We present theoretical investigations of pressure and temperature driven phase transitions in HgTe quantum wells grown on CdTe buffer. Using the 8-band \textbf{k$\cdot$p} Hamiltonian we calculate evolution of energy band structure at different quantum well width with hydrostatic pressure up to 20 kBar and temperature ranging up 300 K. In particular, we show that in addition to temperature, tuning of hydrostatic pressure allows to drive transitions between semimetal, band insulator and topological insulator phases. Our realistic band structure calculations reveal that the band inversion under hydrostatic pressure and temperature may be accompanied by non-local overlapping between conduction and valence bands. The pressure and temperature phase diagrams are presented.
We report on Terahertz detection by inverted band structure HgTe-based Field Effect Transistor up to room temperature. At low temperature, we show that nonlinearities of the transistor channel allows for the observation of the quantum phase transition due to the avoided crossing of zero-mode Landau levels in HgTe 2D topological insulators. These results pave the way towards Terahertz topological Field Effect Transistors.
We report on temperature-dependent magnetospectroscopy of two HgTe/CdHgTe quantum wells below and above the critical well thickness $d_c$. Our results, obtained in magnetic fields up to 16 T and temperature range from 2 K to 150 K, clearly indicate a change of the band-gap energy with temperature. The quantum well wider than $d_c$ evidences a temperature-driven transition from topological insulator to semiconductor phases. At the critical temperature of 90 K, the merging of inter- and intra-band transitions in weak magnetic fields clearly specifies the formation of gapless state, revealing the…
We report ab initio calculations of the electronic band structure and the phonon dispersion relations of the zincblende-type mercury chalcogenides (beta-HgS, HgSe, and HgTe). The latter have been used to evaluate the temperature dependence of the specific heat which has been compared with experimental data. The electronic band structure of these materials has been confirmed to have an inverted direct gap of the alpha-tin type, which makes HgSe and HgTe semimetallic. For beta-HgS, however, our calculations predict a negative spin-orbit splitting which restores semiconducting properties to the m…
In search of materials with three-dimensional flat band dispersions, using {\em ab-initio} computations, we investigate how topological phases evolve as a function of hydrostatic pressure and uniaxial strain in two types of superlattices: HgTe/CdTe and HgTe/HgSe. In short-period HgTe/CdTe superlattices, our analysis unveils the presence of isoenergetic nodal lines, which could host strain-induced three-dimensional flat bands at the Fermi level without requiring doping, when fabricated, for instance, as core-shell nanowires. In contrast, HgTe/HgSe short-period superlattices are found to harbor …
We describe the fine structure of Dirac states in HgTe/CdHgTe quantum wells of critical and close-to-critical thickness and demonstrate the formation of an anticrossing gap between the tips of the Dirac cones driven by interface inversion asymmetry. By combining symmetry analysis, atomistic calculations, and k-p theory with interface terms, we obtain a quantitative description of the energy spectrum and extract the interface mixing coefficient. The zero-magnetic-field splitting of Dirac cones can be experimentally revealed in studying magnetotransport phenomena, cyclotron resonance, Raman scat…
Many-particle hybridization of optical transitions from zero-mode Landau levels in HgTe quantum wells
Laboratoire Charles Coulomb (L2C), UMR 5221 CNRS-Université de Montpellier（勒内·孔洛实验室）；Physics Department, M.V. Lomonosov Moscow State University（莫斯科国立大学物理系）；CEA-LETI, MINATEC Campus, DOPT（CEA-LETI）
The field of topological insulators (TIs) is rapidly growing. Concerning possible applications, the search for materials with an easily controllable TI phase is a key issue. The quantum spin Hall effect, characterized by a single pair of helical edge modes protected by time-reversal symmetry, has been demonstrated in HgTe-based quantum wells (QWs) with an inverted bandgap. We analyze the topological properties of a generically coupled HgTe-based double QW (DQW) and show how in such a system a TI phase can be driven by an inter-layer bias voltage, even when the individual layers are non-inverte…
In this letter, we describe the stabilization of indium antimonide (InSb) in the high-pressure orthorhombic phase (InSb-III) at ambient conditions. Until now, InSb-III has only been observed above 9 GPa, or at around 3 GPa as a metastable structure during the phase transition from cubic zinc blende (InSb-I) to orthorhombic InSb-IV. The crystalline phase transition from InSb-I to InSb-III was driven by an ultrashort, laser-generated, non-hydrostatic pressure pulse. The transition occurred in preferred orientations locked to the initial orientation of the InSb-I crystal, breaking the symmetry of…
We describe observations of a novel hysteresis behavior in the growth of ice crystals under near-vacuum conditions. Above a threshold supersaturation, we find that the ice growth rate often exhibits a sudden increase that we attribute to an impurity-driven growth instability. We examine possible mechanisms for this instability, which can be used to produce clean, faceted ice surfaces.
