Time-resolved near-edge X-ray absorption fine structure of pyrazine from electronic structure and nuclear wave packet dynamics simulations

Tsuru, Shota; Vidal, Marta L.; Pápai, Mátyás; Krylov, Anna I.; Møller, Klaus Braagaard; Coriani, Sonia

doi:10.1063/1.5115154

Cited by 45 publications

(58 citation statements)

References 80 publications

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“…A temporal resolution of 11 fs is measured in a pump-probe experiment. This duration is already 8/10 enough to consider the observation of ultrafast chemical dynamics at the C K-edge 30,31,52,58 . Improved CEP stability and feedback control over the delay will allow attosecond transient absorption experiments in the SXR in the future.…”

Section: Discussionmentioning

confidence: 99%

Efficient table-top dual-wavelength beamline for ultrafast transient absorption spectroscopy in the soft X-ray region

Barreau

Ross

Garg

et al. 2020

Sci Rep

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We present a table-top beamline providing a soft X-ray supercontinuum extending up to 350 eV from high-order harmonic generation with sub-13 fs 1300 nm driving pulses and simultaneous production of sub-5 fs pulses centered at 800 nm. Optimization of the high harmonic generation in a long and dense gas medium yields a photon flux of ~2 x 10 7 photons/s/1% bandwidth at 300 eV. The temporal resolution of X-ray transient absorption experiments with this beamline is measured to be 11 fs for 800 nm excitation. This dual-wavelength approach, combined with high flux and high spectral and temporal resolution soft X-ray absorption spectroscopy, is a new route to the study of ultrafast electronic dynamics in carbon-containing molecules and materials at the carbon K-edge. 2/10 Description of the table-top dual-wavelength beamlineThe beamline is summarized in Figure 1. It uses a 13 mJ , 800 nm, 30 fs, 1 kHz Ti:Sapphire laser (Coherent Legend Elite Duo), whose energy is split into 11 mJ +2 mJ to produce the probe and pump pulses, respectively, used in time-resolved X-ray transient absorption experiments. This section details the simultaneous compression of SWIR (centered at 1300 nm or 1400 nm) and visible-near infrared (centered at 800 nm) pulses, and the characteristics of the soft X-ray spectrometer. Production of few-cycle short-wave infrared pulsesThe few-cycle pulses centered at 1300 nm in the SWIR are produced using an OPA followed by spectral broadening in a hollow-core fiber filled with a rare gas 35 and compression with chirped mirrors 36 . The 11 mJ 800 nm beam is further split into 0.5 mJ and 10.5 mJ for use in a two-stage OPA, which converts the 800 nm to SWIR (1300 nm). The two-stage system is obtained from Light Conversion and is designed to provide CEP stability of the signal pulses. The first stage is a low energy OPA (TOPAS Prime), pumped by 0.5 mJ, which provides 90 J of 2 m pulses in the idler. Due to the parametric amplification process, the idler pulses are passively CEP stabilized, with a stability of <200 mrad. They are then used as the seed for the white light generation in a second, high energy, OPA (HE-TOPAS) pumped with the remaining 10.5 mJ of 800 nm light. This design should ensure the CEP stability of the signal pulses over the 1200-1600 nm tunable range of the OPA, regardless of the CEP stability of the pump laser. However, the following results are obtained with a CEP-averaged signal pulse. The 2.8 mJ, 1300 nm, 40 fs output is focused with a 2-m focusing mirror to a focal size of 390 m (at 1/e 2 ) at the entrance of a 3-m-long, 700-m-inner diameter stretched hollow-core fiber (HCF) filled with 0.4 bar of argon (Few-Cycle Inc.). The ratio of beam

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Section: Discussionmentioning

confidence: 99%

Efficient table-top dual-wavelength beamline for ultrafast transient absorption spectroscopy in the soft X-ray region

Barreau

Ross

Garg

et al. 2020

Sci Rep

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“…From the experimental point of view, the core-to-SOMO peaks are a preferred choice when tracking excited-state dynamics, since they unambiguously originate from the valence-excited states that are probed. 5,11,12,38 Other mechanisms can of course also occur, see e.g. the right scheme in Fig.…”

Section: Intersystem Crossings In Acetylacetonementioning

confidence: 99%

Spin adapted implementation of EOM-CCSD for triplet excited states: Probing intersystem crossings of acetylacetone at the carbon and oxygen K-edges

Faber

Kjønstad

Koch

et al. 2019

The Journal of Chemical Physics

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“…42 Increasing effort is being devoted towards enabling theoretical support for transient X-ray spectroscopies both in terms of accurate calculations of valenceto-core-excited state spectroscopic signals and inclusion of coupled electron-nuclear dynamics. Currently available methods for simulating TRXAS include density functional theory (DFT), 10,[43][44][45][46] restricted active space self-consistent eld without (RASSCF) 47,48 and with second-order perturbation correction (RASPT2), 46,49 algebraic-diagrammatic construction (ADC), [50][51][52] coupled cluster 13,[53][54][55] and combined DFT/ multireference conguration interaction. 56 Effects of nuclear dynamics, and in particular non-adiabatic transitions, have been treated at varying degrees of complexity and accuracy using full-dimensionality trajectory- 10,48 and Gaussian wavepacket-based 46,51,57 dynamics as well as reduced-dimensionality quantum dynamics.…”

Section: Introductionmentioning

confidence: 99%

Probing competing relaxation pathways in malonaldehyde with transient X-ray absorption spectroscopy

et al. 2020

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Time-resolved near-edge X-ray absorption fine structure of pyrazine from electronic structure and nuclear wave packet dynamics simulations

Cited by 45 publications

References 80 publications

Efficient table-top dual-wavelength beamline for ultrafast transient absorption spectroscopy in the soft X-ray region

Efficient table-top dual-wavelength beamline for ultrafast transient absorption spectroscopy in the soft X-ray region

Spin adapted implementation of EOM-CCSD for triplet excited states: Probing intersystem crossings of acetylacetone at the carbon and oxygen K-edges

Probing competing relaxation pathways in malonaldehyde with transient X-ray absorption spectroscopy

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