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Zhihai Zhu

Publications and source records attributed to Zhihai Zhu.

At least 19 recordsLinked to original sources

Anisotropic Surface State Band Splitting and Low Energy Flat Bands in 3d Correlated Topological Kondo Insulator Candidate FeSb$_2$

FeSb$_2$ is a correlated narrow-gap semiconductor that has often been discussed as a $3d$-electron Kondo insulator candidate and exhibits a low-temperature resistance plateau with possible surface-dominated conduction. We carried out a systematic high-resolution laser-based angle-resolved photoemission spectroscopy (ARPES) study of FeSb$_2$ to investigate its electronic structure. The surface states around the zone center show clear anisotropic splitting. When the temperature is lowered into the resistance plateau regime ($<6\,\mathrm{K}$), the surface states remain robust, but their photoemission peaks become much sharper and gain spectral weight. Two distinct flat-band-like features are observed at low energy. One is located at $\sim$127 meV below the Fermi level, which exists only along a specific high-symmetry direction, while the other is located at $\sim$70 meV below the Fermi level and is present along all the measured momentum cuts around the zone center. These results provide new information to understand the renormalization effects, the resistance plateau, and the topological nature of FeSb$_2$.

cond-mat.str-el↗

Granular Superconductivity in La$_{2}$PrNi$_{2}$O$_{7-δ}$ Thin Films

Superconductivity realized in bilayer nickelate thin films enables direct spectroscopic and transport studies at ambient pressure. However, a persistent two-step resistive transition remains a major barrier to achieving optimal superconducting properties. Here, we show that the two-step transition in La$_2$PrNi$_2$O$_{7-δ}$ thin films originates from the granular nature of superconductivity, specifically, the coexistence of two distinct superconducting grain phases coupled by a Josephson junction network. A secondary, lower-temperature transition appears in the $R(T)$ curve, even when residual resistance becomes vanishingly small near 30 K. This two-step behavior significantly lowers the zero-resistance transition temperature, $T_{c, zero}$$\approx$ 10 K, and limits advanced spectroscopic studies. Our findings reveal the microscopic mechanism underlying the two-step transition in thin films and underscore the need for improved oxygen homogeneity to achieve bulk superconductivity in this system.

cond-mat.supr-con↗

Mott-Derived Local Moments and Kondo Hybridization in a d-electron Kagome lattice

Unlike canonical Kondo lattices in f-electron systems, where localized f orbitalsnaturally provide local moments, d-electron Kondo lattices require a distinct mechanism for local-moment formation. However, the study of d-electron Kondo lattices in bulk materials remains far from settled, particularly with regard to the microscopic origin of the local moments. Here, we report a microscopic mechanism for this process in the bilayer kagome metal CsCr6Sb6, where strong correlations drive a Mott splitting of the kagome flat band to supply the requisite local moments. By combining STM/STS and ARPES, we resolve a spectroscopic hierarchy between high-energy correlation effects and low temperature hybridization. Low-temperature STS reveals a robust asymmetric suppression of the density of states near EF that is well captured phenomenologically by a Fano-type lineshape, while ARPES detects a sharp quasiparticlepeak near EF. These low-energy signatures evolveon the same temperature scale and disappear upon warming, consistent with the onset of Kondo hybridization. At the same time, STS resolves symmetric humps at approximately +-50 mV and ARPES identifies a weakly dispersive feature around 50 meV below EF; unlike the near-EF hybridization signatures, these features persist to substantially higher temperatures. This separation of energy and temperature scales supports a two-stage picture in which a kagome flat band first undergoes correlation-driven splitting into lower and upper Hubbard bands, and the occupied lower Hubbard band supplies the local moments that later hybridize with itinerant electrons at lower temperature. Our results therefore move beyond the phenomenology of a kagome Kondo lattice candidate and instead provide a microscopic spectroscopic picture linking Mottness to Kondo hybridization in a frustrated d-electron system.

