arXiv subjects

Zhuoyu Chen

Publications and source records attributed to Zhuoyu Chen.

At least 19 recordsLinked to original sources

arXiv2026

Nearly Isotropic Vortex Solid in $\mathbf{(La,Pr)_{3}Ni_{2}O_{7}}$ Thin Films

The discovery of superconductivity in bulk bilayer nickelates has established a new platform for exploring high-$T_c$ superconductivity beyond the cuprates. The role of the Ni $3d_{z^2}$-derived $γ$ band in the superconductivity of bilayer nickelates remains unresolved. By performing simultaneous resistance and diamagnetism measurements on (La,Pr)$_3$Ni$_2$O$_7$ thin films, we map the vortex melting phase diagram for both in-plane and out-of-plane magnetic fields. For $H\parallel c$, the geometric confinement effect gives rise to pancake vortices. Remarkably, the anisotropy parameter of the vortex melting field $γ_{H_m} \equiv H_m^{ab}/H_m^c$ decreases monotonically with decreasing temperature and approaches unity at low temperatures. Within the anisotropic Ginzburg--Landau scaling, $H_m^{ab}/H_m^c = \sqrt{ρ_s^{ab}/ρ_s^c}$ tracks the superfluid-density anisotropy. Such a vortex solid implies a nearly isotropic superfluid density, which is irreconcilable with the strictly two-dimensional $3d_{x^2-y^2}$-derived bands, but naturally explained by a substantial interlayer superfluid contribution from the $3d_{z^2}$-derived $γ$ band. Our results provide thermodynamic evidence for a substantial contribution of the $γ$ band to superconductivity in bilayer nickelate thin films.

cond-mat.supr-con↗

arXiv2026

Bipolar-doped superconducting infinite-layer cuprates

Distilling the intrinsic physics of the superconducting CuO2 plane from the complexities of charge-reservoir layers is a defining challenge in high-temperature superconductivity. While superconducting electron-doped infinite-layer cuprates have been synthesized, controllable and uniform hole doping has long remained elusive despite exploratory attempts, limiting spectroscopic insights. Here, we realize bipolar doping across infinite-layer (Sr,Eu)CuO2 and (Ca,Li)CuO2+δ single-crystalline thin films, mapping the electronic phase diagram. Both electron- and hole-doped films show pronounced electrical resistance anisotropy, indicating the quasi-two-dimensional nature of the CuO2 planes. Angle-resolved photoemission spectroscopy across electron- and hole-doped regimes reveals persistent antiferromagnetic band folding coexisting with superconductivity. Remarkably, at a hole doping ~0.07 determined by Luttinger volume, the antiferromagnetic folding emerges from Fermi arcs within the film's single Fermi surface, with the onset superconducting transition temperature exceeding 60 K. These findings redefine the interplay between magnetic order and superconductivity and establish a definitive platform to investigate the intrinsic mechanism of high-temperature superconducting cuprates.

cond-mat.supr-con↗

arXiv2026

Atomically resolved intrinsic superconducting gap in (La,Pr)3Ni2O7 films

Ruddlesden-Popper bilayer nickelates provide an emerging platform for studying high-temperature superconductivity, yet the superconducting pairing symmetry remains under debate. Here, we use atomic-resolution scanning tunnelling microscopy and spectroscopy to investigate superconducting 1.5-unit-cell (La,Pr)3Ni2O7 films grown on SrLaAlO4. A cryogenic ultrahigh-vacuum (UHV) sample transfer preserves an ordered sqrt(2) * sqrt(2) surface and yields reproducible U-shaped spectra with two gap scales of ~14 and ~20 meV and extended flat zero-conductance bottoms. By contrast, samples exposed for a longer time in UHV without cooling during transfer show V-shaped spectra despite retaining the surface reconstruction and a transport superconducting transition onset above 40 K. Wide-energy-range spectra indicate that oxygen loss can mix density-wave-related spectral weight. Our measurements provide an atomic-scale observation of the intrinsic nodeless superconducting gap in bilayer nickelate ultrathin films.

