arXiv subjects

P. J. Hirschfeld

Publications and source records attributed to P. J. Hirschfeld.

At least 19 recordsLinked to original sources

arXiv2026

Towards the discovery of high critical magnetic field superconductors

Superconducting materials are of significant technological relevance for a broad range of applications, and intense research efforts aim at enhancing the critical temperature $T_{c}$. Intriguingly, while numerous studies have explored different computational and machine-learning routes to predict $T_{c}$, the fundamental role of the critical magnetic field has so far been overlooked. Here we open a new frontier in superconductor discovery by presenting a consistent computational database of critical fields $H_{c}$, $H_{c1}$, and $H_{c2}$ for over 7300 electron-phonon-paired superconductors covering distinct materials classes. A theoretical framework is developed that combines $α^2F(ω)$ spectral functions and highly accurate Fermi surfaces from density functional theory with clean-limit Eliashberg theory to obtain the coherence lengths, London penetration depths, and Ginzburg-Landau parameters. We discover an unexpectedly large number of Type-I superconductors and show that larger unit cells generically support higher critical fields and Type-II behavior. We identify the importance of going beyond BCS theory by including strong-coupling corrections to the superconducting gap and electron-phonon renormalizations of the effective mass for predictions of critical fields across materials. These results provide a framework for foundational AI models that realize the concept of inverse materials design for high-$T_{c}$ and high-critical-field superconductors.

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arXiv2025

Field-angle-resolved heat transport in UTe$_2$: determination of nodal positions in the superconducting order parameter

One of the recurring hurdles in studying unconventional superconductivity is the challenge of efficiently and conclusively identifying the symmetry of the superconducting order parameter in a new material. Uranium ditelluride (UTe$_2$) exhibits an unprecedented number of superconducting phases as a function of pressure and magnetic field, each presumably characterized by a different symmetry of the superconducting gap function. None of these phases has had its symmetry conclusively identified so far. In this article, we report results of an extensive study of the thermal conductivity of UTe$_2$ in its low-field, low-temperature superconducting state as a function of the angle of an applied magnetic field rotated in the $b$-$c$ plane. We observe clear and substantial oscillations in the thermal conductivity as a function of field angle, which naturally suggests the existence of point nodes in the gap. Utilizing the experimentally determined Fermi surface, we are able to model this phenomenon for all the potential gap structures in UTe$_2$ and positively identify the location of these nodes as being along the crystallographic $b$-axis, implying that the superconducting order parameter belongs to the $B_{2u}$ irreducible representation of the crystal point group. The clarity of this result will accelerate the identification of other superconducting phases in UTe$_2$, and guide future studies through the use of high resolution field-angle-dependent measurements.

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arXiv2025

Inhomogeneity, Fluctuations, and Gap Filling in Overdoped Cuprates

Several recent experiments have challenged the premise that cuprate high-temperature superconductors approach conventional Landau-BCS behavior in the high-doping limit. We argue, based on an analysis of their superconducting spectra, that anomalous properties seen in the most-studied overdoped cuprates require a pairing interaction that is strongly inhomogeneous on nm length scales. This is consistent with recent proposals that the "strange-metal" phase above $T_c$ in the same doping range arises from a spatially random interaction. We show, via mean-field Bogoliubov-de Gennes (BdG) calculations and time-dependent Ginzburg-Landau (TDGL) simulations, that key features of the observed tunneling spectra are reproduced when both inhomogeneity and thermal phase fluctuations are accounted for. In accord with experiments, BdG calculations find that low-$T$ spectra are highly inhomogeneous and exhibit a low-energy spectral shoulder and broad coherence peaks. However, the spectral gap in this approach becomes homogeneous at high $T$, in contrast to experiments. This is resolved when thermal fluctuations are included; in this case, global phase coherence is lost at the superconducting $T_c$ via a broadened BKT transition, while robust phase-coherent superconducting islands persist well above $T_c$. The local spectrum remains inhomogeneous at $T_c$, and the gap is found to fill instead of close with increasing temperature.

