arXiv subjects

Zhibo Kang

Publications and source records attributed to Zhibo Kang.

9 recordsLinked to original sources

arXiv2026

High-Temperature ferromagnetism from site-selective filling in (Fe,Ni)$_{6-\delta}$GeTe$_2$

The discovery of high-temperature ferromagnetism in the metallic van der Waals (vdW) system Fe$_N$GeTe$_2$ has brought two-dimensional (2D) magnets into technologically relevant temperature scales. Specifically at N = 5, dilution of magnetic moments by nickel substitution counterintuitively achieves a record high Curie temperature of 478~K. Unraveling the origin of this nickel-substitution-induced enhancement is complicated by the compound's structural complexity, coexistent itinerant and local magnetic contributions, and mesoscopic compositional domains. Through coordinated structural and electronic characterization, we identify that the high-T$_C$ magnetic phase arises from a strain-stabilized Fe$_6$GeTe$_2$ nano-precipitate. Combining first-principles calculations and spin- and angle-resolved photoemission spectroscopy (ARPES), we uncover a site-specific electronic landscape in which interior iron atoms primarily host localized moments while the outer iron atoms neighboring the tellurium layers produce spin-polarized itinerant carriers that cross the vdW gap. The large energy cost associated with homogeneous nickel substitution is found to favor the spontaneous precipitation of the crystallographically and electronically ``clean'' high-T$_C$ phase. Finally, we compare metal-rich vdW magnets with binary magnetic alloys, and discuss the unifying roles of nano-precipitates in stabilizing otherwise unattainable bulk phases. Our work provides mechanistic insights into the record-high T$_C$ ferromagnetism in (Fe,Ni)$_{5+\delta}$GeTe$_2$, establishing a rigorous foundation for the atomic engineering of vdW magnetic metals informed by direct electronic signatures.

cond-mat.mtrl-sci↗

arXiv2026

Self-Assembled H2NC Molecular Lattices as a Platform for Tunable Quantum Superlattices

Compared to van der Waals moir\'e systems, molecular assembly has emerged as an exciting alternative platform for superlattice engineering via heterointegration. The electronic properties of the self-assembled square lattice monolayer molecular crystal of metal-free naphthalocyanine (H$_2$Nc), in particular the electronic band dispersion and their tunability by metal substrates, remain less explored. Using density functional theory, supported by angle-resolved photoemission and scanning tunneling microscopy, we compare the electronic structure of a free-standing H$_2$Nc monolayer with that of H$_2$Nc lattice assembled on noble metal substrates. In the free-standing film, we identify both nearly flat, molecule-localized states and more dispersive bands, and we show that each can be compactly described by an anisotropic tight-binding Hamiltonian that yields band-resolved hopping anisotropies. We further show theoretically the wide tunability in the inter-site hopping and Coulomb interaction based on dielectric and screening environment, and show two experimental realizations using Ag(100) and Au(111) substrates. On Ag(100), orbital hybridization between molecular frontier states and the substrate drives finite spectral weight at the Fermi level and local interfacial polarization. This hybridization enhances the effective intermolecular hopping roughly thirty-fold, drastically reducing $U/t$. Complementary angle-resolved photoemission spectroscopy resolves substantial interfacial charge redistribution and enhanced bandwidth of the HOMO band, consistent with theoretical predictions. These results clarify how metal substrates and gates convert H$_2$Nc from isolated molecules into a tunable 2D lattice, and highlight molecular superlattices as a promising platform in which the effective interaction parameters can be engineered over a wide range.

