arXiv subjects

Mengwu Huo

Publications and source records attributed to Mengwu Huo.

At least 19 recordsLinked to original sources

arXiv2026

Unconventional Pressure Evolution of Spin-Density-Wave State in La$_{3}$Ni$_{2}$O$_{7}$

The discovery of pressure-induced high temperature superconductivity in the bilayer nickelate La$_{3}$Ni$_{2}$O$_{7}$ has raised the question of how its spin-density-wave (SDW) state evolves toward the superconducting regime. Here, we report a systematic electronic Raman study of La$_{3}$Ni$_{2}$O$_{7}$ single crystals under hydrostatic pressures up to 16.51 GPa. Both the SDW gap energy and the transition temperature $T_{\mathrm{SDW}}$ show an overall increase with pressure, while the dimensionless coupling ratio 2$\Delta_{\text{SDW}}/(k_{\text{B}}T_{\text{SDW}})$ remains constant around $\sim7.5$, indicating a robust strong-coupling character of SDW state. At the same time, the Raman SDW peak broadens as pressure is applied, indicating a gradual weakening of long-range SDW order. These results reveal an unusual pressure evolution in which the SDW energy scale is enhanced while the SDW state becomes progressively less coherent, providing spectroscopic constraints on the magnetic correlations relevant to superconductivity in bilayer nickelates.

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arXiv2026

Regulating oxygen content and superconductivity in La$_3$Ni$_2$O$_{7+\delta}$

The synthesis of high-quality Ruddlesden-Popper (RP) nickelates remains challenging due to variations in oxygen content and the prevalence of intergrown RP phases. Precisely controlling the stoichiometry and characterizing the resulting physical properties are essential for understanding the mechanism of high-$T_c$ superconductivity in these materials. In this work, we synthesize a series of La$_3$Ni$_2$O$_{7+\delta}$ samples with systematically controlled oxygen content and perform comprehensive structural and compositional analyses. Precise oxygen tuning enables us to tailor the microstructure, yielding a pure bilayer phase, a mixture of bilayer and hybrid single-layer-bilayer phases, and a predominantly bilayer phase containing trilayer intergrowths. High-pressure transport measurements reveal distinct superconducting transitions with contrasting $T_c$ values, corresponding to the bilayer phase, the hybrid phase, and trilayer inclusions. Notably, we find that oxygen content not only governs the phase purity$-$i.e., the presence of intergrowth phases$-$but also directly modulates the upper critical field ($H_{c2}$) of the bilayer superconductivity. By establishing a phase diagram of $T_c$ and $H_{c2}$ as functions of oxygen content in La$_3$Ni$_2$O$_{7+\delta}$, this work advances synthetic control and provides new insights into the superconducting mechanism of RP nickelates.

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arXiv2026

High-energy electronic excitations in La3Ni2O7 by time-resolved optical spectroscopy

Recently, high-temperature superconductivity has been established in bilayer La3Ni2O7, which exhibits a density-wave (DW) transition at ~ 150 K under ambient pressure. The DW order is believed to be linked to superconductivity, as it is suppressed upon the emergence of superconductivity at high pressures. Here, we explore the ultrafast dynamics of high-energy electronic excitations from 10 K to room temperature under ambient pressure using time-resolved optical spectroscopy. Two high-energy electronic excitations at ~1.8 and ~ 2.4 eV, arising from distinct interband transitions, are identified. They exhibit different DW gaps of approximately 54 and 67 meV, respectively, along with relaxation dynamics that can be well described by the Rothwarf-Taylor model. In addition, we observe four coherent Raman-active phonon modes that exhibit distinct coupling with different electronic excitations. The phonon softening with increasing temperature can be well described between ~100 K and room temperature by a semi-quantitative model, which includes thermal expansion and anharmonic phonon-phonon coupling. At cryogenic temperatures, deviations from the measured temperature-dependent phonon frequencies and the model fits suggest an additional contribution from electron-phonon coupling. Our study provides direct evidence of the complex gap structure and phonon dynamics in this material, offering critical insights into the DW mechanism and many-body effects.

