Showing 1–9 of 9 results for author: Ohad, G

Square Net TaSiAs Nanowires with Topological Surface Conduction and Linear Magnetoresistance

Authors: Anand Roy, Ofek Goldreich, Guy Ohad, Barun Barick, Olga Brontvein, Ora Bitton, Katya Rechav, Yishay Feldman, Leeor Kronik, Ernesto Joselevich

Abstract: Square-net topological materials exhibit various interesting properties arising from the interplay of their structural diversity, topologically protected bands and different possible electronic features, including intrinsic magnetic ordering and superconductivity. However, little is known about the low-dimensional structures of these materials and their properties. Realization of low-dimensional t… ▽ More Square-net topological materials exhibit various interesting properties arising from the interplay of their structural diversity, topologically protected bands and different possible electronic features, including intrinsic magnetic ordering and superconductivity. However, little is known about the low-dimensional structures of these materials and their properties. Realization of low-dimensional topological square-net materials has the potential of enabling enhancement of their quantum behavior arising from quasi-compact 1D geometry and high surface-to-volume ratio, and their integration into functional devices. This work reports on the synthesis and properties of high-quality, single-crystal nanowires of Si square-net material TaSiAs. The chemical-vapor-transport produces TaSiAs nanowires that are chemically encapsulated with a thin dielectric shell of SiO2, enabling remarkable ambient stability and a pristine surface, which are critical for observing robust topologically protected surface states. Atomic-resolution structural analysis reveals a sharp core-shell interface, and a Si square-net lattice extending along the nanowire axis. These chemically protected nanowires allowed us to observe rich electrical and magnetotransport features, including 4 to 11 times lower room-temperature resistivity than the closest bulk analogues and non-saturating linear magnetoresistance, revealing topologically protected coherent surface transport. First-principles calculations show a wide-range (4 eV) linear band dispersion, alongside different Dirac cones that are protected by either symmorphic (C4) or non-symmorphic symmetries, predicting transport features consistent with our results. The findings demonstrate the unique properties of low-dimensional square-net topological materials and their potential applications, including next-generation interconnects, spintronic devices and quantum computing. △ Less

Submitted 27 July, 2026; originally announced July 2026.

Comments: 5 figures

Automated Workflow for Non-Empirical Wannier-Localized Optimal Tuning of Range-Separated Hybrid Functionals

Authors: Stephen E. Gant, Francesco Ricci, Guy Ohad, Ashwin Ramasubramaniam, Leeor Kronik, Jeffrey B. Neaton

Abstract: We introduce an automated workflow for generating non-empirical Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functionals. WOT-SRSH functionals have been shown to yield highly accurate fundamental band gaps, band structures, and optical spectra for bulk and 2D semiconductors and insulators. Our workflow automatically and efficiently determines the WOT-SRSH functional… ▽ More We introduce an automated workflow for generating non-empirical Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functionals. WOT-SRSH functionals have been shown to yield highly accurate fundamental band gaps, band structures, and optical spectra for bulk and 2D semiconductors and insulators. Our workflow automatically and efficiently determines the WOT-SRSH functional parameters for a given crystal structure and composition, approximately enforcing the correct screened long-range Coulomb interaction and an ionization potential ansatz. In contrast to previous manual tuning approaches, our tuning procedure relies on a new search algorithm that only requires a few hybrid functional calculations with minimal user input. We demonstrate our workflow on 23 previously studied semiconductors and insulators, reporting the same high level of accuracy. By automating the tuning process and improving its computational efficiency, the approach outlined here enables applications of the WOT-SRSH functional to compute spectroscopic and optoelectronic properties for a wide range of materials. △ Less

Submitted 3 November, 2025; originally announced November 2025.

Comments: 16 pages (31 including references), 2 figures, 4 tables. Submitted to Computer Physics Communications. This version includes reviewers comments

Foundations of the ionization potential condition for localized electron removal in density functional theory

Authors: Guy Ohad, María Camarasa-Gómez, Jeffrey B. Neaton, Ashwin Ramasubramaniam, Tim Gould, Leeor Kronik

Abstract: Optimal tuning of functional parameters in density functional theory approximations, based on enforcing the ionization potential theorem, has emerged as the method of choice for the non-empirical prediction of the electronic structure of finite systems. This method has recently been extended to the bulk limit, based on an ansatz that generalizes the ionization potential theorem to the removal of a… ▽ More Optimal tuning of functional parameters in density functional theory approximations, based on enforcing the ionization potential theorem, has emerged as the method of choice for the non-empirical prediction of the electronic structure of finite systems. This method has recently been extended to the bulk limit, based on an ansatz that generalizes the ionization potential theorem to the removal of an electron from a localized Wannier orbital. This Wannier-localization based optimal tuning method has been shown to be highly successful for a wide range of periodic systems, accurately predicting electronic and optical properties. However, a rigorous theoretical justification for its foundational ansatz has been lacking. Here, we establish an ionization potential condition for the removal of a localized electron, by extending the piecewise linearity and Janak's theorems in density functional theory. We also provide numerical evidence supporting our theory. △ Less

Submitted 1 October, 2025; v1 submitted 31 May, 2025; originally announced June 2025.

