Topological Weyl semimetals (WSMs) have attracted widespread interests due to the chiral Weyl fermions and surface Fermi arcs that enable unique optical and transport phenomena. In this work, we present angle-resolved Raman spectroscopy of TaP, a prototypical noncentrosymmetric WSM, for five excitation wavelengths ranging from 364 to 785 nm. The Raman active modes, $A_1$, $B_1^1$, and $B_1^2$ modes, exhibit two main unique features beyond the conventional Raman theory. First, the relative intensities of Raman active modes change as a function of the excitation wavelength. Second, angle-resolved polarized Raman spectra show systematic deviation from the Raman tensor theory. In particular, the $B_1^1$ mode is absent for 633 nm excitation, whereas the $B_1^2$ mode shows an unusual two-fold symmetry instead of a four-fold symmetry for 488, 532, and 633 nm excitations. These unconventional phenomena are attributed to the interference effect in the Raman process owing to the existence of multiple carrier pockets with almost the same energy but different symmetries.
We report a structural study of the Weyl semimetals TaAs, TaP, NbP, and NbAs, utilizing diffraction techniques (single crystal x-ray diffraction and energy dispersive spectroscopy) and imaging techniques (transmission electron microscopy/scanning transmission electron microscopy). We observe defects of various degrees, leading to non-stoichiometric single crystals of all four semimetals. While TaP displays a large pnictide deficiency with composition TaP$_{0.83(3)}$, and stacking faults accompanied by anti-site disorder and site vacancies, TaAs displays transition metal deficiency with composi…
The high pressure phase diagrams of TaAs family (NbP, NbAs, TaP and TaAs) are explored systematically using crystal structure search together with first-principles calculations. Our calculations show that NbAs and TaAs have similar phase diagrams and possess the same structural phase transition sequence of I41md $\rightarrow$ P-6m2 $\rightarrow$ P21/c $\rightarrow$ Pm-3m, with a bit different transition pressures. The phase transition sequence of NbP and TaP are somewhat different from that of NbAs and TaAs. In which new structures emerge, for instance, the Cmcm structure in NbP and the Pmmn s…
We report a comparative polarized Raman study of Weyl semimetals TaAs, NbAs, TaP and NbP. The evolution of the phonon frequencies with the sample composition allows us to determine experimentally which atoms are mainly involved for each vibration mode. Our results confirm previous first-principles calculations indicating that the A$_1$, B$_1(2)$, E$(2)$ and E$(3)$ modes involve mainly the As(P) atoms, the B$_1(1)$ mode is mainly related to Ta(Nb) atoms, and the E$(1)$ mode involves both kinds of atoms. By comparing the energy of the different modes, we establish that the B$_1(1)$, B$_1(2)$, E$…
We report a structural study of the Weyl semimetals TaAs and TaP, utilizing diffraction and imaging techniques, where we show that they contain a high density of defects, leading to non-stoichiometric single crystals of both semimetals. Despite the observed defects and non-stoichiometry on samples grown using techniques already reported in the literature, de Haas-van Alphen measurements on TaP reveal quantum oscillations and a high carrier mobility, an indication that the crystals are of quality comparable to those reported elsewhere. Electronic structure calculations on TaAs reveal that the p…
We investigated the pressure evolution of the electrical transport in the almost compensated Weyl semimetal TaP. In addition, we obtained information on the modifications of the Fermi-surface topology with pressure from the analysis of pronounced Shubnikov-de Haas (SdH) quantum oscillations present in the Hall-effect and magnetoresistance data. The simultaneous analysis of the Hall and longitudinal conductivity data in a two-band model revealed an only weak decrease in the electron- and hole charge-carrier densities up to 1.2 GPa, while the mobilities are essentially pressure independent along…
Unusually high phonon thermal conductivity in the Weyl semimetal TaP: A comparative study with TaAs