cond-mat.supr-con↗

arXiv2026

Field re-entrant superconductivity in Eu-doped infinite-layer nickelates

Intertwined superconducting and magnetic orders may give rise to exotic quantum phases, including field-induced and re-entrant superconductivity. However, such magnetism-enhanced superconductivity has remained elusive in superconductors with higher transition temperatures. While infinite-layer nickelates represent a new class of unconventional superconductors, the impact of rare-earth magnetism on superconducting properties remains largely unexplored. Here, we show that Eu-doped infinite-layer nickelate Sm$_{0.95-x}$Ca$_{0.05}$Eu$_x$NiO$_2$ exhibits a magnetic-field-induced re-entrant superconducting phase in the Eu-rich over-doped regime. Zero-resistance transport and high-field diamagnetic screening confirm the superconducting nature of this phase, which emerges after the initial suppression of low-field superconductivity and remains robust across a broad range of temperatures, fields and field orientations. In the same doping range, we observe nonlinear Hall transport and hysteretic magnetoresistance, indicating the unconventional nature of the re-entrant behaviour. While partially consistent with a compensation mechanism between the Eu-derived exchange field and the applied field, our data reveal pronounced deviations from this model at the highest-doping levels. Our findings establish infinite-layer nickelates as a fertile platform for exploring magnetically driven high-field superconductivity in strongly correlated oxides.

cond-mat.supr-con↗

arXiv2026

$3d_{z^2}$ orbital delocalization and magnetic collapse in superconducting (La,Pr)$_3$Ni$_2$O$_{7-δ}$ films

The recent discovery of Ruddlesden--Popper (RP) nickelate thin-film superconductors has opened a new frontier in unconventional superconductivity. Its realization requires both compressive epitaxial strain and highly oxidative growth conditions, yet the microscopic pathway from the parent phase to the superconducting phase remains elusive. Here, X-ray absorption spectra and resonant inelastic X-ray scattering are employed to track this evolution by independently tuning strain and oxygen content in (La,Pr)$_3$Ni$_2$O$_{7-δ}$ thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge in the same way upon two independent tunings: Spectral weight transfers from a ''Upper Hubbard''-like peak to the hole-like peak associated with O $2p_z$ state, and in parallel, the initially localized Ni $3d_{z^2}$ orbital becomes more itinerant followed by the broadening and weakening of $dd$ orbital excitations. Second, as itinerancy increases, long-range spin-density-wave (SDW) order is suppressed in both intensity and correlation length, indicating direct competition with superconductivity. Yet, short-range magnons persist: they become damped but their bandwidth stays unchanged. Our results paint a coherent picture that both strain and oxygenation drive the RP bilayer nickelates towards the superconducting instability, where the O $2p_z$ and Ni $3d_{z^2}$ orbitals become delocalized. Concomitantly, the long-range magnetic order loses coherence and gets suppressed. These findings establish an orbital-selective route to RP nickelate superconductivity, in which the delocalization of the $2p_z$ and $3d_{z^2}$ orbitals and the robust short-range magnons upon the melting of SDW order are prerequisites, providing strong constraints for theory and the roadmap for designing nickelate superconductors.

cond-mat.supr-con↗

arXiv2026

Electronic structures across superconductor-insulator transition in Ruddlesden-Popper bilayer nickelate films

High-transition-temperature ($T_{C}$) superconductivity is recently discovered in Ruddlesden-Popper (RP) nickelate films with extraordinarily strong oxidation. While investigating phase diagrams is essential for uncovering the superconducting mechanism, the oxygen-tuned superconductor-insulator transition (SIT) in RP nickelates differs fundamentally from that in cuprates or iron-based systems. Here, we unveil the evolution of electronic structure in RP bilayer nickelate thin films across the SIT, combining angle-resolved photoemission spectroscopy (ARPES) and X-ray absorption spectroscopy (XAS) for both occupied and unoccupied states. In the superconducting state, a coherent quasiparticle band near Fermi level ($E_{F}$) coexists with an incoherent waterfall feature at high energy, paralleling that in cuprates. Approaching the insulating state with oxygen deficiency, the spectral weight of the occupied coherent quasiparticle band is gradually suppressed, accompanied by pronounced density of states redistribution and orbital reconfiguration in unoccupied states. These results reveal the electronic origin of the SIT in the phase diagram, which transcends carrier doping effects and oxygen vacancy states. Our findings point to a decisive role of oxygen in shaping the essential electronic landscape of RP bilayer nickelates, offering crucial insights into the superconducting mechanism.

cond-mat.supr-con↗

arXiv2026

Superconductivity and Electronic Structures of Nickelate Thin Film Superstructures

