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Stephen D. Wilson

Publications and source records attributed to Stephen D. Wilson.

At least 19 recordsLinked to original sources

Out-of-equilibrium relaxation dynamics of the superconducting order parameter in CsV$_3$Sb$_5$

The application of a time-varying strain field drives a superconducting order parameter out of equilibrium. How the order parameter relaxes back to equilibrium depends both on the structure of the superconducting gap and on the nature of quasiparticle scattering. We report the discovery of an ultrasonic attenuation peak inside the superconducting state of the kagome superconductor CsV$_3$Sb$_5$. This peak is the natural consequence of the order parameter relaxation time matching the ultrasonic drive frequency near $T_{\rm c}$. From the measured frequency dependence of the peak, we extract a microscopic scattering time of $\tau_N = 25$ ps. This timescale is two orders of magnitude longer than the elastic scattering time as determined by resistivity measurements, but is comparable to the inelastic scattering time determined by thermal transport. Within the conventional framework of order-parameter relaxation, this implies that elastic scattering is ineffective at relaxing the superconducting condensate, consistent with a sign-preserving $s$-wave state obeying Anderson's theorem.

cond-mat.supr-con

Effective Ionic Valence and Local Magnetic Moment in Kagome Superconductors

In order to understand the unexpected similarity and the correlated behavior in kagome superconductor families AV$_3$Sb$_5$ (A = K, Rb, Cs) and ATi$_3$Bi$_5$ (A = Rb, Cs), we investigate the Hartree-scale local electronic structure of these systems. Our result indicates that V and Ti ions are both of 2+ valence such that the corresponding itinerant carrier densities are similar, and the difference in electron count is instead reflected in their quantum fluctuating ionic magnetic moments. However, due to the frustrated lattice geometry of these materials, such local moments are difficult to experimentally observe via standard probes. For verification, we systematically introduce nonmagnetic Sn impurities to locally relieve the geometric frustration and experimentally demonstrate the existence of well-defined local magnetic moments via magnetic susceptibility and muon spin rotation or relaxation ($\mu$SR) measurements. All experiments discover a systematic increase of magnetic susceptibility upon increasing nonmagnetic impurity level. Our discovered ionic moments suggest a paradigm shift from the existing itinerant carrier-only picture to one incorporating strong correlation from local ionic spins. The associated interatomic and local-itinerant correlations offer a solid ground for the emergence of the observed rich correlated behavior in this new family of superconducting materials.

cond-mat.str-el

Competing lattice structures induced by Sn substitution in CsV$_3$Sb$_5$

Understanding the effect of chemical substitution on competing phases of kagome metals is crucial for disentangling the interplay between local structural distortions and electronic instabilities. In \cvs, Sn substitution strongly modifies the electronic phase diagram, yet the microscopic mechanism driving this remains unclear. Here, we combine $^{121}$Sb nuclear quadrupole resonance (NQR) measurements and density functional theory calculations to investigate the atomic-scale effects of Sn substitution in CsV$_3$Sb$_{5-x}$Sn$_x$. At low Sn concentrations, the observed satellite NQR peaks exhibit signatures of local structural distortion induced by Sn substitution, qualitatively consistent with our computational analysis. These impurity-induced features persist across the entire experimentally investigated doping range, up to $x$ = 0.65, and remain observable up to room temperature. For $x=1$, the fully doped idealized case, the estimated dynamical instabilities of the kagome lattice suggest the stabilization of two nearly energy-degenerate equilibrium structures characterized by V-trimers, distinguished by a zero- or $\pi$-phase shift between adjacent layers along the $c$-axis. Together, these results show that Sn substitution drives a complex interplay between local impurity-induced distortions and competing structural instabilities in vanadium-based kagome compounds.

cond-mat.str-el

Evolving charge order in the CDW state of AV$_3$Sb$_5$ metals

AV$_3$Sb$_5$ kagome metals are characterized by intertwined electronic and structural orders, which motivated extensive studies in recent years. Yet the details of the electronic state preceding the superconducting phase remain poorly understood. Here we extend our previous investigation [Phys. Rev. Research 7, L032046 (2025)] of RbV$_3$Sb$_5$ using avoided level crossing (ALC) muon-spin spectroscopy to the $A$ = Cs and K systems. Consistent with our previous study, we identify a second transition whose origin cannot be attributed solely to an internal magnetic field, indicating the involvement of an additional electronic mechanism that subtly modifies the charge distribution within the V plane. In particular, the ALC results point towards an additional charge modulation taking place within the charge density wave (CDW) phase and occurring at $T^{*}<T_{CDW}$ for $A$ = Cs and Rb, or in the vicinity of $T_{CDW}$ for $A$ = K.