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arXiv2025

Developing a Complete AI-Accelerated Workflow for Superconductor Discovery

The quest to identify new superconducting materials with enhanced properties is hindered by the prohibitive cost of computing electron-phonon spectral functions, severely limiting the materials space that can be explored. Here, we introduce a Bootstrapped Ensemble of Equivariant Graph Neural Networks (BEE-NET), a machine-learning model trained to predict the Eliashberg spectral function and superconducting critical temperature with a mean-absolute-error of 0.87 K relative to DFT-based Allen-Dynes calculations. Intriguingly, BEE-NET achieves a true-negative-rate of 99.4\%, enabling highly efficient screening for the rare property of superconductivity. Integrated into a multi-stage, AI-accelerated discovery pipeline that incorporates elemental-substitution strategies and machine-learned interatomic potentials, our workflow reduced over 1.3 million candidate structures to 741 dynamically and thermodynamically stable compounds with DFT-confirmed $T_{\mathrm{c}} > 5$ K. We report the successful synthesis and experimental confirmation of superconductivity in two of these previously unreported compounds. This study establishes a data-driven framework that integrates machine learning, quantum calculations, and experiments to systematically accelerate superconductor discovery.

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arXiv2025

Quasiparticle Interference of Spin-Triplet Superconductors: Application to UTe$_2$

Quasiparticle interference (QPI) obtained from scanning tunneling microscopy (STM) is a powerful method to help extract the pairing symmetry of unconventional superconductors. We examine the general properties of QPI on surfaces of spin-triplet superconductors, where the properties of the $\vec d$-vector order parameter and topological surface bound states offer important differences from QPI on spin-singlet superconducting materials. We then apply the theory to a model specific to UTe$_2$, and compare the resulting QPI with recent STM measurements. We conclude that the two candidate Cooper pair instabilities $B_{2u}$ and $B_{3u}$ exhibit distinct features in the QPI intensity to discriminate these using the experimental data. Characteristic features of the emergent topological surface states protected by chiral symmetry in general, and by mirror symmetries in the case of UTe$_2$, provide further unique signatures to help pinpointing the pairing symmetry channel in this material.

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arXiv2025

Electronic reconstruction and interface engineering of emergent spin fluctuations in compressively strained La$_3$Ni$_2$O$_7$ on SrLaAlO$_4$(001)

Motivated by the recent observation of ambient-pressure superconductivity with $T_c \sim 40$ K in La3Ni2O7 on SrLaAlO4(001) (SLAO), we explore the structural and electronic properties as well as the spin-spin correlation function of this bilayer nickelate system by using density functional theory including a Coulomb repulsion term. We find that the compressive strain exerted by this substrate leads to an unconventional occupation of the antibonding Ni $3d_{z^2}$ states around the $Γ$ point, distinct from the superconducting bulk compound under pressure. While pure strain effects rather modestly enhance the dynamical spin susceptibility, investigation of a reconstructed interface composition as observed in transmission electron microscopy uncovers a strong amplification of the spin fluctuations due to Fermi surface nesting of the antibonding Ni $3d_{z^2}$ states near the interface. These results provide insights into the emergence of superconductivity in strained La$_3$Ni$_2$O$_7$, suggest a possible key role of the interface, and highlight fundamental differences from the hydrostatic pressure scenario.

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arXiv2025

Fermi surface reconstruction and enhanced spin fluctuations in strained La$_3$Ni$_2$O$_{7}$ on LaAlO$_3$(001) and SrTiO$_3$(001)

We explore the structural and electronic properties of the bilayer nickelate La3Ni2O7 on LaAlO3(001) and SrTiO3(001) by using density functional theory including a Coulomb repulsion term. For La$_3$Ni$_2$O$_{7}$/LaAlO$_3$(001), we find that compressive strain and electron doping across the interface result in the unconventional occupation of the antibonding Ni $3d_{z^2}$ states. In sharp contrast, no charge transfer is observed for La$_3$Ni$_2$O$_{7}$/SrTiO$_3$(001). Surprisingly, tensile strain drives a metallization of the bonding Ni $3d_{z^2}$ states, rendering a Fermi surface topology akin to superconducting bulk La$_3$Ni$_2$O$_{7}$ under high pressure, yet with spin fluctuations enhanced considerably beyond pressure effects. Concomitantly, significant octahedral rotations are retained. We discuss the fundamental differences between hydrostatic pressure versus epitaxial strain and establish that strain provides a much stronger control over the Ni $e_g$ orbital polarization. The results suggest epitaxial La$_3$Ni$_2$O$_{7}$, particularly under tensile strain, as interesting system to provide novel insights into the physics of bilayer nickelates and possibly induce superconductivity without external pressure.