College of Physics and Optoelectronic Engineering, Chongqing Normal University（重庆师范大学物理与光电工程学院）；School of Science, Chongqing University of Posts and Telecommunications（重庆邮电大学理学院）；Center for Computational Science and Engineering, Southern University of Science and Technology（南方科技大学计算科学与工程中心）；College of Physics and Electronic Engineering, Chongqing Normal University（重庆师范大学物理与电子工程学院）；College of Physics and Center of Quantum Materials and Devices, Chongqing University（重庆大学物理学院量子材料与器件中心）；Chongqing Key Laboratory for Strongly Coupled Physics, Chongqing University（重庆大学强耦合物理重庆市重点实验室）
We have performed polarized and temperature-dependent Raman scattering measurements on extremely large magnetoresitance compounds TaAs$_2$ and NbAs$_2$. In both crystals, all the Raman active modes, including six A$_g$ modes and three B$_g$ modes, are clearly observed and well assigned with the combination of symmetry analysis and first-principles calculations. The well-resolved periodic intensity modulations of the observed modes with rotating crystal orientations, verify the symmetry of each assigned mode and are fitted to experimentally determine the elements of Raman tensor matrixes. The b…
High pressure Raman spectroscopy of bulk 2H-MoTe$_2$ upto $\sim$ 29 GPa is shown to reveal two phase transitions (at $\sim$ 6 and 16.5 GPa), which are analyzed using first-principles density functional theoretical calculations. The transition at 6 GPa is marked by changes in the pressure coefficients of A$_{1g}$ and E$^{1}_{2g}$ Raman mode frequencies as well as in their relative intensity. Our calculations show that this is an isostructural semiconductor to a semimetal transition. The transition at $\sim$ 16.5 GPa is identified with the changes in linewidths of the Raman modes as well as in t…
Transition metal dichalcogenide MoTe$_2$ is an important candidate for realizing the newly predicted type-IIWeyl fermions, for which the breaking of the inversion symmetry is a prerequisite. Here we present direct spectroscopic evidence for the inversion symmetry breaking in the low temperature phase of MoTe$_2$ by systematic Raman experiments and first principles calculations. We identify five lattice vibrational modes which are Raman active only in noncentrosymmetric structure at low temperature. A hysteresis is also observed in the peak intensity of inversion symmetry activated Raman modes,…
Landau-level spectroscopy, the optical analysis of electrons in materials subject to a strong magnetic field, is a versatile probe of the electronic band structure and has been successfully used in the identification of novel states of matter such as Dirac electrons, topological materials or Weyl semimetals. The latter arise from a complex interplay between crystal symmetry, spin-orbit interaction and inverse ordering of electronic bands. Here, we report on unusual Landau-level transitions in the monopnictide TaP that decrease in energy with increasing magnetic field. We show that these transi…
The asymmetric peak at 212 - 218 cm-1 occurring in InAs micro-nano wires is investigated using spatially resolved Raman spectroscopy (SRRS) of uniform, bent and long tapered MNWs grown on a Si (001) substrate. It is attributed to superposition of E2h phonon (wurtzite : WZ) and TO phonon (zinc blende : ZB) of InAs. Polarized and wavelength dependent SRRS establishes the presence of WZ and ZB phases in these MNWs. However, formation of WZ phase for larger diameter InAs MNWs is not commensurate with existing growth mapping studies, which needs to be understood further. Study of several of these M…
We report high pressure Raman, synchrotron x-ray diffraction and electrical transport studies on Weyl semimetals NbP and TaP along with first-principles density functional theoretical (DFT) analysis. The frequencies of first-order Raman modes of NbP harden with increasing pressure and exhibit a slope change at P$_c$ $\sim$ 9 GPa, and its resistivity exhibits a minimum at P$_c$. The pressure-dependent volume of NbP exhibits a change in its bulk modulus from 207 GPa to 243 GPa at P$_c$. Using DFT calculations, we show that these anomalies are associated with pressure induced Lifshitz transition …
We report a polarized Raman study of Weyl semimetal TaAs. We observe all the optical phonons, with energies and symmetries consistent with our first-principles calculations. We detect additional excitations assigned to multiple-phonon excitations. These excitations are accompanied by broad peaks separated by 140~cm$^{-1}$ that are also most likely associated with multiple-phonon excitations. We also noticed a sizable B$_1$ component for the spectral background, for which the origin remains unclear.