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arXiv2026

Anisotropic Electronic Correlations in the Spin Density Wave State of La$_3$Ni$_2$O$_7$

The bilayer nickelate superconductor La$_3$Ni$_2$O$_7$ undergoes a density wave transition near 150 K that has attracted intensive scrutiny, yet its microscopic origin remains elusive. Here we report polarization-resolved electronic Raman scattering measurements on high-quality single crystals of La$_3$Ni$_2$O$_7$. Below 150\,K, we observe a pronounced, symmetry-dependent redistribution of spectral weight in B$_{1g}$ and B$_{2g}$ channels, consistent with the formation of spin-density-wave (SDW) gaps. Quantitative analysis reveals momentum-selective SDW gap amplitudes, with intermediate-to-strong coupling near X/Y points of the Brillouin zone and weaker coupling along the diagonal direction, indicating an unconventional SDW driven by anisotropic electronic correlations. Our results establish the electronic character of the SDW in La$_3$Ni$_2$O$_7$, and provide a microscopic foundation for understanding the emergence of high-temperature superconductivity under pressure in nickelates.

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arXiv2026

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.

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arXiv2025

Identifying the structure of La3Ni2O7 in the pressurized superconducting state

The crystal structure of La3Ni2O7 in its high-pressure superconducting state has been the subject of intense debate, with conflicting reports proposing orthorhombic (Amam or Fmmm) and tetragonal (I4/mmm) symmetries. Here, using high-pressure Raman spectroscopy down to 3 K, we resolve this controversy by tracking the structural evolution of La3Ni2O7 up to 32.7 GPa. Leveraging rigorous symmetry-based selection rules, we identify a single structural transition from the orthorhombic Amam phase to the Fmmm phase at ~14.5 GPa, signaled by a profound phonon renormalization. Crucially, the persistence of D2h symmetry across the transition rules out the tetragonal I4/mmm phase in the superconducting state in our measurements. The emergence of bulk superconductivity coincides precisely with this transition. Our results establish the orthorhombic Fmmm structure as the intrinsic host of superconductivity in La3Ni2O7 below 19.45 GPa, resolving a central structural controversy and providing a critical foundation for understanding the superconducting mechanism in bilayer nickelates.

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arXiv2025

Evolution of the superconductivity in pressurized La3-xSmxNi2O7

Motivated by the discovery of superconductivity in bilayer La$_3$Ni$_2$O$_7$ at 80 K and the increased superconducting transition temperature, $T_\text{c}$, up to 92 K in single crystals of La$_2$SmNi$_2$O$_7$ under pressure, we systematically study the effect of Sm doping on the superconductivity and structure of La$_{3-x}$Sm$_x$Ni$_2$O$_7$ (0 $\leq$ x $\leq$ 1.5) under pressure. Experimental investigations in polycrystalline samples reveal that Sm doping monotonically decreases the lattice constants $c$ and $a$, thereby enhancing crystal structure distortion and leading to an evolution of the metallic ground state in La$_3$Ni$_2$O$_7$ to an insulating state in La$_{1.5}$Sm$_{1.5}$Ni$_2$O$_7$. The maximum onset $T_\text{c}$ in compounds $x=0.9$ and 1.5 is 89 K, while the pressure that drives the emergence of superconductivity is higher for higher doping levels. The results suggest that the enhancement of $T_\text{c}$ in La$_{3-x}$Sm$_x$Ni$_2$O$_7$ is mainly affected by the compressed $c$ lattice before saturation, and the structure transition is critical for the emergence of superconductivity. Our experimental results provide insight into the influence of elemental substitution on nickelate superconductors, offering a means to increase the transition temperature further.

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arXiv2025

Interlayer coupling enhanced superconductivity near 100 K in La$_{3-x}$Nd$_x$Ni$_2$O$_7$

Systematically controlling the superconducting transition temperature ($T_\text{c}$) in the bilayer Ruddlesden-Popper nickelate La$_3$Ni$_2$O$_7$ remains a significant challenge. Here, we address this by synthesizing high-quality polycrystalline La$_{3-x}$Nd$_x$Ni$_2$O$_7$ ($0 \leq x \leq 2.4$) with record-level rare-earth substitution. Nd doping compresses the lattice, particularly along the $c$ axis, enhances the spin density wave transition temperature, and elevates the pressure required for the orthorhombic-to-tetragonal structural transition. Superconductivity is observed across all doping levels under high pressures, with the onset $T_\text{c}$ rising to $\sim$93~K for $x = 2.1$ and $2.4$ from the electronic transport measurement. Using the radio-frequency transmission technique, newly applied to nickelate superconductors, we detect signatures of superconductivity at $98 \pm 2$~K in the $x=2.4$ compound, pushing the $T_\text{c}$ frontier further. We identify a universal linear relationship where $T_\text{c}$ decreases with the $c$-axis lattice parameter at a rate of approximately $-28$~K/\AA, demonstrating that enhanced interlayer magnetic exchange coupling is the dominant mechanism for superconducting pairing. Our work establishes the critical role of magnetism and provides a unified structural descriptor for elevating $T_\text{c}$ in bilayer nickelates.