cond-mat.str-el↗

Expansion of Momentum Space and Full 2$π$ Solid Angle Photoelectron Collection in Laser-Based Angle-Resolved Photoemission Spectroscopy by Applying Sample Bias

Angle-resolved photoemission spectroscopy (ARPES) directly probes the energy and momentum of electrons in quantum materials, but conventional setups capture only a small fraction of the full 2$π$ solid angle. This limitation is acute in laser-based ARPES, where the low photon energy restricts momentum space despite ultrahigh resolution. Here we present systematic studies of bias ARPES, where applying a sample bias expands the accessible momentum range and enables full 2$π$ solid angle collection in two dimension using our 6.994 eV laser source. An analytical conversion relation is established and validated to accurately map the detector angle to the emission angle and the electron momentum in two dimensions. A precise approach is developed to determine the sample work function which is critical in the angle-momentum conversion of the bias ARPES experiments. Energy and angular resolutions are preserved under biases up to 100 V, and minimizing beam size is shown to be crucial. The technique is effective both near normal and off-normal geometries, allowing flexible Brillouin zone access with lower biases. Bias ARPES thus elevates laser ARPES to a new level, extending momentum coverage while retaining high resolution, and is applicable across a broad photon-energy range.

cond-mat.supr-con↗

Electronic Structure and Superconducting Gap of HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$ Revealed by Laser-Based Angle-Resolved Photoemission Spectroscopy

The spatially-resolved laser-based high resolution angle resolved photoemission spectroscopy (ARPES) measurements have been performed on the optimally-doped HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$ (Hg1223) superconductor with a $T_c$ at 133 K. Two distinct regions are identified on the cleaved surface: the single Fermi surface region where only one Fermi surface is observed, and the double Fermi surface region where two Fermi surface sheets are resolved coming from both the inner (IP) and outer (OP) CuO$_2$ planes. The electronic structure and superconducting gap are measured on both of these two regions. In both cases, the observed electronic states are mainly concentrated near the nodal region. The momentum dependence of superconducting gap deviates from the standard d-wave form. These results indicate that the surface electronic structure of Hg1223 behaves more like that of underdoped cuprates.

cond-mat.supr-con↗

Electronic Origin of Density Wave Orders in a Trilayer Nickelate

The discovery of superconductivity in Ruddlesden-Popper nickelates has established a new frontier in the study of high-temperature superconductors. However, the underlying pairing mechanism and its relationship to the material's electronic and magnetic ground states remain elusive. Since unconventional superconductivity often emerges from a complex interplay of magnetic correlations, elucidating the magnetic ground state of the nickelates at ambient pressure is crucial for understanding the emergence of superconductivity under high pressure. Here, we combine high-resolution angle-resolved photoemission spectroscopy with tight-binding model simulation to investigate the electronic structure of the representative trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$. We provide the first experimental evidence of band splitting induced by interlayer coupling and further resolve the momentum-dependent density wave gap structures along all the Fermi surfaces. Our findings identify the mirror-selective Fermi surface nesting as the origin of the interlayer antiferromagnetic spin density wave and demonstrate the dominant role of Ni-3d$_{z^2}$ orbitals in the low-energy physics of La$_4$Ni$_3$O$_{10}$. These results provide a fundamental framework for understanding the magnetic interactions and high-temperature superconductivity mechanism in the Ruddlesden-Popper nickelate family.

cond-mat.supr-con↗

Stabilizing and Tuning Superconductivity in La$_3$Ni$_2$O$_{7-δ}$ Films: Oxygen Recycling Protocol Reveals Hole-Doping Analogue

