arXiv subjects

Ho-Kwang Mao

Publications and source records attributed to Ho-Kwang Mao.

17 recordsLinked to original sources

arXiv2026

A chemical avenue to manipulate field-reentrant superconducting rivalries in infinite layer nickelates

Recently, preliminary magnetic field-reentrant superconductivity manifested in high-temperature (Tc) Eu-doped infinite-layer (IL) nickelates, beyond analogous discoveries exclusively in low-Tc systems. This evokes intriguing fundamental issues about potential quantum-phase boundary and criticality between unconventional superconductivity and field-reentrant-one, which are inexplicable owing to formidable challenges in growing IL-nickelates towards later-series rare-earths. Herein, we open up chemical avenues to enable effective growth of (RE1-yRE'y)1-xEuxNiO2 (RE/RE': Pr, Nd, Sm, Gd, Dy), giving rise to discoveries of RE-4f-related quantum competition between high-Tc and reentrant superconductivity. Robust magnetic-field-reentrant superconductivity with uniaxial anisotropy is observed at superconducting-dome boundaries, stemming from Eu2+-4f7 associated competition between magnetic-fluctuation promoted pairing and exchange-field interactions. Their quantum-criticality is further modulable via RE(RE')-magnetism, which either reinforces reentrancy or elevates Tc (40.1 K) with more robust critical-current-density (~266 kA/cm2 at 2 K) beyond Sr-/Ca-doped counterparts. Our synthetic route enables the establishment of an ideal platform via IL-nickelates for studying 4f-related unconventional superconductivity and quantum-criticality.

cond-mat.supr-con↗

arXiv2026

Counterintuitive inverse superconducting transition beyond 4He-cooling limit

Thermally driven quantum-orders observed in exceptional instances may redefine the role of thermal-fluctuation from a source of decoherence to a resource for coherent-state engineering. While preliminary signs of counterintuitive temperature-rise-triggered superconductivity manifested in CeCu2Si2, ErRh4B4, Ho1.2Mo6S8 and (La,Ce)Al2, their critical-temperatures (Tc-inv) remain below Kelvin-range, precluding substantial applications. Here, we report field-modulated inverse-superconducting-transitions above 4He-cooling-limit in Eu-based infinite-layer nickelates (EuxNd1-xNiO2 and EuxPr1-xNiO2) grown on a substrate under both overdoped and underdoped regimes. Paradigmatically, superconductivity with zero-resistance is confined between Tc-inv (2.6-5.4 K) and another higher normal-Tc, rising and decreasing with applied magnetic-field, respectively. Starting from the resistive-state below Tc-inv, the inverse-superconducting-transition is driven by not only temperature-rising, but also current-density, while superconductivity further vanishes at higher temperature and current thresholds. The Kelvin-range inverse superconducting transition is plausibly explained by temperature-induced alternating dominance of effective magnetic-fields arising from Eu2+4f7 related compensations relative to the upper-critical-field. Furthermore, an extended-phenomenological-framework is also supported by reemerged superconductivity below 300 mK under magnetic-field, giving rise to an unprecedented temperature-induced reentrant superconductivity. Our findings establish magnetic-interaction-reconfigured high-Tc systems as fertile platforms for exploring quantum phenomena that reverse thermal-decoherence paradigm, also enabling antithetical-designs to unlock untapped application-scenarios for quantum-phase-transition devices.

cond-mat.supr-con↗

arXiv2024

Coexistence of superconductivity and sliding polar metal state in HgPSe3

The simultaneous presence of polarity and metallicity in a material signifies an exotic polar metal state, but such materials are extremely rare, especially in bulk form, due to mutually exclusive nature of the fundamental defining properties. Here, we report experimental findings that HgPSe3 is a robust bulk polar metal at room temperature with a chiral structure stabilized by pressure and, remarkably, this polar metal hosts superconductivity with critical temperature Tc up to 11 K. Theoretical analysis reveals a two-step interlayer sliding-then-compressing mechanism for coexistence of polarity and metallicity in HgPSe3. This work unveils a new paradigm for creating the bulk polar metal state and simultaneous presence of coexisting quantum orders, raising the prospect of discovering novel emergent physics using pressure as a tuning knob.