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arXiv2025

Superconductivity in monolayer-trilayer phase of La$_3$Ni$_2$O$_7$ under high pressure

The discovery of 80 K superconductivity in pressurized bilayer Ruddlesden-Popper (RP) nickelate La$_3$Ni$_2$O$_7$ has established a new high-temperature superconductor family. The quest to understand the governing principles of RP nickelate superconductivity has become a central focus in condensed matter physics. Here, we report a critical advance by synthesizing and investigating a distinct structural polymorph of the same compound: the monolayer-trilayer (1313) hybrid phase of La$_3$Ni$_2$O$_7$. Under high pressure, synchrotron X-ray diffraction and Raman spectroscopy reveal a structural transition from the orthorhombic $Cmmm$ to the tetragonal $P4/mmm$ space group at 13~GPa. Above 19 GPa, the phase exhibits a clear superconducting transition, confirmed by a zero-resistance state, albeit at a significantly reduced temperature of 3.6 K. The stark contrast with the 80 K transition in the bilayer phase provides a uniquely clean experimental comparison. Our results demonstrate that the superconducting transition temperature is directly governed by the nature of the interlayer coupling, and the bilayer NiO$_6$ block as the essential structural motif for achieving high-$T_\text{c}$ superconductivity in the RP nickelates.

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arXiv2025

Distinct orbital contributions to electronic and magnetic structures in La$_{4}$Ni$_{3}$O$_{10}$

High-T$_c$ superconductivity has recently been discovered in Ruddlesden-Popper phase nickelates under pressure, where the low-energy electronic structure is dominated by Ni $d_{x^2 - y^2}$ and $d_{z^2}$ orbitals. However, the respective roles of these orbitals in superconductivity remain unclear. Here, by combining X-ray absorption, electron energy loss spectroscopy, and density functional theory calculations on La$_{4}$Ni$_{3}$O$_{10}$ single crystals, we identify ligand holes in the $p_{x,y}$ orbitals of planar oxygen and the $p_z$ orbitals of apical oxygen, which hybridize with the Ni $d_{x^2-y^2}$ and $d_{z^2}$ orbitals, respectively. These ligand holes enable orbital-selective O K-edge resonant inelastic X-ray scattering (RIXS) study, which reveals that $d_{x^2-y^2}$ states dominate the low-energy charge excitations and are more itinerant. We also observe a $\sim$0.1 eV bimagnon through RIXS and Raman spectroscopy, which leads to an interlayer superexchange interaction J$_z$ of $\sim$50 meV. Our results reveal distinct contributions of Ni $d_{x^2-y^2}$ and $d_{z^2}$ orbitals to the electronic and magnetic structure and provide direct experimental insights to understand the RP-phase nickelate superconductors.

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arXiv2025

Ultrafast Optical Evidence of Coexisting Density Waves in Bilayer Nickelate La$_3$Ni$_2$O$_7$

Utilizing ultrafast optical pump-probe spectroscopy, we investigate the coexistence and competition of electronic orders in the bilayer nickelate La$_3$Ni$_2$O$_7$. Our results reveal two coexisting density waves that can be selectively manipulated with light. We directly identify a spin-density wave (SDW) with electronic nematicity emerging below $T_{\rm SDW}$ $\approx$ 140 K by measuring its spin dynamics, and discover a distinct, nonmagnetic charge order appearing below $T_{\rm DW}$ $\approx$ 115 K. The central finding is the demonstration of differential optical control: the charge order is fragile, completely suppressed by a pump fluence of approximately 40 $\mu$J/cm$^2$, while the SDW is remarkably robust, persisting to 200 $\mu$J/cm$^2$. This work establishes a clear hierarchy in the stability of competing electronic orders and provides a powerful method for disentangling their interplay in quantum materials.