cond-mat.str-el

Direct Evidence of Unconventional Superconductivity in Doped Kagome system RV$_3$Sb$_5$

The superconducting pairing symmetry of kagome metals remains a central unresolved question largely because phase-sensitive experiments capable of distinguishing between different possible order parameters have been difficult to implement. The spatial and energetic characteristics of impurity bound states measured by spectroscopic-imaging scanning tunneling microscopy encode information on the superconducting order parameter. Here, we use impurity-bound state spectroscopy to investigate optimally doped RbV$_3$Sb$_{5}$ where the charge-density wave instability is fully suppressed. We find that the superconducting state is fully gapped and exhibits two distinct energy scales, consistent with a multiband order parameter. Atomic-scale spectroscopy around nonmagnetic defects reveals pronounced particle-hole asymmetric bound states. Comparison with theoretical calculations demonstrates that these bound states are incompatible with conventional $s$-wave and sign-changing $s^{\pm}$ pairing. Our calculations also show that the data are fully consistent with a chiral order parameter. Our results establish impurity-bound-state spectroscopy as a powerful phase-sensitive probe of superconductivity in kagome materials and provide strong evidence that optimally doped RbV$_3$Sb$_{5}$ realizes a fully gapped chiral superconducting state.

cond-mat.supr-con

Near itinerancy and slow singlet formation in the triangular lattice NaRuO2

NaRuO$_2$ forms a delafossite-like structure that contains triangular sublattices of edge-sharing RuO$_6$ octahedra. It shows no evidence of magnetic order down to 100 mK and persistent spin fluctuations, suggestive of a quantum disordered magnetic ground state. In order to characterize the physical regime from which this disordered state arises, we use resonant inelastic X-ray scattering (RIXS) and X-ray absorption spectroscopy (XAS) at the Ru-$L_{2,3}$-edge, along with pulsed high-field magnetization to characterize both the local electronic structure and the magnetic interactions. Despite significant spin-orbit coupling inferred from XAS measurements, a spin-orbit exciton, characteristic of a spin-orbit assisted Mott insulator, was not observed with RIXS due to the presence of damped intraorbital excitations, which are characteristic of a metal. Corroborated by models of the high-field magnetization to a random singlet model, we propose a picture of a nearly itinerant system with strong magnetic and charge fluctuations that destabilize long-range magnetic order.

cond-mat.str-el

Odd-parity electronic order near the semiconductor limit

Identifying materials platforms in which dilute carriers experience strong Coulomb interactions is a central challenge in the search for interaction-driven quantum phases. In such systems, weak carrier screening can promote a variety of collective instabilities beyond the conventional Fermi liquid paradigm, including superconductivity, Wigner crystallization, and odd-parity electronic order. Experimental realizations of such dilute, strongly interacting electronic systems remain rare in crystalline materials. Here we report a spontaneous odd-parity phase transition in the phosphide semiconductor family $\textit{Ln}$Cd$_3$P$_3$ ($\textit{Ln}$ = La, Ce, Pr, Nd). Using optical second harmonic generation, we observe the onset of bulk inversion and rotational symmetry breaking accompanied by the emergence of an in-plane polar axis. Second harmonic microscopy reveals three domain variants related by 120$^\circ$ rotations, while ultrafast transient reflectivity measurements uncover a pronounced electronic reconstruction across the transition. Remarkably, the ordered phase appears only in lightly self-hole-doped compounds and is absent in insulating SmCd$_3$P$_3$, indicating an essential role for itinerant carriers despite their extremely low concentration. Guided by density functional theory, we develop a four-band model of the valence states and show that modest interactions can stabilize odd-parity electronic order. The resulting phase combines a spontaneous Fermi surface distortion with a momentum-dependent bilayer polarization that breaks inversion symmetry. Our results establish a route to interaction-driven parity breaking in dilute-carrier semiconductors and identify honeycomb bilayer systems as a promising platform for odd-parity electronic phases.