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arXiv2025

Beyond Homes scaling: disorder, the Planckian bound and a new universality

Beginning with high-$T_c$ cuprate materials, it has been observed that many superconductors exhibit so-called "Homes scaling", in which the zero-temperature superfluid density, $ρ_{s0}$, is proportional to the product of the normal-state dc conductivity and the superconducting transition temperature, $σ_\mathrm{dc} T_c$. For conventional, s-wave superconductors, such scaling has been shown to be a natural consequence of elastic-scattering disorder, not only in the extreme dirty limit but across a broad range of scattering parameters. Here we show that when an analogous calculation is carried out for elastic scattering in d-wave superconductors, a stark contrast emerges, with $ρ_{s0} \propto \left(σ_\mathrm{dc} T_c \right)^2$ in the dirty limit, in apparent violation of Homes scaling. Within a simple approximate Migdal--Eliashberg treatment of inelastic scattering, we show how Homes scaling is recovered. The normal-state behavior of near optimally doped cuprates is dominated by inelastic scattering, but significant deviations from Homes scaling occur for disorder-dominated cuprate systems, such as underdoped YBCO and overdoped LSCO, and in very clean materials with little inelastic scattering, such as Sr$_2$RuO$_4$. We present a revised analysis where both axes of the original Homes scaling plot are normalized by the Drude plasma weight, $ω_{p,D}^2$, and show that new universal scaling emerges, in which the superfluid fractions of dirty s-wave and dirty d-wave superconductors coalesce to a single point at which normal-state scattering is occurring at the Planckian bound. The combined result is a new tool for classifying superconductors in terms of order parameter symmetry, as well as scattering strength and character. Although our model starts from a Fermi-liquid assumption it describes underdoped cuprates surprisingly well.

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arXiv2024

Superconductivity in WBe2

WBe2, which occurs in space group 194, with hexagonal symmetry P63/mmc, is prepared by arc-melting at temperatures above 2200 C, where Be vapor loss is significant. This study is motivated by recent work on MoB2 and WB2, both superconductors (Tc=32 and 17 K respectively) under high (~70 GPa) pressure. In order to avoid the known Be-rich superconducting phases (WBe13 and WBe22) in the complex phase diagram, both known to be superconducting at 4.1 K, the sample was prepared with a slight (~5%) excess of W. The resultant sample, prepared using high purity (99.999%) Be, is essentially single phase WBe2, with some spread in its superconducting properties due to the known homogeneity range. (WBe2 forms in space group 194 between approximately W1.02Be1.98 and W0.88Be2.12.) Characterization was carried out with x-ray diffraction, electrical resistivity, rho, in zero and applied magnetic fields, and specific heat. The resistivity in zero and applied fields and specific heat data indicate that our sample of WBe2 is a bulk superconductor at ambient pressure with a Tc(onset) in the resistivity at 1.05 K, and Tc(rho->0) at ~0.86 K. There is no signature of superconductivity in rho at 4.1 K, indicating successful avoidance of WBe13 and WBe22. The resistivity data in field indicate an upper critical field of approximately 400 gauss.

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arXiv2024

Optical properties and electronic correlations in La$_3$Ni$_2$O$_7$ bilayer nickelates under high pressure

We explore the optical properties of La3Ni2O7 bilayer nickelates by using density functional theory including a Coulomb repulsion term. Convincing agreement with recent experimental ambient-pressure spectra is achieved for U=3eV, which permits tracing the microscopic origin of the characteristic features. Simultaneous consistency with angle-resolved photoemission spectroscopy and x-ray diffraction suggests the notion of rather moderate electronic correlations in this novel high-Tc superconductor. Oxygen vacancies form predominantly at the inner apical sites and renormalize the optical spectrum quantitatively, while the released electrons are largely accommodated by a defect state. We show that the structural transition occurring under high pressure coincides with a significant enhancement of the Drude weight and a reduction of the out-of-plane interband contribution that act as a fingerprint of the emerging hole pocket. We further calculate the optical spectra for various possible magnetic phases including spin-density waves and discuss the results in the context of experiment. Finally, we investigate the role of the 2-2 versus 1-3 layer stacking and compare the bilayer nickelate to La4Ni3O10, La3Ni2O6, and NdNiO2, unveiling general trends in the optical spectrum as a function of the formal Ni valence in Ruddlesden-Popper versus reduced Ruddlesden-Popper nickelates.

