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Ho-kwang Mao

Publications and source records attributed to Ho-kwang Mao.

At least 19 recordsLinked to original sources

Enhanced and robust superconductivity in La0.8Sr0.2NiO2 membranes compressed up to 210 GPa

The discovery of superconductivity in infinite-layer nickelate thin films has opened a new frontier for exploring unconventional oxide superconductors beyond the copper oxide family. However, the presence of substrate hampers investigations under very high pressure. Recently, this problem was circumvented by a study of freestanding Nd0.85Sr0.15NiO2 membranes, which revealed that superconducting transition temperature kept increasing as the pressure was ramped up to 91 GPa, without showing signs of saturation. Naturally, one wonders what would happen at even higher pressures. Here, we report that superconductivity in a freestanding La0.8Sr0.2NiO2 membrane persists under applied ultrahigh pressures up to 210 GPa. The superconducting transition onset temperature exhibits a continuous dome-like evolution, increasing from 16 K at ambient pressure to a peak of 74.5 K at 146 GPa, and then gradually decreasing to 57.4 K at 210 GPa. Such robustness of superconductivity against ultrahigh pressure has not been observed in high-Tc oxide superconductors before.

cond-mat.supr-con↗

Radio-Frequency Method for Detecting Superconductivity Under High Pressure

We introduce a contactless technique for probing superconductivity and magnetic ordering transitions in micron-sized samples under extreme pressure. Utilizing a multistage Lenz lens system, directly sputtered onto diamond anvils, we realize a radio-frequency (RF, 50 kHz - 200 MHz) transformer with a sample of 50-100 $μ$m in diameter, as its core. This configuration enables efficient transfer and focusing of an electromagnetic field within the diamond anvil cell's chamber. Consequently, the transmitted RF signal exhibits high sensitivity to variations in the sample's surface conductivity and magnetic permeability. We validate this method by determining the critical temperatures ($T_{\text{c}}$) of known superconductors, including NbTi, MgB$_2$, Hg-1223, Bi-2212, YBCO, and REBCO in various magnetic fields, as well as the magnetic ordering temperatures of Gd and Tb. Notably, we apply this technique to the LaH$_{10-x}$, CeH$_{9-10}$, and (La,Ce)H$_{10-12}$ superhydrides at a pressure of about 1-1.5 Mbar. The observed superconducting transitions in Ce and La superhydrides at 90-110 K and 215-242 K, respectively, correlate with the $T_{\text{c}}$'s determined via traditional electrical-resistance measurements. Moreover, we show how multiple repetitions of the RF experiment with the La-Ce superhydride make it possible to detect the increase in $T_{\text{c}}$ over time up to $\approx$ 260-270 K. This finding indicates the possibility of reaching a critical $T_{\text{c}}$ around 0$^\circ$C in the La-based superhydrides.

cond-mat.supr-con↗

Shear-stress-constrained superconductivity in Ruddlesden-Popper nickelates

Ruddlesden-Popper nickelates exhibit superconductivity under pressure in bulk crystals and under epitaxial constraint in thin films, while remaining highly sensitive to sample quality, oxygen content, defects, and stress conditions. We propose that the metastable RP lattice becomes superconducting only when the local constrained deformation of the Ni-O framework falls within a bounded shear-strain window. This deformation controls octahedral rotations, the interlayer Ni-O-Ni bond angle, and coupling between Ni dz2 and dx2-y2 orbitals. This shear-stress-constrained superconductivity scenario unifies the understanding of the pressure threshold, reversibility, spatial inhomogeneity, pressure-medium dependence, film-substrate sensitivity, and reproducibility.

cond-mat.supr-con↗

Pressure Induced 18 K Superconductivity and Two Superconducting Phases in CuIr2S4

We report pressure-induced superconductivity in the spinel CuIr$_{2}$S$_{4}$ with a transition temperature ($T_{\text{c}}$) reaching \textbf{18.2 K}, establishing a new record for this class of materials and surpassing the decades-old limit of 13.7 K. Our electrical transport and synchrotron X-ray diffraction studies up to 224 GPa reveal the emergence of \textbf{two distinct superconducting phases} from a charge-ordered insulating state. The first phase (SC-I) appears around 18 GPa, and forms a dome-shaped superconducting region in which the resistivity exhibits a pronounced, field- and current-sensitive drop without reaching strict zero above our base temperature. Above 111.8 GPa, a second, lower-$T_{\text{c}}$ phase (SC-II) emerges and coexists with SC-I over a broad pressure range, and SC-II ultimately develops a true zero-resistance state above 122.2 GPa. These superconducting phases are intimately linked to a cascade of structural transitions that systematically distort the frustrated pyrochlore lattice of Ir atoms. Our results expand the potential for superconductivity in spinels and demonstrate a pathway to high-$T_{\text{c}}$ pairing directly from a correlated insulating state driven by lattice tuning.

