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Register a new userProbing lattice dynamics and electron-phonon coupling in topological nodal-line semimetal ZrSiS
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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 vibrational patterns along with phonon dispersion spectra. Wavelength and temperature dependent measurements show the complex interplay of electron and phonon degrees of freedom, resulting in resonant phonon and quasielastic electron scatterings through inter-band transitions. Our high-pressure Raman studies reveal vibrational anomalies, which were further investigated from the high-pressure synchrotron x-ray diffraction (HPXRD) spectra. From HPXRD, we have clearly identified pressure-induced structural transitions and coexistence of multiple phases, which also indicate possible electronic topological transitions in ZrSiS. The present study not only provides the fundamental information on the phonon subsystem, but also sheds some light in understanding the topological nodal-line phase in ZrSiS and other iso-structural systems.
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ZrSiS is the most intensively studied topological nodal-line semimetal candidate, which is proposed to host multiple nodal lines in its bulk electronic structure. However, previous angle-resolved photoemission spectroscopy (ARPES) experiments with vacuum ultraviolet lights mainly probed the surface states. Here using bulk-sensitive soft X-ray ARPES, we acquire the bulk electronic states of ZrSiS without any interference from surface states. Our results clearly show two groups of three-dimensional bulk nodal lines located on high-symmetry planes and along high-symmetry lines in the bulk Brillouin zone, respectively. The nodal lines on high-symmetry planes are enforced to pin at the Fermi level by carrier compensation and constitute the whole Fermi surfaces. This means that the carriers in ZrSiS are entirely contributed by nodal-line fermions, suggesting that ZrSiS is a remarkable platform for studying physical properties related to nodal lines.
We instigate the angle-dependent magnetoresistance (AMR) of the layered nodal-line Dirac semimetal ZrSiS for the in-plane and out-of-plane current directions. This material has recently revealed an intriguing butterfly-shaped in-plane AMR that is not well understood. Our measurements of the polar out-of-plane AMR show a surprisingly different response with a pronounced cusp-like feature. The maximum of the cusp-like anisotropy is reached when the magnetic field is oriented in the $a$-$b$ plane. Moreover, the AMR for the azimuthal out-of-plane current direction exhibits a very strong four-fold $a$-$b$ plane anisotropy. Combining the Fermi surfaces calculated from first principles with the Boltzmanns semiclassical transport theory we reproduce and explain all the prominent features of the unusual behavior of the in-plane and out-of-plane AMR. We are also able to clarify the origin of the strong non-saturating transverse magnetoresistance as an effect of imperfect charge-carrier compensation and open orbits. Finally, by combining our theoretical model and experimental data we estimate the average relaxation time of $2.6times10^{-14}$~s and the mean free path of $15$~nm at 1.8~K in our samples of ZrSiS.
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 finding provides some experimental evidence for crystal symmetry protection for the topological semimetal state, which is at the heart of topological relativistic fermion physics.
The topological nodal-line semimetals (NLSMs) possess a loop of Dirac nodes in the k space with linear dispersion, different from the point nodes in Dirac/Weyl semimetals. While the quantum transport associated with the topologically nontrivial Dirac fermions has been investigated extensively, features uniquely associated with the extended nodal lines remain to be demonstrated. Here, we investigate the quantum oscillations (QOs) in the nodal-line semimetal ZrSiS, with the electron transport along the c axis, and magnetic field rotating in the ab plane. The extremal orbits identified through the field orientation dependence of the QOs interlock with the nodal line, leading to a nonzero Berry phase. Most importantly, the Berry phase shows a significant dependence on the magnetic field orientation, which we argue to be due to the finite spin-orbit coupling gap. Our results demonstrate the importance of the spin-orbit coupling and the nodal-line dispersion in understanding the quantum transport of NLSMs.
Dirac semimetal PdTe2 single-crystal temperature-dependent ultrafast carrier and phonon dynamics were studied using ultrafast optical pump-probe spectroscopy. Two distinct carrier and coherent phonons relaxation processes were identified in the 5 K - 300 K range. Quantitative analysis revealed a fast relaxation process ({tau}_f) occurring on a subpicosecond time scale which originated from electron-phonon thermalization. This was followed by a slower relaxation process ({tau}_s) with a time scale of ~ 7-9.5 ps which originated from phonon-assisted electron-hole recombination. Two significant vibrational modes resolved at all measured temperatures and corresponded to Te atoms in-plane (E_g), and out-of-plane (A_1g), motion. As temperature increased both phonon modes softened markedly. A_1g mode frequency monotonically decreased as temperature increased. Its damping rate remained virtually unchanged. As expected, E_g decreased uniformly as temperatures rose. At temperatures above 80 K, there was insignificant change. Test results suggested that pure dephasing played an important role in the relaxation processes. PdTe2 phonon is thought responsible for its superconductive properties. Examining phonons behavior should improve the understanding of its complex superconductivity.
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