arXiv subjects

Ho-kwang Mao

Publications and source records attributed to Ho-kwang Mao.

At least 37 records · Page 2Linked to original sources

arXiv2024

Unveiling a Novel Metal-to-Metal Transition in LuH2: Critically Challenging Superconductivity Claims in Lutetium Hydrides

Following the recent report by Dasenbrock-Gammon et al. (2023) of near-ambient superconductivity in nitrogen-doped lutetium trihydride (LuH3-δNε), significant debate has emerged surrounding the composition and interpretation of the observed sharp resistance drop. Here, we meticulously revisit these claims through comprehensive characterization and investigations. We definitively identify the reported material as lutetium dihydride (LuH2), resolving the ambiguity surrounding its composition. Under similar conditions (270-295 K and 1-2 GPa), we replicate the reported sharp decrease in electrical resistance with a 30% success rate, aligning with Dasenbrock-Gammon et al.'s observations. However, our extensive investigations reveal this phenomenon to be a novel, pressure-induced metal-to-metal transition intrinsic to LuH2, distinct from superconductivity. Intriguingly, nitrogen doping exerts minimal impact on this transition. Our work not only elucidates the fundamental properties of LuH2 and LuH3 but also critically challenges the notion of superconductivity in these lutetium hydride systems. These findings pave the way for future research on lutetium hydride systems while emphasizing the crucial importance of rigorous verification in claims of ambient temperature superconductivity.

cond-mat.supr-con↗

arXiv2023

Structure responsible for the superconducting state in La3Ni2O7 at high pressure and low temperature conditions

Very recently, a new superconductor with Tc = 80 K was reported in nickelate (La3Ni2O7) at around 15 - 40 GPa conditions (Nature, 621, 493, 2023) [1], which is the second type of unconventional superconductor, beside the cuprates, with Tc above liquid nitrogen temperature. However, the phase diagram plotted in this report was mostly based on the transport measurement at low temperature and high pressure conditions, and the assumed corresponding X-ray diffraction (XRD) results was carried out at room temperature. This encouraged us to carry out in situ high pressure and low temperature synchrotron XRD experiments to determine which phase is responsible for the high Tc state. In addition to the phase transition from orthorhombic Amam structure to orthorhombic Fmmm structure, a tetragonal phase with space group of I4/mmm was discovered when the sample was compressed to 19 GPa at 40 K where the superconductivity takes palce in La3Ni2O7. The calculations based on this tetragonal structure reveal that the electronic states approached to the Fermi energy were mainly dominated by the eg orbitals (3dz2 and 3dx2-y2) of Ni atoms, which are located in the oxygen octahedral crystal field. The correlation between Tc and this structural evolution, especially Ni-O octahedra regularity and the in-plane Ni-O-Ni bonding angles, are analyzed. This work sheds new lights to identify what is the most likely phase responsible for superconductivity in the double layered nickelate.

cond-mat.supr-con↗

arXiv2023

Pressure-induced non-monotonic crossover of steady relaxation dynamics in a metallic glass

Relaxation dynamics, as a key to understand glass formation and glassy properties, remains an elusive and challenging issue in condensed matter physics. In this work, in situ high-pressure synchrotron high-energy x-ray photon correlation spectroscopy has been developed to probe the atomic-scale relaxation dynamics of a cerium-based metallic glass during compression. Although the sample density continuously increases, the collective atomic motion initially slows down as generally expected and then counter-intuitively accelerates with further compression (density increase), showing an unusual non-monotonic pressure-induced steady relaxation dynamics crossover at ~3 GPa. Furthermore, by combining in situ high-pressure synchrotron x-ray diffraction, the relaxation dynamics anomaly is evidenced to closely correlate with the dramatic changes in local atomic structures during compression, rather than monotonically scaling with either sample density or overall stress level. These findings could provide new insight into relaxation dynamics and their relationship with local atomic structures of glasses.

cond-mat.mtrl-sci↗

arXiv2023

The near room-temperature upsurge of electrical resistivity in Lu-H-N is not superconductivity, but a metal-to-poor-conductor transition