cond-mat.str-el

Direct Observation of Channelised Supercurrents in a Kagome Superconductor

Superconductors are many-body quantum states in which current flows without dissipation. Theory predicts that supercurrents follow a relatively simple spatial pattern in both conventional and unconventional superconductors. Recent studies into the AV3Sb5 (A = Cs, K, Rb) family of Kagome superconductors indicate that CsV3Sb5 has unconventional transport properties that cannot be accounted for with these simple theories, including reports of intrinsic Josephson junctions, higher order Cooper pairing and the zero field diode effect. Attempts to interpret these findings have focused on the interplay of superconductivity with the unconventional charge density wave (CDW) order in these materials, with which superconductivity competes. A current roadblock to understanding how these kagome superconductors give rise to their intriguing properties is the lack of spatially resolved information about transport. Here we show, using a recently developed superconducting quantum interference device (SQUID) microscope, that flakes of CsV3Sb5-xSnx host a network of narrow supercurrent channels. These supercurrent channels emerge at the critical temperature and remain stable for all temperatures and currents. Their non-linear behaviour is consistent with a network of Josephson junctions linked by narrow supercurrent filaments, which naturally leads to the observed transport anomalies. Intriguingly, these observations are much weaker in undoped samples, which suggests links to the physics of charge density waves, disorder, and electronic correlations, all of which are greatly influenced by the doping strength. These results establish new frontiers for the local investigation of charge transport and competing orders in strongly correlated electron systems, and shine a new light on the anomalous transport properties of the AV3Sb5 kagome superconductors.

cond-mat.supr-con

Distinct lattice and charge excitations in AV3Sb5 kagome superconductors

The kagome superconductor family AV3Sb5 (A=Cs, Rb, K) provides a rich platform for exploring diverse electronic symmetry breaking phenomena, including superconductivity and various forms of density wave orders. Although these compounds share the identical lattice structure in the normal state, they exhibit distinct forms of symmetry breaking upon entering the charge density wave (CDW) phase, and the microscopic origin of which remain elusive. Here, we investigate the lattice and charge degrees of freedom in AV3Sb5 using angle-resolved polarized Raman spectroscopy. Our comprehensive polarization-resolved measurements reveal that the lifting of the twofold-degeneracy of the E2g phonon mode in the CDW phase-previously reported only in CsV3Sb5 with a 3 GHz splitting-also appears ubiquitously in the other two compounds. In contrast, the collective CDW excitations exhibit markedly different polarization dependences depending on the alkali-metal species. These distinct behaviors in the lattice and charge channels provide crucial insight into the enigmatic material-dependent symmetry breaking phenomena that appear in the CDW phase. Furthermore, our experiments, together with first-principles calculations and an effective Hamiltonian model, shed light on the nature of the charge order structure in AV3Sb5 kagome superconductors.

cond-mat.str-el

Magnetic Polarons Enable Exceptional Magnetocaloric Response

Magnetocaloric materials are typically limited by a trade-off between magnetic entropy and field responsiveness. Here we show that magnetic polarons provide an intermediate regime that mitigates this constraint and enables an exceptional magnetocaloric response. Using EuB$_6$ as a model system, we combine thermodynamic and magnetic measurements to demonstrate that nanoscale ferromagnetic clusters emerging near the Curie temperature strongly enhance the field-induced entropy collapse. These clusters possess large effective moments that respond efficiently to applied fields while retaining substantial entropy due to their small size and dynamic fluctuations. As a result, EuB$_6$ exhibits a giant cryogenic magnetocaloric response, with both large isothermal entropy change and adiabatic temperature change in the technologically important 10-40 K range. Our results identify magnetic polarons as an underexplored route for optimizing magnetocaloric performance and establish an intermediate magnetic length scale as a design principle for high-performance cryogenic cooling materials.