cond-mat.supr-con↗

Hydrogen site-dependent physical properties of hydrous magnesium silicates: implications for water storage and transport in the mantle transition zone

The Earth's mantle transition zone (MTZ) is widely recognized as a major water reservoir, exerting significant influence on the planet's water budget and deep cycling processes. Here, we employ crystal structure prediction and first-principles calculations to identify a series of stable hydrous magnesium silicate phases under transition zone conditions. Our results reveal a pressure-induced hydrogen substitution mechanism in wadsleyite, where H+ preferentially migrates from Mg2+ sites to Si4+ sites near 410 km depth. This transformation leads to a substantial decrease in electrical conductivity, consistent with geophysical observations. We estimate the water content in the MTZ to be approximately 1.6 wt%, aligning with seismic and conductivity constraints. Furthermore, using machine learning-enhanced molecular dynamics, we discover double superionicity in hydrous wadsleyite and ringwoodite at temperatures exceeding 2000 K, wherein both H+ and Mg2+ exhibit high ionic mobility. This dual-ion superionic state has potentially profound implications for mass transport, electrical conductivity, and magnetic dynamo generation in rocky super-Earth exoplanets.

physics.geo-ph↗

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/Å, 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.

cond-mat.supr-con↗

Direct Observation of d-Wave Superconducting Gap Symmetry in Pressurized La3Ni2O7-delta Single Crystals

The recent discovery of superconductivity in pressure-stabilized bulk La3Ni2O7-delta, with a critical temperature (Tc) exceeding 77 K, has opened a new frontier in high-temperature superconductivity research beyond cuprates. Yet, the superconducting gap amplitude and symmetry, the key parameters to characterize a superconductor, remain elusive due to the overwhelming challenges of gap studies under high pressure. Here, we introduce in situ directional point-contact spectroscopy conducted under truly hydrostatic pressure, enabling the direct mapping of the superconducting gap in pressurized La3Ni2O7-delta single crystals. Depending on the junction orientation, differential conductance (dI/dV) spectra exhibit distinct V-shaped quasiparticle features and a sharp zero-bias peak, indicating a predominant d-wave-like pairing symmetry. Measurement of the c-axis gap amplitude Delta yields a gap-to-Tc ratio of 2Delta/kBTc = 4.2(5), positioning La3Ni2O7-delta firmly among unconventional, nodal high-Tc superconductors. These findings set stringent constraints on theoretical models for nickelate superconductors and establish a robust spectroscopic approach for understanding superconductors under extreme pressures.

cond-mat.supr-con↗

Superconducting susceptibility signal captured in a record wide pressure range

In recent years, the resistance signature of the high temperature superconductivity above 250 K in highly compressed hydrides (more than 100 GPa) has garnered significant attention within the condensed matter physics community. This has sparked renewed optimism for achieving superconductivity under room-temperature conditions. However, the superconducting diamagnetism, another crucial property for confirming the superconductivity, has yet to be conclusively observed. The primary challenge arises from the weak diamagnetic signals detected from the small samples compressed in diamond anvil cells. Therefore, the reported results of superconducting diamagnetism in hydrides have sparked intense debate, highlighting the urgent need for workable methodology to assess the validity of the experimental results. Here, we are the first to report the ultrahigh pressure measurements of the superconducting diamagnetism on Nb0.44Ti0.56, a commercial superconducting alloy, in a record-wide pressure range from 5 GPa to 160 GPa. We present detailed results on factors such as sample size, the diamagnetic signal intensity, the signal-to-noise ratio and the superconducting transition temperature across various pressures and different pressure transmitting media. These comprehensive results clearly demonstrate that this alloy is an ideal reference sample for evaluating superconductivity in compressed hydrides,validating the credibility of the experimental systems and superconducting diamagnetic results, as well as determining the nature of the superconductivity of the investigated sample. In addition, these results also provide a valuable benchmark for studying the pressure-induced superconductivity in other material families.

cond-mat.supr-con↗

Absence of dehydration due to superionic transition at Earth's core-mantle boundary

The properties and stability of hydrous phases are key to unraveling the mysteries of the water cycle in Earth's interior. Under the deep lower mantle conditions, hydrous phases transition into a superionic state. However, the influence of the superionic effect on their stability and dehydration processes remains poorly understood. Using ab initio calculations and deep-learning potential molecular dynamics simulations, we discovered a doubly superionic transition in delta-AlOOH, characterized by the highly diffusive behavior of ionic hydrogen and aluminum within the oxygen sub-lattice. These highly diffusive elements contribute significant external entropy into the system, resulting in exceptional thermostability. Free energy calculations indicate that dehydration is energetically and kinetically unfavorable when water exists in a superionic state under core-mantle boundary (CMB) conditions. Consequently, water can accumulate in the deep lower mantle over Earth's history. This deep water reservoir plays a crucial role in the global deep water and hydrogen cycles.