Ruddlesden-Popper (RP) nickelates have emerged as a crucial platform for exploring the mechanisms of high-temperature superconductivity. However, the Fermi surface topology required for superconductivity remains elusive. Here, beyond the superconducting pure bilayer (2222) phase, we report the thin film growth and ambient-pressure superconductivity of monolayer-bilayer (1212) and bilayer-trilayer (2323) superstructures, together with the absence of superconductivity in monolayer-trilayer (1313) superstructure, under identical compressive epitaxial strain. The onset superconducting transition temperatures range from 46 to 50 K, exceeding the McMillan limit. Angle-resolved photoemission spectroscopy reveals key Fermi surface differences in these atomically-engineered structures. In superconducting 1212 and 2222 films, a dispersive hole-like band ($γ^{\mathrm{II}}$) forms an underlying Fermi pocket, surrounding the Brillouin zone corner. In contrast, the top of the flat band ($γ^{\mathrm{III}}$) is observed ~70 meV below $E_\text{F}$ in the non-superconducting 1313 films. Particularly, the superconducting 2323 films host both $γ^{\mathrm{II}}$ and $γ^{\mathrm{III}}$ bands. The polarization dependence of the $γ$ bands reveals their Ni $d_{z^2}$ origin. Our findings expand the family of ambient-pressure nickelate superconductors and establish a connection between structural configuration, electronic structure, and the emergence of superconductivity in nickelates.

cond-mat.supr-con↗

arXiv2026

Three-Dimensional Electronic Structures in Superconducting Ruddlesden-Popper Bilayer Nickelate Films

Beyond the quasi-two-dimensional (2D) paradigm of cuprates, the role of the third dimension of the Ruddlesden-Popper bilayer nickelates is essential to decoding their superconducting mechanism. Here, using angle-resolved photoemission spectroscopy (ARPES) with varied photon energies, we systematically investigate the electronic band structures in three dimensions for superconducting (La,Pr,Sm)$_3$Ni$_2$O$_7$/SrLaAlO$_4$ thin films (superconducting onset temperature $T_c^{\text{onset}} \sim 48$ K) transferred via a cryogenic ultra-high vacuum suitcase. We reveal an orbital-dependent dimensionality: while the $d{x^2-y^2}$-dominant bands exhibit a quasi-2D character, the $d{z^2}$-dominant band displays a finite $k_z$ dispersion. Finite energy gaps are identified on all observed bands across multiple high-symmetry directions. Systematic temperature-dependent analysis characterizes the superconducting nature of the gap on the $d{z^2}$-derived band, revealing a large gap $Δ\sim 18$ meV and a ratio $2Δ/k_BT_c\sim 8$ exceeding the weak-coupling BCS limit. The suppression of spectral weight near the Fermi level persists above the superconducting transition temperature. Ubiquitous waterfall-like spectral features evidence the presence of electron interactions. These results underscore the role of the $d_{z^2}$ orbital and correlations, placing constraints on theoretical models for nickelate superconductivity.

cond-mat.supr-con↗

arXiv2026

Multimodal Terahertz Spectroscopy of the Pairing Symmetry and Normal-State Pseudogap in (La,Pr)$_3$Ni$_2$O$_7$ Films

The discovery of ambient-pressure superconductivity in compressively strained (La,Pr)$_3$Ni$_2$O$_7$ thin films has intensified efforts to identify the pairing mechanism. However, the symmetry of the superconducting order parameter and the character of the normal state remain unsettled. Here we combine bulk-sensitive terahertz (THz) time-domain spectroscopy with THz third-harmonic generation to present spectroscopic insights into these issues. Linear THz spectroscopy reveals a bulk superconducting response in the (La,Pr)$_3$Ni$_2$O$_7$ films, evidenced by the suppression of low-frequency spectral weight below the onset critical temperature, $T_\mathrm{c}^{\mathrm{onset}}$. A weak coherence peak near $T_\mathrm{c}^{\mathrm{onset}}$, together with substantial residual low-frequency conductivity as $T\to 0$, is consistent with disordered $s_{\pm}$-wave pairing. In the nonlinear regime, the third-harmonic signal rises sharply on cooling through $T_\mathrm{c}^{\mathrm{onset}}$, providing an independent signature of the transition. Strikingly, the nonlinear response persists above $T_\mathrm{c}^{\mathrm{onset}}$, pointing to either disorder-enhanced nonlinearity or a distinct correlated normal state. Motivated by angle-resolved photoemission spectroscopy on similarly grown films that identifies a comparable temperature scale, we associate the anomalous normal-state terahertz nonlinearity with a pseudogap. These results establish (La,Pr)$_3$Ni$_2$O$_7$ as a bulk superconductor with $s_{\pm}$-like pairing that coexists with, and may compete with, a distinct ordered state, providing a platform for exploring unconventional superconductivity beyond cuprates and pnictides.

