arXiv subjects

Jacob P. C. Ruff

Publications and source records attributed to Jacob P. C. Ruff.

At least 19 recordsLinked to original sources

arXiv2026

Room-temperature multistage metastability in a moiré superstructure

Metastability is fundamental not only to phase ordering and transitions, but also to a broad range of modern technologies, from memory devices to metallic glasses. In condensed-matter physics, charge density waves (CDWs) offer versatile platforms for accessing metastable states due to their sensitivity to external stimuli. However, most metastable CDW states are stabilized only at low temperatures, limiting their practical utility. In this study, we report the observation of electrically driven, room-temperature, nonvolatile metastable states in the bulk form of EuTe$_4$, a recently discovered compound that hosts an innate moiré superlattice characterized by the stacking of incommensurate monolayer and bilayer CDWs. Systematic transport measurements reveal discrete resistivity plateaus and strong electric-field sensitivity, with a large number of metastable states readily induced across a wide temperature window within a giant hysteresis loop, making them well-suited for high-temperature, multi-bit memory applications. By integrating photoemission spectroscopy, diffraction, and in-situ transport measurements, we uncover that these metastable states do not stem from conventional mechanisms such as the emergence of new ordered phases or changes in incommensurate periodicity. Instead, they are characterized by a suppression of the original CDW amplitude and a reduction in correlation length, pointing to a unique electric-field-induced switching of out-of-plane CDW phases in the moiré superstructure. Our findings not only provide critical insights into metastable phenomena in moiré systems with stacked electronic orders but also establish EuTe$_4$ as a promising platform for developing room-temperature, multi-bit memory devices.

cond-mat.str-el↗

arXiv2025

Bidirectional ultrafast control of charge density waves via phase competition

The intricate competition between coexisting charge density waves (CDWs) can lead to rich phenomena, offering unique opportunities for phase manipulation through electromagnetic stimuli. Leveraging time-resolved X-ray diffraction, we demonstrate ultrafast control of a CDW in EuTe$_4$ upon optical excitation. At low excitation intensities, the amplitude of one of the coexisting CDW orders increases at the expense of the competing CDW, whereas at high intensities, it exhibits a nonmonotonic temporal evolution characterized by both enhancement and reduction. This transient bidirectional controllability, tunable by adjusting photo-excitation intensity, arises from the interplay between optical quenching and phase-competition-induced enhancement. Our findings, supported by phenomenological time-dependent Ginzburg-Landau theory simulations, not only clarify the relationship between the two CDWs in EuTe$_4$, but also highlight the versatility of optical control over order parameters enabled by phase competition.

cond-mat.str-el↗

arXiv2025

Dynamics of a jointly commensurate moir\'e charge density wave

The advent of two-dimensional moir\'e systems has revolutionized the exploration of phenomena arising from strong correlations and nontrivial band topology. Recently, a moir\'e superstructure formed by two coexisting charge density waves (CDWs) with slightly mismatched wavevectors has been realized. These incommensurate CDWs can collectively exhibit commensurability, resulting in the jointly commensurate CDW (JC-CDW) and establishing a new paradigm for controlling moir\'e potential and periodicity. Achieving such functionality, however, hinges on a key open question: how do the amplitude, phase coherence, and periodicity of this order respond to external perturbations? Here, we address this question using a suite of time- and momentum-resolved diffraction and spectroscopic techniques to probe light-induced CDW dynamics in EuTe$_4$. Our time-resolved diffraction measurements distinguish the instantaneous quenching of the JC-CDW amplitude, as verified by time-resolved photoemission spectroscopy, from the much slower evolution of phase fluctuations. Furthermore, while the JC-CDW wavevector remains locked along the CDW direction upon photoexcitation, indicating a preserved moir\'e periodicity, the correlation length of JC-CDW shows an exclusive reduction perpendicular to its wavevector, unveiling the formation of previously unexplored shear-type defects. Together, this multimodal methodology reconstructs the spatiotemporal evolution of the JC-CDW upon excitation. These findings not only highlight the remarkable robustness of JC-CDWs out of equilibrium, but also provide insight into optical manipulation and engineering of moir\'e quantum materials through defect control.