The recent achievement of superconductivity in La$_3$Ni$_2$O$_{7-δ}$ with transition temperatures exceeding 40 K in thin films under compressive strain and 80 K in bulk crystals under high pressure opens new avenues for research on high-temperature superconductivity. The realization of superconductivity in thin films requires delicate control of growth conditions, which presents significant challenges in the synthesis process. Furthermore, the stability of superconducting La$_3$Ni$_2$O$_{7-δ}$ films is compromised by oxygen loss, which complicates their characterization. We introduce an effective recycling protocol that involves oxygen removal in a precursor phase followed by ozone-assisted annealing, which restores superconducting properties. By tuning the oxygen content, we construct an electronic phase diagram that highlights oxygen addition as a potential analogue to hole doping via La substitution with Sr, providing insights into the doping mechanism and guiding future material optimization.

cond-mat.supr-con↗

Impact of Electron Correlations on Infinite-Layer Cuprates and Nickelates

Optimization of unconventional superconductivity involves a balance of interaction strengths. Precise determination of correlation strength across different material families is therefore important. Here, we present a combined X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) study of infinite-layer PrNiO$_2$ and SrCuO$_2$ that enables fair comparison of their interaction strengths. For both compounds, we study the orbital and magnetic excitations and extract their dispersions along high-symmetry directions. Using a single-band Hubbard model and including higher-order exchange interactions, we derive the correlation factor $U/t$ for both compounds. A key finding is that despite a smaller Coulomb repulsion $U$, PrNiO$_2$ exhibits a correlation strength that is 20% stronger than that of its isostructural cuprate counterpart SrCuO$_2$. This indicates that a moderation of the correlation strength may further optimize superconductivity in nickelates.

cond-mat.supr-con↗

Persistent paramagnons in high-temperature infinite-layer nickelate superconductors

The recent discovery of high-temperature superconductivity in hole-doped SmNiO$_2$, exhibiting the record-high transition temperature $T_c$ among infinite-layer (IL) nickelates, has opened a new avenue for exploring design principles of superconductivity. Experimentally determining the electronic structure and magnetic interactions in this new system is crucial to elucidating the mechanism behind the enhanced superconductivity. Here, we report a Ni $L$-edge resonant inelastic x-ray scattering (RIXS) study of superconducting Sm-based IL nickelate thin films Sm$_{1-x-y-z}$Eu$_x$Ca$_y$Sr$_z$NiO$_2$ (SECS). Dispersive paramagnonic excitations are observed in both optimally and overdoped SECS samples, supporting a spin-fluctuation-mediated pairing scenario. However, despite the two-fold enhancement of $T_c$ in the Sm-based nickelates compared to their Pr-based counterparts, the effective exchange coupling strength is reduced by approximately $20\%$. This behavior contrasts with hole-doped cuprates, where magnetic interactions correlate positively with $T_c$, highlighting essential differences in their superconducting mechanisms.

cond-mat.supr-con↗

Resolving the Electronic Ground State of La3Ni2O7-δ Films

The recent discovery of a superconductivity signature in La3Ni2O7-δ under a pressure of 14 GPa, with a superconducting transition temperature of around 80 K, has attracted considerable attention. An important aspect of investigating electronic structures is discerning the extent to which the electronic ground state of La3Ni2O7-δ resembles the parent state of the cuprate superconductor, a charge transfer insulator with long-range antiferromagnetism. Through X-ray absorption spectroscopy, we have uncovered the crucial influence of oxygen ligands on the electronic ground states of the Ni ions, displaying a charge transfer nature akin to cuprate but with distinct orbital configurations. Both in-plane and out-of-plane Zhang-Rice singlets associated with Ni d_(x^2-y^2 ) and d_(z^2) orbitals are identified, together with a strong interlayer coupling through inner apical oxygen. Additionally, in La3Ni2O7-δ films, we have detected a superlattice reflection (1/4, 1/4, L) at the Ni L absorption edge using resonant X-ray scattering measurements. Further examination of the resonance profile indicates that the reflection originates from the Ni d orbitals. By evaluating the reflection's azimuthal angle dependence, we have confirmed the presence of collinear antiferromagnetic spin ordering and charge-like anisotropy ordered with the same periodicity. Notably, our findings reveal a microscopic relationship between these two components in the temperature dependence of the scattering intensity of the reflection. This investigation enriches our understanding of high-temperature superconductivity in La3Ni2O7-δ under high pressure.