cond-mat.supr-con↗

arXiv2023

Lattice effect on the superexchange interaction in antiferromagnetic Bi$_2$Sr$_2$CaCu$_2$O$_8$

The in-plane superexchange interaction $J$ of cuprate superconductors has long been suggested to be an important parameter for exploring their high-temperature superconductivity. The bilayer Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ is the most studied system with high-quality single crystals in the wide doping range with the the same structure and phase. So far, the lattice parameter dependence of $J$ in its antiferromagnetic parent compound Bi$_2$Sr$_2$CaCu$_2$O$_{8}$ has not been established. By combining Raman scattering and x-ray diffraction techniques on the same sample in the same pressure environment, we obtain the evolution of both the two-magnon spectrum and the structural parameters with pressure up to nearly 30 GPa, The relationship between pressure or the in-plane lattice parameter and $J$ is thus established for Bi$_2$Sr$_2$CaCu$_2$O$_{8}$. Over the studied pressure range, superconductivity does not appear in this parent compound based on a sensitive magnetic measurement technique. The effects of pressure and chemical doping on the superexchange interaction and structure and their implications for superconductivity are discussed from the comparison of the obtained experimental data with the existing experiments. The results and findings provide valuable information for the understanding of superconductivity and the future theory developments for superconductivity in cuprates.

cond-mat.supr-con↗

arXiv2021

Future Study of Dense Superconducting Hydrides at High Pressure

The discovery of a record high superconducting transition temperature (Tc) of 288 K in a pressurized hydride inspires new hope to realize ambient condition superconductivity. Here, we give a perspective on the theoretical and experimental studies of hydride superconductivity. Predictions based on the BCS-Eliashberg-Midgal theory with the aid of density functional theory have been playing a leading role in the research and guiding the experimental realizations. To date, about twenty hydrides experiments have been reported to exhibit high-Tc superconductivity and their Tc agree well with the predicted values. However, there are still some controversies existing between the predictions and experiments, such as no significant transition temperature broadening observed in the magnetic field, the experimental electron-phonon coupling beyond the Eliashberg-Midgal limit, and the energy dependence of density of states around the Fermi level. To investigate these controversies and the origin of the highest Tc in hydrides, key experiments are required to determine the structure, bonding, and vibrational properties associated with H atoms in these hydrides.

cond-mat.supr-con↗

arXiv2021

Stabilization of S3O4 at High Pressure-Implications for the Sulfur Excess Paradox

The geological conundrum of sulfur excess refers to the finding that predicted amounts of sulfur, in the form of SO2, discharged in volcanic eruptions much exceeds the sulfur available for degassing from the erupted magma. Exploring the source of the excess sulfur has been the subject of considerable interest. Here, from a systematic computational investigation of sulfur-oxygen compounds under pressure, a hitherto unknown S3O4 compound containing a mixture of sulfur oxidation states +II and +IV emerges and is predicted to be stabilized above a pressure of 79 GPa. We predict that S3O4 can be produced via multiple redox reactions involving subducted S-bearing minerals (e.g., sulfates and sulfides) at high pressure conditions relevant to the deep lower mantle, and conversely be decomposed into SO2 and S at shallow depths of Earth. Therefore, S3O4 can be considered as a key intermediate compound to promote the decomposition of sulfates to release SO2, which offers an alternative source of the excess sulfur released during explosive eruptions. These findings provide a possible resolution to the geological paradox of excess sulfur degassing and a viable mechanism for the understanding of S exchange between surface and the lower mantle for the deep sulfur cycle.

