Ho-Kwang Mao

Center for High Pressure Science and Technology Advanced Research, Pootung, Shanghai Shi, China

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Publications (506)2629.96 Total impact

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    ABSTRACT: Pressure-induced polymerization of charged triple-bond monomers like acetylide and cyanide could lead to formation of a conductive metal-carbon network composite, thus providing a new route to synthesize inorganic/organic conductors with tunable composition and properties. The industry application of this promising synthetic method is mainly limited by the reaction pressure needed, which is often too high to be reached for gram amounts of sample. Here we successfully synthesized highly conductive Li3Fe(CN)6 at maximum pressure around 5 GPa and used in situ diagnostic tools to follow the structural and functional transformations of the sample, including in situ X-ray and neutron diffraction and Raman and impedance spectroscopy, along with the neutron pair distribution function measurement on the recovered sample. The cyanide anions start to react around 1 GPa and bond to each other irreversibly at around 5 GPa, which are the lowest reaction pressures in all known metal cyanides and within the technologically achievable pressure range for industrial production. The conductivity of the polymer is above 10(-3) S·cm(-1), which reaches the range of conductive polymers. This investigation suggests that the pressure-induced polymerization route is practicable for synthesizing some types of functional conductive materials for industrial use, and further research like doping and heating can hence be motivated to synthesize novel materials under lower pressure and with better performances.
    Inorganic Chemistry 11/2015; DOI:10.1021/acs.inorgchem.5b01851 · 4.76 Impact Factor
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    Physical Review B 11/2015; 92(17). DOI:10.1103/PhysRevB.92.174106 · 3.74 Impact Factor
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    ABSTRACT: Raman spectroscopy and angle dispersive X-ray diffraction (XRD) experiments of bismuth selenide (Bi2Se3) have been carried out to pressures of 35.6 and 81.2 GPa, respectively, to explore its pressure induced phase transformation. The experiments indicate that a progressive structural evolution occurs from an ambient rhombohedra phase (Space group (SG): R-3m) to monoclinic phase (SG: C2/m) and eventually to a high pressure body-centered tetragonal phase (SG: I4/mmm). Evidenced by our XRD data up to 81.2 GPa, the Bi2Se3 crystallizes into body-centered tetragonal structures rather than the recently reported disordered body-centered cubic (BCC) phase. Furthermore, first principles theoretical calculations favor the viewpoint that the I4/mmm phase Bi2Se3 can be stabilized under high pressure (>30 GPa). Remarkably, the Raman spectra of Bi2Se3 from this work (two independent runs) are still Raman active up to ~35 GPa. It is worthy to note that the disordered BCC phase at 27.8 GPa is not observed here. The remarkable difference in atomic radii of Bi and Se in Bi2Se3 may explain why Bi2Se3 shows different structural behavior than isocompounds Bi2Te3 and Sb2Te3.
    Scientific Reports 11/2015; 5:15939. DOI:10.1038/srep15939 · 5.58 Impact Factor
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    ABSTRACT: The systematic evolution of the structural, vibrational, and superconducting properties of nearly optimally doped Tl2Ba2CaCu2O8+δ with pressure up to 30 GPa is studied by x-ray diffraction, Raman scattering, and magnetic susceptibility measurements. No phase transformation is observed in the studied pressure regime. The obtained lattice parameters and unit-cell volume continuously decrease with pressure by following the expected equation of state. The axial ratio of c/a exhibits an anomaly starting from 9 GPa. At such a pressure level, the deviation from the nonlinear variation of the phonon frequencies is detected. Both the above observations indicate the enhancement of the distortion upon compression. The superconducting transition temperature is found to exhibit a parabolic behavior with a maximum of 114 K around 7 GPa. We demonstrate that the interplay between the intrinsic pressure variables and distortion controls the superconductivity.
    Journal of Physics Condensed Matter 10/2015; 27(44):445701. DOI:10.1088/0953-8984/27/44/445701 · 2.35 Impact Factor
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    ABSTRACT: The addition polymerization of charged monomers like C≡C2– and C≡N– is scarcely seen at ambient conditions but can progress under external pressure with their conductivity significantly enhanced, which expands the research field of polymer science to inorganic salts. The reaction pressures of transition metal cyanides like Prussian blue and K3Fe(CN)6 are much lower than that of alkali cyanides. To figure out the effect of the transition metal on the reaction, the crystal structure and electronic structure of K3Fe(CN)6 under external pressure are investigated by in situ neutron diffraction, in situ X-ray absorption fine structure (XAFS), and neutron pair distribution functions (PDF) up to ∼15 GPa. The cyanide anions react following a sequence of approaching–bonding–stabilizing. The Fe(III) brings the cyanides closer which makes the bonding progress at a low pressure (2–4 GPa). At ∼8 GPa, an electron transfers from the CN to Fe(III), reduces the charge density on cyanide ions, and stabilizes the reaction product of cyanide. From this study we can conclude that bringing the monomers closer and reducing their charge density are two effective routes to decrease the reaction pressure, which is important for designing novel pressure induced conductor and excellent electrode materials.
    The Journal of Physical Chemistry C 09/2015; 119(39):150914115329002. DOI:10.1021/acs.jpcc.5b06793 · 4.77 Impact Factor
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    ABSTRACT: We fabricated mono-dispersed hollow waxberry shaped β-quartz GeO2 by a facile one-step synthesis in emulsion at room temperature. TEM images indicated that hollow waxberry shaped GeO2 were consisted of nano-sphere whose average size were estimated to be 20 nm. The growth mechanism and optical properties of the products were also investigated. It was found that addition of n-butanol and PVP were crucial factors to control the morphology of GeO2. The possible formation mechanism of the hollow interior is proposed as the Ostwald ripening. The optical properties of the β-GeO2 nanoparticles with hollow shapes were also studied with photoluminescence spectrum, which reveals a broad emission, suggesting potential applications in electronic and optoelectronic nanodevices. These attractive results provide us a new simple method further used to fabricate other specific hollow structure and indicate hollow waxberry shaped GeO2 may have potential applications in light-emitting nanodevices.
    Journal of Nanoscience and Nanotechnology 09/2015; 15(2):1732-7. DOI:10.1166/jnn.2015.9062 · 1.56 Impact Factor
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    ABSTRACT: Phase separation is a crucial ingredient of the physics of manganites; however, the role of mixed phases in the development of the colossal magnetoresistance (CMR) phenomenon still needs to be clarified. We report the realization of CMR in a single-valent LaMnO3 manganite. We found that the insulator-to-metal transition at 32 GPa is well described using the percolation theory. Pressure induces phase separation, and the CMR takes place at the percolation threshold. A large memory effect is observed together with the CMR, suggesting the presence of magnetic clusters. The phase separation scenario is well reproduced, solving a model Hamiltonian. Our results demonstrate in a clean way that phase separation is at the origin of CMR in LaMnO3.
    Proceedings of the National Academy of Sciences 09/2015; 112(35):10869-72. DOI:10.1073/pnas.1424866112 · 9.67 Impact Factor
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    Zhimei Sun · Jian Zhou · Zhitang Song · Rajeev Ahuja · Ho-Kwang Mao · Yuanchun Pan ·