physics.geo-ph↗

Isotropic superconductivity in pressurized trilayer nickelate La4Ni3O10

Evidence of superconductivity (SC) has recently been reported in pressurized La3Ni2O7 and La4Ni3O10, providing a new platform to explore high-temperature superconductivity. However, while zero resistance state has been observed, experimental characterization of the superconducting properties of pressurized nickelates is still limited and experimentally challenging. Here, we present the first full temperature dependence of the upper critical field Hc2 measurement in La4Ni3O10 single crystal, achieved by combining high magnetic field and high-pressure techniques. Remarkably, the Hc2 of La4Ni3O10 is nearly isotropic, with the anisotropic parameter monotonically increasing from 1.4 near Tc to 1 at lower temperatures. By analyzing the Hc2 using the two-band model, we uncover that the anisotropic diffusivity of the bands, primarily originating from d(z2 ) and d(x2-y2 ) orbitals, is well compensated, resulting in an unusually isotropic superconducting state. These findings provide critical experimental evidence that underscores the significant role of the d(z2 ) orbital in enabling superconductivity in pressurized Ruddlesden-Popper nickelates.

cond-mat.supr-con↗

Observation of a $Pbca$ phase and robust metallicity in $\rm{RuO_2}$ under pressure

$\rm{RuO_2}$ stands as a quintessential rutile-type compound under ambient conditions, with its structural exploration under pressure bearing significant implications for both phase transition investigations and Earth science. Nonetheless, the precise phase transition sequence remains a debate. In this study, we disclose the emergence of the $Pbca$ phase alongside the enduring metallic character of $\rm{RuO_2}$ under megabar pressure. Employing state-of-the-art synchrotron X-ray diffraction, our observations delineate a phase transition trajectory progressing through rutile, $\rm{CaCl_2}$, and ultimately $Pbca$ phases. Notably, the $Pbca$ phase manifests immediately just after the rutile-$\rm{CaCl_2}$ transition, confining a narrow pressure regime for the pure $\rm{CaCl_2}$-type phase. Within the pressure range of 15.5 to 35.0 GPa, a coexistence of the $\rm{CaCl_2}$-type and $Pbca$ phases is observed, transforming to a sole presence of the $Pbca$ phase beyond 35.0 GPa. Electrical transport measurements conducted on both single crystal and powder samples confirm the enduring metallic conductivity of $\rm{RuO_2}$, persisting up to at least $\sim$120 GPa, albeit exhibiting a diminished conductivity at ultrahigh pressures due to a reduction in electronic density of states at the Fermi level. This study furnishes compelling evidence for the presence of the $Pbca$ phase across a broad pressure range, diverging from the previously widely acknowledged $Pa\bar{3}$ phase, thereby offering crucial insights into phase transition phenomena in other metal dioxides and advancing our comprehension of electronic behaviors within 4d and 5d electron systems.

cond-mat.mtrl-sci↗

Investigations of key issues on the reproducibility of high-Tc superconductivity emerging from compressed La3Ni2O7

Recently, the signatures of superconductivity near 80 K have been discovered in the single crystal of La3Ni2O7 under pressure, which makes it a new candidate of the high-temperature superconductors dominated by 3d transition elements after the cuprate and iron-pnictide superconductors. However, there are several critical questions that have been perplexing the scientific community. These questions include (1) what factors contribute to the inconsistent reproducibility of the experimental results? (2) what is the fundamental nature of pressure-induced superconductivity: bulk or non-bulk (filamentary-like)? (3) where does the superconducting phase locate within the sample if it is filamentary-like? (4) is the oxygen content important for developing and stabilizing its superconductivity? In this study, we employ comprehensive high-pressure techniques to address these crucial issues. Through our modulated ac susceptibility measurements, we are the first to find that the superconductivity in this nickelate is filamentary-like. Our scanning transmission electron microscopy (STEM) investigations suggest that the filamentary-like superconductivity most likely emerges at the interface between the La3Ni2O7 and La4Ni3O10 phases. By tuning the oxygen content on the polycrystalline La3Ni2O7, we also find that the oxygen content plays vital role for developing and stabilizing its superconductivity. The upper and lower bounds of the oxygen content are 7.35 and 6.89, respectively. Our results provide not only new insights into understanding the puzzling issues in this material, but also significant information for achieving a better understanding on the superconductivity of this material.