We investigate the elementary steps at the microscopic level for proton diffusion in brucite under high pressure, which results from a complex interplay between two processes: the O-H reorientations motion around the $\mathbf c$ axis and O-H covalent bond dissociations. First-principle path-integral molecular dynamics simulations reveal that the increasing pressure tends to lock the former motion, while, in contrast, it activates the latter which is mainly triggered by nuclear quantum effects. These two competing effects therefore give rise to a pressure sweet spot for proton diffusion within …
We have observed a massive reconstruction of the Fermi surface of single crystal chromium as a function of high pressure and high magnetic fields caused by the spin-flip transition, with multiple new orbits appearing above 0.93 GPa. Additionally, some orbits have field-induced effective masses of ~0.06-0.07 me, seen only at high magnetic fields. Based on the temperature insensitivity displayed by the oscillation amplitudes at these frequencies, we attribute the orbits to quantum interference rather than to Landau quantization.
The effect of hydrostatic pressure up to 27 GPa on the Raman scattering (RS) in bulk HfS$_2$ is investigated. There are two transformations of RS spectra, which take place during compression at pressure between 5.7 GPa and 9.8 GPa as well as between 12.8 GPa and 15.2 GPa. Seven vibrational modes can be observed after the transformation, as compared to four modes before the transformation. The observed change suggests structural change in the material of yet unknown nature. The frequencies of the RS modes observed above the transformation change linearly with pressure and corresponding pressure…
A detailed high pressure investigation is carried out on $Fe_4Nb_2O_9$ using angle resolved x-ray diffraction and Raman spectroscopy measurements. We find a structural transition from the ambient trigonal phase to a monoclinic phase above 8.8 GPa. The structural transition is assumed to be driven by a large distortion of $Nb-O_6$ octahedra as seen from x-ray diffraction analysis and a large pressure dependence of $Nb-O_6$ octahedra breathing Raman mode. Anomalous behaviour of Raman modes and increase in the phonon life time at the phase transition pressure indicate a trigonal paramagnetic phas…
We present a high-pressure investigation of the semiconductor-to-metal transition in MoS2 and WS2 carried out by synchrotron-based far-infrared spectroscopy, to reconcile the controversial estimates of the metallization pressure found in the literature and gain new insight into the mechanisms ruling this electronic transition. Two spectral descriptors are found indicative of the onset of metallicity and of the origin of the free carriers in the metallic state: the absorbance spectral weight, whose abrupt increase defines the metallization pressure threshold, and the asymmetric lineshape of the…
Layered transition-metal compounds with controllable magnetic behaviors provide many fascinating opportunities for the fabrication of high-performance magneto-electric and spintronic devices. The tuning of their electronic and magnetic properties is usually limited to the change of layer thickness, electrostatic doping, and the control of electric and magnetic fields. However, pressure has been rarely exploited as a control parameter for tailoring their magneto-electric properties. Here, we report a unique pressure-driven isostructural phase transition in layered CrCl3 accompanied by a simulta…
Dehydrogenation of alkanes is of increasing importance in fulfilling global demand for olefins and offers a potential source of carbon-neutral hydrogen as a co-product. Currently commercial dehydrogenation processes occur at high-temperatures (500-900$^\circ$C) which is energy intensive and results in side reactions and rapid coking of the catalysts. In addition the hydrogen produced is often burned to maintain temperature and to inhibit the back reaction. Here we demonstrate pressure as a parameter to enable novel chemical catalytic processes and demonstrate ambient-temperature dehydrogenatio…
The pressure induced bcc to hcp transition in Fe has been investigated via ab-initio electronic structure calculations. It is found by the disordered local moment (DLM) calculations that the temperature induced spin fluctuations result in the decrease of the energy of Burgers type lattice distortions and softening of the transverse $N$-point $TA_1$ phonon mode with $[\bar{1}10]$ polarization. As a consequence, spin disorder in an system leads to the increase of the amplitude of atomic displacements. On the other hand, the exchange coupling parameters obtained in our calculations strongly decre…