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arXiv2025

Ground state and magnetic transitions of the orthorhombic antiferromagnet CaCo$_2$TeO$_6$

We report the systematic synthesis, crystal structure, magnetization, and powder neutron diffraction of single crystalline and polycrystalline CaCo$_2$TeO$_6$ samples. CaCo$_2$TeO$_6$ crystallizes in an orthorhombic structure with $Pnma$ space group, featuring chains of edge-shared CoO$_6$ octahedra arranged in a honeycomb pattern. Two antiferromagnetic transitions are observed at $T$$_{N1}$ = 14.4 K and $T$$_{N2}$ = 16.2 K, corresponding to two long-range magnetic orders with propagation vectors of $\bf{k}$$_1$ = (0, 0, 0) and $\bf{k}$$_2$ = (0.125, 0, 0.25), respectively. The ground state is determined as a canted up-up-down-down zigzag spin configuration along the $c$ axis, wherein the magnetic moments of Co1 and Co2 ions are 3.4(1) and 2.1(1)$\mu$$_B$, respectively. Successive spin-flop transitions appear with the increasing magnetic field applied along the easy axis ($c$ axis), accompanied by depression of the antiferromagnetic orders and enhancement of residual magnetic entropy. The field-induced spin-disordered state suggests that CaCo$_2$TeO$_6$ may be an ideal candidate for studying frustrated magnetism.

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arXiv2025

Collapse of density wave and emergence of superconductivity in pressurized-La$_4$Ni$_3$O$_{10}$ evidenced by ultrafast spectroscopy

Recent discoveries of superconductivity in Ruddlesden-Popper nickelates realize a rare category of superconductors. However, the use of high-pressure diamond anvil cells limits spectroscopic characterization of the density waves and superconducting gaps. Here, we systematically studied the pressure evolution of La$_{4}$Ni$_{3}$O$_{10}$ using ultrafast optical pump-probe spectroscopy. We found that the transition temperature and energy gap of density waves are suppressed with increasing pressure and disappear suddenly near 17 GPa where structural transition appears. In addition, the observation of a single density wave gap indicates that the spin density wave and charge density wave remain coupled as pressure increases, rather than decoupling. After the density wave collapse, a distinct low-temperature regime emerges, characterized by a small gap consistent with potential superconducting pairing. The separated phase region of superconductivity and density waves suggests that superconductivity in pressurized-La$_4$Ni$_3$O$_{10}$ competes strongly with density waves, offering new insights into the interplay between these two phenomena.

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arXiv2025

Low volume fraction of high-Tc superconductivity in La3Ni2O7 at 80 K and ambient pressure

The discovery of superconductivity in pressurized La3Ni2O7 with a transition temperature of approximately 80 K above the boiling point of liquid nitrogen has sparked significant attention. It is essential to search for high-temperature superconductivity in bulk samples and at ambient pressure in nickelates. In this study, we report influential factors that affect the appearance of superconductivity in La3Ni2O7 at ambient pressure. From direct-current magnetic measurements, we observe a clear diamagnetic response at 80 K in post-annealed single crystals of La3Ni2O7 in oxygen. The superconducting volume fraction is estimated to be within 0.2%, resulting in a decrease in resistivity. This work presents a practical approach for further investigating high-temperature superconductivity in nickelates at ambient pressure.

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arXiv2024

Low-temperature mean valence of nickel ions in pressurized La$_3$Ni$_2$O$_7$

The discovery of high critical temperature (Tc) superconductivity in pressurized La$_3$Ni$_2$O$_7$ has ignited renewed excitement in the search of novel high-Tc superconducting compounds with 3d transition metals. Compared to other ambient-pressure superconductors, such as copper-oxide and iron-oxypnictides, unraveling the mechanisms of the pressure-induced superconductivity poses significant and unique challenges. A critical factor in this phenomenon seems to be related to the electronic configuration of 3d orbitals, which may play a fundamental role in driving high-Tc superconductivity. However, the pressure effects on the mixed-valence states of 3d-orbital cations and their influence on the emergence of high-Tc superconductivity remain poorly understood. Here, we use high-pressure (P) and low-temperature synchrotron X-ray absorption spectroscopy to investigate the influence of pressure on the mean valence change of Ni ions in La$_3$Ni$_2$O$_7$. Our results demonstrate that at a low-temperature of 20 K, the mean valence remains relatively stable across the pressures range from 1 atm to 40 GPa. Based on analyzing the absorption data, we find that, at a critical pressure, the ambient-pressure ordered phases disappear and both the structural and the superconducting phase transition occur. The pressure-induced structural phase transition revealed by our absorption results is consistent with that determined by X-ray diffraction, offering new information for a comprehensive understanding on the pressure-induced superconductivity in La$_3$Ni$_2$O$_7$.

