Supersolid phases are quantum-entangled states of matter exhibiting the dual characteristics of superfluidity and solidity. Theory predicts that hard-core bosons on a triangular lattice can form such phases at half filling and near complete filling. Leveraging an exact mapping between bosons and spin- 1 2 degrees of freedom, here we show that these phases are realized in the triangular-lattice antiferromagnet K2Co(SeO3)2. At zero field, neutron diffraction reveals the development of quasi-two-dimensional 3 × 3 magnetic order with Z3 translational symmetry breaking (solidity), though with reduced amplitude indicating strong quantum fluctuations. These fluctuations manifest as equidistant bands of continuum neutron scattering, where the lowest-energy mode is gapless at K ( 1 3 1 3 ) , consistent with broken U(1) spin rotational symmetry (superfluidity). For c-axis-oriented magnetic fields near saturation, we find a second phase consistent with a high-field supersolid. These two supersolids are separated by a pronounced 1/3 magnetization plateau phase that supports coherent spin waves, from which we determine the underlying spin Hamiltonian.
How ordered phases melt in low-dimensional quantum materials remain difficult to resolve because the relevant fluctuations are dynamic and charge neutral. In this work, we show that thermal transport provides a sensitive probe of these hidden fluctuations in the layered transition metal dichalcogenide 2H-TaSe2. We observe a striking V-shaped temperature dependence of the thermal conductivity that cannot be explained by conventional phonon-phonon scattering. Instead, it originates from scattering by persistent local charge-density-wave (CDW) correlations, consistent with our phenomenological model linking thermal transport to spatial CDW fluctuation. Electron diffraction reveals short-range periodic lattice distortions persisting to at least 300 K, while X-ray diffraction shows thermal hysteresis of the CDW wavevector. Together, these results reveal a dislocation- and fluctuation-driven weak first-order melting of the CDW state.
Tantalum (Ta) based superconducting circuits have been demonstrated to enable record qubit coherence times and quality factors, motivating a careful study of the microscopic origin of the remaining losses that limit their performance. We have recently shown that the losses in Ta-based resonators are dominated by two-level systems (TLSs) at low microwave powers and millikelvin temperatures. We also observe that some devices exhibit loss that is exponentially activated at a lower temperature inconsistent with the superconducting critical temperature (Tc) of the constituent film. Specifically, dc resistivity measurements show a Tc of over 4 K, while microwave measurements of resonators fabricated from these films show losses that increase exponentially with temperature with an activation energy as low as 0.3 K. Here, we present a comparative study of the structural and thermodynamic properties of Ta-based resonators and identify vortex motion-induced loss as the source of thermally activated microwave loss. Through careful magnetoresistance and x-ray diffraction measurements, we observe that the increased loss occurs for films that are in the clean limit, where the superconducting coherence length is shorter than the mean free path. Vortex motion-induced losses are suppressed for films in the dirty limit, which show evidence of structural defects that can pin vortices. We verify this hypothesis by explicitly pinning vortices via patterning and find that we can suppress the loss by microfabrication.
Superconductivity in La_4Ni_3O_10 has been reported to emerge upon suppression of intertwined spin and charge density wave (SDW/CDW) order, suggesting a possible connection to the pairing mechanism. Here we report a systematic investigation of La_4Ni_3-xCu_xO_10+δ (0 ≤ x ≤ 0.7), focusing on the evolution of the SDW/CDW order as a function of chemical substitution. Temperature-dependent resistivity, magnetic susceptibility, and Hall effect measurements reveal a linear suppression of density wave transition temperature Tdw and a concurrent enhancement of hole concentration with increasing Cu content. At higher substitution levels (x > 0.15), the transition-induced anomaly in the resistivity becomes undetectable while a magnetic signature persists, indicating a partial decoupling of spin and charge components and the possible survival of short-range spin correlations. The absence of superconductivity across the substitution series highlights the importance of additional factors in stabilizing the superconducting state in pressurized La_4Ni_3O_10.
The discovery of novel superconducting materials is a long-standing challenge in materials science, with a wealth of potential for applications in energy, transportation and computing. Recent advances in artificial intelligence (AI) have enabled expediting the search for new materials by efficiently utilizing vast materials databases. In this study, we developed an approach based on deep learning (DL) to predict new superconducting materials. We have synthesized a compound derived from our DL network and confirmed its superconducting properties in agreement with our prediction. Our approach is also compared to previous work based on random forests (RFs). In particular, RFs require knowledge of the chemical properties of the compound, while our neural net inputs depend solely on the chemical composition. With the help of hints from our network, we discover a new ternary compound Mo20Re6Si4, which becomes superconducting below 5.4 K. We further discuss the existing limitations and challenges associated with using AI to predict and, along with potential future research directions.