Through model Hamiltonian studies and first-principle electronic structure calculations, we have examined the effect of inversion symmetry breaking (ISB) field and hydrostatic pressure on the band topology of halide perovskites by taking MAPbI$_3$ as a prototype. Our study shows that while hydrostatic pressure induces normal to topological insulator continuous phase transition, the ISB field makes it first order. The pressure smoothly reduces the normal bandgap, and without ISB, the system achieves a gapless state before it produces a non-trivial bandgap with inverted characters. The ISB field…
Hybrid perovskites have been at the forefront of condensed matter research particularly in context of device applications primarily in relation to applications in the field of solar cells. In this article, we demonstrate that several new functionalities may be added to the arsenal of hybrid perovskites, in terms of external stimuli driven spin transitions as well as piezochromism. As an example, we study Dimethylammonium Manganese Formate (DMAMnF), a hybrid perovskite investigated quite extensively experimentally. We show by employing first principles DFT+U calculations with the aid of ab init…
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 undulat…
We study lanthanum mononitride LaN by first-principles calculations. The commonly reported rock-salt structure of $Fm\bar{3}m$ symmetry for rare-earth monopnictides is found dynamically unstable for LaN at zero temperature. Using density functional theory and evolutionary crystal prediction, we discover a new, dynamically stable structure with $P1$ symmetry at 0 K. This $P1$-LaN exhibits spontaneous electric polarization. Our ab initio molecular dynamics simulations of finite-temperature phonon spectra further suggest that LaN will undergo ferroelectric and structural transitions from $P1$ to …
The transformation pathways of carbon at high pressures are of broad interest for synthesis of novel materials and for revealing the Earth's geological history. We have applied large plastic shear on graphite in rotational anvils to form hexagonal and nanocrystalline cubic diamond at extremely low pressures of 0.4 and 0.7 GPa, which are 50 and 100 times lower than the transformation pressures under hydrostatic compression and well below the phase equilibrium. Large shearing accompanied with pressure elevation to 3 GPa also leads to formation of a new orthorhombic diamond phase. Our results dem…
The high-pressure properties of fluorine and chlorine are not yet well understood because both are highly reactive and volatile elements, which has made conducting diamond anvil cell and x-ray diffraction experiments a challenge. Here we use ab initio methods to search for stable crystal structures of both elements at megabar pressures. We demonstrate how symmetry and geometric constraints can be combined to efficiently generate crystal structures that are composed of diatomic molecules. Our algorithm extends the symmetry driven structure search method [Phys. Rev. B 98 (2018) 174107] by adding…
Crystal structure prediction with theoretical methods is particularly challenging when unit cells with many atoms need to be considered. Here we employ a symmetry-driven structure search (SYDSS) method and combine it with density functional theory (DFT) to predict novel crystal structures at high pressure. We sample randomly from all 1,506 Wyckoff positions of the 230 space groups to generate a set of initial structures. During the subsequent structural relaxation with DFT, existing symmetries are preserved, but the symmetries and the space group may change as atoms move to more symmetric posi…
High-Pressure Structural Evolution of Na2ZrSi2O7 and Na2ZrSi2O7.H2O: Topology-Driven Compression Behaviors, Phase Stability, and Electronic Transitions
Universitat de Valencia（瓦伦西亚大学）；Center for High Pressure Science and Technology Advanced Research (HPSTAR)（高压科学和技术先进研究中心）；Nankai University（南开大学）；CELLS-ALBA Synchrotron Light Facility（CELLS-ALBA同步辐射光源设施）；Bhabha Atomic Research Center (BARC)（巴哈原子研究中心）
Charged nitrogen dimers are ubiquitous in high-pressure binary metal-nitrogen systems. They are known to possess integer formal charges x varying from one through four. Here, we present the investigation of the binary alkali- and alkaline earth metal-nitrogen systems, Na-N, Ca-N, Sr-N, Ba-N to 70 GPa. We report on compounds-Na3(N2)4, Ca3(N2)4, Sr3(N2)4, and Ba(N2)3-featuring charged nitrogen dimers with paradigm-breaking non-integer charges, x = 0.67, 0.75 and 1.5. The metallic nature of all four compounds is deduced from ab initio calculations. The conduction electrons occupy the pi* antibond…