cond-mat.supr-con↗

arXiv2026

Pressure-enhanced superconductivity and its correlation with suppressed resistance dip in (La,Pr)3Ni2O7 films

The discovery of superconductivity with a transition temperature (Tc) exceeding 40 K in La3Ni2O7 and (La,Pr)3Ni2O7 thin films at ambient pressure provides a viable platform for the experiments that can only be conducted under ambient-pressure conditions, and for the theoretical investigations aimed at understanding the commonalities and peculiarities of the behaviors related to the superconductivity between the film and the compressed bulk systems - including the effects of oxygen vacancies and strain. Consequently, it is crucial to determine whether Tc can be further enhanced and to uncover the underlying physics that controls the Tc value in these ambient-pressure superconducting thin films. Here, we report a systematic study of hydrostatic pressure effects on the superconducting properties of (La,Pr)3Ni2O7 thin films. We find that external pressure universally enhances Tc of the film samples regardless of their initial Tc value. The onset Tc of 68.5 K at 2.0 GPa demonstrates a notable increase from 62 K at 0.3 GPa. Furthermore, we observe that the samples without zero resistance show a resistance dip just above the superconducting transition, whereas the samples that exhibit zero resistance do not display this dip. Applying pressure can suppress the dips and drive the system toward zero resistance. Based on our results, we propose that this feature is associated with oxygen vacancies and that the depth of the dip can serve as an indicator of the concentration of the vacancies. It is plausible that the dip is caused by the localization of mobile electrons at the vacancy sites. Applying pressure can delocalize these electrons, which in turn may contribute to the increase in Tc.

cond-mat.supr-con↗

arXiv2026

Superconductivity onset above 60 K in ambient-pressure nickelate films

Ambient-pressure superconductivity in nickelates has been capped at an onset transition temperature ($T_{c}^{onset}$) of ~50 K, a value that remains lower than the cuprate (~133 K) and iron-based (~55 K) counterparts, despite the promise shown under high pressure. Here, we report ambient-pressure superconductivity onset at ~63 K in epitaxial (La,Pr)3Ni2O7 thin films grown under compressive strain on SrLaAlO4 substrates. This $T_{c}$ leap is enabled by pushing our gigantic-oxidative atomic-layer-by-layer epitaxy (GAE) method into an extreme non-equilibrium growth regime. It simultaneously enhances kinetics via higher temperatures and achieves full oxygenation in situ without post-annealing. Synchrotron X-ray diffraction and scanning transmission electron microscopy confirm that this approach yields films of large-scale crystalline purity, overcoming the inherent metastability of the strained superconducting phase. Transport measurements reveal a zero-resistance temperature ($T_{c}^{zero}$) reaching ~37 K, while mutual inductance measurements demonstrate a robust diamagnetic transition starting at ~23 K. These films exhibit a systematic evolution in their normal-state resistivity-temperature curve: the power-law exponent $α$ evolves from Fermi-liquid-like ($α$ ~2) at lower $T_{c}^{onset}$ to strange-metal-like ($α$ ~1) in higher $T_{c}^{onset}$ samples, directly linking the enhanced superconductivity to non-Fermi liquid behavior. Mapping the vortex melting phase diagram by the mutual inductance technique further reveals 2D melting limit suppressed to near zero, which demonstrates significantly stronger interlayer coupling than that of cuprates. These results identify the nickelates as an ambient-pressure strange-metal high-temperature superconductors with strong interlayer coupling.

cond-mat.supr-con↗

arXiv2026

Time-reversal symmetry breaking superconductivity with electronic glass in nickelate (La, Pr, Sm)3Ni2O7 films

