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Using time- and angle-resolved photoemission spectroscopy, we study the response of metallic single layer TaS$_2$ in the 1H structural modification to the generation of excited carriers by a femtosecond laser pulse. A complex interplay of band structure modifications and electronic temperature increase is observed and analyzed by direct fits of model spectral functions to the two-dimensional (energy and $k$-dependent) photoemission data. Upon excitation, the partially occupied valence band is found to shift to higher binding energies by up to 150 meV, accompanied by electronic temperatures exceeding 3000~K. These observations are explained by a combination of temperature-induced shifts of the chemical potential, as well as temperature-induced changes in static screening. Both contributions are evaluated in a semi-empirical tight-binding model. The shift resulting from a change in the chemical potential is found to be dominant.
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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 absence of inversion symmetry leads to a strong spin-orbit splitting of the upper valence band of semiconducting single layer transition metal dichalchogenides such as MoS$_2$ or WS$_2$. This permits a direct comparison of the electron-phonon coupling strength in states that only differ by their spin. Here, the electron-phonon coupling in the valence band maximum of single-layer WS$_2$ is studied by first principles calculations and angle-resolved photoemission. The coupling strength is found to be drastically different for the two spin-split branches, with calculated values of $lambda_K=$0.0021 and 0.40 for the upper and lower spin-split valence band of the free-standing layer, respectively. This difference is somewhat reduced when including scattering processes involving the Au(111) substrate present in the experiment and the experimental results confirm the strongly branch-dependent coupling strength.
Our detailed Angle Resolved Photoemission Spectroscopy (ARPES) study of $2H$-TaS$_2$, a canonical incommensurate charge density wave (CDW) material, illustrates pronounced many-body renormalization in the system, which is manifested by the presence of multiple kink structures in the electronic dispersions. Temperature-dependent measurements reveal that these kink structures persist even at temperatures higher than the charge density wave transition temperature $it{T}_{text{cdw}},$ and the energy locations of the kinks are practically temperature-independent. Correlating kink energies with the published Raman scattering data and the theoretically calculated phonon spectrum of $2H$-TaS$_2$, we conclude phononic mechanism for these kinks. We have also detected momentum-anisotropy in the band renormalization, which in turn indicates momentum-dependence of the electron-phonon coupling of the system.
The dynamics of S=1/2 quantum spins on a 2D square lattice lie at the heart of the mystery of the cuprates cite{Hayden2004,Vignolle2007,Li2010,LeTacon2011,Coldea2001,Headings2010,Braicovich2010}. In bulk cuprates such as LCO{}, the presence of a weak interlayer coupling stabilizes 3D N{e}el order up to high temperatures. In a truly 2D system however, thermal spin fluctuations melt long range order at any finite temperature cite{Mermin1966}. Further, quantum spin fluctuations transfer magnetic spectral weight out of a well-defined magnon excitation into a magnetic continuum, the nature of which remains controversial cite{Sandvik2001,Ho2001,Christensen2007,Headings2010}. Here, we measure the spin response of emph{isolated one-unit-cell thick layers} of LCO{}. We show that coherent magnons persist even in a single layer of LCO{} despite the loss of magnetic order, with no evidence for resonating valence bond (RVB)-like spin correlations cite{Anderson1987,Hsu1990,Christensen2007}. Thus these excitations are well described by linear spin wave theory (LSWT). We also observe a high-energy magnetic continuum in the isotropic magnetic response. This high-energy continuum is not well described by 2 magnon LSWT, or indeed any existing theories.
1T-TaS$_2$ is a prototypical charge-density-wave (CDW) system with a Mott insulating ground state. Usually, a Mott insulator is accompanied by an antiferromagnetic state. However, the antiferromagnetic order had never been observed in 1T-TaS$_2$. Here, we report the stabilization of the antiferromagnetic order by the intercalation of a small amount of Fe into the van der Waals gap of 1T-TaS$_2$, i.e. forming 1T-Fe$_{0.05}$TaS$_2$. Upon cooling from 300~K, the electrical resistivity increases with a decreasing temperature before reaching a maximum value at around 15~K, which is close to the Neel temperature determined from our magnetic susceptibility measurement. The antiferromagnetic state can be fully suppressed when the sample thickness is reduced, indicating that the antiferromagnetic order in Fe$_{0.05}$TaS$_2$ has a non-negligible three-dimensional character. For the bulk Fe$_{0.05}$TaS$_2$, a comparison of our high pressure electrical transport data with that of 1T-TaS$_2$ indicates that, at ambient pressure, Fe$_{0.05}$TaS$_2$ is in the nearly commensurate charge-density-wave (NCCDW) phase near the border of the Mott insulating state. The temperature-pressure phase diagram thus reveals an interesting decoupling of the antiferromagnetism from the Mott insulating state.
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