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Deyuan Hu

Publications and source records attributed to Deyuan Hu.

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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.

cond-mat.supr-con

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.

cond-mat.supr-con

Dissecting superconductivity in the Ruddlesden-Popper nickelates: The role of electron correlation and interlayer magnetic exchange

The discovery of superconductivity in the Ruddlesden-Popper (RP) nickelates has opened a new chapter in the search for high superconducting transition temperatures ($T_\mathrm{c}$) materials. A central and puzzling feature of this family is the wide variation in $T_\mathrm{c}$ despite their common NiO$_2$ building blocks, as highlighted by the recent observation of superconductivity at $\sim$ 30 K in trilayer $\mathrm{La_4Ni_3O_{10}}$, significantly lower than 80 K reported in bilayer $\mathrm{La_3Ni_2O_7}$. Understanding the factors that control $T_\mathrm{c}$ in this family is therefore of paramount importance. Here, we use resonant inelastic x-ray scattering (RIXS) to investigate the electronic and magnetic excitations of $\mathrm{La_4Ni_3O_{10}}$ in direct comparison with its bilayer counterpart. Our results reveal a markedly different landscape. $\mathrm{La_4Ni_3O_{10}}$ exhibits a more itinerant character, evidenced by broader Ni $dd$ orbital excitations and a strong Ni 3$d$ fluorescence continuum, suggesting weaker electronic correlations than in the bilayer. Despite this, well-defined collective spin excitations persist, including dispersive acoustic and optical magnon branches alongside an incommensurate spin density wave. Using linear spin wave theory, we extract the interlayer superexchange interaction ($J_z$) to be $\sim$ 22 meV, much smaller than that in $\mathrm{La_3Ni_2O_7}$. The weaker correlation and reduced interlayer exchange together provide a consistent explanation for the substantially lower $T_\mathrm{c}$ in the trilayer compound. Our findings establish interlayer magnetic coupling and electronic correlation as key parameters governing superconductivity in layered nickelates and offer critical constraints for understanding the pairing mechanism in this emerging family.

cond-mat.supr-con

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.

cond-mat.supr-con

Highly Anisotropic Charge Dynamics and Spectral Weight Redistribution in the Trilayer Nickelate La$_{4}$Ni$_{3}$O$_{10}$

We study the $ab$-plane and $c$-axis charge dynamics of La$_{4}$Ni$_{3}$O$_{10}$ using optical spectroscopy. While a pronounced Drude profile, i.e. metallic response, is observed in the $ab$-plane optical conductivity $σ_{1}^{ab}(ω)$, the $c$-axis optical spectra $σ_{1}^{c}(ω)$ exhibit semiconducting behavior. The zero-frequency extrapolation of the optical conductivity $σ_{1}(ω\rightarrow 0) \equiv 1/ρ_{\text{dc}}$ gives a resistivity anisotropy of $ρ_{c}/ρ_{ab} \simeq 366$ at 300~K for La$_{4}$Ni$_{3}$O$_{10}$, which is much larger than the values in iron-based superconductors but comparable to those in high-$T_{c}$ cuprates. The interband response is also highly anisotropic, showing salient orbital selectivity for light polarized in the $ab$ plane and along the $c$ axis. The interband-transition peaks in both $σ_{1}^{ab}(ω)$ and $σ_{1}^{c}(ω)$ are located at lower energies compared to density-functional-theory predictions, signifying considerable electronic correlations. By investigating the spectral weight transfer, we find that in the pristine phase, Coulomb correlations have a marked impact on the charge dynamics of \LNO, whereas in the density-wave state, a gap opens with the Ni-$d_{z^{2}}$ orbital being involved.

cond-mat.supr-con

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.

cond-mat.supr-con

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.

cond-mat.supr-con

Revealing superconducting gap in La$_3$Ni$_2$O$_7$-$δ$ by Andreev reflection spectroscopy under high pressure

The recent discovery of compressed superconductivity at 80~K in La$_3$Ni$_2$O$_7$-$δ$ has brought nickelates into the family of unconventional high-temperature superconductors. However, due to the challenges of directly probing the superconducting pairing mechanism under high pressure, the pairing symmetry and gap structures of nickelate superconductors remain under intense debate. In this work, we successfully determine the microscopic information on the superconducting gap structure of La$_3$Ni$_2$O$_7$-$δ$ samples subjected to pressures exceeding 20~GPa, by constructing different conductance junctions within diamond anvil cells. By analyzing the temperature-dependent differential conductance spectra within the Blonder--Tinkham--Klapwijk (BTK) model, we have determined the superconducting energy gap at high pressure. The differential conductance curves reveal a two-gap structure with $Δ_{1} = 23~\mathrm{meV}$ and $Δ_{2} = 6~\mathrm{meV}$, while the BTK fitting is consistent with an $s$-like, two-gap spectrum. The gap ratio $2Δ_{s1}(0) / k_{\mathrm{B}}T_{c}$ is found to be 7.61, belonging to a family of strongly coupled superconductors. Our findings provide valuable insights into the superconducting gap structures of the pressure-induced superconducting nickelates.

cond-mat.supr-con

Evidence for the Meissner effect in the nickelate superconductor La3Ni2O7-delta single crystal using diamond quantum sensors

Quantum sensing with nitrogen-vacancy (NV) centers in diamond enables the characterization of magnetic properties in the extreme situation of tiny sample with defects. Recent studies have reported superconductivity in La3Ni2O7-delta under pressure, with zero-resistance near 80 K, though the Meissner effect remains debated due to low superconducting volume fractions and limited high-pressure magnetic measurement techniques. In this work, we use diamond quantum sensors and four-probe detection to observe both zero resistance and the Meissner effect in the same La3Ni2O7-delta single crystal. By mapping the Meissner effect, we visualized superconducting regions and revealed sample inhomogeneities. Our combined magnetic and electrical measurements on the same crystal provide dual evidence of superconductivity, supporting the high-temperature superconductivity of La3Ni2O7-delta. This study also offers insights into its structural and magnetic properties under high pressure.

