arXiv subjects

Ho-kwang Mao

Publications and source records attributed to Ho-kwang Mao.

At least 55 records · Page 3Linked to original sources

arXiv2018

Diffusion-controlled Alloying of Single-phase Multi-principal Covalent Transition Metal Carbides with Enhanced Damage tolerance and Exceptional Thermal Properties

Multicomponent alloying has displayed extraordinary potential for producing exceptional structural and functional materials. However, the synthesis of single-phase, multi-principal covalent compounds remains a challenge. Here we present a diffusion-controlled alloying strategy for the successful realization of covalent multi-principal transition metal carbides (MPTMCs) with a single face-centered cubic (FCC) phase. The increased interfacial diffusion promoted by the addition of a nonstoichiometric compound leads to rapid formation of the new single phase at much lower sintering temperature. Direct atomic-level observations via scanning transmission electron microscopy demonstrate that MPTMCs are composed of a single phase with a random distribution of all cations, which holds the key to the unique combinations of improved fracture toughness, superior Vickers hardness, and extremely lower thermal diffusivity achieved in MPTMCs. The present discovery provides a promising approach toward the design and synthesis of next-generation high-performance materials.

cond-mat.mtrl-sci↗

arXiv2018

On the Reactivity of Hydrogen-Helium and Hydrogen-Nitrogen at High Pressures

Through a series of Raman spectroscopy studies, we investigate the behaviour of hydrogen-helium and hydrogen-nitrogen mixtures at high pressure across wide ranging concentrations. We find that there is no evidence of chemical association, miscibility, nor any demixing of hydrogen and helium in the solid state up to pressures of 250 GPa at 300 K. In contrast, we observe the formation of concentration-dependent N$_2$-H$_2$ van der Waals solids, which react to form N-H bonded compounds above 50 GPa. Through this combined study, we can demonstrate that the recently claimed chemical association of H$_2$-He can be attributed to significant N$_2$ contamination and subsequent formation of N$_2$-H$_2$ compounds.

cond-mat.mtrl-sci↗

arXiv2018

Prolonged mixed phase induced by high pressure in MnRuP

Hexagonally structured MnRuP was studied under high pressure up to 35 GPa from 5 to 300 K using synchrotron X-ray diffraction. We observed that a partial phase transition from hexagonal to orthorhombic symmetry started at 11 GPa. The new and denser orthorhombic phase coexisted with its parent phase for an unusually long pressure range, ΔP ~ 50 GPa. We attribute this structural transformation to a magnetic origin, where a decisive criterion for the boundary of the mixed phase lays in the different distances between the Mn-Mn atoms. In addition, our theoretical study shows that the orthorhombic phase of MnRuP remains steady even at very high pressures up to ~ 250 GPa, when it should transform to a new tetragonal phase.

cond-mat.mtrl-sci↗

arXiv2016

Simultaneous band gap narrowing and carrier lifetime prolongation of organic-inorganic trihalide perovskites

The organic-inorganic hybrid lead trihalide perovskites have been emerging as the most attractive photovoltaic material. As regulated by Shockley-Queisser theory, a formidable materials science challenge for the next level improvement requires further band gap narrowing for broader absorption in solar spectrum, while retaining or even synergistically prolonging the carrier lifetime, a critical factor responsible for attaining the near-band gap photovoltage. Herein, by applying controllable hydrostatic pressure we have achieved unprecedented simultaneous enhancement in both band gap narrowing and carrier lifetime prolongation (up to 70~100% increase) under mild pressures at ~0.3 GPa. The pressure-induced modulation on pure hybrid perovskites without introducing any adverse chemical or thermal effect clearly demonstrates the importance of band edges on the photon-electron interaction and maps a pioneering route towards a further boost in their photovoltaic performance.

cond-mat.mtrl-sci↗

arXiv2016

Pressure-Induced Confined Metal from the Mott Insulator Sr3Ir2O7

The spin-orbit Mott insulator Sr3Ir2O7 provides a fascinating playground to explore insulator-metal transition driven by intertwined charge, spin, and lattice degrees of freedom. Here, we report high pressure electric resistance and resonant inelastic x ray scattering measurements on single crystal Sr3Ir2O7 up to 63 65 GPa at 300 K. The material becomes a confined metal at 59.5 GPa, showing metallicity in the ab plane but an insulating behavior along the c axis. Such an unusual phenomenon resembles the strange metal phase in cuprate superconductors. Since there is no sign of the collapse of spin orbit or Coulomb interactions in x-ray measurements, this novel insulator metal transition is potentially driven by a first-order structural change at nearby pressures. Our discovery points to a new approach for synthesizing functional materials.

