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Register a new userScattering dominated high-temperature phase of 1T-TiSe2: an optical conductivity study
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The controversy regarding the precise nature of the high-temperature phase of 1T-TiSe2 lasts for decades. It has intensified in recent times when new evidence for the excitonic origin of the low-temperature charge-density wave state started to unveil. Here we address the problem of the high-temperature phase through precise measurements and detailed analysis of the optical response of 1T-TiSe2 single crystals. The separate responses of electron and hole subsystems are identified and followed in temperature. We show that neither semiconductor nor semimetal pictures can be applied in their generic forms as the scattering for both types of carriers is in the vicinity of the Ioffe-Regel limit with decay rates being comparable to or larger than the offsets of band extrema. The nonmetallic temperature dependence of transport properties comes from the anomalous temperature dependence of scattering rates. Near the transition temperature the heavy electrons and the light holes contribute equally to the conductivity. This surprising coincidence is regarded as the consequence of dominant intervalley scattering that precedes the transition. The low-frequency peak in the optical spectra is identified and attributed to the critical softening of the L-point collective mode.
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The charge density wave phase transition of 1T-TiSe2 is studied by angle-resolved photoemission over a wide temperature range. An important chemical potential shift which strongly evolves with temperature is evidenced. In the framework of the exciton condensate phase, the detailed temperature dependence of the associated order parameter is extracted. Having a mean-field-like behaviour at low temperature, it exhibits a non-zero value above the transition, interpreted as the signature of strong excitonic fluctuations, reminiscent of the pseudo-gap phase of high temperature superconductors. Integrated intensity around the Fermi level is found to display a trend similar to the measured resistivity and is discussed within the model.
The transient optical conductivity of photoexcited 1T-TaS2 is determined over a three-order-of-magnitude frequency range. Prompt collapse and recovery of the Mott gap is observed. However, we find important differences between this transient metallic state and that seen across the thermally-driven insulator-metal transition. Suppressed low-frequency conductivity, Fano phonon lineshapes, and a mid-infrared absorption band point to polaronic transport. This is explained by noting that the photo-induced metallic state of 1T-TaS2 is one in which the Mott gap is melted but the lattice retains its low-temperature symmetry, a regime only accessible by photo-doping.
The simultaneous condensation of electronic and structural degrees of freedom gives rise to new states of matter, including superconductivity and charge-density-wave formation. When exciting such a condensed system, it is commonly assumed that the ultrafast laser pulse disturbs primarily the electronic order, which in turn destabilizes the atomic structure. Contrary to this conception, we show here that structural destabilization of few atoms causes melting of the macroscopic ordered charge-density wave in 1T-TiSe2. Using ultrafast pump-probe non-resonant and resonant X-ray diffraction, we observe full suppression of the Se 4p orbital order and the atomic structure at excitation energies more than one order of magnitude below the suggested excitonic binding energy. Complete melting of the charge-density wave occurs 4-5 times faster than expected from a purely electronic charge-screening process, strongly suggesting a structurally assisted breakup of excitonic correlations. Our experimental data clarifies several questions on the intricate coupling between structural and electronic order in stabilizing the charge-density-wave in 1T-TiSe2. The results further show that electron-phonon-coupling can lead to different, energy dependent phase-transition pathways in condensed matter systems, opening new possibilities in the conception of non-equilibrium phenomena at the ultrafast scale.
The correlation between electronic and crystal structures of 1T-TiSe2 in the charge density wave (CDW) state is studied by x-ray diffraction. Three families of reflections are used to probe atomic displacements and the orbital asymmetry in Se. Two distinct onset temperatures are found, TCDW and a lower T* indicative for an onset of Se out-of-plane atomic displacements. T* coincides with a DC resistivity maximum and the onset of the proposed gyrotropic electronic structure. However, no indication for chirality is found. The relation between the atomic displacements and the transport properties is discussed in terms of Ti 3d and Se 4p states that only weakly couple to the CDW order.
Compounds with intermediate-size transition metals such as Fe or Mn are close to the transition between charge-transfer systems and Mott-Hubbard systems. We study the optical conductivity sigma(omega) of insulating layered LaSrFeO_4 in the energy range 0.5 - 5.5 eV from 15 K to 250 K by the use of spectroscopic ellipsometry in combination with transmittance measurements. A multipeak structure is observed in both sigma^a(omega) and sigma^c(omega). The layered structure gives rise to a pronounced anisotropy, thereby offering a means to disentangle Mott-Hubbard and charge-transfer absorption bands. We find strong evidence that the lowest dipole-allowed excitation in LaSrFeO_4 is of Mott-Hubbard type. This rather unexpected result can be attributed to Fe 3d - O 2p hybridization and in particular to the layered structure with the associated splitting of the e_g level. In general, Mott-Hubbard absorption bands may show a strong dependence on temperature. This is not the case in LaSrFeO_4, in agreement with the fact that spin-spin and orbital-orbital correlations between nearest neighbors do not vary strongly below room temperature in this compound with a high-spin 3d^5 configuration and a Neel temperature of T_N = 366 K.
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