Since the discovery of superconductivity in mercury at 4 K in 1911, searching for materials with superconductivity at higher temperatures towards practical conditions has been a primary enduring goal. The recent report of room-temperature superconductivity at near-ambient pressure in nitrogen-doped lutetium hydride (Lu-H-N) by Dasenbrock-Gammon et al. (Hereafter referred as D-G) seems a great step approaching the ultimate goal. Specifically, they claimed evidence of superconductivity on Lu-H-N with a maximum Tc of 294 K at 1 GPa. However, the failure to observe the drastic temperature-dependent resistance change above 200 K in high-pressure synthesized Lu-H-N compounds, a prerequisite for superconductivity, by researchers worldwide in all independent follow-up studies casts a heavy shadow on the authenticity of the claims. The sober questions are: what is the sample that produces the sharp resistance jump near room temperature? What are the reasons for the non-reproducibility of others who follow the D-G method of synthesis and the inscrutable low success rate (35%) in synthesizing the right sample even for the authors in Ref. 1? What causes the observed sharp resistance jump? Here, with a well-controlled experiment protocol, we repeatedly reproduced the near room-temperature sudden change of electrical resistance in the Lu-H-N sample, and we could quantitatively compare its behavior with the initial pure Lu in a normal metallic state. These results enable us to scrutinize the origin for the near-room temperature sharp resistance change, which is attributed to a metal-to-poor-conductor transition rather than superconductivity.

cond-mat.supr-con↗

arXiv2023

Origin of superionic state in Earth's inner core

Earth's inner core (IC) serves as a reservoir for volatile elements, which significantly affects its behavior and properties. Recent studies suggest that superionicity can be observed in ice and iron hydrides under high-pressure and temperature conditions, providing an alternative understanding of the planet's interior. In this study, we demonstrated that electride formation drives the superionic state in iron hydride under IC pressure conditions. The electride stabilizes the iron lattice and provides a pathway for volatile diffusion. The coupling between lattice stability and superionicity is triggered near 100 GPa and enhanced at higher pressures. The electride-driven superionicity can also be generalized for volatiles in other rocky planetary cores. These findings provide new insights into the mechanisms of core formation and evolution of rocky planets.

physics.geo-ph↗

arXiv2023

Robust magnetism against pressure in non-superconducting samples prepared from lutetium foil and H2/N2 gas mixture

Recently, the claim of "near-ambient superconductivity" in a N-doped lutetium hydride attracted enormous following-up investigations in the community of condensed matter physics and material sciences. But quite soon, the experimental results from different groups indicate consistently that no evidence of near-ambient superconductivity is found in the samples synthesized by the same method as the reported one, or by the other alternative methods. From our extended high-pressure heat capacity and magnetic susceptibility measurements on the samples prepared with the lutetium foil and H2/N2 gas mixture, we report the finding of a magnetic transition at the temperature about 56 K. Our results show that this magnetic phase is robust against pressure up to 4.3 GPa, which covers the critical pressure of boosting the claimed near room temperature superconductivity.

cond-mat.supr-con↗

arXiv2023

No evidence of superconductivity in the compressed sample prepared from the lutetium foil and H2/N2 gas mixture

A material described as lutetium-hydrogen-nitrogen (Lu-H-N in short) was recently claimed to have near-ambient superconductivity[Gammon et al, Nature 615, 244, 2023]. If the results could be reproduced by other teams, it would be a major scientific breakthrough. Here, we report our results of transport and structure measurements on a material prepared using the same method as that reported by Gammon et al. Our X-ray diffraction measurements indicated that the obtained sample contained three substances: the FCC-1 phase (Fm-3m) with a lattice parameter a=5.03 Å, the FCC-2 phase (Fm-3m) with a lattice parameter a= 4.755 Å and Lu metal. These two FCC phases are identical to the those reported in the so-called near-ambient superconductor. However, we found that the samples had no evidence of superconductivity, through our resistance measurements in the temperature range of 300 - 4 K and pressure range of 0.9 - 3.4 GPa, and our magnetic susceptibility measurements in the pressure range of 0.8-3.3 GPa and temperature down to 100 K. We also used a laser heating technique to heat the sample to 1800°C and found no superconductivity in the produced dark blue samples below 6.5 GPa. In addition, the color of the both samples remain dark blue in the pressure range investigated.