Resolving Contradictory Estimates of Band Gaps of Bulk PdSe$_2$: A Wannier-Localized Optimally-Tuned Screened Range-Separated Hybrid Density Functional Theory Study

Authors: Fred Florio, María Camarasa-Gómez, Guy Ohad, Doron Naveh, Leeor Kronik, Ashwin Ramasubramaniam

Abstract: Palladium diselenide (PdSe$_2$) -- a layered van der Waals material -- is attracting significant attention for optoelectronics due to the wide tunability of its band gap from the infrared through the visible range as a function of the number of layers. However, there continues to be disagreement over the precise nature and value of the optical band gap of bulk PdSe$_2$, owing to the rather small v… ▽ More Palladium diselenide (PdSe$_2$) -- a layered van der Waals material -- is attracting significant attention for optoelectronics due to the wide tunability of its band gap from the infrared through the visible range as a function of the number of layers. However, there continues to be disagreement over the precise nature and value of the optical band gap of bulk PdSe$_2$, owing to the rather small value of this gap that complicates experimental measurements and their interpretation. Here, we design and employ a Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional to investigate the electronic bandstructures and optical absorption spectra of bulk and monolayer PdSe$_2$. In particular, we account carefully for the finite exciton center-of-mass momentum within a time-dependent WOT-SRSH framework to calculate the \emph{indirect} optical gap and absorption onset accurately. Our results agree well with the best available photoconductivity measurements, as well as with state-of-the-art many-body perturbation theory calculations, confirming that bulk PdSe$_2$ has an optical gap in the mid-infrared (upper-bound of 0.44 eV). More generally, this work further bolsters the utility of the WOT-SRSH approach for predictive modeling of layered semiconductors. △ Less

Submitted 25 January, 2025; originally announced January 2025.

Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional

Authors: Francisca Sagredo, Stephen E. Gant, Guy Ohad, Jonah B. Haber, Marina R. Filip, Leeor Kronik, Jeffrey B. Neaton

Abstract: Halide double perovskites are a chemically-diverse and growing class of compound semiconductors that are promising for optoelectronic applications. However, the prediction of their fundamental gaps and optical properties with density functional theory (DFT) and {\it ab initio} many-body perturbation theory has been a significant challenge. Recently, a nonempirical Wannier-localized optimally-tuned… ▽ More Halide double perovskites are a chemically-diverse and growing class of compound semiconductors that are promising for optoelectronic applications. However, the prediction of their fundamental gaps and optical properties with density functional theory (DFT) and {\it ab initio} many-body perturbation theory has been a significant challenge. Recently, a nonempirical Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has been shown to accurately produce the fundamental band gaps of a wide set of semiconductors and insulators, including lead halide perovskites. Here we apply the WOT-SRSH functional to five halide double perovskites, and compare the results with those obtained from other known functionals and previous $GW$ calculations. We also use the approach as a starting point for $GW$ calculations and we compute the band structures and optical absorption spectrum for Cs\textsubscript{2}Ag{Bi}Br\textsubscript{6}, using both time-dependent DFT and the $GW$-Bethe-Salpeter equation approach. We show that the WOT-SRSH functional leads to accurate fundamental and optical band gaps, as well as optical absorption spectra, consistent with spectroscopic measurements, thereby establishing WOT-SRSH as a viable method for the accurate prediction of optoelectronic properties of halide double perovskites. △ Less

Submitted 7 August, 2024; originally announced August 2024.

Electronic and Optical Excitations in van der Waals Materials from a Non-Empirical Wannier-Localized Optimally-Tuned Screened Range-Separated Hybrid Functional

Authors: María Camarasa-Gómez, Stephen E. Gant, Guy Ohad, Jeffrey B. Neaton, Ashwin Ramasubramanian, Leeor Kronik

Abstract: Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recently proposed Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for various covalent and ionic… ▽ More Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recently proposed Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for various covalent and ionic crystals. However, for vdW materials the tuning of the material- and structure-dependent functional parameters has, until now, only been attained semi-empirically. Here, we present a non-empirical WOT-SRSH approach applicable to vdW materials, with the optimal functional parameters transferable between monolayer and bulk. We apply this methodology to prototypical vdW materials: black phosphorus, molybdenum disulfide, and hexagonal boron nitride (in the latter case including zero-point renormalization). We show that the WOT-SRSH approach consistently achieves accuracy levels comparable to experiments and ab initio many-body perturbation theory (MBPT) calculations for band structures and optical absorption spectra, both on its own and as an optimal starting point for MBPT calculations. △ Less

Submitted 1 May, 2024; originally announced May 2024.