cond-mat.str-el↗

arXiv2016

Novel chemistry of lithium oxides and superconducting low-pressure LiO4

We study the stability of Li-O compounds as a function of pressure, with Li ion battery applications and fundamental chemical interest in mind. Using the ab initio evolutionary algorithm, we predict stability of novel compounds LiO4, Li5O3 and Li6O under pressure. LiO4, formed at the pressure of just 6 GPa, can be seen as ε-O8 accepting two electrons from two Li atoms. This phase is superconducting, with Tc up to 12.2 K at 10 GPa. This is remarkable, because elemental oxygen becomes superconducting at much higher pressure (96 GPa) and has much lower Tc (<0.6 K), and suggests that chemical alloying with other elements has the potential of not only decreasing metallization pressure, but also of increasing Tc. Since ε-O8 is called red oxygen, LiO4 can be identified "lithium red-oxid", and is distinct from superoxide. Additionally, Li5O3 is stable at pressures above 70 GPa and can be represented as a hybrid structure 4Li2O {\cdot} Li2O2, and electride suboxide Li6O is stable above 62 GPa.

cond-mat.mtrl-sci↗

arXiv2014

Pressure-induced Superconductivity in CaC2

Carbon can exist as isolated dumbbell, one-dimensional (1D) chain, 2D plane, and 3D network in carbon solids or carbon-based compounds, which attributes to its rich chemical binding way, including sp-, sp2-, and sp3-hybridized bonds. Sp2 hybridizing carbon always captures special attention due to its unique physical and chemical property. Here, using evolutionary algorithm in conjunction with ab initio method, we found that under compression, dumbbell carbon in CaC2 can be polymerized firstly into one-dimensional chain and then into ribbon and further into two dimensional graphite sheet at higher pressure. The C2m structure transforms into an orthorhombic Cmcm phase at 0.5 GPa, followed by another orthorhombic Immm phase, which is stabilized at wide pressure range of 15.2-105.8 GPa and then forced into MgB2-type phase with wide range stability up to at least 1 TPa. Strong electron-phonon coupling in cold compressed CaC2 is found, in particular for Immm phase, which has the highest lambda value (0.562-0.564) among them, leading to its high superconducting critical temperature (7.9~9.8 K), wihich is comparable to 11.5K value of CaC6. Our research results show that calcium can not only stabilize carbon sp2 hybridization at larger range of pressure but make them present superconducting behavior, which would further ignite experimental and theoretical research interests on Alkali-Earth metal carbides to uncover their peculiar physical properties under extreme conditions.

cond-mat.supr-con↗

arXiv2013

A Novel High-Pressure Monoclinic Metallic Phase of V2O3

Vanadium sesquioxide, V2O3, is a prototypical metal-to-insulator system where, in temperature-dependent studies, the transition always coincides with a corundum-to-monoclinic structural transition. As a function of pressure, V2O3 follows the expected behavior of increased metallicity due to a larger bandwidth for pressures up to 12.5 GPa. Surprisingly, for higher pressures when the structure becomes unstable, the resistance starts to increase. Around 32.5 GPa at 300 K, we observe a novel pressure-induced corundum-to-monoclinic transition between two metallic phases, showing that the structural phase transition can be decoupled from the metal-insulator transition. Using X-ray Raman scattering, we find that screening effects, which are strong in the corundum phase, become weakened at high pressures. Theoretical calculations indicate that this can be related to a decrease in coherent quasiparticle strength, suggesting that the high-pressure phase is likely a critical correlated metal, on the verge of Mott-insulating behavior.

cond-mat.str-el↗

arXiv2012

Pressure dependence of the monoclinic phase in (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 solid solutions

We combine high-pressure x-ray diffraction, high-pressure Raman scattering, and optical microscope to investigate a series of PMN-xPT solid solutions (x=0.2, 0.3, 0.33, 0.35, 0.37, 0.4) in diamond anvil cells up to 20 GPa at 300 K. The Raman spectra show a peak centered at 380 cm-1 above 6 GPa for all samples, in agreement with previous observations. X-ray diffraction measurements are consistent with this spectral change indicating structural phase transition; we find that the triplet at the pseudo cubic (220) Bragg peak merges into a doublet above 6 GPa. Our results indicate that the morphotropic phase boundary region (x=0.33 to 0.37) with the presence of monoclinic symmetry persists up to 7 GPa. The pressure dependence of ferroelectric domains in PMN-0.32PT single crystals was observed using a polarizing optical microscope. The domain wall density decreases with pressure and domains disappear at a modest pressure of 3 GPa. We propose a pressure-composition phase diagram for PMN-xPT solid solutions.