The layered ternary compound TaIrTe4 is an important candidate to host the recently predicted type-II Weyl Fermions. However, a direct and definitive proof of the absence of inversion symmetry in this material, a prerequisite for the existence of Weyl Fermions, has so far remained evasive. Herein, an unambiguous identification of the broken inversion symmetry in TaIrTe4 is established using angle-resolved polarized Raman spectroscopy. Combining with high-resolution transmission electron microscopy, we demonstrate an efficient and nondestructive recipe to determine the exact crystallographic or…
The recent discoveries of Dirac fermions in graphene and on the surface of topological insulators have ignited worldwide interest in physics and materials science. A Weyl semimetal is an unusual crystal where electrons also behave as massless quasi-particles but interestingly they are not Dirac fermions. These massless particles, Weyl fermions, were originally considered in massless quantum electrodynamics but have not been observed as a fundamental particle in nature. A Weyl semimetal provides a condensed matter realization of Weyl fermions, leading to unique transport properties with novel d…
Weyl Semimetals (WSMs), a recently discovered topological state of matter, exhibit an electronic structure governed by linear band dispersions and degeneracy (Weyl) points leading to rich physical phenomena, which are yet to be exploited in thin film devices. While WSMs were established in the monopnictide compound family several years ago, the growth of thin films has remained a challenge. Here, we report the growth of epitaxial thin films of NbP and TaP by means of molecular beam epitaxy. Single crystalline films are grown on MgO (001) substrates using thin Nb (Ta) buffer layers, and are fou…
LaAgSb$_{2}$ is a rare material, which offers the opportunity to investigate the complex interplay between charge density wave (CDW) ordering and topology protected electronic band structure. As both of these phenomena are governed by the structural symmetries, a comprehensive study of the lattice dynamics is highly desirable. In this report, we present the results of temperature and pressure dependent Raman spectroscopy and x-ray diffraction in single crystalline LaAgSb$_{2}$. Our results confirm that Raman spectroscopy is a highly sensitive tool to probe CDW ordering phenomenon, particularly…
Very recently the topological Weyl semimetal (WSM) state was predicted in the noncentrosymmetric compounds TaAs, TaP, NbAs, and NbP and soon led to photoemission and transport experiments to verify the presumed topological properties such as Fermi arcs (unclosed Fermi surfaces) and the chiral anomaly. In this work, we have performed fully \textit{ab initio} calculations of the surface band structures of these four WSM materials and revealed the Fermi arcs with spin-momentum-locked spin texture. On the (001) polar surface, the shape of the Fermi surface depends sensitively on the surface termin…
Weyl semimetals (WSMs) are topological quantum states wherein the electronic bands linearly disperse around pairs of nodes, the Weyl points, of fixed (left or right) chirality. The recent discovery of WSM materials triggered an experimental search for the exotic quantum phenomenon known as the chiral anomaly. Via the chiral anomaly nonorthogonal electric and magnetic fields induce a chiral density imbalance that results in an unconventional negative longitudinal magnetoresistance, the chiral magnetic effect. Recent theoretical work suggests that this effect does not require well-defined Weyl n…
The semimetal NbIrTe4 has been proposed to be a Type-II Weyl semimetal with 8 pairs of opposite Chirality Weyl nodes which are very close to the Fermi energy. This topological electronic structure is made possible because of the broken inversion symmetry of NbIrTe4 which is an orthorhombic crystal with Td symmetry. Using micro-Raman scattering as a probe, we observe the frequencies and symmetries of 19 phonon modes (ranging from 40 to 260 cm-1) in this material and compare to Density Functional Theory calculations. Using angular and polarization resolved Raman scattering for green (514 nm) and…
Discovery of Weyl fermions in semimetallic tansition-metal monopnictides is a major breakthrough in condensed matter physics. A Weyl semimetal is characterized by the existence of robust Weyl points and unclosed topological surface states in the form of Fermi arc. All the four compounds of the Weyl semimetal transition monopnictide family i.e. NbP, TaP, NbAs and TaAs exhibit extremely high mobility and unsaturated high magnetoresistance (MR). For example, MR values are 8.5x10^5% at 1.85 K for NbP and 1.5x10^5% at 3 K in 9 T for TaAs. NbP also achieves very low value of residual resistivity 0.6…