cond-mat.supr-con↗

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↗

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$_7$.

cond-mat.supr-con↗

Observation of the Josephson effect in superhydrides: DC SQUID based on (La,Ce)H$_{10+x}$ with operating temperature of 179 K

Among known materials, hydride superconductors have the highest critical temperatures and are very promising as a basis for electronic sensors. Superconducting quantum interference devices (SQUID), due to its unique sensitivity to magnetic fields, are the most important applications of superconductors in microelectronics. In this work, we describe a direct current SQUID made of lanthanum-cerium superhydride (La, Ce)H$_{10+x}$ at a pressure of 148 GPa, with an operating temperature of 179 K and a bias current of about 2 mA. When placing (La, Ce)H$_{10+x}$ in a modulated magnetic field (0.1-0.005 Hz, 5 G), we observed the generation of higher harmonics up to 18$ν$$_0$ and a periodic dependence of the sample resistance on the magnetic flux density R ${\propto}$ sin($π$$Φ$/$Φ$$_0$). We demonstrate that the (La, Ce)H$_{10+x}$ SQUID with a size of about 6 $μ$m, operates in the mode of low thermal fluctuations and can be used to detect magnetic fields below 0.1 G. Our findings pave the road to more advanced applications of the Josephson effect and SQUIDs made of hydride superconductors.

cond-mat.supr-con↗

Superconducting-transition-temperature dependence of superfluid density and conductivity in pressurized cuprate superconductors

What factors fundamentally determine the value of superconducting transition temperature (Tc) in high temperature superconductors has been the subject of intense debate. Following the establishment of an empirical law known as Homes'law, there is a growing consensus in the community that the Tc value of the cuprate superconductors is closely linked to its superfluid density and conductivity. However, all the data supporting this empirical law have been obtained from the ambient-pressure superconductors. In this study, we present the first high-pressure results about the connection of these two quantities with Tc, through the studies on the Bi1.74Pb0.38Sr1.88CuO6+delta and Bi2Sr2CaCu2O8+delta, in which the value of their high-pressure resistivity (the reciprocal of conductivity) is achieved by adopting our newly established method, while the value of superfluid density is extracted using the Homes'law. We highlight that the Tc values are strongly linked the two joint response factors of magnetic field and electric field, i.e. superfluid density and conductivity, respectively, implying that the physics governing the determination of Tc is influenced by the intrinsic electromagnetic fields of the system.

cond-mat.supr-con↗

Narrowing band gap chemically and physically: Conductive dense hydrocarbon

Band gap energy of an organic molecule can be reduced by intermolecular interaction enhancement, and thus, certain polycyclic aromatic hydrocarbons (PAHs), which are insulators with wide band gaps, are expected to undergo insulator-metal transitions by simple compression. Such a pressure-induced electronic transition can be exploited to transform non-metallic organic materials into states featuring intriguing electronic characteristics such as high-temperature superconductivity. Numerous attempts have been made to metalize various small PAHs, but so far only pressure-induced amorphization well below the megabar region was observed. The wide band gap energy of the small PAHs and low chemical stability under simple compression are the bottlenecks. We have investigated the band gap energy evolution and the crystal structural compression of the large PAH molecules, where the band gap energy is significantly reduced by increasing the number of π-electrons and improved chemical stability with fully benzenoid molecular structure. Herein, we present a pressure-induced transition in dicoronylene, C48H20, an insulator at ambient conditions that transforms into a semi-metallic state above 23.0 GPa with a three-order-of-magnitude reduction in resistivity. In-situ UV-visible absorption, transport property measurement, Raman spectroscopy, X-ray diffraction and density functional theory calculations were performed to provide tentative explanations to the alterations in its electronic structure at high pressure. The discovery of an electronic transition at pressures well below the megabar is a promising step towards realization of a single component purely hydrocarbon molecular metal in the near future.

cond-mat.mtrl-sci↗

A novel method for determining the resistivity of compressed superconducting materials

The resistivity of a superconductor in its normal state plays a critical role in determining its superconducting ground state. However, measuring the resistivity of a material under high pressure has long presented a significant technical challenge due to pressure-induced changes in the crystallographic directions, especially for samples with anisotropic layered structures like high-Tc superconductors and other intriguing quantum materials. Here, we are the first to propose a novel and effective method for determining high-pressure resistivity, which relies on the ambient-pressure resistivity, initial sample sizes, lattice parameters, high-pressure resistance, and lattice parameters measured from the same sample. Its validity has been confirmed through our investigations of pressurized copper-oxide superconductors, which demonstrates that this method provides new possibilities for researchers conducting high-pressure studies related to resistivity of these materials.

cond-mat.str-el↗