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Register a new userPressure-induced reconstructive phase transition in Cd$_3$As$_2$
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Cadmium arsenide Cd$_3$As$_2$ hosts massless Dirac electrons in its ambient-conditions tetragonal phase. We report X-ray diffraction and electrical resistivity measurements of Cd$_3$As$_2$ upon cycling pressure beyond the critical pressure of the tetragonal phase and back to ambient conditions. We find that at room temperature the transition between the low- and high-pressure phases results in large microstrain and reduced crystallite size both on rising and falling pressure. This leads to non-reversible electronic properties including self-doping associated with defects and a reduction of the electron mobility by an order of magnitude due to increased scattering. Our study indicates that the structural transformation is sluggish and shows a sizable hysteresis of over 1~GPa. Therefore, we conclude that the transition is first-order reconstructive, with chemical bonds being broken and rearranged in the high-pressure phase. Using the diffraction measurements we demonstrate that annealing at ~200$^circ$C greatly improves the crystallinity of the high-pressure phase. We show that its Bragg peaks can be indexed as a primitive orthorhombic lattice with a_HP~8.68 A b_HP~17.15 A and c_HP~18.58 A. The diffraction study indicates that during the structural transformation a new phase with another primitive orthorhombic structure may be also stabilized by deviatoric stress, providing an additional venue for tuning the unconventional electronic states in Cd3As2.
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We report a room-temperature optical reflectivity study performed on [112]-oriented Cd$_3$As$_2$ single crystals over a broad energy range under external pressure up to 10 GPa. The abrupt drop of the band dispersion parameter ($z$-parameter) and the interruption of the gradual redshift of the bandgap at $sim$4~GPa confirms the structural phase transition from a tetragonal to a monoclinic phase in this material. The pressure-induced increase of the overall optical conductivity at low energies and the continuous redshift of the high-energy bands indicate that the system evolves towards a topologically trivial metallic state, although a complete closing of the band gap could not be observed in the studied pressure range. Furthermore, a detailed investigation of the low-pressure regime suggests the possible existence of an intermediate state between 2 and 4~GPa , that might be a precursor of the structural phase transition or due to the lifted degeneracy of the Dirac nodes. Several optical parameters show yet another anomaly at 8~GPa, where low-temperature superconductivity was found in an earlier study.
Nitride perovskites are supposed to exhibit excellent properties as oxide analogues and may even have better performance in specific fields for their more covalent characters. However, till now, very limited nitride perovskites have been reported. In this work, a nitride perovskite LaMoN$_3$ has been systematically studied by first-principles calculations. The most interesting physical property is its ferroelectric $R3c$ phase, which can be stabilized under a moderate hydrostatic pressure ($sim1.5$ GPa) and probably remain meta-stable under the ambient condition. Its ferroelectric polarization is considerable large, $80.3$ $mu$C/cm$^2$, driven by the nominal $4d^0$ rule of Mo$^{6+}$, and the covalent hybridization between Mos $4d$ and Ns $2p$ orbitals is very strong. Our calculation not only predicts a new ferroelectric material with prominent properties, but also encourages more studies on pressure engineering of functional nitrides.
Thermoelectric materials can be used to convert heat to electric power through the Seebeck effect. We study magneto-thermoelectric figure of merit (ZT) in three-dimensional Dirac semimetal Cd$_3$As$_2$ crystal. It is found that enhancement of power factor and reduction of thermal conductivity can be realized at the same time through magnetic field although magnetoresistivity is greatly increased. ZT can be highly enhanced from 0.17 to 1.1 by more than six times around 350 K under a perpendicular magnetic field of 7 Tesla. The huge enhancement of ZT by magnetic field arises from the linear Dirac band with large Fermi velocity and the large electric thermal conductivity in Cd$_3$As$_2$. Our work paves a new way to greatly enhance the thermoelectric performance in the quantum topological materials.
We study the low-energy electronic structure of three-dimensional Dirac semimetal, Cd$_3$(As$_{1-x}$P$_x$)$_2$ [$x$ = 0 and 0.34(3)], by employing the angle-resolved photoemission spectroscopy (ARPES). We observe that the bulk Dirac states in Cd$_3$(As$_{0.66}$P$_{0.34}$)$_2$ are gapped out with an energy of 0.23 eV, contrary to the parent Cd$_3$As$_2$ in which the gapless Dirac states have been observed. Thus, our results confirm the earlier predicted topological phase transition in Cd$_3$As$_2$ with perturbation. We further notice that the critical P substitution concentration, at which the two Dirac points that are spread along the $c$-axis in Cd$_3$As$_2$ form a single Dirac point at $Gamma$, is much lower [x$_c$(P)$<$ 0.34(3)] than the predicted value of x$_c$(P)=0.9. Therefore, our results suggest that the nontrivial band topology of Cd$_3$As$_2$ is remarkably sensitive to the P substitution and can only survive over a narrow substitution range, i.e., 0 $leq$ x (P) $<$ 0.34(3).
We report ultrafast transient-grating measurements of crystals of the three-dimensional Dirac semimetal cadmium arsenide, Cd3As2, at both room temperature and 80 K. After photoexcitation with 1.5-eV photons, charge-carriers relax by two processes, one of duration 500 fs and the other of duration 3.1 ps. By measuring the complex phase of the change in reflectance, we determine that the faster signal corresponds to a decrease in absorption, and the slower signal to a decrease in the lights phase velocity, at the probe energy. We attribute these signals to electrons filling of phase space, first near the photon energy and later at lower energy. We attribute their decay to cooling by rapid emission of optical phonons, then slower emission of acoustic phonons. We also present evidence that both the electrons and the lattice are strongly heated.
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