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arXiv2024

Superconductivity in pressurized Re$_{0.10}$Mo$_{0.90}$B$_2$

The recent surprising discovery of superconductivity with critical temperature $T_c$ = 32 K in MoB$_2$ above 70 GPa has led to the search for related materials that may superconduct at similarly high $T_c$ values and lower pressures. We have studied the superconducting and structural properties of Re$_{0.10}$Mo$_{0.90}$B$_2$ to 170 GPa. A structural phase transition from R3m to P6/mmm commences at 48 GPa, with the first signatures of superconductivity appearing above 44 GPa. The critical temperature is observed to increase with pressure. A complete resistive transition is observed only above 150 GPa, where the highest onset $T_c$ of 30 K is also achieved. Upon releasing pressure, the high pressure superconducting phase is found to be metastable. During unloading, a complete resistive superconducting transition is observed all the way down to 20 GPa (with onset $T_c \sim 20$ K). Our results suggest that the P6/mmm structure is responsible for the observed superconductivity.

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arXiv2024

Effect of low-temperature compression on superconductivity and crystal structure in strontium metal

The superconducting and structural properties of elemental strontium metal were investigated under pressures up to 60 GPa while maintaining cryogenic conditions during pressure application. Applying pressure at low temperatures reveals differences in superconducting and structural phases compared to previous reports obtained at room temperatures. Notably, the superconducting critical temperature exhibits a twofold increase under compression after cryogenic cooling within the pressure range of 35-42 GPa, compared to cryogenic cooling after room-temperature compression. Subsequently, the transition width becomes significantly sharper above 42 GPa. Low-temperature X-ray diffraction measurements under pressure reveal that this change corresponds to the Sr-III to Sr-IV transition, with no evidence of any metastable structure. Furthermore, the monoclinic Sr-IV structure was observed to remain stable to much higher pressures - at least up to 60 GPa, without the appearance of the incommensurate Sr-V phase present at room temperature. This implies that thermal activation energy plays an important role in overcoming the presence of a kinetic barrier to the Sr-V phase at room temperature.

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arXiv2024

Theory of Josephson scanning microscopy with $s$-wave tip on unconventional superconducting surface: application to Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$

Josephson scanning tunneling microscopy (JSTM) is a powerful probe of the local superconducting order parameter, but studies have been largely limited to cases where superconducting sample and superconducting tip both have the same gap symmetry -- either s-wave or d-wave. It has been generally assumed that in an ideal $s$-to-$d$ JSTM experiment the critical current would vanish everywhere, as expected for ideal $c$-axis planar junctions. We show here that this is not the case. Employing first-principles Wannier functions for Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$, we develop a scheme to compute Josephson critical current ($I_{c}$) and quasiparticle tunneling current measured by JSTM with sub-angstrom resolution. We demonstrate that the critical current for tunneling between an s-wave tip and a superconducting cuprate sample has largest magnitude above O sites and it vanishes above Cu sites. $I_{c}$ changes sign under $π/2$-rotation and its average over a unit cell vanishes, as a direct consequence of the $d$-wave gap symmetry in cuprates. Further, we show that $I_{c}$ is strongly suppressed in the close vicinity of a Zn-like impurity owing to suppression of the superconducting order parameter. More interestingly, $I_{c}$ acquires non-vanishing values above the Cu sites near the impurity. The critical current modulations produced by the impurity occur at characteristic wavevectors distinct from the quasiparticle interference (QPI) analogue. Furthermore, the quasiparticle tunneling spectra in the JSTM set-up shows coherence peaks and impurity-induced resonances shifted by the $s$-wave tip gap. We discuss similarities and differences in JSTM observables and conventional STM observables, making specific predictions that can be tested in future JSTM experiments.

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arXiv2024

Thermal conductivity of nonunitary triplet superconductors: application to UTe$_2$

There is considerable evidence that the heavy fermion material UTe$_2$ is a spin-triplet superconductor, possibly manifesting time-reversal symmetry breaking, as measured by Kerr effect and muon spin resonance experiments below the critical temperature, in some samples. Such signals can arise due to a chiral orbital state, or possible nonunitary pairing. Although experiments at low $T$ appear to be consistent with point nodes in the spectral gap, the detailed form of the order parameter and even the nodal positions are not yet determined. Thermal conductivity measurements can extend to quite low temperatures, with varying heat current direction can therefore provide information on the order parameter structure. Here we derive a general expression for the thermal conductivity of a spin triplet superconductor, and use it to compare the low-temperature behavior of various states proposed for UTe$_2$.