cond-mat.str-el↗

arXiv2025

Strong long-wavelength electron-phonon coupling in Ta$_2$Ni(Se,S)$_5$

The search for intrinsic excitonic insulators (EI) has long been confounded by coexisting electron-phonon coupling in bulk materials. Although the ground state of an EI may be difficult to differentiate from density-wave orders or other structural instabilities, excited states offer distinctive signatures. One way to provide clarity is to directly inspect the phonon spectral function for long wavelength broadening due to phonon interaction with the high velocity EI phason. Here, we report that the quasi-one-dimensional (quasi-1D) EI candidate Ta$_2$NiSe$_5$ shows extremely anisotropic phonon broadening and softening in the semimetallic normal state. In contrast, such a behavior is completely absent in the broken symmetry state of Ta$_2$NiSe$_5$ and in the isostructural Ta$_2$NiS$_5$, where the latter has a fully gapped normal state. By contrasting the expected phonon lifetimes in the BCS and BEC limits of a putative EI, our results suggest that the phase transition in Ta$_2$Ni(Se,S)$_5$ family is closely related to strong interband electron-phonon coupling. We experimentally determine the dimensionless coupling $\frac{g}{\omega_0}\sim10$, showing Ta$_2$Ni(Se,S)$_5$ as a rare "ultra-strong coupling" material.

cond-mat.str-el↗

arXiv2025

Large asymmetric anomalous Nernst effect in the antiferromagnet SrIr$_{0.8}$Sn$_{0.2}$O$_3$

A large anomalous Nernst effect is essential for thermoelectric energy harvesting in the transverse geometry without external magnetic field. It is often connected with anomalous Hall effect, especially when electronic Berry curvature is believed to be the driving force. This approach implicitly assumes the same symmetry for the Nernst and Hall coefficients, which is however not necessarily true. Here we report a large anomalous Nernst effect in antiferromagnetic SrIr$_{0.8}$Sn$_{0.2}$O$_3$ that defies the antisymmetric constraint on the anomalous Hall effect imposed by the Onsager reciprocal relation. The observed spontaneous Nernst thermopower quickly reaches the sub-$μ$V/K level below the Néel transition around 250 K, which is comparable with many topological antiferromagnetic semimetals and far excels other magnetic oxides. Our analysis indicates that the coexistence of significant symmetric and antisymmetric contributions plays a key role, pointing to the importance of extracting both contributions and a new pathway to enhanced anomalous Nernst effect for transverse thermoelectrics

cond-mat.mtrl-sci↗

arXiv2025

In-plane anisotropy of charge density wave fluctuations in 1$T$-TiSe$_2$

We report measurements of anisotropic triple-$q$ charge density wave (CDW) fluctuations in the transition metal dichalcogenide 1$T$-TiSe$_2$ over a large volume of reciprocal space with X-ray diffuse scattering. Above the transition temperature, $T_{\text{CDW}}$, the out-of-plane diffuse scattering is characterized by rod-like structures which indicate that the CDW fluctuations in neighboring layers are largely decoupled. In addition, the in-plane diffuse scattering is marked by ellipses which reveal that the in-plane fluctuations are anisotropic. Our analysis of the diffuse scattering line shapes and orientations suggests that the three charge density wave components contain independent phase fluctuations. At $T_{\text{CDW}}$, long range coherence is established in both the in-plane and out-of-plane directions, consistent with the large observed value of the CDW gap compared to $T_{\text{CDW}}$, and the predicted presence of a hierarchy of energy scales.

cond-mat.str-el↗

arXiv2025

Large moiré superstructure of stacked incommensurate charge density waves

Recent advances in van der Waals heterostructures have opened the new frontier of moiré physics, whereby tuning the interlayer twist angle or adjusting lattice parameter mismatch have led to a plethora of exotic phenomena such as unconventional superconductivity and fractional quantum spin Hall effect. We extend the concept of moiré engineering to materials that host incommensurate orders, where we discovered a long-period, thermally-hysteretic moiré superlattice in a layered charge density wave (CDW) compound, EuTe$_\text{4}$. Using high-momentum-resolution X-ray diffraction performed on ultrathin flakes, we found two coexisting, incommensurate CDWs with slightly mismatched in-plane wavevectors. The interaction between these two CDWs leads to their joint commensuration with the high-symmetry lattice as well as a large moiré superstructure with an in-plane period of 13.6~nm. Due to different out-of-plane orders of the incommensurate CDWs, the moiré superstructure exhibits a clear thermal hysteresis, accounting for the large hysteresis observed in electrical resistivity and numerous metastable states induced by light or electrical pulses. Our findings pave the way for a new development in moiré engineering based on an incommensurate lattice. They further highlight the important role of interlayer ordering in determining the macroscopic properties of these stacked incommensurate structures.