cond-mat.supr-con↗

Two Distinct Charge Orders in Infinite-layer PrNiO2+δ revealed by Resonant X-ray Diffraction

A broken translation symmetry has recently been revealed in infinite-layer nickelates, which has piqued considerable interest in its origin and relation to superconductivity, as well as in its comparison to charge order in cuprates. Here, by performing resonant x-ray scattering measurements in thin films of infinite-layer PrNiO2+δ, we find that the superlattice reflection at the Ni L3 absorption edge differs considerably from that at the Pr M5 resonance in their dependence on energy, temperature, and local symmetry, indicating they are two distinct charge orders despite the same in-plane wavevectors. These dissimilarities might be related to the excess oxygen dopants, considering that the resonant reflections were observed in an incompletely reduced PrNiO2+δ film. In addition, our azimuthal analysis suggests that the oxygen ligands should play a pivotal role in the charge modulation revealed at the Ni L3 resonance.

cond-mat.supr-con↗

Spin fluctuations sufficient to mediate superconductivity in nickelates

Infinite-layer nickelates show high-temperature superconductivity, and the experimental phase diagram agrees well with the one simulated within the dynamical vertex approximation (D$Γ$A). Here, we compare the spin-fluctuation spectrum behind these calculations to resonant inelastic X-ray scattering experiments. The overall agreement is good. This independent cross-validation of the strength of spin fluctuations strongly supports the scenario, advanced by D$Γ$A, that spin-fluctuations are the mediator of the superconductivity observed in nickelates.

cond-mat.supr-con↗

ARPES Detection of Superconducting Gap Sign in Unconventional Superconductors

Superconductivity is realized by opening a gap in the superconducting state. The gap symmetry is crucial in understanding the underlying superconductivity mechanism. The magnitude and the phase are essential in fully characterizing the superconducting gap. Angle-resolved photoemission spectroscopy (ARPES) has played a key role in determining the gap symmetry in unconventional superconductors. However, it has been considered so far that ARPES can only measure the magnitude of the superconducting gap but not its phase; the phase has to be detected by other phase-sensitive techniques. Here we propose a new method to directly detect the superconducting gap sign by using ARPES. This method is successfully validated in a cuprate superconductor with a well-known $d$-wave gap symmetry. When two bands are nearby in momentum space and have a strong interband interaction, the resulted electronic structures in the superconducting state are sensitive to the relative gap sign between the two bands which can be captured by ARPES measurements. Our present work provides a new way to detect the gap sign and can be applied to various superconductors, particularly those with multiple orbitals like the iron-based superconductors. It also makes ARPES more powerful to determine both the gap magnitude and the phase that are significant in understanding the superconductivity mechanism of unconventional superconductors.

cond-mat.supr-con↗

Magnetic Excitations in Strained Infinite-layer Nickelate PrNiO2

Strongly correlated materials often respond sensitively to the external perturbations. In the recently discovered superconducting infinite-layer nickelates, the superconducting transition temperature can be dramatically enhanced via only ~1% compressive strain-tuning enabled by substrate design. However, the root of such enhancement remains elusive. While the superconducting pairing mechanism is still not settled, magnetic Cooper pairing - similar to the cuprates has been proposed. Using resonant inelastic x-ray scattering, we investigate the magnetic excitations in infinite-layer PrNiO2 thin films for different strain conditions. The magnon bandwidth of PrNiO2 shows only marginal response to strain-tuning, in sharp contrast to the striking enhancement of the superconducting transition temperature Tc in the doped superconducting samples. These results suggest the enhancement of Tc is not mediated by spin excitations and thus provide important empirics for the understanding of superconductivity in infinite-layer nickelates.