cond-mat.mtrl-sci↗

arXiv2012

Pressure tuning of Fermi surface topology of optimally doped BaFe$_{1.9}$Ni$_{0.1}$As$_{2}$

The superconducting, transport, and structural properties of optimally electron-doped BaFe$_{1.9}$Ni$_{0.1}$As$_{2}$ are investigated by combining the electrical resistance and synchrotron X-ray diffraction measurements at high pressures. The superconducting transition temperature of this system is found to decrease in a similar way of the axial ratio of $c/a$ with increasing pressure but vanishing at a critical pressure of 7.5 GPa where $c/a$ has a dip and an isostructural transformation from a tetragonal to a collapsed tetragonal phase takes place. The resistance is found to obey a linear temperature dependence, evidencing the antiferromagnetic spin-fluctuations transport mechanism. The pressure effects are interpreted within the framework of pressure-induced Fermi surface topology modification in which pressure suppresses both the quasiparticle effective mass and the strength of the antiferromagnetic spin fluctuations leading to the reduction of superconductivity, accordingly. The absent superconductivity in the collapsed tetragonal phase is suggested to result from the complete suppression of the antiferromagnetic spin fluctuations.

cond-mat.supr-con↗

arXiv2012

Pressure-Driven Quantum Criticality in An Iron-Selenide Superconductor

The discovery of superconductivity of about 30 K in iron selenides with very large magnetic moments simulates the examination of completing orders. Here we report a finding of pressure- induced suppression of the superconducting transition temperature Tc and enhancement of the temperature of the resistance hump TH through charge transfer between two iron sites with different occupancies. The activation energy for the electric transport of the high-temperature resistance is observed to go to zero at a critical pressure of 8.7 GPa, at which superconductivity tends to disappear and the semiconductor-to-metal transition takes place. Beyond the critical point, the resistance exhibits a metallic behavior over the whole temperature range studied. All these features indicate the existence of quantum criticality in iron-selenide superconductors.

cond-mat.supr-con↗

arXiv2012

Pressure-induced amorphization and polyamorphism in one-dimensional single crystal TiO2 nanomaterials

The structural phase transitions of single crystal TiO2-B nanoribbons were investigated in-situ at high-pressure using the synchrotron X-ray diffraction and the Raman scattering. Our results have shown a pressure-induced amorphization (PIA) occurred in TiO2-B nanoribbons upon compression, resulting in a high density amorphous (HDA) form related to the baddeleyite structure. Upon decompression, the HDA form transforms to a low density amorphous (LDA) form while the samples still maintain their pristine nanoribbon shape. HRTEM imaging reveals that the LDA phase has an α-PbO2 structure with short range order. We propose a homogeneous nucleation mechanism to explain the pressure-induced amorphous phase transitions in the TiO2-B nanoribbons. Our study demonstrates for the first time that PIA and polyamorphism occurred in the one-dimensional (1D) TiO2 nanomaterials and provides a new method for preparing 1D amorphous nanomaterials from crystalline nanomaterials.

cond-mat.mtrl-sci↗

arXiv2012

Reemerging superconductivity at 48 K across quantum criticality in iron chalcogenides

Pressure plays an essential role in the induction1 and control2,3 of superconductivity in iron-based superconductors. Substitution of a smaller rare-earth ion for the bigger one to simulate the pressure effects has surprisingly raised the superconducting transition temperature Tc to the record high 55 K in these materials4,5. However, Tc always goes down after passing through a maximum at some pressure and the superconductivity eventually tends to disappear at sufficiently high pressures1-3. Here we show that the superconductivity can reemerge with a much higher Tc after its destruction upon compression from the ambient-condition value of around 31 K in newly discovered iron chalcogenide superconductors. We find that in the second superconducting phase the maximum Tc is as high as 48.7 K for K0.8Fe1.70Se2 and 48 K for (Tl0.6Rb0.4)Fe1.67Se2, setting the new Tc record in chalcogenide superconductors. The presence of the second superconducting phase is proposed to be related to pressure-induced quantum criticality. Our findings point to the potential route to the further achievement of high-Tc superconductivity in iron-based and other superconductors.