physics.comp-ph↗

arXiv2019

Synthesis and electronic structure characterization of diamane

Atomically thin graphite, known as graphene, has been a marvel in material science because of its exceptional properties, novel physics and promising applications. Atomically thin diamond, called diamane, has also attracted considerable scientific interest due to its potential physical and mechanical properties. However, until now there has been no reports of successful synthesis of a free-standing pristine diamane film. Here, we report the synthesis and electronic structure characterization of diamane. Electrical measurements, x-ray diffraction and theoretical simulations reveal that trilayer and thicker graphene transform to hexagonal diamane (h-diamane) when compressed to above 20 GPa, which can be preserved down to few GPa. Raman studies indicate that the sample quenched from high pressure and high temperature also has a h-diamane structure, i.e., h-diamane is recovered back to ambient conditions. Optical absorption and band structure calculations reveal an indirect energy gap of 2.8 eV in the diamane film. Compared to gapless graphene, diamane with sizable bandgap may open up new applications of carbon semiconductors.

cond-mat.mtrl-sci↗

arXiv2018

Electronic Spin transition in FeO$_{2}$: evidence for Fe(II) with peroxide O$_{2}^{2-}$

The discovery of FeO$_{2}$ containing more oxygen than hematite (Fe$_{2}$O$_{3}$) that was previously believed to be the most oxygen rich iron compounds, has important implications on the study of the deep lower mantle compositions. Compared to other iron compounds, there are limited reports on FeO$_{2}$ making studies of its physical properties of great interest in fundamental condensed matter physics and geoscience. Even the oxidation state of Fe in FeO$_{2}$ is the subject of debate in theoretical works and there have not been reports from experimental electronic and magnetic properties measurements. Here, we report the pressure-induced spin state transition from synchrotron experiments and our computational results explain the underlying mechanism. Using density functional theory and dynamical mean field theory, we calculated spin states of Fe with volume and Hubbard interaction $U$ change, which clearly demonstrate that Fe in FeO$_{2}$ consists of Fe(II) and peroxide O$_{2}^{2-}$. Our study suggests that localized nature of both Fe 3$d$ orbitals and O$_{2}$ molecular orbitals should be correctly treated for unveiling the structural and electronic properties of FeO$_{2}$.

cond-mat.str-el↗

arXiv2017

Spin Quenching Assisted by a Strongly Anisotropic Compression Behavior in MnP

We studied the crystal structure and spin state of MnP under high pressure with synchrotron X-ray diffraction and X-ray emission spectroscopy. MnP has an exceedingly strong anisotropy in compressibility, with the primary compressible direction along the b axis of the Pnma structure. X-ray emission spectroscopy reveals a pressure-driven quenching of the spin state in MnP. Firstprinciples calculations suggest that the strongly anisotropic compression behavior significantly enhances the dispersion of the Mn d-orbitals and the splitting of the d orbital levels compared to the hypothetical isotropic compression behavior. Thus, we propose spin quenching results mainly from the significant enhancement of the itinerancy of d electrons and partly from spin rearrangement occurring in the split d-orbital levels near the Fermi level. This explains the fast suppression of magnetic ordering in MnP under high pressure. The spin quenching lags behind the occurrence of superconductivity at ~8 GPa implying that spin fluctuations govern the electron pairing for superconductivity.

cond-mat.supr-con↗

arXiv2017

X-ray driven first-order phase transition in GeO2 glass under pressure

Unprecedented bright and intense synchrotron X-rays have been widely used to unravel numerous compelling electronic and structural properties using a large variety of physical techniques, while the puzzling phenomenon is the uncertainties of measurements due to X-ray induced considerable electronic and structural changes of a matter under study. Here, we report an X-ray driven first-order tetrahedral-octahedral phase transition in GeO2 glass at high pressure using X-ray absorption fine structure (XAFS) with a nano-polycrystalline diamond anvil (NPD) cell. Upon X-ray irradiation from an undulator device, the XAFS spectrum at 5.4 GPa, which is below the threshold pressure of tetrahedral to pentahedral transition, starts to progressively approach the spectrum of octahedral GeO2 at 20.4 GPa. Detailed analysis indicates that both the nearest distance and coordination number of GeO2 glass at 5.4 GPa increase to those of a fully octahedral glass above 20 GPa, while negligible changes were found at other low pressures. These observations demonstrate that X-ray irradiation can be served as an alternative stimulus for forming dense matter under pressure, as the well-known external stimuli of pressure and temperature. Dense matter formed under external stimuli is crucial for understanding the formation, differentiation and evolution of planet and Earth. Attention for the X-ray induced structural uncertainties is called, especially for addressing metastable states under extreme conditions which may become undetectable in terms of intense synchrotron X-rays as structural tools.

