arXiv subjects

Ruoshi Jiang

Publications and source records attributed to Ruoshi Jiang.

13 recordsLinked to original sources

arXiv2026

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↗

arXiv2025

Charge order through crystallization of Frenkel excitons: realization in kagome metals

Charge order is a widely observed and representative example of spontaneous broken symmetries in quantum states of matter. Owing to the large intra-atomic Coulomb energy, the charge redistribution in such an order typically implies significant alteration of the electronic and lattice properties of materials. While the standard description of charge order, namely a "charge density wave" instability of the Fermi surface, has been broadly and successfully applied to good metals, its applicability to correlated ionic materials has been rather limited. Here, we propose an alternative general scenario of charge order - crystallization of long-lived Frenkel excitons - suitable for these ionic materials. We demonstrate this scenario on the recently discovered kagome superconductors and successfully reproduce all the characteristics of experimental observations on both local charge correlations and long-range ordering. The proposed generic scenario offers a long-sought understanding of charge order applicable to modern correlated functional materials.

cond-mat.str-el↗

arXiv2025

2D ferroelectricity accompanying antiferro-orbital order in semi-metallic WTe$_2$

The first switchable electric polarization in metals was recently discovered in bilayer and trilayer WTe2. Strangely, despite the tininess of the ordered polarization, the ferroelectricity survives up to 350 K, rendering the mechanism of such ferroelectricity challenging for standard understandings. Here, via a density-functional-based multi-energy-scale analysis of the system's broken symmetries, we identify a weak out-of-plane ferroelectricity accompanying a strong in-plane antiferro-orbital order. This unusual low-energy correlation, which emerges from an antiferroelectric structure formed at much higher energy, naturally explains the above puzzling observation. This result reveals an unprecedented paradigm of electronic ferroelectricity generally applicable to 2D polar metals with ultrafast-switchable polarization ideal for the next-generation non-volatile memory and other devices.

cond-mat.mtrl-sci↗

arXiv2025

Band-Gap Tunability in Anharmonic Perovskite-like Semiconductors Driven by Polar Electron-Phonon Coupling

The ability to finely tune optoelectronic properties in semiconductors is crucial for the development of advanced technologies, ranging from photodetectors to photovoltaics. In this work, we propose a novel strategy to achieve such tunability by utilizing electric fields to excite low-energy polar optical phonon modes, which strongly couple to electronic states in anharmonic semiconductors. We conducted a high-throughput screening of over $10,000$ materials, focusing on centrosymmetric compounds with imaginary polar phonon modes and suitable band gaps, and identified $310$ promising candidates with potential for enhanced optoelectronic tunability. From this set, three perovskite-like compounds --Ag$_3$SBr, BaTiO$_3$, and PbHfO$_3$-- were selected for in-depth investigation based on their contrasting band-gap behavior with temperature. Using first-principles calculations, \textit{ab initio} molecular dynamics simulations, tight-binding models, and anharmonic Fr\"ohlich theory, we analyzed the underlying physical mechanisms. Our results show that polar phonon distortions can induce substantial band-gap modulations at ambient conditions, including reductions of up to $70\%$ in Ag$_3$SBr and increases of nearly $23\%$ in BaTiO$_3$, relative to values calculated at zero temperature, while PbHfO$_3$ exhibits minimal change. These contrasting responses arise from distinct electron-phonon coupling mechanisms and orbital hybridization at the band edges. This work establishes key design principles for harnessing polar lattice dynamics to engineer tunable optoelectronic properties, paving the way for adaptive technologies such as wavelength-selective optical devices and solar absorbers.

cond-mat.mtrl-sci↗

arXiv2025

Pressure-induced trans-proximate correlation in La$_4$Ni$_3$O$_{10}$ and possible routes to enhance its superconductivity

We report an unexpected trans-proximate interlayer correlation (stronger correlation between disjoint layers than the adjacent ones) in the high-pressure phase of the recently discovered La$_4$Ni$_3$O$_{10}$ superconductors. Accompanied by an unusual pressure-induced fractionalization of Ni$^{2+}$ ionic spin from the standard spin-1 to spin-$\frac{1}{2}$, this trans-proximate correlation results from the emergence of a cross-layer trimer in our multi-energy-scale derivation of the electron dynamics. The resulting low-energy effective description resembles that of the cuprates and suggests a universal superconducting mechanism in all existing nickelate and cuprate superconductors. The rare trans-proximate correlation not only explains the weaker superconductivity in comparison with the related La$_3$Ni$_2$O$_7$ samples, but it also indicates a viable strategy to improve superconductivity in this trilayer nickelate by lowering layer symmetry. Such pressure-induced trans-proximate correlation is expected in many materials and examplifies the engineering of rich uncharted quantum states of matter through pressure.

