Search

The correlation between electronic and crystal structures of 1T-TiSe_{2} in the charge-density wave (CDW) state is studied by x-ray diffraction in order to clarify basic properties in the CDW state, transport properties, and chirality. Three families of reflections are used to probe atomic displacements and the orbital asymmetry in Se. Two distinct onset temperatures are found: T_{CDW} 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 (chiral) 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.

Ultrafast electron delocalization induced by a femtosecond laser pulse is a well-known process in which electrons are ejected from the ions within the laser pulse duration. However, very little is known about the speed of electron localization out of an electron gas in correlated metals, i.e., the capture of an electron by an ion. Here, we demonstrate by means of pump-probe x-ray techniques across the Eu L_{3} absorption edge that an electron localization process in the EuNi_{2}(Si_{0.21}Ge_{0.79})_{2} intermetallic material occurs within a few hundred femtoseconds after the optical excitation. Spectroscopy and diffraction data collected simultaneously at low temperature and for various laser fluences show that the localization dynamics process is much faster than the thermal expansion of the unit cell along the c direction which occurs within picoseconds. Nevertheless, this latter process is still much slower than pure electronic effects, such as screening, and the subpicosecond timescale indicates an optical phonon driven origin. In addition, comparing the laser fluence dependence of the electronic response with that found in other intermediate 4f valence materials, we suggest that the electron localization process observed in this Eu-based correlated metal is mainly related to changes in the 4f hybridization. The observed ultrafast electron localization process sparks fundamental questions for our understanding of electron correlations and their coupling to the lattice.

In this work, we use ultrafast pump-probe nonresonant and resonant x-ray diffraction to track the periodic lattice distortion and the electronic charge density wave in 1T-TiSe_{2} upon optical excitation. We observe a fluence regime in which the periodic lattice deformation is strongly suppressed but the charge density wave related Se 4p orbital order remains mostly intact. Complete melting of both structural and electronic order occurs four to five times faster than expected from a purely electronic charge-screening process, strongly suggesting a structurally assisted weakening of excitonic correlations. Our experimental data provide insight on the intricate coupling between structural and electronic order in stabilizing the periodic-lattice-distortion/charge-density-wave state in 1T-TiSe_{2}. The results further show that electron-phonon coupling can lead to different, energy dependent phase-transition pathways in condensed matter systems, opening different possibilities in the conception of nonequilibrium phenomena at the ultrafast scale.

We investigate the structural dynamics of the incommensurately modulated phase of Sn 2 P 2 Se 6 by means of time-resolved X-ray diffraction following excitation by an optical pump. Tracking the incommensurable distortion in the time domain enables us to identify the transport effects leading to a complete disappearance of the incommensurate phase over the course of 100 ns. These observations suggest that a thin surface layer of the high-temperature phase forms quickly after photo-excitation and then propagates into the material with a constant velocity of 3.7 m/s. Complementary static structural measurements reveal previously unreported higher-order satellite reflection in the incommensurate phase. These higher-order reflections are attributed to cubic vibrational terms in the Hamiltonian.