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    Xiaozhi Yan · Dayong Tan · Xiangting Ren · Wenge Yang · Duanwei He · Ho-Kwang Mao ·
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    ABSTRACT: In this article, we present the abnormal compression and plastic behavior of germanium during the pressure-induced cubic diamond to β-tin structure transition. Between 8.6 GPa and 13.8 GPa, in which pressure range both phases are co-existing, first softening and followed by hardening for both phases were observed via synchrotron x-ray diffraction and Raman spectroscopy. These unusual behaviors can be interpreted as the volume misfit between different phases. Following Eshelby, the strain energy density reaches the maximum in the middle of the transition zone, where the switch happens from softening to hardening. Insight into these mechanical properties during phase transformation is relevant for the understanding of plasticity and compressibility of crystal materials when different phases coexist during a phase transition.
    Applied Physics Letters 04/2015; 106(17):171902. DOI:10.1063/1.4919003 · 3.30 Impact Factor
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    ABSTRACT: 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$_{8+\delta}$ 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.
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    ABSTRACT: 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.
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    ABSTRACT: 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.
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    ABSTRACT: 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.
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    ABSTRACT: Phase transition of solid-state materials is a fundamental research topic in condensed matter physics, materials science and geophysics. It has been well accepted and widely proven that isostructural compounds containing different cations undergo same pressure-induced phase transitions but at progressively lower pressures as the cation radii increases. However, we discovered that this conventional law reverses in the structural transitions in 122-type iron-based superconductors. In this report, a combined low temperature and high pressure X-ray diffraction (XRD) measurement has identified the phase transition curves among the tetragonal (T), orthorhombic (O) and the collapsed-tetragonal (cT) phases in the structural phase diagram of the iron-based superconductor AFe2As2 (A = Ca, Sr, Eu, and Ba). The cation radii dependence of the phase transition pressure (T → cT) shows an opposite trend in which the compounds with larger ambient radii cations have a higher transition pressure.
    Scientific Reports 11/2014; 4:7172. DOI:10.1038/srep07172 · 5.58 Impact Factor
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    Chang-Sheng Zha · R E Cohen · Ho-Kwang Mao · Russell J Hemley ·