cond-mat.supr-con

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.

cond-mat.supr-con

Squeezing enhanced sensing at an exceptional point

Pushing the boundaries of measurement precision is central for sensing and metrology, pursued by nonclassical resources such as squeezing, and non-Hermitian degeneracies with distinct spectral response. Their convergence, however, remains challenging. We find extraordinary enhancement of sensitivity by unifying both effects in a general framework for quantum sensing in open systems. At the parametric oscillation threshold and an exceptional point, the sensing precision exhibits a unique quartic scaling with the perturbation strength. The result generalizes to multimode squeezed-state sensors with higher-order exceptional points catered to various quantum sensing platforms.

quant-ph

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.

cond-mat.supr-con

Revealing nanoscale structural phase separation in La$_{3}$Ni$_{2}$O$_{7-δ}$ single crystal via scanning near-field optical microscopy

The discovery of superconductivity in La3Ni2O7-$δ$ under high pressure,with an onset critical temperature around 80 K, has sparked significant interest in the superconducting phases of Ruddlesden-Popper nickelates, Lan+1NinO3n+1. While La4Ni3O10 exhibits nearly 100% superconductivity with Tc~30 K under high pressure, magnetic susceptibility studies on La3Ni2O7-$δ$, however, reveal a more complex picture, indicating either filamentary superconductivity or that approximately 50% of crystal phase becomes superconducting in polycrystalline samples. In this study, we employed scattering-type scanning near-field optical microscopy to visualize nanoscale structural phase separation in La3Ni2O7-$δ$, identifying enhanced optical conductivity with stripes approximately 183 nm wide. These stripes run diagonally with respect to the Ni-O-Ni bond directions in the a-b plane, ruling out the possibility that they arise from impurity phases, like the '1313', '214' or '4310' structures. The dark regions and bright stripes exhibit optical conductivities ~ 22% and 29% of gold's, respectively. Additionally, we find that the bright stripes constitute about 38% of the total field of view, while the remainder consists of dark regions and the transitional region between dark regions and bright stripes. Our results suggest that optical conductivity stripes originate from nanoscale structural phase separation. In contrast, La4Ni3O10 exhibits uniform and higher optical conductivity with no observable evidence of phase separation. Thus, our study represents a pioneering effort to directly image nanoscale phase separation in Lan+1NinO3n+1 nickelates. This observation could provide crucial insights into the factors that limit the superconducting volume fraction of La3Ni2O7-$δ$, highlighting SNOM as a powerful probe for exploring nanoscale low-energy physics in correlated quantum materials.

cond-mat.supr-con

Origin of the density wave instability in trilayer nickelate La$_{4}$Ni$_{3}$O$_{10}$ revealed by optical and ultrafast spectroscopy

In the intricate phase diagram of unconventional superconductors characterized by intertwined electronic orders and superconductivity, a key step in understanding the superconducting mechanism is to investigate the parent compounds from which superconductivity emerges through doping or pressure. In this study, we employed optical spectroscopy and ultrafast reflectivity measurements to examine the density wave instability in the trilayer nickelate La$_{4}$Ni$_{3}$O$_{10}$, which displays pressure-induced superconductivity up to 30 K. Our optical spectroscopy measurements reveal that La$_{4}$Ni$_{3}$O$_{10}$ behaves as a metal with a high plasma frequency. Upon cooling, we observed a distinct formation of a density wave energy gap in both optical conductivity and pump-probe measurements. The gap feature is more pronounced compared to the bilayer nickelate La$_{3}$Ni$_{2}$O$_{7}$. Through a comparison of the experimentally determined plasma frequency with first-principles calculations, we classify La$_{4}$Ni$_{3}$O$_{10}$ as a moderately electron-correlated material, resembling the parent compound of iron-based superconductors but exhibiting weaker correlation than the bilayer nickelate La$_{3}$Ni$_{2}$O$_{7}$. The enhanced gap feature and weaker electronic correlation in La$_{4}$Ni$_{3}$O$_{10}$ may explain its lower superconductivity transition temperature under high pressure. These findings significantly advance our comprehension of the density wave and superconductivity mechanisms in the trilayer nickelate La$_{4}$Ni$_{3}$O$_{10}$.

cond-mat.str-el

Identification of the superconductivity in bilayer nickelate La$_3$Ni$_2$O$_7$ upon 100 GPa

Identification of superconductivity in the Ruddlesden-Popper phases of nickelates under high pressure remains challenging. Here, we report a comprehensive study of the crystal structure, resistance, and Meissner effect in single crystals of La$_3$Ni$_2$O$_7$ with hydrostatic pressures up to 104 GPa. X-ray diffraction measurements reveal a structural transition from the orthorhombic to a tetragonal phase above 40 GPa. Zero resistance of the superconductivity was achieved with a maximum onset $T_c^{onset}$ of 83 K at 18.0 GPa. Superconductivity is gradually suppressed until it disappears above 80 GPa, resulting in a right-triangle-like superconducting region. The direct-current magnetic susceptibility technique successfully detected the Meissner effect in La$_3$Ni$_2$O$_7$ under pressure; the maximum superconducting volume fraction is estimated to be 62.7% at 22.0 GPa. Thus, we demonstrate the bulk nature of superconductivity in the bilayer nickelate La$_3$Ni$_2$O$_7$ single crystals under high pressure. The results reveal intimate connections among the superconductivity, oxygen content, and structure in La$_3$Ni$_2$O$_7$.

cond-mat.supr-con