The co-occurrence of phase transitions with local and global order parameters, such as the entangled magnetization and topological invariant, is attractive but has been seldom realized experimentally. Here, by using high-pressure in-situ X-ray diffraction, high-pressure electric transport measurements and high-pressure first-principles calculations, we report a magneto-topological phase transition, i.e., the phenomenon of magnetic materials undergoing different magnetic and topological phases during the process of pressure loading, in a recently discovered magnetic Weyl semimetal Co3Sn2S2. By …
Intrinsic magnetic topological insulators provide an ideal platform to achieve various exciting physical phenomena. However, this kind of materials and related research are still very rare. In this work, we reported the electronic and structural phase transitions in intrinsic magnetic topological insulator MnSb2Te4 driven by hydrostatic pressure. Electric transport results revealed that temperature dependent resistance showed a minimum value near short-range antiferromagnetic (AFM) ordering temperature TN', the TN' values decline with pressure, and the AFM ordering was strongly suppressed near…
By first-principles calculation based on the density functional theory (DFT) with the modified Becke-Johnson local density approximation plus Hubbard U (MBJLDA+U), we studied the band structures of the Yb chalcogenides YbO and YbS under ambient and high pressures. It was revealed that both YbO and YbS have a trivial band topology under ambient pressure, and a nontrivial band topology under high pressure. The topological phase transition is reduced by the pressure-driven single-band inversion between 5d- and 4f -orbitals at the time-reversal invariant momentum (TRIM) point X. A bulk Dirac cone …
Application of about 0.8 GPa pressure is sufficient to induce the neutral-ionic transition in the mixed stack charge-transfer crystal 2-chloro-5-methyl-$p$-phenylenediamine--2,5-dimethyl-dicyanoquinonediimine ({\CD}). The ionicity increases continuously from $\sim$ 0.35 at ambient conditions to $\sim$ 0.65 when the pressure is raised up to 2 GPa. Moreover, stack dimerization begins well before the crossing of the neutral-ionic interface. The evolution of the transition is similar to what observed in the temperature induced phase change in the same compound. (cond-mat/0101179) A distinguishing …
The metal-insulator and spin state transitions of CoO under high pressure are studied by using density functional theory combined with dynamical mean-field theory. Our calculations predict that the metal-insulator transition in CoO is a typical orbital selective Mott transition, where the $t_{2g}$ orbitals of Co 3d shell become metallic firstly around 60 GPa while the $e_g$ orbitals still remain insulating until 170 GPa. Further studies of the spin states of Co 3d shell reveal that the orbital selective Mott phase in the intermediate pressure regime is mainly stabilized by the high-spin state …
Radiation hydrodynamics simulations were used to study the effect of plastic ablators in laser-driven shock experiments. The sensitivity to composition and equation of state was found to be 5-10% in ablation pressure. As was found for metals, a laser pulse of constant irradiance gave a pressure history which decreased by several percent per nanosecond. The pressure history could be made more constant by adjusting the irradiance history. The impedance mismatch with the sample gave an increase o(100%) in the pressure transmitted into the sample, for a reduction of several tens of percent in the …
The Local Density Approximation combined with Dynamical Mean-Field Theory (LDA+DMFT method) is applied to the study of the paramagnetic and magnetically ordered phases of hematite Fe$_2$O$_3$ as a function of volume. As the volume is decreased, a simultaneous 1st order insulator-metal and high-spin to low-spin transition occurs close to the experimental value of the critical volume. The high-spin insulating phase is destroyed by a progressive reduction of the charge gap with increasing pressure, upon closing of which the high spin phase becomes unstable. We conclude that the transition in Fe$_…