cond-mat.str-el↗

arXiv2024

Pseudosymmetry in Tetragonal Perovskite SrIrO$_3$ Synthesized under High Pressure

In this study, we report a tetragonal perovskite structure of SrIrO$_3$ (P4/mmm, a = 3.9362(9) Å, c = 7.880(3) Å) synthesized at 6 GPa and 1400 $°$C, employing the ambient pressure monoclinic SrIrO$_3$ with distorted 6H structure as a precursor. The crystal structure of tetragonal SrIrO3 was evaluated on the basis of single crystal and powder X-ray diffraction. A cubic indexing was observed attributed to overlooked superlattice reflections. Weak fractional peaks in the H and K dimensions suggest possible structure modulation by oxygen defects. Magnetization study reveals weak paramagnetic behavior down to 2 K, indicative of the interplay between spin-orbit coupling, electron correlations, and crystal electric field. Additionally, measurements of electrical resistivity display metallic behavior with an upturn at about 54 K, ascribed to weak electron localization and possible structural defects.

cond-mat.mtrl-sci↗

arXiv2023

Structural Transition and Magnetic Anisotropy in $α$-RuCl$_{3}$

We report X-ray diffraction and magnetic susceptibility studies of the structural phase transition in $α$-RuCl$_{3}$. By utilizing a single crystal sample with predominantly single twin domain, we show that $α$-RuCl$_{3}$ goes from high-temperature C2/m structure to a rhombohedral structure with R$\bar{3}$ symmetry at low temperature. While the defining feature of the structural transition is changing the stacking direction from the monoclinic a-axis to the b-axis, bond-anisotropy disappears when the structural change occurs, indicating that the local $C_3$ symmetry is restored within the honeycomb layer. The symmetry change is corroborated by the vanishing magnetic anisotropy in the low-temperature structure. Our study demonstrates that magnetic interaction is extremely sensitive to structural details in $α$-RuCl$_{3}$, which could explain the sample dependence found in this material.

cond-mat.str-el↗

arXiv2023

Frustrated charge order and cooperative distortions in ScV6Sn6

Here we study the stability of charge order in the kagome metal ScV6Sn6. Synchrotron x-ray diffraction measurements reveal high-temperature, short-range charge correlations at the wave vectors along q=(1/3,1/3,1/2) whose inter-layer correlation lengths diverge upon cooling. At the charge order transition, this divergence is interrupted and long-range order freezes in along q=(1/3,1/3,1/3), as previously reported, while disorder enables the charge correlations to persist at the q=(1/3,1/3,1/2) wave vector down to the lowest temperatures measured. Both short-range and long-range charge correlations seemingly arise from the same instability and both are rapidly quenched upon the introduction of larger Y ions onto the Sc sites. Our results validate the theoretical prediction of the primary lattice instability at q=(1/3,1/3,1/2), and we present a heuristic picture for viewing the frustration of charge order in this compound.

cond-mat.str-el↗

arXiv2023

Anomalous excitonic phase diagram in band-gap-tuned Ta2Ni(Se,S)5

During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators -- an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta2Ni(Se,S)5. A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta2NiSe5, but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems.

cond-mat.str-el↗

arXiv2023

YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$, vanadium-based kagome metals with Yb$^{2+}$ and Eu$^{2+}$ zig-zag chains

Here we present YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$, two new compounds exhibiting slightly distorted vanadium-based kagome nets interleaved with zig-zag chains of divalent Yb$^{2+}$ and Eu$^{2+}$ ions. Single crystal growth methods are reported alongside magnetic, electronic, and thermodynamic measurements. YbV$_3$Sb$_4$ is a nonmagnetic metal with no collective phase transitions observed between 60mK and 300K. Conversely, EuV$_3$Sb$_4$ is a magnetic kagome metal exhibiting easy-plane ferromagnetic-like order below $T_\text{C}$=32K with signatures of noncollinearity under low field. Our discovery of YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$ demonstrate another direction for the discovery and development of vanadium-based kagome metals while incorporating the chemical and magnetic degrees of freedom offered by a rare-earth sublattice.