A Weyl semimetal possesses spin-polarized band-crossings, called Weyl nodes, connected by topological surface arcs. The low-energy excitations near the crossing points behave the same as massless Weyl fermions, leading to exotic properties like chiral anomaly. To have the transport properties dominated by Weyl fermions, Weyl nodes need to locate nearly at the chemical potential and enclosed by pairs of individual Fermi surfaces with nonzero Fermi Chern numbers. Combining angle-resolved photoemission spectroscopy and first-principles calculation, here we show that TaP is a Weyl semimetal with o…
Topological materials provide an exclusive platform to study the dynamics of relativistic particles in table-top experiments and offer the possibility of wide-scale technological applications. ZrSiS is a newly discovered topological nodal-line semimetal and has drawn enormous interests. In this report, we have investigated the lattice dynamics and electron-phonon interaction in single crystalline ZrSiS using Raman spectroscopy. Polarization and angle resolved measurements have been performed and the results have been analyzed using crystal symmetries and theoretically calculated atomic vibrati…
A giant planar Hall effect (PHE) and anisotropic magnetoresistance (AMR) is observed in TaP, a nonmagnetic Weyl semimetal with ultrahigh mobility. The perpendicular resistivity (i.e., the planar magnetic field applied normal to the current) far exceeds the zero-field resistivity, which thus rules out the possible origin of negative longitudinal magnetoresistance. The giant PHE/AMR is finally attributed to the large anisotropic orbital magnetoresistance that stems from the ultrahigh mobility. Furthermore, the mobility-enhanced current jetting effects are found to strongly deform the line shape …
The search for highly efficient and low-cost catalysts is one of the main driving forces in catalytic chemistry. Current strategies for the catalyst design focus on increasing the number and activity of local catalytic sites, such as the edge-sites of molybdenum disulfides in the hydrogen evolution reaction (HER). Here, we propose and demonstrate a different principle that goes beyond local site optimization by utilizing topological electronic states, a global property of the material, to spur catalytic activity. For HER, we have found excellent catalysts among the transition-metal monopnictid…
GaGeTe is a layered material composed of germanene and GaTe sublayers that has been recently predicted to be a basic Z2 topological semimetal. To date, only one polytype of GaGeTe is known with trigonal centrosymmetric structure (alpha phase, space group R-3m, No. 166). Here we show that as-grown samples of GaGeTe show traces of at least another polytype with hexagonal non-centrosymmetric structure (beta phase, space group P63mc, No. 186). Moreover, we suggest that another bulk hexagonal polytype (gamma phase, space group P-3m1, No. 164) could also be found near room conditions. Both alpha and…
Tunable symmetry breaking plays a crucial role for the manipulation of topological phases of quantum matter. Here, through combined high-pressure magneto-transport measurements, Raman spectroscopy, and X-ray diffraction, we demonstrate a pressure-induced topological phase transition in nodal-line semimetal ZrSiS. Symmetry analysis and first-principles calculations suggest that this pressure-induced topological phase transition may be attributed to weak lattice distortions by non-hydrostatic compression, which breaks some crystal symmetries, such as the mirror and inversion symmetries. This fin…
Raman scattering in the three-dimensional Dirac semimetal Cd3As2 shows an intricate interplay of electronic and phonon degrees of freedom. We observe resonant phonon scattering due to interband transitions, an anomalous anharmonicity of phonon frequency and intensity, as well as quasielastic (E~0) electronic scattering. The latter two effects are governed by a characteristic temperature scale T* ~ 100 K that is related to mutual fluctuations of lattice and electronic degrees of freedom. A refined analysis shows that this characteristic temperature corresponds to the energy of optical phonons w…
