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Register a new userDoublon bottleneck in the ultrafast relaxation dynamics of hot electrons in 1T-TaS_2
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Employing time-resolved photoelectron spectroscopy we analyze the relaxation dynamics of hot electrons in the charge density wave / Mott material 1T-TaS_2. At 1.2 eV above the Fermi level we observe a hot electron lifetime of 12 +- 5 fs in the metallic state and of 60 +- 10 fs in the broken symmetry ground state - a direct consequence of the reduced phase space for electron-electron scattering determined by the Mott gap. Boltzmann equation calculations which account for the interaction of hot electrons in a Bloch band with a doublon-holon excitation in the Mott state provide insight into the unoccupied electronic structure in the correlated state.
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Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic in- teractions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS$_2$, we identify a spectroscopic signature of double occupied sites (doublons) that are reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycle $hbar/Japprox$ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained by purely electronic effects captured by the single band Hubbard model, where thermalization is fast in the small-gap regime. Qualitative agreement with the experimental results however requires the assumption of an intrinsic hole-doping. The sensitivity of the doublon dynamics on the doping level provides a way to control ultrafast processes in such strongly correlated materials.
The dynamical properties of single crystal 1T-TaS$_{2}$ are investigated both in commensurate charge density wave state (CCDW state) and hidden charge density wave state (HCDW state). We develop a useful criterion in time-domain transmission terahertz measurement to judge whether the compound is driven into a metastable state or still in its virgin state. An increase of terahertz conductivity by two orders of magnitude from CCDW state to HCDW state is obtained by taking account of the penetration depth mismatch, which is in agreement with reported emph{dc} transport measurement. Upon weak pumping, only transient processes with rapid decay dynamics are triggered in both CCDW and HCDW states. We compare the conductivity increases in terahertz frequency range between transient and HCDW states and suggest that fluctuated metallic domain walls may develop in the transient states.
Through a series of transverse magnetic focusing experiments, we show that hot electrons in a two-dimensional electron gas system undergo an ultrafast relaxation when generated by a quantum dot (QD) instead of a quantum point contact (QPC). We find here that QPC hot electrons were well described by the non-interacting Fermi gas model for excitations up to 1.5 meV above the Fermi level of 7.44 meV, whereas QD hot electrons exhibited an energy loss quadratic to the excitation. The energy relaxation was a sizeable fraction of the tested excitations, up to about 55%. With the proposal that the hot electrons are relaxed by the QD immediately after emission, we present a toy model in which a capacitive coupling between the QD and its leads results in a finite, ultrafast energy relaxation.
Frequency and dc magnetic field dependences of dynamic susceptibility in diluted paramagnets LiYF$_4$:Ho$^{3+}$ have been measured at liquid helium temperatures in the ac and dc magnetic fields parallel to the symmetry axis of a tetragonal crystal lattice. Experimental data are analyzed in the framework of microscopic theory of relaxation rates in the manifold of 24 electron-nuclear sublevels of the lowest non-Kramers doublet and the first excited singlet in the Ho$^{3+}$ ground multiplet $^5I_8$ split by the crystal field of S$_4$ symmetry. The one-phonon transition probabilities were computed using electron-phonon coupling constants calculated in the framework of exchange charge model and were checked by optical piezospectroscopic measurements. The specific features observed in field dependences of the in- and out-of-phase susceptibilities (humps and dips, respectively) at the crossings (anti-crossings) of the electron-nuclear sublevels are well reproduced by simulations when the phonon bottleneck effect and the cross-spin relaxation are taken into account.
A prototypical quasi-2D metallic compound, 1T-TaS_2 has been extensively studied due to an intricate interplay between a Mott-insulating ground state and a charge density-wave (CDW) order. In the low-temperature phase, 12 out of 13 Ta_{4+} 5textit{d}-electrons form molecular orbitals in hexagonal star-of-David patterns, leaving one 5textit{d}-electron with textit{S} = 1/2 spin free. This orphan quantum spin with a large spin-orbit interaction is expected to form a highly correlated phase of its own. And it is most likely that they will form some kind of a short-range order out of a strongly spin-orbit coupled Hilbert space. In order to investigate the low-temperature magnetic properties, we performed a series of measurements including neutron scattering and muon experiments. The obtained data clearly indicate the presence of the short-ranged phase and put the upper bound on ~ 0.4 textit{mu}_B for the size of the magnetic moment, consistent with the orphan-spin scenario.
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