cond-mat.supr-con↗

arXiv2022

Novel Valence Transition in Elemental Metal Europium around 80 GPa

Valence transition could induce structural, insulator-metal, nonmagnetic-magnetic and superconducting transitions in rare-earth metals and compounds, while the underlying physics remains unclear due to the complex interaction of localized 4f electrons as well as their coupling with itinerant electrons. The valence transition in the elemental metal europium (Eu) still has remained as a matter of debate. Using resonant x-ray emission scattering and x-ray diffraction, we pressurize the states of 4f electrons in Eu and study its valence and structure transitions up to 160 GPa. We provide compelling evidence for a valence transition around 80 GPa, which coincides with a structural transition from a monoclinic (C2/c) to an orthorhombic phase (Pnma). We show that the valence transition occurs when the pressure-dependent energy gap between 4f and 5d electrons approaches the Coulomb interaction. Our discovery is critical for understanding the electrodynamics of Eu, including magnetism and high-pressure superconductivity.

cond-mat.str-el↗

arXiv2021

Atomistic Evidence of Nucleation Mechanism for the Direct Graphite-to-Diamond Transformation

The direct graphite-to-diamond transformation mechanism has been a subject of intense study and remains debated concerning the initial stages of the conversion, the intermediate phases, and their transformation pathways. Here, we successfully recover samples at early conversion stage by tuning high-pressure/high-temperature conditions and reveal direct evidence supporting the nucleation-growth mechanism. Atomistic observations show that intermediate orthorhombic graphite phase mediates the growth of diamond nuclei. Furthermore, we observe that quenchable orthorhombic and rhombohedra graphite are stabilized in buckled graphite at lower temperatures. These intermediate phases are further converted into hexagonal and cubic diamond at higher temperatures following energetically favorable pathways in the order: graphite -> orthorhombic graphite -> hexagonal diamond, graphite -> orthorhombic graphite -> cubic diamond, graphite -> rhombohedra graphite -> cubic diamond. These results significantly improve our understanding of the transformation mechanism, enabling the synthesis of different high-quality forms of diamond from graphite.

cond-mat.mtrl-sci↗

arXiv2021

Oxygen-driven enhancement of electron correlation in hexagonal iron at Earth's inner core conditions

Earth's inner core consists of mainly iron with a bit of light elements. Understanding of its structure and related physical properties has been elusive for both experiment and theory due to its required extremely high pressure and temperature conditions. Here, using density functional theory plus dynamical mean field theory, we demonstrate that oxygen atoms energetically stabilize hexagonal structured iron at the inner core condition. Electrical resistivity is much enhanced compared with pure hcp-Fe, supporting the conventional thermal convection model. Moreover, our calculated seismic velocity shows a quantitative match with geologically observed Preliminary Reference Earth Model data.

physics.geo-ph↗

arXiv2021

Lonsdaleite: The diamond with optimized bond lengths and enhanced hardness

Diamond is known as the hardest substance due to its ultra-strong tetrahedral sp3 carbon bonding framework. The only weak link is its cubic cleavage planes between (111) buckled honeycomb layers. Compressing graphite single crystals and heating to moderate temperatures, we synthesized a bulk, pure, hexagonal diamond (lonsdaleite) with distorted carbon tetrahedrons that shorten the bond between its hexagonal (001) buckled honeycomb layers, thus strengthening their linkage. We observed direct transformation of graphite (100) to lonsdaleite (002) and graphite (002) to lonsdaleite (100). We find the bulk lonsdaleite has superior mechanical properties of Vicker hardnesses HV = 164+/-11 GPa and 124+/-13 GPa, measured on the surface corresponding to the original graphite (001) and (100) surfaces, respectively. Properties of lonsdaleite as the supreme material can be further enhanced by purifying the starting material graphite carbon and fine-tuning the high pressure-temperature synthesis conditions.

cond-mat.mtrl-sci↗

arXiv2020

Origin of superconductivity and giant phonon softening in TlInTe$_2$ under pressure