Ultrathin ferroelectric films with out-of-plane polarization and high Curie temperatures are key to miniaturizing electronic devices. Most ferroelectrics employed in devices are proper ferroelectrics, where spontaneous polarization is the primary order parameter. Unfortunately, the Curie temperature of proper ferroelectrics is drastically reduced as the ferroelectric becomes thin; nearly all proper ferroelectrics need to be thicker than several unit cells. The absence of an ultrathin limit has been predicted, but not verified for improper ferroelectrics. These are ferroelectrics where the polarization emerges secondary to the primary order parameter, such as a structural distortion. Here we report improper ferroelectricity with an undiminished Curie temperature in a 0.75-unit-cell-thick hexagonal LuFeO3 (h-LuFeO3) film grown on a SrCo2Ru4O11 bottom electrode with an atomically engineered monolayer bridging layer. Our results demonstrate the absence of a critical thickness for improper ferroelectricity and provide a methodology for creating ultrathin improper ferroelectrics by stabilizing their primary order parameters.
Entanglement between photons and a quantum memory is a key component of quantum repeaters, which allow long-distance quantum entanglement distribution in the presence of fiber losses. Spin-photon entanglement has been implemented with a number of different atomic and solid-state qubits with long spin coherence times, but none directly emit photons into the 1.5-mu m telecom band where losses in optical fibers are minimized. Here, we demonstrate spin-photon entanglement using a single rare earth ion in the solidstate Er3coupled to a silicon nanophotonic cavity, which directly emits photons at 1532.6 nm. We infer an entanglement fidelity of 73(3)% after propagating through 15.6 km of optical fiber. This work opens the door to large-scale quantum networks based Er3ions, leveraging scalable silicon device fabrication and spectral multiplexing.
Materials improvements are a powerful approach to reducing loss and decoherence in superconducting qubits because such improvements can be readily translated to large scale processors. Recent work improved transmon coherence by utilizing tantalum (Ta) as a base layer and sapphire as a substrate. The losses in these devices are dominated by two-level systems (TLSs) with comparable contributions from both the surface and bulk dielectrics, indicating that both must be tackled to achieve major improvements in the state of the art. Here we show that replacing the substrate with high-resistivity silicon (Si) dramatically decreases the bulk substrate loss, enabling 2D transmons with time-averaged quality factors (Q) exceeding 1.5 x 10^7, reaching a maximum Q of 2.5 x 10^7, corresponding to a lifetime (T_1) of up to 1.68 ms. This low loss allows us to observe decoherence effects related to the Josephson junction, and we use improved, low-contamination junction deposition to achieve Hahn echo coherence times (T_2E) exceeding T_1. We achieve these material improvements without any modifications to the qubit architecture, allowing us to readily incorporate standard quantum control gates. We demonstrate single qubit gates with 99.994 that can potentially be fabricated at wafer scale, and therefore can be readily translated to large-scale quantum processors.
The existence of a quantum critical point (QCP) and fluctuations around it are believed to be important for understanding the phase diagram in unconventional superconductors such as cuprates, iron pnictides, and heavy fermion superconductors. However, the QCP is usually buried deep within the superconducting dome and is difficult to investigate. The connection between quantum critical fluctuations and superconductivity remains an outstanding problem in condensed matter. Here combining both electrical transport and Nernst experiments, we explicitly demonstrate the onset of superconductivity at an unconventional QCP in gate-tuned monolayer tungsten ditelluride (WTe2), with features incompatible with the conventional Bardeen-Cooper-Schrieffer scenario. The results lead to a superconducting phase diagram that is distinguished from other known superconductors. Two distinct gate-tuned quantum phase transitions are observed at the ends of the superconducting dome. We find that quantum fluctuations around the QCP of the underdoped regime are essential for understanding how the monolayer superconductivity is established. The unconventional phase diagram we report here illustrates a previously unknown relation between superconductivity and QCP.