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arXiv2024

Why Scanning Tunneling Microscopy on Sr$_2$RuO$_4$ sometimes doesn't see the superconducting gap

Scanning tunneling microscopy (STM) is perhaps the most promising way to detect the superconducting gap size and structure in the canonical unconventional superconductor Sr$_2$RuO$_4$ directly. However, in many cases, researchers have reported being unable to detect the gap at all in simple STM conductance measurements. Recently, an investigation of this issue on various local topographic structures on a Sr-terminated surface found that superconducting spectra appeared only in the region of small nanoscale canyons, corresponding to the removal of one RuO surface layer. Here, we analyze the electronic structure of various possible surface structures using first principles methods, and argue that bulk conditions favorable for superconductivity can be achieved when removal of the RuO layer suppresses the RuO$_4$ octahedral rotation locally. We further propose alternative terminations to the most frequently reported Sr termination where superconductivity surfaces should be observed.

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arXiv2024

Spontaneous time-reversal symmetry breaking by disorder in superconductors

A growing number of superconducting materials display evidence for spontaneous time-reversal symmetry breaking (TRSB) below their critical transition temperatures. Precisely what this implies for the nature of the superconducting ground state of such materials, however, is often not straightforward to infer. We review the experimental status and survey different theoretical mechanisms for the generation of TRSB in superconductors. In cases where a TRSB complex combination of two superconducting order parameter components is realized, defects, dislocations and sample edges may generate superflow patterns that can be picked up by magnetic probes. However, even single-component condensates that do not break time-reversal symmetry in their pure bulk phases can also support signatures of magnetism inside the superconducting state. This includes, for example, the generation of localized orbital current patterns or spin-polarization near atomic-scale impurities, twin boundaries and other defects. Signals of TRSB may also arise from a superconductivity-enhanced Ruderman-Kittel-Kasuya-Yosida exchange coupling between magnetic impurity moments present in the normal state. We discuss the relevance of these different mechanisms for TRSB in light of recent experiments on superconducting materials of current interest.

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arXiv2024

Spin fluctuations in the ultranodal superconducting state of Fe(Se,S)

The iron-based superconductor FeSe isovalently substituted with S displays an abundance of remarkable phenomena that have not been fully understood, at the center of which are apparent zero-energy excitations in the superconducting state in the tetragonal phase. The phenomenology has been generally consistent with the proposal of the so-called ultranodal states where Bogoliubov Fermi surfaces are present. Recently, nuclear magnetic resonance measurements have seen unusually large upturns in the relaxation rate as temperature decreases to nearly zero in these systems, calling for theoretical investigations. In this paper, we calculate the spin susceptibility of an ultranodal superconductor including correlation effects within the random phase approximation. Although the non-interacting mean-field calculation rarely gives an upturn in the low temperature relaxation rate within our model, we found that correlation strongly enhances scattering between coherent parts of the Bogoliubov Fermi surface, resulting in robust upturns when the interaction is strong. Our results suggest that in addition to the presence of Bogoliubov Fermi surfaces, correlation and multiband physics also play important roles in the system's low energy excitations.

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arXiv2024

Structural transitions, octahedral rotations, and electronic properties of $A_3$Ni$_2$O$_7$ rare-earth nickelates under high pressure

Motivated by the recent observation of superconductivity with $T_c \sim 80$ K in pressurized La3Ni2O7 [Nature 621, 493 (2023)], we explore the structural and electronic properties in A3Ni2O7 bilayer nickelates (A=La-Lu, Y, Sc) as a function of hydrostatic pressure (0-150 GPa) from first principles including a Coulomb repulsion term. At $\sim 20$ GPa, we observe an orthorhombic-to-tetragonal transition in La$_3$Ni$_2$O$_7$ at variance with recent x-ray diffraction data, which points to so-far unresolved complexities at the onset of superconductivity, e.g., charge doping by variations in the oxygen stoichiometry. We compile a structural phase diagram with particular emphasis on the $b/a$ ratio, octahedral anisotropy, and octahedral rotations. Intriguingly, chemical and external pressure emerge as two distinct and counteracting control parameters. We find unexpected correlations between $T_c$ and the in-plane Ni-O-Ni bond angles for La$_3$Ni$_2$O$_7$. Moreover, two novel structural phases with significant $c^+$ octahedral rotations and in-plane bond disproportionations are uncovered for A=Nd-Lu, Y, Sc that exhibit a surprising pressure-driven electronic reconstruction in the Ni $e_g$ manifold. By disentangling the involvement of basal versus apical oxygen states at the Fermi surface, we identify Tb$_3$Ni$_2$O$_7$ as an interesting candidate for superconductivity at ambient pressure. These results suggest a profound tunability of the structural and electronic phases in this novel materials class and are key for a fundamental understanding of the superconductivity mechanism.

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