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arXiv2024

Unveiling the multiband metallic nature of the normal state in nickelate La3Ni2O7

The discovery of unconventional superconductivity around 80 K in perovskite nickelates under high pressure has furnished a new platform to explore high-temperature unconventional superconductivity in addition to cuprates. Understanding the normal state of nickelate superconductors is crucial to uncovering the origin of this unconventional superconductivity and gaining further insight into its underlying mechanism. In this study, we systemically studied the transport properties of La3Ni2O7 by tuning the pressure under high magnetic fields. Magnetoresistance (MR) consistently exhibits a quasi-quadratic dependence on the magnetic field across all measured pressures and temperatures. Increased pressure enhances the metallicity of the system and leads to a monotonic increase in MR, which follows the extended Kohler's rule. These results suggest that the normal state of La3Ni2O7 to be a multiband metallic nature.

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arXiv2024

Strongly Anisotropic Charge Dynamics in La3Ni2O7 with Coherent-to-Incoherent Crossover of Interlayer Charge Dynamics

We report an optical spectroscopy study of the charge-dynamics anisotropy in the La3Ni2O7 single crystals with the electric field of the incident light parallel to the crystalline c-axis and ab-plane respectively. The evolution of the low-energy part of its c-axis optical conductivity spectra ({\sigma}1c({\omega})) from a Drude component to a finite-energy peak, together with the change in the c-axis electron mean-free-path which is distinctly longer than the c-axis lattice constant at 10 K but is shorter than the c-axis lattice constant at 300 K, demonstrates a crossover from coherent to incoherent interlayer charge dynamics in La3Ni2O7, which is associated with the variation from weak to strong dissipation within its ab-plane. In contrast, the Drude component robust in its {\sigma}1ab({\omega}) and the long ab-plane electron mean-free-path greater than the a-axis and b-axis unit-cell lengths manifest the persistence of coherent in-plane charge dynamics from 10 to 300 K. Thus, the charge dynamics in La3Ni2O7 shows a remarkable anisotropy at high temperatures. At low temperatures, the large values of the ratio between the ab-plane and c-axis Drude weights and the ratio {\sigma}1ab({\omega} -> 0)/{\sigma}1c({\omega} -> 0) indicate a strong anisotropy of the low-temperature charge dynamics in La3Ni2O7.

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arXiv2024

Evolution of Electronic Correlations in the Ruddlesden-Popper Nickelates

We report on optical studies of the Ruddlesden-Popper nickelates La$_{n+1}$Ni$_{n}$O$_{3n+1}$ with $n = 2$ (La$_{3}$Ni$_{2}$O$_{7}$), $n = 3$ (La$_{4}$Ni$_{3}$O$_{10}$) and $n = \infty$ (LaNiO$_{3}$). As the number of the NiO$_{6}$ octahedra layers $n$ grows, the ratio of the kinetic energy determined from the experimental optical conductivity and that from band theory $K_{\text{exp}}/K_{\text{band}}$ increases, suggesting a reduction of electronic correlations. While the strong electronic correlations in the bilayer La$_{3}$Ni$_{2}$O$_{7}$ place it on the verge of the Mott insulating phase, the trilayer La$_{4}$Ni$_{3}$O$_{10}$ and infinite-layer LaNiO$_{3}$ exhibit moderate electronic correlations, falling into the regime of correlated metals. The evolution of the electronic correlations in La$_{n+1}$Ni$_{n}$O$_{3n+1}$ is likely to be dominated by the Ni-$d_{z^2}$ orbital. Our results provide important information for understanding the superconductivity in Ruddlesden-Popper nickelates.

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