The interplay of crystal electric field, temperature, and spin-orbit coupling can yield a Kramers ion and thus an effective S = 1/2 ground state for Co2+ ions (3d7), which is often the case for low dimensional materials. This is because a highly anisotropic structural motif can force the spins to point either up or down, hence becoming a system where spins communicate via Ising interactions. Cobalt-based quasi-1-dimensional materials have been studied in this context since the latter half of the 20th century, but due to the development of modern characterization techniques and advances in sample preparation, the exotic physical phenomena that have generated the most interest have only emerged in the most recent three to four decades. This topical review mainly summarizes progress in cobalt-based quasi-1-dimensional quantum magnets, and comments on a few research directions of potential future interest.
Single $\text{Er}^{3+}$ ions in CaW04 coupled to nanophotonic cavities enable indistinguishable single-photon emission and spin-photon entanglement in the telecom band, forming building blocks for quantum repeater networks. However, spin decoherence from paramagnetic impurities limits fidelity. We investigate spin dynamics of near-surface Er ions ($~$ 10–15 nm from surface) as a step toward quantum repeaters and memory.
We successfully synthesized the erbium (Er)-doped optical material calcium tungstate (CaWO4) while maintaining charge balance by codoping Er with vanadium (V5+) and niobium (Nb5+) into the optical material calcium tungstate (CaWO4). The synthesized samples, with the general formula Ca1- x Erx W1- x Mx O4 (M = V or Nb), were annealed at 1200 °C in air. Er3+ dopants introduced localized visible-light transition states within the band gap, thus adding pink hues to the white CaWO4 for both codoping systems. Phase-pure materials were obtained up to the doping levels of x = 0.10, beyond which impurity peaks in powder X-ray diffraction patterns emerged. Reduction in lattice constants and grain sizes due to dopant substitution was observed. No evidence was seen for long-range magnetic ordering above 0.5 K, and the local crystal field of Er3+ was different for the two codopants. Charge-compensated codoping is thus shown to be an effective strategy for tailoring scheelite optical properties.
The solid-state synthesis at an applied pressure of 6 GPa, crystal structure, and elementary electronic properties of the previously unreported compound TiSe3 are described. The crystal structure, which is based on 1D chains of Ti-Se triangular prisms that are coupled to each other, with two-thirds of the Se involved in a Se-Se pair, is similar to that of TiS3. Unlike the trisulfide, the triselenide is only made under pressure at temperatures between 800 and 900 °C. The material is semiconducting and weakly diamagnetic.
Utilizing tantalum (Ta) in superconducting circuits has led to significant improvements, such as high qubit lifetimes and quality factors in both qubits and resonators, underscoring the importance of material optimization in quantum device performance. In this work, we explore superconducting gap engineering in Ta-based devices as a strategy to expand the range of viable host materials. By alloying 20 atomic percent hafnium (Hf) into Ta thin films, we achieve a superconducting transition temperature (T_c) of 6.09 K, as measured by DC transport, reflecting an increased superconducting gap. We systematically vary deposition conditions to control film orientation and transport properties of the Ta-Hf alloy films. The enhancement in T_c is further confirmed by microwave measurements at millikelvin temperatures. Despite the 40% increase in T_c relative to pure Ta, the loss contributions from two-level systems (TLS) and quasiparticles (QPs) remain unchanged in the low-temperature regime. These findings highlight the potential of material engineering to improve superconducting circuit performance and motivate further exploration of engineered alloys for quantum technologies.
We present terahertz spectroscopic measurements of quantum spin dynamics in the honeycomb magnet K_2Co_2TeO_6 as a function of temperature, polarization and in an external magnetic field applied in the honeycomb plane. Magnetic excitations are resolved below the magnetic ordering temperature of T_N = 12 K. In the applied magnetic field, we reveal characteristic field dependence not only for the magnetic excitations observed at zero field, but also a rich set of modes emerging in finite fields. The observed magnetic excitations exhibit clear dependence on the terahertz polarization, and characteristic features at field-induced phase transitions consistent with our high-field magnetization data. We cannot evidently resolve a continuumlike feature, even when the long-range magnetic order is presumably suppressed in the strong magnetic field, indicating that a Kitaev-type interaction, if existing, is subleading in this compound.
