arXiv subjects

Hualei Sun

Publications and source records attributed to Hualei Sun.

At least 19 recordsLinked to original sources

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.

cond-mat.supr-con↗

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

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

The recent discovery of compressed superconductivity at 80~K in La$_3$Ni$_2$O$_7$-$\delta$ 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$_7$-$\delta$ 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 $\Delta_{1} = 23~\mathrm{meV}$ and $\Delta_{2} = 6~\mathrm{meV}$, while the BTK fitting is consistent with an $s$-like, two-gap spectrum. The gap ratio $2\Delta_{s1}(0) / k_{\mathrm{B}}T_{c}$ 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.

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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.

cond-mat.str-el↗

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

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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arXiv2024

Signature of Superconductivity in Pressurized Trilayer-nickelate Pr$_4$Ni$_3$O$_{10-\delta}$

The discovery of high-temperature superconductivity in La$_3$Ni$_2$O$_7$ and La$_4$Ni$_3$O$_{10}$ under pressure has drawn extensive attention. Herein, we report systematic investigations on the evolutions of structure, magnetism, and electrical resistance of Pr$_4$Ni$_3$O$_{10-\delta}$ polycrystalline samples under various pressures. Pr$_4$Ni$_3$O$_{10-\delta}$ exhibits density wave transitions on Ni and Pr sublattices at about 158 K and 4.3 K, respectively, and the density wave can be progressively suppressed by pressure. A structural transformation from the monoclinic $P2_1/a$ space group to the tetragonal $I4/mmm$ occurs at around 20 GPa. An apparent drop in resistance with evident magnetic field dependence is observed as pressure above 20 GPa, indicating the emergence of superconductivity in Pr$_4$Ni$_3$O$_{10-\delta}$ polycrystalline samples. The discovery of the signature of superconductivity in Pr$_4$Ni$_3$O$_{10-\delta}$ broadens the family of nickelate superconductors and provides a new platform for investigating the mechanisms of superconductivity in the Ruddlesden-Popper phases of nickelates.

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arXiv2024

Density-wave-like gap evolution in La$_3$Ni$_2$O$_7$ under high pressure revealed by ultrafast optical spectroscopy

Density wave (DW) order is believed to be correlated with superconductivity in the recently discovered high-temperature superconductor La$_3$Ni$_2$O$_7$. However, experimental investigations of its evolution under high pressure are still lacking. Here, we explore the quasiparticle dynamics in bilayer nickelate La$_3$Ni$_2$O$_7$ single crystals using ultrafast optical pump-probe spectroscopy under high pressures up to 34.2 GPa. At ambient pressure, the temperature-dependent relaxation dynamics demonstrate a phonon bottleneck effect due to the opening of an energy gap around 151 K. The energy scale of the DW-like gap is determined to be 66 meV by the Rothwarf-Taylor model. Combined with recent experiential results, we propose that this DW-like transition at ambient pressure and low temperature is spin density wave (SDW). With increasing pressure, this SDW order is significantly suppressed up to 13.3 GPa before it completely disappears around 26 GPa. Remarkably, at pressures above 29.4 GPa, we observe the emergence of another DW-like order with a transition temperature of approximately 135 K, which is probably related to the predicted charge density wave (CDW) order. Our study provides the experimental evidence of the evolution of the DW-like gap under high pressure, offering critical insights into the correlation between DW order and superconductivity in La$_3$Ni$_2$O$_7$.

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arXiv2024

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$_7$.

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arXiv2024

Neutron Scattering Studies on the High-$T_c$ Superconductor La$_3$Ni$_2$O$_{7-\delta}$ at Ambient Pressure

After several decades of studies of high-temperature superconductivity, there is no compelling theory for the mechanism yet; however, the spin fluctuations have been widely believed to play a crucial role in forming the superconducting Cooper pairs. The recent discovery of high-temperature superconductivity near 80 K in the bilayer nickelate La$_3$Ni$_2$O$_7$ under pressure provides a new platform to elucidate the origins of high-temperature superconductivity. We perform elastic and inelastic neutron scattering studies on a polycrystalline sample of La$_3$Ni$_2$O$_{7-\delta}$ at ambient pressure. No magnetic order can be identified down to 10 K. The absence of long-range magnetic order in neutron diffraction measurements may be ascribed to the smallness of the magnetic moment. However, we observe a weak flat spin-fluctuation signal at $\sim$ 45 meV in the inelastic scattering spectra. The observed spin excitations could be interpreted as a result of strong interlayer and weak intralayer magnetic couplings for stripe-type antiferromagnetic orders. Our results provide crucial information on the spin dynamics and are thus important for understanding the superconductivity in La$_3$Ni$_2$O$_7$.