The discovery of Ruddlesden-Popper (R-P) nickelate superconductors under high pressure heralds a new chapter of high-transition temperature (high-Tc) superconductivity. Recently, ambient-pressure superconductivity is achieved in R-P bilayer nickelate thin films through epitaxial compressive strain, unlocking the potential for understanding the nature of the unconventional superconductivity. Here, through electrical transport study, we report the discovery of time-reversal symmetry (TRS) breaking superconductivity with electronic glass in bilayer nickelate (La, Pr, Sm)3Ni2O7 films. It emerges in the lower-temperature regime of superconducting transition to the zero-resistance state, and is captured by three remarkable characteristics: 1. Unconventional magnetoresistance hysteresis, the direct evidence of TRS breaking, which is robust under different magnetic field orientations and differs fundamentally from trapped vortices or long-range-ordered magnetism. Successive oxygen reductions simultaneously weaken both the superconductivity and hysteresis, revealing their mutual connections to selective electronic orbitals. 2. Magnetic field history-dependence and zero-field non-reciprocity in the current-voltage responses, further substantiating the intrinsic and spontaneous TRS breaking. 3. Logarithmically slow resistance relaxations upon the removal of magnetic field, the hallmarks of glassy dynamics. Distinguished by the striking magnetic field history- and time-dependent properties, our findings uncover an unprecedented superconducting state in the nickelate superconductors, providing phenomenological and conceptual advances for future research on high-Tc superconductivity.

cond-mat.supr-con↗

arXiv2026

Preparation and optimization of high-temperature superconducting Ruddlesden-Popper nickelate thin films

The discovery of ambient-pressure nickelate high-temperature superconductivity provides a new platform for probing the underlying superconducting mechanisms. However, the thermodynamic metastability of Ruddlesden-Popper nickelates Lnn+1NinO3n+1 (Ln = lanthanide) presents significant challenges in achieving precise control over their structure and oxygen stoichiometry. This study establishes a systematic approach for growing phase-pure, high-quality Ln3Ni2O7 thin films on LaAlO3 and SrLaAlO4 substrates using gigantic-oxidative atomic-layer-by-layer epitaxy. The films grown under an ultrastrong oxidizing ozone atmosphere are superconducting without further post annealing. Specifically, the optimal Ln3Ni2O7/SrLaAlO4 superconducting film exhibits an onset transition temperature (Tc,onset) of 50 K. Four critical factors governing the crystalline quality and superconducting properties of Ln3Ni2O7 films are identified: 1) precise cation stoichiometric control suppresses secondary phase formation; 2) complete atomic layer-by-layer coverage coupled with 3) optimized interface reconstruction minimizes stacking faults; 4) accurate oxygen content regulation is essential for achieving a single superconducting transition and high Tc,onset. These findings provide valuable insights for the layer-by-layer epitaxy growth of diverse oxide high-temperature superconducting films.

cond-mat.supr-con↗

arXiv2026

Non-equilibrium transport reveals energy level degeneracy

We demonstrate a method to determine energy level degeneracies using non-equilibrium electronic transport through voltage-biased quantum dots. We establish the general validity of this approach using single and double quantum dots in bilayer graphene and GaAs. Unlike established methods based on entropy measurements or time-resolved tunneling statistics, our approach achieves comparable precision without requiring calibrated electron heating or real-time charge detection. We resolve the predicted symmetric shell structure in bilayer graphene quantum dots, including a singlet ground state at half filling and the ground state degeneracies of the first 13 carriers. Extending the method to double quantum dots, we observe degeneracy doubling associated with bonding and antibonding orbitals for a single carrier and a fourfold degeneracy for two carriers, previously inaccessible with existing techniques. These results establish a conceptually general and experimentally straightforward approach for probing energy level degeneracies in complex quantum systems.

cond-mat.mes-hall↗

arXiv2026

Bosonic phases across the superconductor-insulator transition in infinite-layer samarium nickelate

Superconductivity arises from the global phase coherence of Cooper pairs. Modulation of phase coherence leads to quantum phase transitions, serving as an important tool for studying unconventional superconductivity. Here, we demonstrate bosonic phases across the superconductor-insulator transition in infinite-layer nickelate superconducting films by the control of spatially periodic network patterns. Magnetoresistance oscillations with a periodicity of h/2e provide direct evidence of 2e Cooper pairing in nickelates. The phase transition is predominantly driven by enhanced superconducting fluctuations, and Cooper pairs are involved in charge transport across the transition. Notably, we observe two types of anomalous metallic phases, emerging respectively at finite magnetic fields and down to zero magnetic field. They can be characterized by bosonic excitations, suggesting the dynamic roles of vortices in the ground states. Our work establishes nickelates as a key platform for investigating the rich landscape of bosonic phases controlled via the phase coherence of Cooper pairs.

