Flexible attosecond beamline for high harmonic spectroscopy and XUV/near-IR pump probe experiments requiring long acquisition times

Weber, Sébastien J.; Manschwetus, Bastian; Billon, M.; Böttcher, Martin; Bougeard, M.; Breger, P.; Géléoc, Marie; Gruson, Vincent; Huetz, A.; Lin, Nan; Picard, Y. J.; Ruchon, Thierry; Salières, P.; Carré, B.

doi:10.1063/1.4914464

Cited by 30 publications

(32 citation statements)

References 67 publications

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“…The experiments were conducted on the PLFA beamline (CEA Saclay) 60 where the XUV pulses generated by the bichromatic field were focused in a COLTRIMS-type reaction microscope 61 to induce photoionization of randomly oriented NO target molecules (Fig. 4 and Methods section).…”

Section: Resultsmentioning

confidence: 99%

Evidence of depolarization and ellipticity of high harmonics driven by ultrashort bichromatic circularly polarized fields

et al. 2018

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High harmonics generated by counter-rotating laser fields at the fundamental and second harmonic frequencies have raised important interest as a table-top source of circularly polarized ultrashort extreme-ultraviolet light. However, this emission has not yet been fully characterized: in particular it was assumed to be fully polarized, leading to an uncertainty on the effective harmonic ellipticity. Here we show, through simulations, that ultrashort driving fields and ultrafast medium ionization lead to a breaking of the dynamical symmetry of the interaction, and consequently to deviations from perfectly circular and fully polarized harmonics, already at the single-atom level. We perform the complete experimental characterization of the polarization state of high harmonics generated along that scheme, giving direct access to the ellipticity absolute value and sign, as well as the degree of polarization of individual harmonic orders. This study allows defining optimal generation conditions of fully circularly polarized harmonics for advanced studies of ultrafast dichroisms.

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Section: Resultsmentioning

confidence: 99%

Evidence of depolarization and ellipticity of high harmonics driven by ultrashort bichromatic circularly polarized fields

et al. 2018

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“…We now turn to the combination of the 3D-momentum spectrometry with APT generation. The experiments have been conducted on the PLFA beamline at SLIC facility of CEA Saclay 52 . A schematic of the setup is shown in Figure 3.…”

Section: Combining 3d-momentum Spectrometry With Apt Generation: Expementioning

confidence: 99%

Molecular frame photoemission by a comb of elliptical high-order harmonics: a sensitive probe of both photodynamics and harmonic complete polarization state

et al. 2016

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Due to the intimate anisotropic interaction between an XUV light field and a molecule resulting in photoionization (PI), molecular frame photoelectron angular distributions (MFPADs) are most sensitive probes of both electronic/nuclear dynamics and the polarization state of the ionizing light field. Consequently, they encode the complex dipole matrix elements describing the dynamics of the PI transition, as well as the three normalized Stokes parameters s, s, s characterizing the complete polarization state of the light, operating as molecular polarimetry. The remarkable development of advanced light sources delivering attosecond XUV pulses opens the perspective to visualize the primary steps of photochemical dynamics in time-resolved studies, at the natural attosecond to few femtosecond time-scales of electron dynamics and fast nuclear motion. It is thus timely to investigate the feasibility of measurement of MFPADs when PI is induced e.g., by an attosecond pulse train (APT) corresponding to a comb of discrete high-order harmonics. In the work presented here, we report MFPAD studies based on coincident electron-ion 3D momentum imaging in the context of ultrafast molecular dynamics investigated at the PLFA facility (CEA-SLIC), with two perspectives: (i) using APTs generated in atoms/molecules as a source for MFPAD-resolved PI studies, and (ii) taking advantage of molecular polarimetry to perform a complete polarization analysis of the harmonic emission of molecules, a major challenge of high harmonic spectroscopy. Recent results illustrating both aspects are reported for APTs generated in unaligned SF molecules by an elliptically polarized infrared driving field. The observed fingerprints of the elliptically polarized harmonics include the first direct determination of the complete s, s, s Stokes vector, equivalent to (ψ, ε, P), the orientation and the signed ellipticity of the polarization ellipse, and the degree of polarization P. They are compared to so far incomplete results of XUV optical polarimetry. We finally discuss the comparison between the outcomes of photoionization and high harmonic spectroscopy for the description of molecular photodynamics.

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“…This remarkable property underlies the 'molecular polarimetry' (MP) method [16] which is tunable and available over a spectral range spanning from VUV to x-ray photon energies [14,17,18], where polarimetry is a challenging task. We recently applied the MP method to retrieve the complete polarization state of individual high-order harmonics (HHs) in an attosecond pulse train (APT) produced by the HHG-based XUV source of the PLFA facility of CEA-Saclay [19], for different schemes involving symmetry breaking in the generation process [20,21]. For these experiments, we chose process (I) which possesses fingerprint properties to act as an efficient 'polarimeter'.…”

Section: Introductionmentioning

confidence: 99%

Dissociative photoionization of NO across a shape resonance in the XUV range using circularly polarized synchrotron radiation

Veyrinas

Saquet

Poullain

et al. 2019

The Journal of Chemical Physics

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We report benchmark results for dissociative photoionization (DPI) spectroscopy and dynamics of the NO molecule in the region of the σ* shape resonance in the ionization leading to the NO + (c 3 Π) ionic state. The experimental study combines well characterized XUV circularly polarized synchrotron radiation (SR), delivered at the DESIRS beamline (SOLEIL), with ionelectron coincidence 3D momentum spectroscopy. The measured (N + , e) kinetic energy correlation diagrams reported at four discrete photon energies in the extended 23-33 eV energy range allow for resolving the different active DPI reactions, and indicate the importance of spectrally-resolved studies using SR in the context of time-resolved studies where PI is induced by broadband XUV attosecond pulses. In the dominant DPI reaction which leads to the NO + (c 3 Π) ionic state, PI dynamics across the σ* shape resonance are probed by molecular frame photoelectron angular distributions where the parallel and perpendicular transitions are highlighted, as well as the circular dichroism CDAD(θ e ) in the molecular frame. The latter also constitute benchmark references for molecular polarimetry. The measured dynamical parameters are well described by multichannel Schwinger configuration interaction calculations. Similar results are obtained for the DPI spectroscopy of highly excited NO + electronic states populated in the explored XUV photon energy range.

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Flexible attosecond beamline for high harmonic spectroscopy and XUV/near-IR pump probe experiments requiring long acquisition times

Cited by 30 publications

References 67 publications

Evidence of depolarization and ellipticity of high harmonics driven by ultrashort bichromatic circularly polarized fields

Evidence of depolarization and ellipticity of high harmonics driven by ultrashort bichromatic circularly polarized fields

Molecular frame photoemission by a comb of elliptical high-order harmonics: a sensitive probe of both photodynamics and harmonic complete polarization state

Dissociative photoionization of NO across a shape resonance in the XUV range using circularly polarized synchrotron radiation

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