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Strong Photothermoelectric Response and Contact Reactivity of the Dirac Semimetal ZrTe5

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 Added by Francois Leonard
 Publication date 2017
  fields Physics
and research's language is English




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The family of three-dimensional topological insulators opens new avenues to discover novel photophysics and to develop novel types of photodetectors. ZrTe5 has been shown to be a Dirac semimetal possessing unique topological electronic and optical properties. Here we present spatially-resolved photocurrent measurements on devices made of nanoplatelets of ZrTe5, demonstrating the photothermoelectric origin of the photoresponse. Due to the high electrical conductivity and good Seebeck coefficient, we obtain noise-equivalent powers as low as 42 pW/Hz1/2 at room temperature for visible light illumination at zero bias. We also show that these devices suffer from significant ambient reactivity such as the formation of a Te-rich surface region driven by Zr oxidation, as well as severe reactions with the metal contacts. This reactivity results in significant stresses in the devices, leading to unusual geometries that are useful for gaining insight into the photocurrent mechanisms. Our results indicate that both the large photothermoelectric response and reactivity must be considered when designing or interpreting photocurrent measurements in these systems.



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Novel phases of matter with unique properties that emerge from quantum and topological protection present an important thrust of modern research. Of particular interest is to engineer these phases on demand using ultrafast external stimuli, such as photoexcitation, which offers prospects of their integration into future devices compatible with optical communication and information technology. Here, we use MeV Ultrafast Electron Diffraction (UED) to show how a transient three-dimensional (3D) Dirac semimetal state can be induced by a femtosecond laser pulse in a topological insulator ZrTe$_5$. We observe marked changes in Bragg diffraction, which are characteristic of bond distortions in the photoinduced state. Using the atomic positions refined from the UED, we perform density functional theory (DFT) analysis of the electronic band structure. Our results reveal that the equilibrium state of ZrTe$_5$ is a topological insulator with a small band gap of $sim$25 meV, consistent with angle-resolved photoemission (ARPES) experiments. However, the gap is closed in the presence of strong spin-orbit coupling (SOC) in the photoinduced transient state, where massless Dirac fermions emerge in the chiral band structure. The time scale of the relaxation dynamics to the transient Dirac semimetal state is remarkably long, $tau sim$160 ps, which is two orders of magnitude longer than the conventional phonon-driven structural relaxation. The long relaxation is consistent with the vanishing density of states in Dirac spectrum and slow spin-repolarization of the SOC-controlled band structure accompanying the emergence of Dirac fermions.
Topological materials with broken inversion symmetry can give rise to nonreciprocal responses, such as the current rectification controlled by magnetic fields via magnetochiral anisotropy. Bulk nonreciprocal responses usually stem from relativistic corrections and are always found to be very small. A large magnetochiral anisotropy of novel origin has been proposed for topological semimetals, but no concrete example has been known so far. Here we report our discovery that ZrTe5 crystals in proximity to a topological quantum phase transition present gigantic magnetochiral anisotropy which is at least 1000 times larger than in any known material. We argue that a very low carrier density, inhomogeneities, and a torus-shaped Fermi surface induced by breaking of inversion symmetry in a Dirac material are central to explain this extraordinary property.
Resistivity anomaly, a sharp peak of resistivity at finite temperatures, in the transition-metal pentatellurides ZrTe5 and HfTe5 was observed four decades ago, and more exotic and anomalous behaviors of electric and thermoelectric transport were revealed recent years. Here we present a theory of Dirac polarons, composed by massive Dirac electrons and holes in an encircling cloud of lattice displacements or phonons at finite temperatures. The chemical potential of Dirac polarons sweeps the band gap of the topological band structure by increasing the temperature, leading to the resistivity anomaly. Formation of a nearly neutral state of Dirac polarons accounts for the anomalous behaviors of the electric and thermoelectric resistivity.
We combine transport, magnetization, and torque magnetometry measurements to investigate the electronic structure of ZrTe5 and its evolution with temperature. At fields beyond the quantum limit, we observe a magnetization reversal from paramagnetic to diamagnetic response, which is characteristic of a Dirac semi-metal. We also observe a strong non-linearity in the magnetization that suggests the presence of additional low-lying carriers from other low-energy bands. Finally, we observe a striking sensitivity of the magnetic reversal to temperature that is not readily explained by simple band-structure models, but may be connected to a temperature dependent Lifshitz transition proposed to exist in this material.
Hydrodynamic fluidity in condensed matter physics has been experimentally demonstrated only in a limited number of compounds due to the stringent conditions that must be met. Herein, we demonstrate phonon hydrodynamic-like properties in three-dimensional topological semimetal ZrTe5 thanks to its ultrahigh-purity and intrinsic structural instability. By measuring the thermal properties in a wide temperature range, two representative experimental evidences of phonon hydrodynamics are seen in an interesting temperature window between the ballistic and diffusive regimes: a faster evolution of the thermal conductivity than in the ballistic regime and the non-monotonic temperature-dependent effective phonon mean-free-path. In addition, magneto-thermal conductivity results indicate us that charged quasiparticles, as well as phonons, may also play an important role in the hydrodynamic flow in the ZrTe5 system.
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