cond-mat.supr-con↗

arXiv2026

Superconductor-insulator transitions in infinite-layer nickelates controlled via ${operando}$ monitored reduction

Nickelates represent an emerging class of superconductors that demand innovative approaches for structural and electronic phase modulations. Continuous control over superconductor-insulator transition (SIT) in nickelates remains particularly challenging, hindering both fundamental understanding and potential applications. Here, we demonstrate SIT in infinite-layer nickelate superconductors utilizing multiple techniques, including an ${operando}$ monitored reduction (OMR) method. OMR enables ultrawide-range continuous modulation of the Ni 3${d}$ orbital electron occupancy from ~3${d}^7$ to ~3${d}^9$. The 3${d}$ occupancy is calibrated through systematic synchrotron X-ray absorption (XAS), combined with scanning transmission electron microscopy (STEM) annular bright field (ABF) analysis of oxygen atoms. SIT is further modulated via ionic liquid gating and magnetic field. Strikingly different from cuprates, our Nernst effect measurements show that pairing initiates at the onset of the resistive drop. The subsequent emergence of the Meissner effect at zero resistance marks the establishment of global phase coherence. Angle-dependent magnetotransport within the transition temperature regime indicates a mixture of two-dimensional (2D) and three-dimensional (3D) superconducting characters, suggesting the observed SIT deviates from the canonical 2D model. Our results provide a unique perspective on the interplay of structural and electronic phase transitions in the infinite-layer nickelates across the oxygen content-magnetic field-temperature parameter space.

cond-mat.supr-con↗

arXiv2025

Enhanced Superconductivity and Mixed-dimensional Behaviour in Infinite-layer Samarium Nickelate Thin Films

Rare-earth infinite-layer nickelates represent an emerging class of unconventional superconductors, with materials synthesis largely limited to early lanthanide compounds. Here, we report the synthesis and characterization of phase-pure superconducting samarium-based infinite-layer nickelate thin films, including the first demonstration of Sm$_{1-x}$Sr$_x$NiO$_2$, along with co-doped variants incorporating europium and calcium. These films, grown on LSAT (001) substrates, exhibit coherent lattice structures up to $\sim$ 9 nm thickness with minimal stacking faults. The co-doped compounds achieve a record-small $c$-axis parameter of 3.26 Å and display remarkable superconducting transition temperatures up to 32.5 K. These results establish a clear correlation between decreasing $c$-axis parameter and increasing critical temperature across different rare-earth systems. In addition, angle-dependent magnetoresistance investigations reveal the existence of a hybrid mixture of 2D and 3D superconductivity in this novel system with enhanced coupling between the rare-earth 5d and Ni 3d orbitals, confirmed by resonant inelastic X-ray scattering experiments. As the concentration of Eu increases, the system exhibits a clear tendency towards 3D superconductivity. Furthermore, we observe distinctive negative magnetoresistance in the europium-containing samples. These findings advocate clear materials design principles for higher transition temperatures and exotic physics in infinite-layer nickelate superconductors through structural engineering of the rare-earth site.

cond-mat.supr-con↗

arXiv2025

Orbital-selective charge transfer drives two-step negative thermal expansion structural transitions in PbTa2Se4

The negative thermal expansion (NTE) effect has been found generally combined with structural phase transitions. However, the charge and orbital freedoms of the NTE has not been well studied. This study employs angle-resolved photoemission spectroscopy and first-principles calculations to elucidate the charge and orbital kinetics of the anomalous two-step negative thermal expansion structural phase transitions in PbTa2Se4. As the temperature decreases, each transition undergoes a similar block-layer sliding, although the charge transfer behaviors differ significantly. During the first transition, charge is mainly transferred from the Pb 6pz orbital to an M-shaped band below the Fermi level, barely altering the Fermi surface. In contrast, the second transition involves modifications to both the Fermi surface and charge-transfer orbitals, with charge selectively transferred from Pb 6px/py orbitals to Ta 5dz2 orbitals and a decrease of the Fermi pockets formed by Pb 6px/py orbitals. Furthermore, a small pressure can easily tune the base structure phase among the three phases and the corresponding superconductivity. Therefore, our findings reveal that the orbital-selective charge transfer drives the unusual structure transition in PbTa2Se4, offering new insights into the NTE mechanisms and providing a unique window to study the pressure-tuned superconductivity in this metal-intercalated transition chalcogenides.

cond-mat.mtrl-sci↗