cond-mat.mtrl-sci↗

arXiv2015

Signature of a polyamorphic transition in the THz spectrum of vitreous GeO2

The THz spectrum of density fluctuations, $S(Q, ω)$, of vitreous GeO$_2$ at ambient temperature was measured by inelastic x-ray scattering from ambient pressure up to pressures well beyond that of the known $α$-quartz to rutile polyamorphic (PA) transition. We observe significant differences in the spectral shape measured below and above the PA transition, in particular, in the 30-80 meV range. Guided by first-principle lattice dynamics calculations, we interpret the changes in the phonon dispersion as the evolution from a quartz-like to a rutile-like coordination. Notably, such a crossover is accompanied by a cusp-like behavior in the pressure dependence of the elastic response of the system. Overall, the presented results highlight the complex fingerprint of PA phenomena on the high-frequency phonon dispersion.

cond-mat.dis-nn↗

arXiv2015

Pressure tuning of superconductivity independent of disorder in Tl$_{2}$Ba$_{2}$CaCu$_{2}$O$_{8+δ}$

Varying the superconducting transition temperature over a large scale of a cuprate superconductor is a necessary step for identifying the unsettled mechanism of superconductivity. Chemical doping or element substitution has been proven to be effective but also brings about lattice disorder. Such disorder can completely destroy superconductivity even at a fixed doping level. Pressure has been thought to be the most clean method for tuning superconductivity. However, pressure-induced increase of disorder was recognized from recent experiments. By choosing a disordered Tl$_{2}$Ba$_{2}$CaCu$_{2}$O$_{8+δ}$ at the optimal doping, we perform single-crystal x-ray diffraction and magnetic susceptibility measurements at high pressures. The obtained structural data provides evidence for the robust feature for the disorder of this material in the pressure range studied. This feature ensures the pressure effects on superconductivity distinguishable from the disorder. The derived parabolic-like behavior of the transition temperature with pressure up to near 30 GPa, having a maximum around 7 GPa, offers a platform for testing any realistic theoretical models in a nearly constant disorder environment. Such a behavior can be understood when considering the carrier concentration and the pairing interaction strength as two pressure intrinsic variables.

cond-mat.supr-con↗

arXiv2015

Superconductivity in Dense Rashba Semiconductor BiTeCl

Layered non-centrosymmetric bismuth tellurohalides are being examined as candidates for topological insulators. Pressure is believed to be essential for inducing and tuning topological order in these systems. Through electrical transport and Raman scattering measurements, we find superconductivity in two high-pressure phases of BiTeCl with the different normal state features, carrier characteristics, and upper critical field behaviors. Superconductivity emerges when the resistivity maximum or charge density wave is suppressed by the applied pressure and then persists till the highest pressure of 51 GPa measured. The huge enhancement of the resistivity with three magnitude of orders indicates the possible achievement of the topological order in the dense insulating phase. These findings not only enrich the superconducting family from topological insulators but also pave the road on the search of topological superconductivity in bismuth tellurohalides.

cond-mat.supr-con↗

arXiv2015

Superconductivity in efficient thermoelectric Cu$_3$Sb$_{0.98}$Al$_{0.02}$Se$_4$

Both superconductivity and thermoelectricity offer promising prospects for daily energy efficiency applications. The advancements of thermoelectric materials have led to the huge improvement of the thermoelectric figure of merit in the past decade. By applying pressure on a highly efficient thermoelectric material Cu$_{3}$Sb$_{0.98}$Al$_{0.02}$Se$_4$, we achieve dome-shape superconductivity developing at around 8.5 GPa but having a maximum critical temperature of 3.2 K at pressure of 12.7 GPa. The novel superconductor is realized through the first-order structural transformation from its initial phase to an orthorhombic one. The superconducting phase is determined in the ultimate formation of the Cu-Al-Sb-Se alloy.

