New Method for Measuring Angle-Resolved Phases in Photoemission

You, Daehyun; Ueda, Kiyoshi; Грызлова, Е. В.; Grum–Grzhimailo, A. N.; Popova, Maria M.; Staroselskaya, Ekaterina I.; Tugs, Oyunbileg; Orimo, Yuki; Sato, Takeshi; Ishikawa, Kenichi L.; Carpeggiani, Paolo; Csizmadia, Tamás; Füle, Miklós; Sansone, G.; Maroju, Praveen Kumar; D׳Elia, A.; Mazza, Tommaso; Meyer, Michael; Callegari, Carlo; Fraia, Michele Di; Plekan, Oksana; Richter, Robert; Giannessi, L.; Allaria, E.; Ninno, G. De; Trovò, M.; Badano, L.; Diviacco, B.; Gaio, G.; Gauthier, David; Mirian, Najmeh; Penco, G.; Ribič, Primož Rebernik; Spampinati, S.; Spezzani, C.

doi:10.1103/physrevx.10.031070

Cited by 39 publications

(41 citation statements)

References 57 publications

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“…For atomic targets, one-photon ionization delays could be retrieved from the time-dependence of the oscillatory two-photon ionization signal demonstrating, e.g., relative photoionization time delays of few tens of attoseconds between electron ejection from n s and n p electronic orbitals in Ne and Ar 7 , 8 or addressing the characterization of autoionizing Fano resonances in the ionization continuum 9 – 11 . More insight into such ionization dynamics described by two-photon transition matrix elements was then demonstrated in angular resolved studies in the laboratory frame 12 – 18 .…”

Section: Introductionmentioning

confidence: 97%

Influence of shape resonances on the angular dependence of molecular photoionization delays

et al. 2021

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Characterizing time delays in molecular photoionization as a function of the ejected electron emission direction relative to the orientation of the molecule and the light polarization axis provides unprecedented insights into the attosecond dynamics induced by extreme ultraviolet or X-ray one-photon absorption, including the role of electronic correlation and continuum resonant states. Here, we report completely resolved experimental and computational angular dependence of single-photon ionization delays in NO molecules across a shape resonance, relying on synchrotron radiation and time-independent ab initio calculations. The angle-dependent time delay variations of few hundreds of attoseconds, resulting from the interference of the resonant and non-resonant contributions to the dynamics of the ejected electron, are well described using a multichannel Fano model where the time delay of the resonant component is angle-independent. Comparing these results with the same resonance computed in e-NO+ scattering highlights the connection of photoionization delays with Wigner scattering time delays.

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Section: Introductionmentioning

confidence: 97%

Influence of shape resonances on the angular dependence of molecular photoionization delays

et al. 2021

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“…Changing the relative phase and the strength of harmonics provides a way to control the PADs as it was realized in the ω + 2ω process 30 years ago in the optical domain [16][17][18]. Recently, with the advent of longitudinally coherent free-electron lasers, experimental studies of the coherent control in the ω + 2ω process in the XUV wavelength range became possible and the first such measurements have been done [19][20][21].…”

Section: Introductionmentioning

confidence: 99%

Symmetry Violation in Bichromatic Ionization by a Free-Electron Laser: Photoelectron Angular Distribution and Spin Polarization

et al. 2021

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A fundamental phenomenon of coherent control is investigated theoretically using the example of neon photoionization by the bichromatic field of a free-electron laser. A system exposed to coherent fields with commensurable frequencies loses some symmetry, which manifests itself in the angular distribution and spin polarization of the electron emission. We predict several such effects, for example, the violation of symmetry with respect to the plane perpendicular to the polarization vector of the second harmonic and the appearance of new components of spin polarization. Furthermore, we predict a very efficient control of spin polarization via manipulation of the phase between the harmonics. Experimental observation of these effects is accessible with modern free-electron lasers operating in the extreme ultraviolet wavelength regime.

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“…where the quantization axis is defined by the laser polarization vector, θ and φ are the polar and azimuthal angles of photoelectron emission directionn, Y lm is the spherical harmonics, and β lm are expansion coefficients. Traditional RABBITT measurements 29 using parallel-polarized extreme ultraviolet attosecond pulse trains (XUV-APT) and near infrared (NIR) laser fields report a cylindrically symmetric PAD and a large angle-dependent phase shift, close to π, which is ascribed to the incomplete quantum interference following Fano's propensity rule [29][30][31] . However, as the relative polarization direction between the XUV-APT and NIR is skewed 32,33 , the symmetry is broken.…”

Section: Introductionmentioning

confidence: 99%

Symmetry resolved atomic photoionization phase shift by attosecond coincidence metrology

Jiang

Armstrong

Tong

et al. 2021

Preprint

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Attosecond chronoscopy is central to the understanding of ultrafast electron dynamics from gas to condensed phase with attosecond temporal resolution. It has, however, not yet been able to determine the timing of individual partial waves, and steering their contribution has been a substantial challenge. Here, we develop a polarization-skewed attosecond chronoscopy to reveal their roles from the angle-resolved photoionization phase shifts in rare gas atoms. By scanning the relative polarization angle between an extreme-ultraviolet attosecond pulse train and a phase-locked near-infrared laser field serving as a partial wave meter, we break the cylindrical symmetry and observe an emission direction dependent phase shift in the photoionized electron momenta. The experimental observations are well supported by numerical simulations using the R-matrix with time-dependence method, and by analytical analysis using the soft-photon approximation. Our symmetry-resolved, partial-wave analysis identifies the transition rate and phase shifts of each individual ionization pathway in the attosecond photoelectron emission dynamics. Our findings provide critical insights into the ubiquitous attosecond optical timer and the underlying attosecond photoionization dynamics, thereby offer new perspectives for the control, manipulation, and exploration of ultrafast electron dynamics in complex systems.

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New Method for Measuring Angle-Resolved Phases in Photoemission

Cited by 39 publications

References 57 publications

Influence of shape resonances on the angular dependence of molecular photoionization delays

Influence of shape resonances on the angular dependence of molecular photoionization delays

Symmetry Violation in Bichromatic Ionization by a Free-Electron Laser: Photoelectron Angular Distribution and Spin Polarization

Symmetry resolved atomic photoionization phase shift by attosecond coincidence metrology

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