cond-mat.supr-con↗

arXiv2012

Spiral Chain O4 Form of Dense Oxygen

Oxygen is in many ways a unique element: the only known diatomic molecular magnet and the capability of stabilization of the hitherto unexpected O8 cluster structure in its solid form at high pressure. Molecular dissociations upon compression as one of the fundamental problems were reported for other diatomic solids (e.g., H2, I2, Br2, and N2), but it remains elusive for solid oxygen, making oxygen an intractable system. We here report the theoretical prediction on the dissociation of molecular oxygen into a polymeric spiral chain O4 structure (θ-O4) by using first-principles calypso method on crystal structure prediction. The θ-O4 stabilizes above 2 TPa and has been observed as the third high pressure phase of sulfur (S-III). We find that the molecular O8 phase remains extremely stable in a large pressure range of 0.008 - 2 TPa, whose breakdown is driven by the pressure-induced instability of a transverse acoustic phonon mode at zone boundary, leading to the ultimate formation of θ-O4. Remarkably, stabilization of θ-O4 turns oxygen from a superconductor into an insulator with a wide band gap (approximately 5.9 eV) originating from the sp3-like hybridized orbitals of oxygen and the localization of valence electrons. (This is a pre-print version of the following article: Li Zhu et al, Spiral chain O4 form of dense oxygen, Proc. Natl. Acad. Sci. U.S.A. (2011), doi: 10.1073/pnas.1119375109, which has been published online at http://www.pnas.org/content/early/2011/12/27/1119375109 .)

cond-mat.mtrl-sci↗

arXiv2005

Crystal structures of superconducting phases of S and Se

Compressed S and Se are studied by x-ray diffraction with synchrotron radiation up to 160 GPa. The S-IV phase is shown to have a body-centered monoclinic structure and to be stable between 83 and 150 GPa on pressure increase, where it transform to S-V with a primitive rhombohedral $β$-Po structure. Observation of the modulation reflections in S-IV up to 135 GPa shows that its crystal structure is incommensurately modulated, as recently reported for Se and Te. The modulated body-centered monoclinic phase of Se, Se-IV, is shown to transform to the $β$-Po phase Se-V at around 80 GPa. Se-V transforms to a body-centered cubic phase at 140 GPa in accordance with previous studies. Pressure dependence of the structural parameters of these high-pressure phases in S and Se are discussed in relation to their superconducting behaviour.

cond-mat.other↗

arXiv2004

High-pressure phase relations of Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ single crystals

We have investigated the pressure dependence of the superconducting transition temperature $T_{c}$ up to 18 GPa of Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+δ}$ single crystals ranging from the highly underdoped through the nearly optimally doped to the highly overdoped level. For all three samples studied, $T_{c}$ is found to increase initially and then saturate at a critical pressure $P_{c}$ but decrease modestly with further compression. Oxygen doping tends to reduce the increase in $T_{c}$ and $P_{c}$. A new high-pressure phase diagram between the saturated $T_{c}$ and $P_{c}$ is then obtained. Theoretical interpretation is given by using the competition between the hole carrier density and pairing interaction strength based on the high-pressure transport data of the resistivity and Hall coefficient in this system.

cond-mat.supr-con↗

arXiv2004

Pressure-induced phonon frequency shifts in transition-metal nitrides

We report the first experiments on the high pressure phonon spectra of transition-metal nitrides HfN, ZrN, and NbN, obtained by Raman scattering measurements. Two pronounced bands, which are related to the acoustic part at low frequency around 200 cm$^{-1}$ and the optical part at high frequency around 550 cm$^{-1}$ of the phonon spectrum, respectively, shift to high frequency values with increasing pressure. An analysis of the results allows us to reproduce the experimental pressure dependence of the superconducting transition temperature $T_{c}$ of ZrN and NbN.

cond-mat.supr-con↗

arXiv2002

New Methods for Investigating Superconductivity at Very High Pressures

We review recent advances in diamond anvil cell development, focusing on the details of magnetic susceptibility techniques. We have developed and implemented highly sensitive technique that allowed observations of superconductivity using magnetic susceptibility at megabar pressures, including the observation of a Tc in sulfur to above 230 GPa. The advancement of the technique should enable the most demanding diamond anvil cell applications. The Tc(P) data for simple s-p metals (Se,S, MgB_2) are presented and analyzed. The possibility for a phonon-assisted electronic topological transition (ETT) in MgB_2 at high pressure is discussed.

cond-mat.supr-con↗