cond-mat.mtrl-sci↗

arXiv2026

Photoinduced metastable cation disorder in metal halide double perovskites

Lead-free perovskites have emerged as environmentally benign alternatives to lead-halide counterparts for optoelectronics. Among them, the double perovskite Cs2AgInCl6 family exhibits remarkable white-light emission with proper composition engineering, enabled by strong electron-phonon coupling and the formation of self-trapped excitons (STEs). Despite these advantages, the fundamental photo- and structural dynamics governing their excited-state behavior remain poorly understood. Here, we report a long-lived metastable phase in the Cs2AgInCl6 double perovskite family and unravel this process and the concomitant electronic and structural evolution using a suite of tools including transient optical spectroscopy, time-resolved X-ray diffraction (TR-XRD) and X-ray absorption (TR-XAS). We show that the photoinduced, transient metastable phase is associated with B-site (Ag-In) disorder, which induces a dramatically reduced optical bandgap. Supported by TR-XRD and first-principles calculations, the Ag-In disorder drives the formation of Ag-rich and In-rich domains with millisecond lifetimes, with lifetimes increasing at lower temperatures. TR-XAS further reveals that photogenerated STEs oxidize Ag+ to Ag2+, facilitating this highly temporally asymmetric order-disorder transition. Our findings demonstrate a new mechanism, mediated by hole-localized STE formation, that enables prolongation of transient light-induced states to the multi-millisecond regime in double perovskites, opening possibilities to harvesting the functional properties of metastable phases of these materials.

cond-mat.mtrl-sci↗

arXiv2025

Superconductivity suppression and bilayer decoupling in Pr substituted YBa$_2$Cu$_3$O$_{7-\delta}$

The mechanism behind superconductivity suppression induced by Pr substitutions in YBa$_2$Cu$_3$O$_{7-\delta}$ (YBCO) has been a mystery since its discovery: in spite of being isovalent to Y$^{3+}$ with a small magnetic moment, it is the only rare-earth element that has a dramatic impact on YBCO's superconducting properties. Using angle-resolved photoemission spectroscopy (ARPES) and DFT+$U$ calculations, we uncover how Pr substitution modifies the low-energy electronic structure of YBCO. Contrary to the prevailing Fehrenbacher-Rice (FR) and Liechtenstein-Mazin (LM) models, the low energy electronic structure contains no signature of any $f$-electron hybridization or new states. Yet, strong electron doping is observed primarily on the antibonding Fermi surface. Meanwhile, we reveal major electronic structure modifications to Cu-derived states with increasing Pr substitution: a pronounced CuO$_2$ bilayer decoupling and an enhanced CuO chain hopping, implying indirect electron-release pathways beyond simple 4$f$ state ionization. Our results challenge the long-standing FR/LM mechanism and establish Pr substituted YBCO as a potential platform for exploring correlation-driven phenomena in coupled 1D-2D systems.

cond-mat.supr-con↗

arXiv2025

Sub-tesla on-chip nanomagnetic metamaterial platform for angle-resolved photoemission spectroscopy

Magnetically controlled states in quantum materials are central to their unique electronic and magnetic properties. However, direct momentum-resolved visualization of these states via angle-resolved photoemission spectroscopy (ARPES) has been hindered by the disruptive effect of magnetic fields on photoelectron trajectories. Here, we introduce an \textit{in-situ} method that is, in principle, capable of applying magnetic fields up to 1 T. This method uses substrates composed of nanomagnetic metamaterial arrays with alternating polarity. Such substrates can generate strong, homogeneous, and spatially confined fields applicable to samples with thicknesses up to the micron scale, enabling ARPES measurements under magnetic fields with minimal photoelectron trajectory distortion. We demonstrate this minimal distortion with ARPES data taken on monolayer graphene. Our method paves the way for probing magnetic field-dependent electronic structures and studying field-tunable quantum phases with state-of-the-art energy-momentum resolutions.

cond-mat.mes-hall↗

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↗

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

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↗

arXiv2019

Quantum oscillations in the non-centrosymmetric superconductor and topological nodal-line semimetal PbTaSe$_2$

We observed quantum oscillations in thermoelectric and magnetic torque signals in non-centrosymmetric superconductor PbTaSe$_2$. One oscillatory frequency stems from the orbits formed by magnetic breakdown, while others are from two-dimensional-like Fermi surfaces near the topological nodal rings. Our comprehensive understanding of the Fermi surface topology of PbTaSe$_2$, including nailing down the Fermi level and detecting the Berry phases near the nodal rings, is crucial for searching plausible topological superconductivity in its bulk and surface states.

cond-mat.supr-con↗