Comments: 11 pages + 4 figures; Supporting Information (15 pages + 2 figures)

Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals

Authors: Guy Ohad, Stephen E. Gant, Dahvyd Wing, Jonah B. Haber, María Camarasa-Gómez, Francisca Sagredo, Marina R. Filip, Jeffrey B. Neaton, Leeor Kronik

Abstract: Using both time-dependent density functional theory (TDDFT) and the ``single-shot" $GW$ plus Bethe-Salpeter equation ($GW$-BSE) approach, we compute optical band gaps and optical absorption spectra from first principles for eight common binary and ternary closed-shell metal oxides (MgO, Al$_2$O$_3$, CaO, TiO$_2$, Cu$_2$O, ZnO, BaSnO$_3$, and BiVO$_4$), based on the non-empirical Wannier-localized… ▽ More Using both time-dependent density functional theory (TDDFT) and the ``single-shot" $GW$ plus Bethe-Salpeter equation ($GW$-BSE) approach, we compute optical band gaps and optical absorption spectra from first principles for eight common binary and ternary closed-shell metal oxides (MgO, Al$_2$O$_3$, CaO, TiO$_2$, Cu$_2$O, ZnO, BaSnO$_3$, and BiVO$_4$), based on the non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional. Overall, we find excellent agreement between our TDDFT and $GW$-BSE results and experiment, with a mean absolute error less than 0.4 eV, including for Cu$_2$O and ZnO, traditionally considered to be challenging for both methods. △ Less

Submitted 5 September, 2023; originally announced September 2023.

An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids

Authors: Stephen E. Gant, Jonah B. Haber, Marina R. Filip, Francisca Sagredo, Dahvyd Wing, Guy Ohad, Leeor Kronik, Jeffrey B. Neaton

Abstract: The dependence of ab initio many-body perturbation theory within the $GW$ approximation on the eigensystem used in calculating quasiparticle corrections limits this method's predictive power. Here, we investigate the accuracy of the recently developed Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional as a generalized Kohn-Sham starting point for single-shot… ▽ More The dependence of ab initio many-body perturbation theory within the $GW$ approximation on the eigensystem used in calculating quasiparticle corrections limits this method's predictive power. Here, we investigate the accuracy of the recently developed Wannier-localized optimally tuned screened range-separated hybrid (WOT-SRSH) functional as a generalized Kohn-Sham starting point for single-shot $GW$ ($G_0W_0$) calculations for a range of semiconductors and insulators. Comparison to calculations based on well-established functionals, namely PBE, PBE0, and HSE, as well as to self-consistent $GW$ schemes and to experiment, shows that band gaps computed via $G_0W_0$@WOT-SRSH have a level of precision and accuracy that is comparable to that of more advanced methods such as quasiparticle self-consistent $GW$ (QS$GW$) and eigenvalue self-consistent $GW$ (ev$GW$). We also find that $G_0W_0$@WOT-SRSH improves the description of states deeper in the valence band manifold. Finally, we show that $G_0W_0$@WOT-SRSH significantly reduces the sensitivity of computed band gaps to ambiguities in the underlying WOT-SRSH tuning procedure. △ Less

Submitted 24 May, 2022; v1 submitted 1 February, 2022; originally announced February 2022.

Journal ref: Phys. Rev. Materials 6, 053802 (2022)

Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional

Authors: Dahvyd Wing, Guy Ohad, Jonah B. Haber, Marina R. Filip, Stephen E. Gant, Jeffrey B. Neaton, Leeor Kronik

Abstract: Accurate prediction of fundamental band gaps of crystalline solid state systems entirely within density functional theory is a long standing challenge. Here, we present a simple and inexpensive method that achieves this by means of non-empirical optimal tuning of the parameters of a screened range-separated hybrid functional. The tuning involves the enforcement of an ansatz that generalizes the io… ▽ More Accurate prediction of fundamental band gaps of crystalline solid state systems entirely within density functional theory is a long standing challenge. Here, we present a simple and inexpensive method that achieves this by means of non-empirical optimal tuning of the parameters of a screened range-separated hybrid functional. The tuning involves the enforcement of an ansatz that generalizes the ionization potential theorem to the removal of an electron in an occupied state described by a localized Wannier function in a modestly sized supercell calculation. The method is benchmarked against experiment for a set of systems ranging from narrow band gap semiconductors to large band gap insulators, spanning a range of fundamental band gaps from 0.2 to 14.2 eV and is found to yield quantitative accuracy across the board, with a mean absolute error of $\sim$0.1 eV and a maximal error of $\sim$0.2 eV. △ Less

Submitted 11 October, 2021; v1 submitted 6 December, 2020; originally announced December 2020.

Comments: 10 pages, 2 figures