Analogous to 2D layered transition metal dichalcogenides, the TlSe family of 1D chain materials with Zintl-type structure exhibits exotic phenomena under high-pressure. In the present work, we have systematically investigated the high-pressure behavior of TlInTe 2 using Raman spectroscopy, synchrotron X-ray diffraction, and transport measurements, in combination with crystal structure prediction (CSP) based on the evolutionary approach and first principles calculations. We found that TlInTe$_2$ undergoes a pressure driven semiconductor to semimetal transition at 4 GPa, followed by a superconducting transition at 5.7 GPa (with Tc = 3.8 K) induced by a Lifshitz transition. The Lifshitz transition is initiated by the appearance of new electron pockets on the Fermi surface, which evolve with pressure and connect to the adjacent electron pockets forming an umbrella shaped Fermi surface at the top and bottom of the Brillouin zone. An unusual giant phonon softening (Ag mode) concomitant with a V-shaped Tc behavior appears at 10-12 GPa as a result of the interaction of optical phonons with the conduction electrons, resulting in Fano line shaped asymmetry in Ag mode. A prominent Tc anomaly concurrent with the Ag mode softening at 19-20 GPa is correlated to the semimetal to metal transition. The CSP calculations reveal that these transitions are not accompanied by any structural phase transitions up to the maximum pressure achieved, 33.5 GPa. Our findings on TlInTe$_2$ open up a new platform to study a plethora of unexplored high pressure novel phenomena in TlSe family induced by Lifshitz transition (electronic driven), phonon softening and electron-phonon coupling.

cond-mat.supr-con↗

arXiv2020

Novel Superstructure-Phase Two-Dimensional Material 1$\textit{T}$-VSe$_2$ at High Pressure

A superstructure can elicit versatile new properties of materials by breaking their original geometrical symmetries. It is an important topic in the layered graphene-like two-dimensional transition-metal dichalcogenides (TMDs), but its origin remains unclear. Using diamond-anvil cell techniques, synchrotron x-ray diffraction, x-ray absorption, and the first-principles calculations, we show that the evolution from the weak Van der Waals bonding to the Heisenberg covalent bonding between layers induces an isostructural transition in quasi-two-dimensional 1$\textit{T}$-type VSe$_2$ at high pressure. Furthermore, our results show that high-pressure induce a novel superstructure at 15.5 GPa, rather than suppress as it would normally, which is unexpected. It is driven by the Fermi surface nesting, enhanced by the pressure-induced distortion. The results suggest that the superstructure not only appears in the two-dimensional structure but also can emerge in the pressure-tuned three-dimensional structure with new symmetry and develop superconductivity.

cond-mat.mtrl-sci↗

arXiv2019

Intermolecular coupling and fluxional behavior of hydrogen in phase IV

We performed Raman and infrared (IR) spectroscopy measurements of hydrogen at 295 K up to 280 GPa at an IR synchrotron facility of SSRF. To reach the highest pressure, hydrogen was loaded into toroidal diamond anvils with 40 micrometers central culet. The intermolecular coupling has been determined by concomitant measurements of the IR and Raman vibron modes. In phase IV, we find that the intermolecular coupling is much stronger in the graphene (G) like layer of elongated molecules compared to the Br2 like layer of shortened molecules and it increases with pressure much faster in the G layer compared to the Br2 layer. These heterogeneous lattice dynamical properties are unique features of highly fluxional hydrogen phase IV.

cond-mat.mtrl-sci↗

arXiv2019

Lattice frustration in spin-orbit Mott insulator Sr3Ir2O7 at high pressure

The intertwined charge, spin, orbital, and lattice degrees of freedom could endow 5d compounds with exotic properties. Current interest is focused on electromagnetic interactions in these materials, whereas the important role of lattice geometry remains to be fully recognized. For this sake, we investigate pressure-induced phase transitions in the spin-orbit Mott insulator Sr3Ir2O7 with Raman, electrical resistance, and x-ray diffraction measurements. We reveal an interesting magnetic transition coinciding with a structural transition at 14.4 GPa, but without a concurrent insulator-metal transition. The conventional correlation between magnetic and Mott insulating states is thereby absent. The observed softening of the one-magnon mode can be explained by a reduced tetragonal distortion, while the actual magnetic transition is associated with tilting of the IrO6 octahedra. This work highlights the critical role of lattice frustration in determining the high-pressure phases of Sr3Ir2O7. The ability to control electromagnetic properties via manipulating the crystal structure with pressure promises a new way to explore new quantum states in spin-orbit Mott insulators.