cond-mat.mtrl-sci

Discovery of an odd-parity f-wave charge order in a kagome metal

The spontaneous breaking of symmetries is a cornerstone of physics, defining the phases of matter from the cosmological scale to the quantum realm. In condensed matter, electronic orders are classified by their behavior under fundamental symmetries like spatial inversion (parity). While even-parity orders, such as conventional superconductivity and charge density waves, are ubiquitous, their odd-parity counterparts--predicted to host exotic phenomena such as gapless quasiparticle excitations and novel collective modes--are comparatively elusive states of quantum matter. Here, using high-resolution scanning tunneling microscopy and angle-resolved photoemission spectroscopy on the kagome metal CsV$_3$Sb$_5$, we report the discovery of an inversion symmetry-breaking $f$-wave charge bond order. We show that this phase, which preserves translation symmetry, is stabilized by the spontaneous opening of a spectral gap at a previously overlooked Dirac point, providing a textbook condensed-matter realization of the Gross-Neveu model for dynamical mass generation and parity breaking. Intriguingly, this $f$-wave order is itself a intervening phase, vanishing abruptly below a temperature of 10\,K and pointing to a subsequent transition into a `hidden' electronic state that is invisible to local STM probes. Our findings establish odd-parity charge order as a novel phase of matter, here, embedded within the intricate hierarchy of correlated electronic orders on the kagome lattice.

cond-mat.str-el

Collinear spin density wave state in distorted square-lattice GdNiSn$_4$

We characterize the magnetic ground state of the newly synthesized lanthanide intermetallic GdNiSn$_4$ via resonant elastic x-ray scattering measurements. This compound forms distorted square nets of Gd that initially order magnetically below 23 K followed by a lower temperature transition at 16 K. Our scattering data identify the ground state order as a single-$q$ incommensurate, collinear order that slides towards a commensurate wave vector above the 16 K transition. Magnetic symmetry analysis combined with azimuthal dependence resolves the ground state magnetic structure as a moment-modulated spin density wave state with Gd moments oriented parallel to the in-plane a-axis. We discuss connections between the observed magnetic order and electronic properties in this square-net compound.

cond-mat.str-el

New Crystal Structures Hide in Plain Sight: A Stress Test for AI-Guided Materials Discovery

New types of crystal structures are discovered only rarely, and the artificial intelligence (AI) models now reshaping materials discovery have so far produced new chemical compositions within known structural families rather than genuinely new structures. We report GdNiSn4 and LuNiSn4, intermetallics that adopt a previously unreported structure type, found not by computation but by exploratory synthesis. Single-crystal diffraction shows that the structure is an intergrowth of two known structural units. We then use this system as a benchmark for two leading generative models, MatterGen and DiffCSP++. For DiffCSP++, the benchmark is performed in its crystallographically constrained setting, using the required space-group and Wyckoff-position inputs. Under our sampling budget, neither model recovers the experimentally reported monoclinic structure within the structural-matching tolerance. The generated structures are evaluated without further structural relaxation using the nonmagnetic analog LuNiSn4, where we rule out 4f magnetism as the cause. Because the new structure is built from familiar building blocks, it should be derivable. We argue that encoding chemical reasoning, such as the stacking of known motifs, is a concrete path toward AI that can discover structurally novel materials.

cond-mat.mtrl-sci

Raman scattering spectroscopic observation of a ferroelastic crossover in bond-frustrated PrCd$_3$P$_3$

2D magnetism in triangular lattices has already shown potential for hosting exotic magnetic states. Control of these magnetic states, both in terms of magnetic properties and in terms of charge doping would be the next step. This makes materials which combine triangular lattice magnetic layers with layers hosting interesting structural or electronic properties particularly useful. PrCd$_3$P$_3$, studied in this work, is one of a family of materials where triangular lattice layers of magnetic rare earth ions alternate with semiconducting hexagonal CdP layers. Using Raman scattering spectroscopy we uncover a structural instability in the CdP layers, associated with a soft mode behavior of a phonon in these layers. Raman scattering detects crystal electric field excitations, and confirms a singlet ground state for Pr$^{3+}$ and splitting of the doublet levels as a result of the structural instability in CdP layers. While Pr$^{3+}$ is non-magnetic in PrCd$_3$P$_3$ we speculate that this family of materials can realize control of the magnetic layer through the CdP layer which can become ferroelectric under strain that would relieve frustration.

cond-mat.mtrl-sci

Electron-electron and electron-phonon collision cross sections in CsV3Sb5

AV3Sb5 (A=K, Rb, Cs) are kagome metals and superconductors, attracting much recent attention as nexus of multiple quantum states. Here, through a systematic study of electric and thermal transport of CsV3Sb5, we identify it as a metallic Fermi liquid with moderate electronic correlations ans strong electron-phonon (e-ph) collision cross section. We observe contributions to the inelastic electrical resistivity, each dominating within a distinct temperature window. The prefactor of the T2 is consistent with the Kadowaki-Woods scaling for a Fermi liquid with moderate correlation. By performing thermal conductivity measurements at zero and finite magnetic field, we separate the electronic and the lattice contributions to the thermal conductivity. The Wiedemann-Franz law is satisfied in the zero-temperature limit, while a downward deviation emerges at finite temperature due to the mismatch between the prefactors of the electrical and thermal quadratic resistivities, as reported in other metals. The Bloch-Gr\"uneisen description of electron-phonon scattering successfully accounts for both electronic thermal and electrical transport, indicating a remarkably large e-ph collision cross section in CsV3Sb5.