cond-mat.mtrl-sci↗

arXiv2023

Multimodal Operando X-ray Mechanistic Studies of a Bimetallic Oxide Electrocatalyst in Alkaline Media

Furthering the understanding of the catalytic mechanisms in the oxygen reduction reaction (ORR) is critical to advancing and enabling fuel cell technology. In this work, we use multimodal operando synchrotron X-ray diffraction (XRD) and resonant elastic X-ray scattering (REXS) to investigate the interplay between the structure and oxidation state of a Co-Mn spinel oxide electrocatalyst, which has previously shown ORR activity that rivals Pt in alkaline fuel cells. During cyclic voltammetry, the electrocatalyst exhibited a reversible and rapid increase in tensile strain at low potentials, suggesting robust structural reversibility and stability of Co-Mn oxide electrocatalysts during normal fuel cell operating conditions. At low potential holds, exploring the limit of structural stability, an irreversible tetragonal-to-cubic phase transition was observed, which may be correlated to reduction in both Co and Mn valence states. Meanwhile, joint density-functional theory (JDFT) calculations provide insight into how reactive adsorbates induce strain in spinel oxide nanoparticles. Through this work, strain and oxidation state changes that are possible sources of degradation during the ORR in Co-Mn oxide electrocatalysts are uncovered, and the unique capabilities of combining structural and chemical characterization of electrocatalysts in multimodal operando X-ray studies are demonstrated.

cond-mat.mtrl-sci↗

arXiv2023

Reversible Non-Volatile Electronic Switching in a Near Room Temperature van der Waals Ferromagnet

The ability to reversibly toggle between two distinct states in a non-volatile method is important for information storage applications. Such devices have been realized for phase-change materials, which utilizes local heating methods to toggle between a crystalline and an amorphous state with distinct electrical properties. To expand such kind of switching between two topologically distinct phases requires non-volatile switching between two crystalline phases with distinct symmetries. Here we report the observation of reversible and non-volatile switching between two stable and closely-related crystal structures with remarkably distinct electronic structures in the near room temperature van der Waals ferromagnet Fe$_{5-δ}$GeTe$_2$. From a combination of characterization techniques we show that the switching is enabled by the ordering and disordering of an Fe site vacancy that results in distinct crystalline symmetries of the two phases that can be controlled by a thermal annealing and quenching method. Furthermore, from symmetry analysis as well as first principle calculations, we provide understanding of the key distinction in the observed electronic structures of the two phases: topological nodal lines compatible with the preserved global inversion symmetry in the site-disordered phase, and flat bands resulting from quantum destructive interference on a bipartite crystaline lattice formed by the presence of the site order as well as the lifting of the topological degeneracy due to the broken inversion symmetry in the site-ordered phase. Our work not only reveals a rich variety of quantum phases emergent in the metallic van der Waals ferromagnets due to the presence of site ordering, but also demonstrates the potential of these highly tunable two-dimensional magnets for memory and spintronics applications.

cond-mat.str-el↗

arXiv2023

Role of electron-phonon coupling in excitonic insulator candidate Ta2NiSe5

Electron-hole bound pairs, or excitons, are common excitations in semiconductors. They can spontaneously form and ``condense'' into a new insulating ground state -- the so-called excitonic insulator -- when the energy of electron-hole Coulomb attraction exceeds the band gap. In the presence of electron-phonon coupling, a periodic lattice distortion often concomitantly occurs with this exciton condensation. However, similar structural transition can also be induced by electron-phonon coupling itself, therefore hindering the clean identification of bulk excitonic insulators based on reductionistic reasoning (e.g. which instability is the ``driving force'' of the phase transition). Using high-resolution synchrotron x-ray diffraction and angle-resolved photoemission spectroscopy techniques, we identify key electron-phonon coupling effects in a leading excitonic insulator candidate Ta2NiSe5. These include an extensive unidirectional lattice fluctuation and an electronic pseudogap in the normal state, as well as a negative electronic compressibility in the charge-doped broken-symmetry state. In combination with first principles and model calculations, we determine a minimal lattice model and the corresponding interaction parameters that capture the experimental observations. More importantly, we show how the Coulomb and electron-phonon coupling effects can be separated on the level of lattice model, and demonstrate a general framework beyond the reductionist approach in the investigation of correlated systems with intertwined orders.