cond-mat.str-el↗

arXiv2019

Pressure enhanced interplay among lattice, spin and charge in La2FeMnO6 mixed perovskite

Spin crossover plays a central role in the structural instability, net magnetic moment modification, metallization, and even in superconductivity in corresponding materials. Most reports on the pressure-induced spin crossover with a large volume collapse so far focused on compounds with single transition metal. Here we report a comprehensive high-pressure investigation of a mixed Fe-Mn perovskite La2FeMnO6. Under pressure, the strong coupling between Fe and Mn leads to a combined valence/spin transition: Fe3+(S = 5/2) to Fe2+(S = 0) and Mn3+(S = 2) to Mn4+(S = 3/2), with an isostructural phase transition. The spin transitions of both Fe and Mn are offset by ~ 20 GPa of the onset pressure, and the lattice collapse occurs in between. Interestingly, Fe3+ ion shows an abnormal behavior when it reaches a lower valence state (Fe2+) accompanied by a + 0.5 eV energy shift in Fe K-absorption edge at 15 GPa. This process is associated with the charge-spin-orbital state transition from high spin Fe3+ to low spin Fe2+, caused by the significantly enhanced t2g-eg crystal field splitting in the compressed lattice under high pressure. Density Functional Theory calculations confirm the energy preference of the high-pressure state with charge redistribution accompanied by spin state transition of Fe ions. Moreover, La2FeMnO6 maintains semiconductor behaviors even when the pressure reached 144.5 GPa as evidenced by the electrical transport measurements, despite the huge resistivity decreasing 7 orders of magnitude compared with that at ambient pressure. The investigation carried out here demonstrates high flexibility of double perovskites and their good potentials for optimizing the functionality of these materials.

cond-mat.str-el↗

arXiv2019

Anomalous behavior of the quasi-one-dimensional quantum material Na$_{2}$OsO$_{4}$ at high pressure

Na$_{2}$OsO$_{4}$ is an unusual quantum material that, in contrast to the common 5${d}^{2}$ oxides with spins = 1, owns a magnetically silent ground state with spin = 0 and a band gap at Fermi level attributed to a distortion in the OsO$_{6}$ octahedral sites. In this semiconductor, our low-temperature electrical transport measurements indicate an anomaly at 6.3 K with a power-law behavior inclining through the semiconductor-to-metal transition observed at 23 GPa. Even more peculiarly, we discover that before this transition, the material becomes more insulating instead of merely turning into a metal according to the conventional wisdom. To investigate the underlying mechanisms, we applied experimental and theoretical methods to examine the electronic and crystal structures comprehensively, and conclude that the enhanced insulating state at high pressure originates from the enlarged distortion of the OsO$_{6}$. It is such a distortion that widens the band gap and decreases the electron occupancy in Os's ${t}_{2g}$ orbital through an interplay of the lattice, charge, and orbital in the material, which is responsible for the changes observed in our experiments.

cond-mat.mtrl-sci↗

arXiv2018

Superionic hydrogen in Earth's deep interior

Superionic hydrogen was previously thought to be an exotic state predicted and confirmed only in pure H2O ice. In Earth's deep interior, H2O exists in the form of O-H groups in ultra-dense hydrous minerals, which have been proved to be stable even at the conditions of the core-mantle boundary (CMB). However, the superionic states of these hydrous minerals at high P-T have not been investigated. Using first-principles calculations, we found that pyrite structured FeO2Hx (0 <= x <= 1) and d-AlOOH, which have been proposed to be major hydrogen-bearing phases in the deep lower mantle (DLM), contain superionic hydrogen at high P-T conditions. Our observations indicate a universal pathway of the hydroxyl O-H at low pressure transforming to symmetrical O-H-O bonding at high-P low-T, and a superionic state at high-P high-T. The superionicity of hydrous minerals has a major impact on the electrical conductivity and hydrogen transportation behaviors of Earth's lower mantle as well as the CMB.

cond-mat.mtrl-sci↗