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Abstract: Quantum materials display exotic behaviours related to the interplay between temperature-driven phase transitions. Here, we study the electron dynamics in one such material, CaFe$_2$As$_2$, a parent Fe-based superconductor, employing time and angle-resolved photoemission spectroscopy. CaFe$_2$As$_2$ exhibits concomitant transition to spin density wave state and tetragonal to orthorhombic structure below 170 K. The Fermi surface of this material consists of three hole pockets ($\alpha$, $\beta$ and $\gamma$) around $\Gamma$-point and two electron pockets around $X$-point. The hole pockets have $d_{xy}$, $d_{yz}$ and $d_{zx}$ orbital symmetries. The $\beta$ band constituted by $d_{xz}$/$d_{yz}$ orbitals exhibit a gap across the magnetic phase transition. We discover that polarized pump pulses can induce excitations of electrons of a selected symmetry. More specifically, while $s$-polarized light (polarization vector perpendicular to the $xz$-plane) excites electrons corresponding to all the three hole bands, $p$-polarized light excites electrons essentially from ($\alpha$,$\beta$) bands which are responsible for magnetic order. Interestingly, within the magnetically ordered phase, the excitation due to the $p$-polarized pump pulses occur at a time scale of 50 fs, which is significantly faster than the excitation induced by $s$-polarized light ($\sim$ 200 fs). These results suggest that the relaxation of different ordered phases occurs at different time scales and this method can be used to achieve selective excitations to disentangle complexity in the study of quantum materials.
Keywords: Electronic structure, Pnictides and chalcogenides, Time-resolved spectroscopy
Published in RUNG: 13.10.2021; Views: 3153; Downloads: 9
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Abstract: Photons have fixed spin and unbounded orbital angular momentum (OAM). While the former is manifested in the polarization of light, the latter corresponds to the spatial phase distribution of its wavefront1. The distinctive way in which the photon spin dictates the electron motion upon light– matter interaction is the basis for numerous well-established spectroscopies. By contrast, imprinting OAM on a mat- ter wave, specifically on a propagating electron, is gener- ally considered very challenging and the anticipated effect undetectable2. In refs. 3,4, the authors provided evidence of OAM-dependent absorption of light by a bound electron. Here, we seek to observe an OAM-dependent dichroic photo- electric effect, using a sample of He atoms. Surprisingly, we find that the OAM of an optical field can be imprinted coher- ently onto a propagating electron wave. Our results reveal new aspects of light–matter interaction and point to a new kind of single-photon electron spectroscopy.
Keywords: FEL, OAM, Photoelectric effect
Published in RUNG: 09.09.2020; Views: 4190; Downloads: 0
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Abstract: The initial deactivation pathways of gaseous 2-nitrophenol excited at 268 nm were investigated by time-resolved photoelectron spectroscopy (TRPES) with femtosecond-VUV light, produced by a monochromatized high harmonic generation source. TRPES allowed us to obtain new, valuable experimental information about the ultrafast excited-state dynamics of 2-nitrophenol in the gas phase. In accord with recent ab initio on-the-fly nonadiabatic molecular dynamic simulations, our results validate the occurrence of an ultrafast intersystem crossing leading to an intermediate state that decays on a subpicosecond time scale with a branched mechanisms. Two decay pathways are experimentally observed. One probably involves proton transfer, leading to the most stable triplet aci-form of 2-nitrophenol; the second pathway may involve OH rotation. We propose that following intersystem crossing, an ultrafast fragmentation channel leading to OH or HONO loss could also be operative.
Keywords: Ultrafast photoemission, nitrophenol
Published in RUNG: 12.02.2019; Views: 4797; Downloads: 0
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Abstract: We report on orbital-dependent quasiparticle dynamics in EuFe 2 As 2, a parent compound of Fe-based superconductors, and a way to experimentally identify this behavior using time-and angle-resolved photoelectron spectroscopy across the spin density wave transition. We observe two different relaxation timescales for photoexcited d x z/d y z and d x y electrons. While the itinerant d x z/d y z electrons relax faster through the electron-electron scattering channel, d x y electrons form a quasiequilibrium state with the lattice due to their localized character, and the state decays slowly. Our findings suggest that electron correlation in Fe pnictides is an important property, which should carefully be taken into account when describing the electronic properties of both parent and carrier-doped compounds, and therefore establish a strong connection with cuprates
Keywords: photoelectron dynamics, Fe based superconductors
Published in RUNG: 29.11.2018; Views: 4756; Downloads: 0
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Keywords: Cobalt Phtalocyanine, photoemission spectroscopy, gas phase, solid state
Published in RUNG: 07.02.2018; Views: 5570; Downloads: 0
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