cond-mat.supr-con↗

arXiv2015

Tripling the critical temperature of KFe$_{2}$As$_{2}$ by carrier switch

Superconductivity of high critical temperature ($T_{c}$) superconductors is usually realized through chemical dopant or application of pressure in a similar way to induce charge carriers of either electrons or holes into their parent compounds. For chemical doping, superconductivity behaves asymmetrically with the maximum $T_{c}$ often higher for optimal hole-doping than that of optimal electron-doping on the same parent compound. However, whether electron carriers could be in favour of higher $T_{c}$ than holes in such high-$T_{c}$ superconductors is unknown but attractive. Here we show that the application of pressure can drive KFe$_{2}$As$_{2}$ from hole- to electron-superconductivity after passing the previously reported $V$-shape or oscillation regime. The maximum $T_{c}$ in the electron-dominated region is tripled to the initial value of 3.5 K or the average in the low-pressure hole-dominated region. The structural transition takes place from the tetragonal to collapsed tetragonal phase when the carrier characteristic is changed upon compression. Our results unambiguously offer a new route to further improve superconductivity with huge $T_{c}$ enhancement for a compound through carrier switch. The strong electronic correlations in KFe$_{2}$As$_{2}$ are suggested to account for the unexpected enhancement of superconductivity in the collapsed tetragonal phase.

cond-mat.supr-con↗

arXiv2013

Sustainable high critical temperature in a hydrocarbon superconductor

Organic superconductors are unique materials with a crystal structure made primarily of a complex carbon based network, an element associated directly with life, which were postulated to have a high critical temperature, $T_{C}$, even above room temperature, from a theoretical viewpoint. Pressure plays an essential role in the study of superconductivity in such organic materials, including creation of the first organic superconductor as well as the achievement of the highest $T_{C}$ of 14.2 K for charge transfer salts and 38 K for metal-doped fullerides. However, superconductivity in these organic systems is only sustainable within a very narrow pressure range (a few GPa) and is readily destroyed upon further compression. Here we report high-pressure magnetic susceptibility and structure measurements on a newly discovered superconductor, LaPhenanthrene. It is found that the application of pressure not only significantly increases $T_{C}$ from its ambient-pressure value of 4.8 K to 12.3 K at 18.4 GPa but also stabilizes the high $T_{C}$ over the entire pressure range (61 GPa) of the study. The evolution of $T_{C}$ with pressure is closely correlated with the angle $β$ of the monoclinic unit cell. Both $T_{C}$ and $β$ change sharply with increasing pressure initially but remain constant above 40 GPa, indicating that molecule orientation is essential to superconductivity. These behaviors can be understood in terms of pressure tuning of electron correlations, illustrating the unconventional nature of superconductivity in these hydrocarbon superconductors.

cond-mat.supr-con↗

arXiv2007

Brillouin scattering and molecular dynamics study of the elastic properties of Pb(Mg1/3Nb2/3)O3

We report the complete set of elastic constants and the bulk modulus for single crystal Pb(Mg1/3Nb2/3)O3 (PMN) at room temperature obtained from Brillouin spectroscopy and molecular dynamics (MD) simulations. The bulk modulus from Brillouin is found to be 103 GPa, in a good agreement with earlier x-ray studies. We also derived the refractive index along all principal axes and found PMN to be optically isotropic, with a refractive index of 2.52 +/- 0.02. PMN shows mechanical anisotropy with A=1.7. The MD simulations of PMN using the random site model overestimate the elastic constants by 20-50 GPa and the bulk modulus is 148 GPa, but the mechanical anisotropy matches the Brillouin results of A = 1.7. We also determined the elastic constants for various models of PMN and we find variation in the elastic constants based on chemical ordering.

cond-mat.mtrl-sci↗