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.
We investigate the low-temperature charge-density-wave (CDW) state of bulk TaS$_2$ with a fully self-consistent DFT+U approach, over which the controversy has remained unresolved regarding the out-of-plane metallic band. By examining the innate structure of the Hubbard U potential, we reveal that the conventional use of atomic-orbital basis could seriously misevaluate the electron correlation in the CDW state. By adopting a generalized basis, covering the whole David star, we successfully reproduce the Mott insulating nature with the layer-by-layer antiferromagnetic order. Similar consideration should be applied for description of the electron correlation in molecular solid.
The Drude model describes the free-electron conduction in simple metals, governed by the freedom that the mobile electrons have within the material. In strongly correlated systems, however, a significant deviation of the optical conductivity from the simple metallic Drude behavior is observed. Here, we investigate the optical conductivity of the heavy-fermion system CeCu$_{mathrm{6-x}}$Au$_{mathrm{x}}$, using time-resolved, phase-sensitive terahertz spectroscopy. Terahertz electric field creates two types of excitations in heavy-fermion materials: First, the intraband excitations that leave the heavy quasiparticles intact. Second, the resonant interband transitions between the heavy and light parts of the hybridized conduction band that break the Kondo singlet. We find that the Kondo-singlet breaking interband transitions do not create a Drude peak, while the Kondo-retaining intraband excitations yield the expected Drude response; thus, making it possible to separate these two fundamentally different correlated contributions to the optical conductivity.
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.
We demonstrate terahertz time-domain spectroscopy (THz-TDS) to be an accurate, rapid and scalable method to probe the interaction-induced Fermi velocity renormalization { u}F^* of charge carriers in graphene. This allows the quantitative extraction of all electrical parameters (DC conductivity {sigma}DC, carrier density n, and carrier mobility {mu}) of large-scale graphene films placed on arbitrary substrates via THz-TDS. Particularly relevant are substrates with low relative permittivity (< 5) such as polymeric films, where notable renormalization effects are observed even at relatively large carrier densities (> 10^12 cm-2, Fermi level > 0.1 eV). From an application point of view, the ability to rapidly and non-destructively quantify and map the electrical ({sigma}DC, n, {mu}) and electronic ({ u}F^* ) properties of large-scale graphene on generic substrates is key to utilize this material in applications such as metrology, flexible electronics as well as to monitor graphene transfers using polymers as handling layers.
In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the $pi$ band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.
Z. X. Wang
,Q. M. Liu
,L. Y. Shi
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(2019)
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"Photoinduced hidden CDW state and relaxation dynamics of 1T-TaS_2 probed by time-resolved terahertz spectroscopy"
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Zixiao Wang
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