Superconductivity in La$_{4}$Ni$_{3}$O$_{10}$ has been reported to emerge upon suppression of intertwined spin and charge density wave (SDW/CDW) order, suggesting a possible connection to the pairing mechanism. Here we report a systematic investigation of La$_{4}$Ni$_{3-x}$Cu$_{x}$O$_{10+\delta}$ ($0 \leq x \leq 0.7$), focusing on the evolution of the SDW/CDW order as a function of chemical substitution. Temperature-dependent resistivity, magnetic susceptibility, and Hall effect measurements reveal a linear suppression of density wave transition temperature $T{\text{dw}}$ and a concurrent enhancement of hole concentration with increasing Cu content. At higher substitution levels ($x > 0.15$), the transition-induced anomaly in the resistivity becomes undetectable while a magnetic signature persists, indicating a partial decoupling of spin and charge components and the possible survival of short-range spin correlations. The absence of superconductivity across the substitution series highlights the importance of additional factors in stabilizing the superconducting state in pressurized La$_{4}$Ni$_{3}$O$_{10}$.
We study the magnetic properties of the metallic kagome system (Fe_1-xCo_x) Sn by a combination of Muon Spin Relaxation (μSR), magnetic susceptibility and Scanning Tunneling Microscopy (STM) measurements, in single crystal specimens with Co concentrations x=0,0.11,0.8. In the undoped antiferromagnetic compound FeSn, we find possible signatures for a previously unidentified phase that sets in at T^*∼ 50 K, well beneath the Neel temperature T_N ∼ 376 K, as indicated by a peak in the relaxation rate 1/T_1 observed in zero field (ZF) and longitudinal field (LF) μSR measurements, with a corresponding anomaly in the ac and dc-susceptibility, and an increase in the static width 1/T_2 in ZF measurements. No signatures of spatial symmetry breaking are found in STM down to 7 K. In Fe_0.2Co_0.8Sn, we find canonical spin glass behavior with freezing temperature T_g∼ 3.5 K; the ZF and LF time spectra exhibit results similar to those observed in dilute alloy spin glasses CuMn and AuFe, with a critical behavior of 1 / T_1 at T_g and 1 / T_1→ 0 as T → 0. The absence of spin dynamics at low temperatures makes a clear contrast to the spin dynamics observed by μSR in many geometrically frustrated spin systems on insulating kagome, pyrochlore, and triangular lattices. The spin glass behavior of CoSn doped with dilute Fe moments is shown to originate primarily from the randomness of doped Fe moments rather than due to geometrical frustration of the underlying lattice.
Billions of organic molecules have been computationally generated, yet functional inorganic materials remain scarce due to limited data and structural complexity. Here we introduce Structural Constraint Integration in a GENerative model (SCIGEN), a framework that enforces geometric constraints, such as honeycomb and kagome lattices, within diffusion-based generative models to discover stable quantum materials candidates. SCIGEN enables conditional sampling from the original distribution, preserving output validity while guiding structural motifs. This approach generates ten million inorganic compounds with Archimedean and Lieb lattices, over 10% of which pass multistage stability screening. High-throughput density functional theory calculations on 26,000 candidates shows over 95% convergence and 53% structural stability. A graph neural network classifier detects magnetic ordering in 41% of relaxed structures. Furthermore, we synthesize and characterize two predicted materials, TiPd0.22Bi0.88 and Ti0.5Pd1.5Sb, which display paramagnetic and diamagnetic behaviour, respectively. Our results indicate that SCIGEN provides a scalable path for generating quantum materials guided by lattice geometry.
Van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and the fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent x-ray absorption spectroscopy and x-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7)) in the ferromagnetic state, and (b) an instability of the orbital moment in proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment, and establish VI3 as a prime candidate for the study of orbital quantum effects.
Billions of organic molecules are known, but only a tiny fraction of the functional inorganic materials have been discovered, a particularly relevant problem to the community searching for new quantum materials. Recent advancements in machine learning-based generative models, particularly diffusion models, show great promise for generating new, stable materials. However, integrating geometric patterns into materials generation remains a challenge. Here, we introduce Structural Constraint Integration in the GENerative model (SCIGEN). Our approach can modify any trained generative diffusion model by strategic masking of the denoised structure with a diffused constrained structure prior to each diffusion step to steer the generation toward constrained outputs. Furthermore, we mathematically prove that SCIGEN effectively performs conditional sampling from the original distribution, which is crucial for generating stable constrained materials. We generate eight million compounds using Archimedean lattices as prototype constraints, with over 10% surviving a multi-staged stability pre-screening. High-throughput density functional theory (DFT) on 26,000 survived compounds shows that over 50% passed structural optimization at the DFT level. Since the properties of quantum materials are closely related to geometric patterns, our results indicate that SCIGEN provides a general framework for generating quantum materials candidates.