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

Barreau, Lou; Veyrinas, K.; Gruson, Vincent; Weber, Sébastien J.; Auguste, T.; Hergott, J.-F.; Lepetit, F.; Carré, B.; Houver, J. C.; Dowek, D.; Salières, P.

doi:10.1038/s41467-018-07151-8

Cited by 60 publications

(32 citation statements)

References 72 publications

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“…2e . As shown in Supplementary Note 9 , we extracted the Stokes polarization parameters of the harmonics from these measurements and estimated a value of the degree of polarization of 0.8 ± 0.2 for all harmonics, similar to reported values for the generation of circular harmonics from atomic and molecular gases 29 , 30 . Moreover, we find in Si that the harmonic ellipticities | ε HH | are all close to 1, independent of sample rotation θ (see Fig.…”

Section: Resultssupporting

confidence: 60%

Polarization-state-resolved high-harmonic spectroscopy of solids

et al. 2019

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Attosecond metrology sensitive to sub-optical-cycle electronic and structural dynamics is opening up new avenues for ultrafast spectroscopy of condensed matter. Using intense lightwaves to precisely control the fast carrier dynamics in crystals holds great promise for next-generation petahertz electronics and devices. The carrier dynamics can produce high-order harmonics of the driving field extending up into the extreme-ultraviolet region. Here, we introduce polarization-state-resolved high-harmonic spectroscopy of solids, which provides deeper insights into both electronic and structural sub-cycle dynamics. Performing high-harmonic generation measurements from silicon and quartz, we demonstrate that the polarization states of the harmonics are not only determined by crystal symmetries, but can be dynamically controlled, as a consequence of the intertwined interband and intraband electronic dynamics. We exploit this symmetry-dynamics duality to efficiently generate coherent circularly polarized harmonics from elliptically polarized pulses. Our experimental results are supported by ab-initio simulations, providing evidence for the microscopic origin of the phenomenon.

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Section: Resultssupporting

confidence: 60%

Polarization-state-resolved high-harmonic spectroscopy of solids

et al. 2019

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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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“…4(b), the driving conditions are not right to drive the electrons into regions in which the varying m * k changes the polarization of HH5 over the course of the pulse significantly. In any case, depolarization effects have been discussed recently in gas HHG [39] and we predict that the influence of the band structure can cause an even stronger depolarization in solid HHG, although this remains yet to be observed.…”

Section: Zinc Sulfidementioning

confidence: 59%

Role of intraband dynamics in the generation of circularly polarized high harmonics from solids

et al. 2020

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Recent studies have demonstrated that the polarization states of high harmonics from solids can differ from those of the driving pulses. To gain insights on the microscopic origin of this behavior, we perform one-particle intraband-only calculations and reproduce some of the most striking observations. For instance, our calculations yield circularly polarized harmonics from elliptically polarized pulses that sensitively depend on the driving conditions. Furthermore, we perform experiments on ZnS and find partly similar characteristics as reported from silicon. Comparison to our intraband-only calculations shows reasonable qualitative agreement for a below-band-gap harmonic. We show that intraband dynamics predict depolarization effects for higher field strengths. For harmonics above the band gap, interband dynamics become important and the high-harmonic response to elliptical excitation looks systematically different. Our work proposes a method to distinguish between different high-harmonic generation mechanisms and it could pave the way to compact solid-state high-harmonic sources with controllable polarization states.

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

Cited by 60 publications

References 72 publications

Polarization-state-resolved high-harmonic spectroscopy of solids

Polarization-state-resolved high-harmonic spectroscopy of solids

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

Role of intraband dynamics in the generation of circularly polarized high harmonics from solids

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