We report the first observation of the non-magnetic Barkhausen effect in van der Waals layered crystals, specifically, between the Td and 1T' phases in type-II Weyl semimetal MoTe2. Thinning down the MoTe2 crystal from bulk material to about 25nm results in a drastic strengthening of the hysteresis in the phase transition, with the difference in critical temperature increasing from 40K to more than 300K. The Barkhausen effect appears for thin samples and the temperature range of the Barkhausen zone grows approximately linearly with reducing sample thickness, pointing to a surface origin of the…
Based on first principle calculations, we show that a family of nonmagnetic materials including TaAs, TaP, NbAs and NbP are Weyl semimetal (WSM) without inversion center. We find twelve pairs of Weyl points in the whole Brillouin zone (BZ) for each of them. In the absence of spin-orbit coupling (SOC), band inversions in mirror invariant planes lead to gapless nodal rings in the energy-momentum dispersion. The strong SOC in these materials then opens full gaps in the mirror planes, generating nonzero mirror Chern numbers and Weyl points off the mirror planes. The resulting surface state Fermi a…
Recently, Cd3As2 has attracted intensive research interest as an archetypical Dirac semimetal, hosting three-dimensional linear-dispersive electronic bands near the Fermi level. Previous studies have shown that single-crystalline Cd3As2 has an anomalously low lattice thermal conductivity, ranging from 0.3 W/mK to 0.7 W/mK at 300 K, which has been attributed to point defects. In this work, we combine first-principles lattice dynamics calculations and temperature-dependent high-resolution Raman spectroscopy of high-quality single-crystal thin films grown by molecular beam epitaxy to reveal the e…
Thermoelectrics are promising by directly generating electricity from waste heat. However, (sub-)room-temperature thermoelectrics have been a long-standing challenge due to vanishing electronic entropy at low temperatures. Topological materials offer a new avenue for energy harvesting applications. Recent theories predicted that topological semimetals at the quantum limit can lead to a large, non-saturating thermopower and a quantized thermoelectric Hall conductivity approaching a universal value. Here, we experimentally demonstrate the non-saturating thermopower and quantized thermoelectric H…
Model for charge carrier spectra in topological semimetals of the TaAs family
B. Verkin Institute for Low Temperature Physics & Engineering of the National Academy of Sciences of Ukraine（乌克兰国家科学院B.维尔金低温物理与工程研究所）；Institute of Low Temperature and Structure Research, Polish Academy of Sciences（波兰科学院低温结构研究所）
A model is constructed to describe the thermal-field emission of electrons from a three-dimensional ($3$D) topological semimetal hosting Dirac/Weyl node(s). The traditional thermal-field electron emission model is generalised to accommodate the $3$D non-parabolic energy band structures in the topological Dirac/Weyl semimetals, such as cadmium arsenide (\ch{Cd3As2}), sodium bismuthide (\ch{Na3Bi}), tantalum arsenide (\ch{TaAs}) and tantalum phosphide (\ch{TaP}). Due to the unique Dirac cone band structure, an unusual dual-peak feature is observed in the total energy distribution (TED) spectrum.…
Orbital Hall Effect in Weyl Semimetals from quantum geometric band interference
University of Bologna（博洛尼亚大学）；Max Planck Institute for the Structure and Dynamics of Matter（马普结构动力学研究所）；Universität Würzburg（维尔茨堡大学）；Universidad del País Vasco（巴斯克大学）；The Flatiron Institute（平顿研究所）
We present experimental evidence of an intriguing phase transition between distinct topological states in the type-II Weyl semimetal MoTe2. We observe anomalies in the Raman phonon frequencies and linewidths as well as electronic quasielastic peaks around 70 K, which, together with structural, thermodynamic measurements, and electron-phonon coupling calculations, demonstrate a temperature-induced transition between two topological phases previously identified by contrasting spectroscopic measurements. An analysis of experimental data suggests electron-phonon coupling as the main driving mechan…
In this work, we have studied the structural, elastic, mechanical, electronic, bonding, acoustic, thermal and optical properties of TaX (X = P, As) in detail via first-principles method using the density functional theory. A comprehensive study of elastic constants and moduli shows that both TaP and TaAs possesses low to medium level of elastic anisotropy (depending on the measure), reasonably good machinability, mixed bonding characteristics with ionic and covalent contributions, brittle nature and relatively high Vickers hardness with a low Debye temperature and melting temperature. The mini…