Activating metamagnetic transitions between ordered states in van der Waals magnets and devices bring great opportunities in spintronics. We show that external pressure, which enhances the interlayer hopping without introducing chemical disorders, triggers multiple metamagnetic transitions upon cooling in the topological van der Waals magnets Mn(Bi$_{1-x}$Sb$_x$)$_4$Te$_7$, where the antiferromagnetic interlayer superexchange coupling competes with the ferromagnetic interlayer coupling mediated by the antisite Mn spins. The temperature-pressure phase diagrams reveal that while the ordering tem…
This paper presents results for systems formed in a solid glassy state after nanocrystallization process above the glass temperature. We analyze electric conductivity and relaxation processes after such treatment under high temperature (HT) and high pressure (HP-HT) as well. The latter leads to ca. 8% increase of density, two decades (100) increase of electric conductivity as well as qualitative changes in relaxation processes. The previtreous-type changes of the relaxation time on cooling is analyzed by the use of critical-like and the 'critical-activated' description. Presented results corre…
In rare-earth compounds with valence fluctuation, the proximity of the 4f level to the Fermi energy leads to instabilities of the charge configuration and the magnetic moment. Here, we provide direct experimental evidence for an induced magnetic polarization of the Eu$^{3+}$ atomic shell with J=0, due to intra-atomic exchange and spin-orbital coupling interactions with Eu$^{2+}$ atomic shell. By applying external pressure, a transition from antiferromagnetic to a fluctuating behavior in a EuNiGe$_3$ single crystals is probed. Magnetic polarization is observed for both valence states of Eu$^{2+…
In the context of a nonequilibrium statistical thermodynamics, based on a nonequilibrium statistical ensemble formalism, a generalized hydrodynamics of fluids under driven flow and shear stress is derived. At the thermodynamic level, the nonequilibrium equations of state are derived, which are coupled to the evolution of the basic variables that describe the hydrodynamic motion in such a system. Generalized diffusion-advection and Maxwell-Cattaneo advection equations are obtained in appropriate limiting situations. This nonlinear higher-order hydrodynamics is applied, in an illustration, to th…
The localized-itinerant nature of Ce-4$f$ valence electrons in heavy fermion compound CeIn$_{3}$ under pressure is studied thoroughly by means of the combination of density functional theory and single-site dynamical mean-field theory. The detailed evolutions of electronic structures of CeIn$_{3}$, including total and partial density of states, momentum-resolved spectral functions, and valence state histograms etc., are calculated in a wide pressure range where the corresponding volume compression $V/V_0 \in [0.6,1.0]$ (here $V_0$ is the experimental crystal volume) at $T \cong 116$ K. Upon in…
We report the development of a technique to measure heat capacity at large uniaxial pressure using a piezoelectric-driven device generating compressive and tensile strain in the sample. Our setup is optimized for temperatures ranging from 8 K down to millikelvin. Using an AC heat-capacity technique we are able to achieve an extremely high resolution and to probe a homogeneously strained part of the sample. We demonstrate the capabilities of our setup on the unconventional superconductor Sr$_2$RuO$_4$. By replacing thermometer and adjusting the remaining setup accordingly the temperature regime…
Structural responses incipient to pressure-driven antiferromagnetic quantum critical point of van der Waals heavy-fermion metal CeSiI
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院）；School of Physics and Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education), Renmin University of China（中国人民大学物理学院）；Department of Advanced Materials Science, Graduate School of Frontier Sciences, University of Tokyo（东京大学前沿科学研究生院先进材料科学系）；Department of Natural Sciences, Faculty of Science and Engineering, Tokyo City University（东京都市大学理工学部自然科学科）
We present a piezoelectric-driven uniaxial pressure cell that is optimized for muon spin relaxation and neutron scattering experiments, and that is operable over a wide temperature range including cryogenic temperatures. To accommodate the large samples required for these measurement techniques, the cell is designed to generate forces up to 1000 N, and to minimize the background signal the space around the sample is kept as open as possible. We demonstrate here that by mounting plate-like samples with epoxy, a uniaxial stress exceeding 1 GPa can be achieved in an active volume of 5 mm3. We sho…