cond-mat.supr-con↗

Strain-induced enhancement of $T_c$ in infinite-layer Pr$_{0.8}$Sr$_{0.2}$NiO$_2$ films

The mechanism of unconventional superconductivity in correlated materials remains a great challenge in condensed matter physics. The recent discovery of superconductivity in infinite-layer nickelates, as analog to high-Tc cuprates, has opened a new route to tackle this challenge. By growing 8 nm Pr0.8Sr0.2NiO2 films on the (LaAlO3)0.3(Sr2AlTaO6)0.7 substrate, we successfully raise the transition temperature Tc from 9 K in the widely studied SrTiO3-substrated nickelates into 15 K. By combining x-ray absorption spectroscopy with the first-principles and many-body simulations, we find a positive correlation between Tc and the pre-edge peak intensity, which can be attributed to the hybridization between Ni and O orbitals induced by the strain. Our result suggests that structural engineering can further enhance unconventional superconductivity, and the charge-transfer property plays a crucial role in the pairing strength.

cond-mat.supr-con↗

Electronic Nature of Charge Density Wave and Electron-Phonon Coupling in Kagome Superconductor KV$_3$Sb$_5$

The Kagome superconductors AV3Sb5 (A=K, Rb, Cs) have received enormous attention due to their nontrivial topological electronic structure, anomalous physical properties and superconductivity. Unconventional charge density wave (CDW) has been detected in AV3Sb5. High-precision electronic structure determination is essential to understand its origin. Here we unveil electronic nature of the CDW phase in our high-resolution angle-resolved photoemission measurements on KV3Sb5. We have observed CDW-induced Fermi surface reconstruction and the associated band folding. The CDW-induced band splitting and the associated gap opening have been revealed at the boundary of the pristine and reconstructed Brillouin zones. The Fermi surface- and momentum-dependent CDW gap is measured and the strongly anisotropic CDW gap is observed for all the V-derived Fermi surface. In particular, we have observed signatures of the electron-phonon coupling in KV3Sb5. These results provide key insights in understanding the nature of the CDW state and its interplay with superconductivity in AV3Sb5 superconductors.

cond-mat.supr-con↗

Ultrafast signatures of spin and orbital order in antiferromagnetic $α$-Sr$_2$CrO$_4$

We used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in the antiferromagnetic Mott insulator $α$-Sr$_2$CrO$_4$. This chromate system possesses multiple spin and orbital ordered phases, and therefore could enable us to study the unique interplay between these collective phases through their non-equilibrium response to photoexcitation. Here, by varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr $t_{2g}$ orbitals and charge transfer-type transitions between oxygen 2$p$ and Cr $e_{g}$ orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the N${\textrm{é}}$el temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in $α$-Sr$_2$CrO$_4$ and provide experimental evidence for the phase transition at $T_\textrm{O}$, possibly related to antiferro-type orbital ordering.

cond-mat.str-el↗

Electronic Structure Examination on the Topological Properties of CaMnSb$_{2}$ by Angle-Resolved Photoemission Spectroscopy

We have carried out detailed high resolution ARPES measurements and band structure calculations to study the electronic structure of CaMnSb$_{2}$. The observed Fermi surface mainly consists of one hole pocket around $Γ$ point and one tiny hole pocket at Y point. Strong spectral weight accumulation along the $Γ$-X direction is observed on the hole-like Fermi surface around $Γ$ point, suggesting strong anisotropy of the density of states along the Fermi surface. The tiny hole pocket at Y point originates from an anisotropic Dirac-like band with the crossing point of the linear bands lying $\sim$ 10 meV above the Fermi level. These observations are in a good agreement with the band structure calculations. In addition, we observe additional features along the $Γ$-Y line that cannot be accounted for by the band structure calculations. Our results provide important information in understanding and exploration of novel properties in CaMnSb$_{2}$ and related materials.

cond-mat.mtrl-sci↗