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Register a new userOptical spectroscopy study on pressure-induced phase transitions in the three-dimensional Dirac semimetal Cd$_3$As$_2$
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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.
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Harmonic generation is a general characteristic of driven nonlinear systems, and serves as an efficient tool for investigating the fundamental principles that govern the ultrafast nonlinear dynamics. In atomic gases, high-harmonic radiation is produced via a three-step process of ionization, acceleration, and recollision by strong-field infrared laser. This mechanism has been intensively investigated in the extreme ultraviolet and soft X-ray regions, forming the basis of attosecond research. In solid-state materials, which are characterized by crystalline symmetry and strong interactions, yielding of harmonics has just recently been reported. The observed high-harmonic generation was interpreted with fundamentally different mechanisms, such as interband tunneling combined with dynamical Bloch oscillations, intraband thermodynamics and nonlinear dynamics, and many-body electronic interactions. Here, in a distinctly different context of three-dimensional Dirac semimetal, we report on experimental observation of high-harmonic generation up to the seventh order driven by strong-field terahertz pulses. The observed non-perturbative high-harmonic generation is interpreted as a generic feature of terahertz-field driven nonlinear intraband kinetics of Dirac fermions. We anticipate that our results will trigger great interest in detection, manipulation, and coherent control of the nonlinear response in the vast family of three-dimensional Dirac and Weyl materials.
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.
Three dimensional (3D) topological Dirac materials are under intensive study recently. The layered compound ZrTe$_5$ has been suggested to be one of them by transport and ARPES experiments. Here, we perform infrared reflectivity measurement to investigate the underlying physics of this material. The derived optical conductivity exhibits linear increasing with frequency below normal interband transitions, which provides the first optical spectroscopic proof of a 3D Dirac semimetal. Apart from that, the plasma edge shifts dramatically to lower energy upon temperature cooling, which might be associated with the consequence of lattice parameter shrinking. In addition, an extremely sharp peak shows up in the frequency dependent optical conductivity, indicating the presence of a Van Hove singularity in the joint density of state.
Using first-principles density functional theory calculations, combined with a topological analysis, we have investigated the electronic properties of $Cd_3As_2$ and $Na_3Bi$ Dirac topological semimetals doped with non-magnetic and magnetic impurities. Our systematic analysis shows that the selective breaking of the inversion, rotational and time-reversal symmetry, controlled by specific choices of the impurity doping, induces phase transitions from the original Dirac semimetal to a variety of topological phases such as, topological insulator, trivial semimetal, non-magnetic and magnetic Weyl semimetal, and Chern insulator. The Dirac semimetal phase can exist only if the rotational symmetry $C_n$ with $n > 2$ is maintained. One particularly interesting phase emerging in doped $Cd_3As_2$ is a coexisting Dirac-Weyl phase, which occurs when only inversion symmetry is broken while time-reversal symmetry and rotational symmetry are both preserved. To further characterize the low-energy excitations of this phase, we have complemented our density functional results with a continuum four-band $kcdot p$ model, which indeed displays nodal points of both Dirac and Weyl type. The coexisting phase appears as a transition point between two topologically distinct Dirac phases, but may also survive in a small region of parameter space controlled by external strain.
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).
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