cond-mat.supr-con↗

arXiv2024

Giant Electron-Phonon Coupling Induced Band-Gap Renormalization in Anharmonic Silver Chalcohalide Antiperovskites

Silver chalcohalide antiperovskites (CAP), Ag$_{3}$XY (X = S, Se; Y = Br, I), are a family of highly anharmonic inorganic compounds with great potential for energy applications. However, a substantial and unresolved discrepancy exists between the optoelectronic properties predicted by theoretical first-principles methods and those measured experimentally at room temperature, hindering the fundamental understanding and rational engineering of CAP. In this work, we employ density functional theory, tight-binding calculations, and anharmonic Fr\"ohlich theory to investigate the optoelectronic properties of CAP at finite temperatures. Near room temperature, we observe a giant band-gap ($E_{g}$) reduction of approximately $20$-$60$\% relative to the value calculated at $T = 0$ K, bringing the estimated $E_{g}$ into excellent agreement with experimental measurements. This relative $T$-induced band-gap renormalization is roughly twice the largest value previously reported in the literature for similar temperature ranges. Low-energy optical polar phonon modes, which break inversion symmetry and promote the overlap between silver and chalcogen $s$ electronic orbitals in the conduction band, are identified as the primary contributors to this giant $E_{g}$ reduction. Furthermore, when considering temperature effects, the optical absorption coefficient of CAP increases by nearly an order of magnitude for visible light frequencies. These insights not only bridge a crucial gap between theory and experiment but also open pathways for future technologies where temperature, electric fields, or light dynamically tailor optoelectronic behavior, positioning CAP as a versatile platform for next-generation energy applications.

cond-mat.mtrl-sci↗

arXiv2024

`Interaction annealing' to determine effective quantized valence and orbital structure: an illustration with ferro-orbital order in WTe$_2$

Correlated materials are known to display qualitatively distinct emergent behaviors at low energy. Conveniently, upon absorbing rapid quantum fluctuations, these rich low-energy behaviors can always be effectively described by dressed particles with fully quantized charge, spin, and orbital structure. Such a powerful and simple description is, however, difficult to access through bare particles used in most many-body computations, especially when fluctuations are strong such as in $4d$ and $5d$ compounds. To decipher the dominant quantized structure, we propose an easy-to-implement `interaction annealing' approach that utilizes suppressed charge fluctuation through enhancing ionic charging energy. We establish its theoretical foundation using an exactly treated two-site Hubbard model as a generic example. We then demonstrate its applications with more affordable density functional calculations to a representative $3d$ Mott insulator La${_2}$CuO${_4}$ and a highly fluctuating $5d$ semi-metal WTe${_2}$. In the latter, it reveals an emergent local electronic structure that makes possible an unprecedented explanation of several experimental observations. Finally, we demonstrate the effectiveness of this approach in studying competing local electronic structures in functional materials.

cond-mat.str-el↗

arXiv2024

Universal low-temperature fluctuation of unconventional superconductors revealed: 'Smoking gun' leaves proper bosonic superfluidity the last theory standing

Low-temperature thermal fluctuations offer an essential window in characterizing the true nature of a quantum state of matter, a quintessential example being Fermi liquid theory. Here, we examine the leading thermal fluctuation of the superfluid density across numerous families ranging from relatively conventional to highly unconventional superconductors (MgB$_2$, bismuthates, doped buckyballs, heavy fermions, UTe$_2$, doped SrTiO$_3$, Chevrel clusters, intermetallics, organic superconductors, transition metal dichalcogenides, ruthenates, iron-pnictides, cuprates, and kagome metals). Amazingly, in all of them an unprecedented universal $T^3$ depletion materializes in the low-temperature superfluid density, even in the believed-to-be-conventional MgB$_2$. This reveals a new quantum superfluid state of matter and requires a necessary change of paradigm in describing modern superconductors. We demonstrate that such unorthodox yet generic behavior can be described by a strictly Galilean consistent theory of bosonic superfluidity hosting a long-lived 'true condensate'.

cond-mat.supr-con↗

arXiv2024

Geometric inhibition of superflow in single-layer graphene suggests a staggered-flux superconductivity in bilayer and trilayer graphene

In great contrast to the numerous discoveries of superconductivity in layer-stacked graphene systems, the absence of superconductivity in the simplest and cleanest monolayer graphene remains a big puzzle. Here, through realistic computation of electronic structure, we identify a systematic trend that superconductivity appears to emerge only upon alteration of the low-energy electronic lattice from the underlying honeycomb atomic structure. We then demonstrate that this inhibition can result from from geometric frustration of the bond lattice that disables quantum phase coherence of the order parameter residing on it. In comparison, upon deviating from the honeycomb lattice, relief of geometric frustration allows robust superfluidity with non-trivial spatial structure. For the specific examples of bilayer and trilayer graphene under an external electric field, such bond centered order parameter would develop superfluidity with staggered flux that breaks the time-reversal symmetry. Our study also suggests the possible realization of the long-sought superconductivity in single-layer graphene via the application of uni-directional strain.