cond-mat.str-el↗

arXiv2023

Structural evolution of the kagome superconductors $A$V$_3$Sb$_5$ ($A$ = K, Rb, and Cs) through charge density wave order

The kagome superconductors KV$_3$Sb$_5$, RbV$_3$Sb$_5$, and CsV$_3$Sb$_5$ are known to display charge density wave (CDW) order which impacts the topological characteristics of their electronic structure. Details of their structural ground states and how they evolve with temperature are revealed here using single crystal X-ray crystallographic refinements as a function of temperature, carried out with synchrotron radiation. The compounds KV$_3$Sb$_5$ and RbV$_3$Sb$_5$ present 2$\times$2$\times$2 superstructures in the $Fmmm$ space group with a staggered tri-hexagonal deformation of vanadium layers. CsV$_3$Sb$_5$ displays more complex structural evolution, whose details have been unravelled by applying machine learning methods to the scattering data. Upon cooling through the CDW transition, CsV$_3$Sb$_5$ displays a staged progression of ordering from a 2$\times$2$\times$1 supercell and a 2$\times$2$\times$2 supercell into a final 2$\times$2$\times$4 supercell that persists to $T$ = 11 K and exhibits an average structure where vanadium layers display both tri-hexagonal and Star of David patterns of deformations. Diffraction from CsV$_3$Sb$_5$ under pulsed magnetic fields up to $μ_0H$ = 28 T suggest the real component of the CDW state is insensitive to external magnetic fields.

cond-mat.supr-con↗

arXiv2022

Thermal cycling induced alteration of the stacking order and spin-flip in the room temperature van der Waals magnet Fe$_5$GeTe$_2$

The magnetic properties of the quasi-two-dimensional van der Waals magnet Fe$_{5-δ}$GeTe$_2$ (F5GT), which has a high ferromagnetic ordering temperature $T_{\text{C}}$ $\sim$ 315 K, remains to be better understood. It has been demonstrated that the magnetization of F5GT is sensitive to both the Fe deficiency $δ$ and the thermal cycling history. Here, we investigate the structural and magnetic properties of F5GT with a minimal Fe deficiency ($|δ|$ $\le$ 0.1), utilizing combined x-ray and neutron scattering techniques. Our study reveals that the quenched F5GT single crystals experience an irreversible, first-order transition at $T_{\text{S}}$ $\sim$ 110 K upon first cooling, where the stacking order partly or entirely converts from ABC-stacking to AA-stacking order. Importantly, the magnetic properties, including the magnetic moment direction and the enhanced $T_{\text{C}}$ after the thermal cycling, are intimately related to the alteration of the stacking order. Our work highlights the significant influence of the lattice symmetry to the magnetism in F5GT.

cond-mat.str-el↗

arXiv2022

Bond Ordering and Molecular Spin-Orbital Fluctuations in the Cluster Mott Insulator GaTa$_4$Se$_8$

For materials where spin-orbit coupling is competitive with electronic correlations, the spatially anisotropic spin-orbital wavefunctions can stabilize degenerate states that lead to many and diverse quantum phases of matter. Here, we find evidence for a dynamical spin-orbital state preceding a T$^*$=50 K order-disorder spin-orbital ordering transition in the $j\!=\!3/2$ lacunar spinel GaTa$_4$Se$_8$. Above T$^*$, GaTa$_4$Se$_8$ has an average cubic crystal structure, but total scattering measurements indicate local non-cubic distortions of Ta$_4$ tetrahedral clusters for all measured temperatures $2 < T < 300$ K. Inelastic neutron scattering measurements reveal the dynamic nature of these local distortions through symmetry forbidden optical phonon modes that modulate $j\!=\!3/2$ molecular orbital occupation as well as intercluster Ta-Se bonds. Spin-orbital ordering at T$^*$ cannot be attributed to a classic Jahn-Teller mechanism and based on our findings, we propose that intercluster interactions acting on the scale of T$^*$ act to break global symmetry. The resulting staggered intercluster dimerization pattern doubles the unit cell, reflecting a spin-orbital valence bond ground state.

cond-mat.str-el↗