cond-mat.str-el

Observation of Room-temperature Charge Density Wave Correlations via Coherent Phonon Spectroscopy in Sn-doped Kagome Superconductor CsV$_3$Sb$_5$

In this work, we perform ultrafast time-resolved reflectivity measurements to track the evolution of charge density wave (CDW) correlations in Sn-doped Kagome superconductor CsV$_3$Sb$_{5-x}$Sn$_x$. By extracting the coherent phonon spectrum, we evidence robust signatures of CDW correlations at temperature and doping ranges far beyond the phase boundary of long-range CDW order. Remarkably, we unveil short-range CDW correlations survive up to room temperature in $x = 0.32$ Sn-doped CsV$_3$Sb$_5$, supported by synchrotron X-ray diffraction measurements. We point out the introduction of quenched disorder by Sn doping can pin the CDW and form static short-range CDW, which can explain the observed persistent CDW signatures. Our results thus corroborate the ubiquity and robustness of CDW correlations in Sn-doped CsV$_3$Sb$_5$ and provide new insights on the role of disorders on the CDW correlations in AV$_3$Sb$_5$ family.

cond-mat.str-el

Common sublattice-pure van Hove singularities in the kagome superconductors $\textit{A}$V$_{3}$Sb$_{5}$ ($\textit{A}$ = K, Rb, Cs)

Kagome materials offer a versatile platform for exploring correlated and topological quantum states, where van Hove singularities (VHSs) play a pivotal role in driving electronic instabilities, exhibiting distinct behaviors depending on electron filling and interaction settings. In the recently discovered kagome superconductors $\textit{A}$V$_{3}$Sb$_{5}$ ($\textit{A}$ = K, Rb, Cs), unconventional charge density wave order, superconductivity, and electronic chirality emerge, yet the nature of VHSs near the Fermi level ($\textit{E}$$_{F}$) and their connection to these exotic orders remain elusive. Here, using high-resolution polarization-dependent angle-resolved photoemission spectroscopy, we uncover a universal electronic structure across $\textit{A}$V$_{3}$Sb$_{5}$ that is distinct from density-functional theory predictions that show noticeable discrepancies. We identify multiple common sublattice-pure VHSs near $\textit{E}$$_{F}$, arising from strong V-$\textit{d}$/Sb-$\textit{p}$ hybridization, which significantly promote bond-order fluctuations and likely drive the observed charge density wave order. These findings provide direct spectroscopic evidence for hybridization-driven VHS formation in kagome metals and establish a unified framework for understanding the intertwined electronic instabilities in $\textit{A}$V$_{3}$Sb$_{5}$.

cond-mat.supr-con

Interplay between charge correlations and superconductivity across the superconducting domes of CsV$_{3}$Sb$_{5-x}$Sn$_x$

The kagome metal CsV$_3$Sb$_5$ shows an unconventional interplay between charge density wave (CDW) order and superconductivity. Tuning the band filling is known to rapidly suppress long-range CDW order and drive the formation of two superconducting ``domes" upon increasing hole concentration. Here we determine the detailed evolution of charge correlations across this phase diagram and resolve their interplay with the superconducting state. Upon light hole-doping, the suppression of a metastable $2\times 2\times 4$ CDW state coincides with the suppression of superconducting fluctuations present in the parent CsV$_3$Sb$_5$ compound. Continued doping suppresses long-range $2\times 2\times 2$ CDW order, leaving remnant short-range, quasi-1D correlations that persist across the second superconducting dome. These higher temperature charge correlations are seemingly essential to the lower temperature superconducting state, as charge correlations vanish coincident with superconductivity as a function of hole-doping. A multidomain model of short-range V-V dimer formation within the kagome plane is proposed in the second superconducting dome, where rotational and translational symmetry remain locally broken even in the absence of long-range CDW order.

cond-mat.supr-con