cond-mat.supr-con↗

arXiv2023

Pressure Driven Fractionalization of Ionic Spins Results in Cupratelike High-$T_c$ Superconductivity in La$_3$Ni$_2$O$_7$

Beyond 14GPa of pressure, bi-layered La$_3$Ni$_2$O$_7$ was recently found to develop strong superconductivity above the liquid nitrogen boiling temperature. An immediate essential question is the pressure-induced qualitative change of electronic structure that enables the exciting high-temperature superconductivity. We investigate this timely question via a numerical multi-scale derivation of effective many-body physics. At the atomic scale, we first clarify that the system has a strong charge transfer nature with itinerant carriers residing mainly in the in-plane oxygen between spin-1 Ni$^{2+}$ ions. We then elucidate in eV- and sub-eV-scale the key physical effect of the applied pressure: It induces a cupratelike electronic structure through partially screening the Ni spin from 1 to 1/2. This suggests a high-temperature superconductivity in La$_3$Ni$_2$O$_7$ with microscopic mechanism and ($d$-wave) symmetry similar to that in the cuprates.

cond-mat.supr-con↗

arXiv2022

Variation of carrier density in semimetals via short-range correlation: A case study with nickelate NdNiO$_2$

Carrier density is one of the key controlling factors of material properties, particularly in controlling the essential correlations in strongly correlated materials. Typically, carrier density is externally tuned by doping or gating and remains fixed below room temperature. Strangely, the carrier density in correlated semimetals is often found to vary sensitively against weak external controls such as temperature, magnetic field, and pressure. Here, we develop a realistic simulation scheme that incorporates interatomic noncollinear magnetic correlation without a long-range order. Using the recently discovered nickelate superconductor as an example, we demonstrate a rather generic low-energy mechanism that in semimetals short-range correlation can reversely modulate the carrier density as well. Such a mutual influence between correlation and carrier density provides an extra ingredient for sensitive bifurcating behavior. This special feature of correlated semimetals explains their versatile carrier density at low energy and opens up new possibilities of functionalizing these materials.

cond-mat.str-el↗

arXiv2021

Proposal to improve Ni-based superconductors via enhanced charge transfer

Recently discovered superconductivity in hole-doped nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ has attracted intensive attention in the field. An immediate question is how to improve its superconducting properties. Guided by the key characteristics of electronic structures of the cuprates and the nickelates, we propose that nickel chalcogenides with a similar lattice structure should be a promising family of materials. Using NdNiS$_2$ as an example, through first-principle structural optimization and phonon calculation, we find this particular crystal structure a stable one. We justify our proposal by comparing with CaCuO$_2$ and NdNiO$_2$ with regard to strength of the charge-transfer characteristics and the trend in their low-energy many-body effective Hamiltonians of doped hole carriers. This analysis indicates that nickel chalcogenides host low-energy physics closer to that of the cuprates, with stronger magnetic interaction than the nickelates, and thus they deserve further experimental exploration. Our proposal also opens up the possibility of a wide range of parameter tuning through ligand substitution among chalcogenides, to further improve superconducting properties.

cond-mat.supr-con↗

arXiv2020

Strongly correlated doped hole carriers in the superconducting nickelates: Their location, local many-body state, and low-energy effective Hamiltonian

The families of high-temperature superconductors recently welcomed a new member: hole doped nickelate Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ with a $\sim$15K transition temperature. To understand its emergent low-energy behaviors and experimental properties, an immediate key question is whether the superconducting hole carriers reside in oxygen as in the cuprates, or in nickel as in most nickelates. We answer this crucial question via a ``(LDA+$U$)+ED'' scheme: deriving an effective interacting Hamiltonian of the hole carriers from density functional LDA+$U$ calculation, and studying its local many-body states via exact diagonalization. Surprisingly, distinct from the expected Ni$^{2+}$ spin-triplet state found in most nickelates, the local ground state of two holes is actually a Ni-O spin-singlet state with second hole greatly residing in oxygen. The emerged eV-scale model therefore resembles that of the cuprates, advocating further systematic experimental comparisons. Tracing the microscopic origin of this unexpected result to the lack of apical oxygen in this material, we proposed a route to increase superconducting temperature, and a possible quantum phase transition absent in the cuprates.

cond-mat.supr-con↗