We compare two crystallographic phases of the low-dimensional WP$_2$ to better understand features of electron-electron and electron-phonon interactions in topological systems. The topological $β$-phase, a Weyl semimetal with a giant magneto-resistance, shows a larger intensity of electronic Raman scattering compared to the topologically trivial $α$-phase. This intensity sharply drops for $T < T^* = 20$ K which evidences a crossover in the topological phase from marginal quasiparticles to a coherent low temperature regime. In contrast, the non-topological $α$-phase shows more pronounced signat…
We generalize the notion of dissipationless, topological Hall viscosity tensor to optical phonons in thin film Weyl semimetals. By using the strained Porphyrin thin film Weyl semimetal as a model example, we show how optical phonons can couple to Weyl electrons as chiral pseudo gauge fields. These chiral vector fields lead to a novel dissipationless two-rank viscosity tensor in the effective dynamics of optical phonons whose origin is the chiral anomaly. We also compute the contribution to this two rank Hall viscosity tensor due to the presence of an external magnetic field, whose origin is th…
Topological semimetals have revealed a wide array of novel transport phenomena, including electron hydrodynamics, quantum field theoretic anomalies, and extreme magnetoresistances and mobilities. However, the scattering mechanisms central to these behaviors remain largely unexplored. Here we reveal signatures of significant phonon-electron scattering in the type-II Weyl semimetal WP$_{2}$ via temperature-dependent Raman spectroscopy. Over a large temperature range, we find that the decay rates of the lowest energy $A_{1}$ modes are dominated by phonon-electron rather than phonon-phonon scatter…
The Weyl semimetal phase is a recently discovered topological quantum state of matter characterized by the presence of topologically protected degeneracies near the Fermi level. These degeneracies are the source of exotic phenomena, including the realization of chiral Weyl fermions as quasiparticles in the bulk and the formation of Fermi arc states on the surfaces. Here, we demonstrate that these two key signatures show distinct evolutions with the bulk band topology by performing angle-resolved photoemission spectroscopy, supported by first-principle calculations, on transition-metal monophos…
We study the possibility of pressure-induced transitions from a normal semiconductor to a topological insulator (TI) in bismuth tellurohalides using density functional theory and tight-binding method. In BiTeI this transition is realized through the formation of an intermediate phase, a Weyl semimetal, that leads to modification of surface state dispersions. In the topologically trivial phase, the surface states exhibit a Bychkov-Rashba type dispersion. The Weyl semimetal phase exists in a narrow pressure interval of 0.2 GPa. After the Weyl semimetal--TI transition occurs, the surface electron…
The electron-phonon interaction (EPI) is instrumental in a wide variety of phenomena in solid-state physics, such as electrical resistivity in metals, carrier mobility, optical transition and polaron effects in semiconductors, lifetime of hot carriers, transition temperature in BCS superconductors, and even spin relaxation in diamond nitrogen-vacancy centers for quantum information processing. However, due to the weak EPI strength, most phenomena have focused on electronic properties rather than on phonon properties. One prominent exception is the Kohn anomaly, where phonon softening can emerg…
We have studied theoretically the Weyl semimetals the point symmetry group of which has reflection planes and which contain equivalent valleys with opposite chiralities. These include the most frequently studied compounds, namely the transition metals monopnictides TaAs, NbAs, TaP, NbP, and also Bi$_{1-x}$Sb$_x$ alloys. The circular photogalvanic current, which inverts its direction under reversal of the light circular polarization, has been calculated for the light absorption under direct optical transitions near the Weyl points. In the studied materials, the total contribution of all the val…
Charge dynamics in the Weyl semimetals NbIrTe$_4$ and TaIrTe$_4$ under pressure: Signatures of an electronic phase transition
University of Augsburg（奥格斯堡大学）；Tanta University（坦塔大学）；National High Magnetic Field Laboratory, Florida State University（佛罗里达州立大学国家高磁场实验室）；Baylor University（贝勒大学）；Pennsylvania State University（宾夕法尼亚州立大学）