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    ABSTRACT: A 75 kW, 915 MHz microwave plasma-assisted chemical vapor deposition system was adapted and utilized to scale up production of high-quality single-crystal diamonds at high growth rates. A 300 mm diameter plasma discharge was achieved with uniform temperature distributions of ±250 °C on up to 300 single-crystal diamond substrates. Diamond single crystals were synthesized from H2/CH4/N2 gas mixtures at pressures between 90 and 180 Torr, with recorded growth rates from 10 to 30 μm/h. The source of N2 was from vacuum chamber leakage, and it greatly affected synthesis chemistry. Optical emission spectroscopy was used to probe the localized plasma chemistry and plasma uniformity at different gas pressures. Production rates of up to 100 g/day of single-crystal diamonds were demonstrated, with 25% of the material categorized as colorless. Crystals up to 3.5 mm in thickness could be produced during a single deposition run. The quality of the crystals produced was assessed by photoluminescence and UV–visible absorption spectroscopies.
    Crystal Growth & Design 06/2014; 14(7):3234–3238. DOI:10.1021/cg500693d · 4.89 Impact Factor
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    ABSTRACT: We report an anomalous phase transition in compressed In2Se3. The high-pressure studies indicate that In2Se3 transforms to a new isosymmetric R-3m structure at 0.8 GPa whilst the volume collapses by 7%. This phase transition involves a pressure-induced interlayer shear glide with respect to one another. Consequently, the outer Se atoms of one sheet locate into the interstitial sites of three Se atoms in the neighboring sheets that are weakly connected by van der Waals interaction. Interestingly, this interlayer shear glide changes the stacking sequence significantly but leaves crystal symmetry unaffected. This study provides an insight to the mechanisms of the intriguing isosymmetric phase transition.
    Applied Physics Letters 05/2014; 104(21):212102. DOI:10.1063/1.4879832 · 3.30 Impact Factor
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    ABSTRACT: The mineralogical constitution of the Earth’s mantle dictates the geophysical and geochemical properties of this region. Previous models of a perovskite-dominant lower mantle have been built on the assumption that the entire lower mantle down to the top of the D″ layer contains ferromagnesian silicate [(Mg,Fe)SiO3] with nominally 10 mole percent Fe. On the basis of experiments in laser-heated diamond anvil cells, at pressures of 95 to 101 gigapascals and temperatures of 2200 to 2400 kelvin, we found that such perovskite is unstable; it loses its Fe and disproportionates to a nearly Fe-free MgSiO3 perovskite phase and an Fe-rich phase with a hexagonal structure. This observation has implications for enigmatic seismic features beyond ~2000 kilometers depth and suggests that the lower mantle may contain previously unidentified major phases.
    Science 05/2014; 344(6186):877-82. DOI:10.1126/science.1250274 · 33.61 Impact Factor

Publication Stats

16k Citations
2,629.96 Total Impact Points


  • 2012-2015
    • Center for High Pressure Science and Technology Advanced Research
      Pootung, Shanghai Shi, China
    • Ehime University
      • Geodynamics Research Center
      Matuyama, Ehime, Japan
  • 1974-2013
    • Carnegie Institution for Science
      • Geophysical Laboratory
      Washington, WV, United States
  • 2002-2012
    • Carnegie Institute
      Washington, Washington, D.C., United States
  • 2008-2011
    • Jilin University
      • State Key Lab of Superhard Materials
      Jilin, Jilin Sheng, China
    • University of Nevada, Las Vegas
      Las Vegas, Nevada, United States
  • 2006-2011
    • Zhejiang University
      • Department of Material Science and Engineering
      Hang-hsien, Zhejiang Sheng, China
    • James Cook University
      Townsville, Queensland, Australia
  • 1986-2011
    • The Washington Institute
      Washington, Washington, D.C., United States
  • 2005-2008
    • Argonne National Laboratory
      • Division of Materials Science
      Lemont, Illinois, United States
  • 2007
    • The University of Tokyo
      • Institute for Solid State Physics
      Tokyo, Tokyo-to, Japan
  • 2003-2005
    • University of Chicago
      • • James Franck Institute
      • • Department of Geophysical Sciences
      Chicago, IL, United States
  • 2001
    • Princeton University
      Princeton, New Jersey, United States
  • 2000
    • Loyola University Maryland
      • Department of Physics
      Baltimore, Maryland, United States
  • 1993
    • Johns Hopkins University
      • Department of Earth and Planetary Sciences
      Baltimore, Maryland, United States