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arXiv2024

Electronic and magnetic excitations in La$_3$Ni$_2$O$_7$

The striking discovery of high-temperature superconductivity (HTSC) of 80 K in a bilayer nickelate La$_3$Ni$_2$O$_7$ under a moderately high pressure of about 14 GPa ignited a new wave of studying HTSC in nickelates. The properties of the parental phase at ambient pressure may contain key information on basic interactions therein and bosons that may mediate pairing giving birth to superconductivity. Moreover, the bilayer structure of La$_3$Ni$_2$O$_7$ may suggest a distinct minimal model in comparison to cuprate superconductors. Here using X-ray absorption spectroscopy and resonant inelastic X-ray scattering, we studied La$_3$Ni$_2$O$_7$ at ambient pressure, and found that Ni 3$d_{x^2-y^2}$, Ni 3$d_{z^2}$, and ligand oxygen 2$p$ orbitals dominate the low-energy physics with a small charge-transfer energy. Remarkably, well-defined optical-like magnetic excitations were found to soften into a quasi-static spin-density-wave ordering, evidencing the strong electronic correlations and rich magnetic properties. Based on a Heisenberg spin model, we found that the inter-layer effective magnetic superexchange interaction is much larger than the intra-layer ones, and proposed two viable magnetic structures. Our results set the foundation for further exploration of La$_3$Ni$_2$O$_7$ superconductor.

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arXiv2023

Visualization of Oxygen Vacancies and Self-doped Ligand Holes in La3Ni2O7-{\delta}

The recent discovery of superconductivity in La3Ni2O7-{\delta} under high pressure with a transition temperature around 80 K has sparked extensive experimental and theoretical efforts. Several key questions regarding the pairing mechanism remain to be answered, such as the most relevant atomic orbitals and the role of atomic deficiencies. Here, we develop a new energy-filtered multislice electron ptychography technique, assisted with electron energy loss spectroscopy, to address these critical issues. Oxygen vacancies are directly visualized and are found to primarily occupy the inner apical sites, which have been proposed to be crucial to superconductivity. We precisely determine the nanoscale stoichiometry and its correlation to the oxygen K edge spectra, which reveals a significant inhomogeneity in the oxygen content and electronic structure within the sample. The spectroscopic results also unveil that stoichiometric La3Ni2O7 is in the charge-transfer regime, with holes that are self-doped from Ni sites into O sites. The outer apical oxygen is found to be less relevant to the low-energy physics and can be safely disregarded in theoretical models. These observations will assist in further development and understanding of superconducting nickelate materials. Our imaging technique for quantifying atomic deficiencies can also be widely applied in materials science and condensed matter physics.

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arXiv2023

Structural transition, electric transport, and electronic structures in the compressed trilayer nickelate La4Ni3O10

Atomic structure and electronic band structure are fundamental properties for understanding the mechanism of superconductivity. Motivated by the discovery of pressure-induced high-temperature superconductivity at 80 K in the bilayer Ruddlesden-Popper nickelate La3Ni2O7, the atomic structure and electronic band structure of the trilayer nickelate La4Ni3O10 under pressure up to 44.3 GPa are investigated. A structural transition from the monoclinic P21/a space group to the tetragonal I4/mmm around 12.6-13.4 GPa is identified, accompanying with a drop of resistance below 7 K. Density functional theory calculations suggest that the bonding state of Ni 3dz2 orbital rises and crosses the Fermi level at high pressures, which may give rise to possible superconductivity observed in resistance under pressure in La4Ni3O10. The trilayer nickelate La4Ni3O10 shows some similarities with the bilayer La3Ni2O7 and has unique properties, providing a new platform to investigate the underlying mechanism of superconductivity in nickelates.

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