskite and perovskite-like materials has only begun to be tapped experimentally, recent advances in theoretical and computational methods, as well as in computing infrastructure, have led to the possibility of understanding the photophysics of ever more complex systems. We illustrate this progress in our review by summarizing representative studies of first-principles calculations of halide perovskites with various degrees of complexity.
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2019-present
Electronic Structure
doi: 10.1088/issn.2516-1075
Online ISSN: 2516-1075