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Abstract: In devices based on organic semiconductors, aggregation and inter-molecular interactions play a key role in affecting the photo-physical and dynamical carrier properties of the material, potentially becoming a limiting factor to achieving high efficiency. As a consequence, a detailed understanding of the interplay between the film molecular structure and the material properties is essential to properly design devices with optimized performance. Here we demonstrate how different molecular structural arrangements modulate the charge transfer (CT) dynamics in cobalt phthalocyanine (CoPc) thin films. By transient absorption spectroscopy and time-resolved photoemission spectroscopy, we study the influence of different CoPc structures on the dynamical electronic properties, the CoPc intra and inter- molecular de-excitation pathways up to 7 ns. We rationalize the ultrafast formation of triplet states in the CoPc through an electron exchange process between the single-occupied Co3dz2 orbital and p orbitals of the macrocycle, which obviate for an energetically unfavourable spin-flip. We found enhanced CT exciton lifetime in the case of the herringbone structure with respect to the brickwork one, possibly explainable by a more efficient CT exciton delocalization along the stacking axis.
Keywords: Charge transfer, organic molecules, time resolved spectroscopies
Published in RUNG: 30.06.2023; Views: 571; Downloads: 2
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Keywords: harge density wave, Brillouin zone, angle-resolved photoemission spectroscopy, time-resolved photoemission spectroscopy., angle-resolved photoemission spectroscopy
Published in RUNG: 21.06.2023; Views: 594; Downloads: 0
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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: 1536; Downloads: 5
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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: 2582; 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: 3276; Downloads: 0
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