Abstract

Nonlinear light–matter interactions in the extreme ultraviolet (XUV) are a prerequisite to perform XUV-pump/XUV-probe spectroscopy of core electrons. Such interactions are now routinely investigated at free-electron laser (FEL) facilities. Yet, electron dynamics are often too fast to be captured with the femtosecond resolution of state-of-the-art FELs. Attosecond pulses from laser-driven XUV-sources offer the necessary temporal resolution. However, intense attosecond pulses supporting nonlinear processes have only been available for photon energy below 50 eV, precluding XUV-pump/XUV-probe investigation of typical inner-shell processes. Here, we surpass this limitation by demonstrating two-photon absorption from inner electronic shells of xenon at photon energies around 93 eV and 115 eV. This advance opens the door for attosecond real-time observation of nonlinear electron dynamics deep inside atoms.

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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2017 (6)

S. Huang, Y. Ding, Y. Feng, E. Hemsing, Z. Huang, J. Krzywinksi, A. A. Lutman, A. Marinelli, T. J. Maxwell, and D. Zhu, “Generating single-spike hard x-ray pulses with nonlinear bunch compression in free-electron lasers,” Phys. Rev. Lett. 119, 154801 (2017).
[Crossref]

T. R. Barillot, P. Matia-Hernando, D. Greening, D. J. Walke, T. Witting, L. J. Frasinkski, J. P. Marangos, and J. W. G. Tisch, “Towards XUV pump-probe experiments in the femtosecond to sub-femtosecond regime: new measurement of the helium two-photon ionization cross-section,” Chem. Phys. Lett. 683, 38–42 (2017).
[Crossref]

S. Chatziathanasiou, S. Kahaly, E. Skantzakis, G. Sansone, R. Lopez-Martens, S. Haessler, K. Varju, G. D. Tsakiris, D. Charalambidis, and P. Tzallas, “Generation of attosecond light pulses from gas and solid state media,” Photonics 4, 26 (2017).
[Crossref]

D. E. Rivas, A. Borot, D. E. Cardenas, G. Marcus, X. Gu, D. Herrmann, J. Xu, J. Tan, D. Kormin, G. Ma, W. Dallari, G. D. Tsakiris, I. B. Földes, S.-W. Chou, M. Weidman, B. Bergues, T. Wittmann, H. Schröder, P. Tzallas, D. Charalambidis, O. Razskazovskaya, V. Pervak, F. Krausz, and L. Veisz, “Next generation driver for attosecond and laser-plasma physics,” Sci. Rep. 7, 5224 (2017).
[Crossref]

A. Karamatskou, “Nonlinear effects in photoionization over a broad photon-energy range within the TDCIS scheme,” J. Phys. B 50, 013002 (2017).
[Crossref]

S. Kühn, M. Dumergue, S. Kahaly, S. Mondal, M. Füle, T. Csizmadia, B. Farkas, B. Major, Z. Várallyay, E. Cormier, M. Kalashnikov, F. Calegari, M. Devetta, F. Frassetto, E. Månsson, L. Poletto, S. Stagira, C. Vozzi, M. Nisoli, P. Rudawski, S. Maclot, F. Campi, H. Wikmark, C. L. Arnold, C. M. Heyl, P. Johnsson, A. L’Huillier, R. Lopez-Martens, S. Haessler, M. Bocoum, F. Boehle, A. Vernier, G. Iaquaniello, E. Skantzakis, N. Papadakis, C. Kalpouzos, P. Tzallas, F. Lépine, D. Charalambidis, K. Varjú, K. Osvay, and G. Sansone, “The ELI-ALPS facility: the next generation of attosecond sources,” J. Phys. B 50, 132002 (2017).
[Crossref]

2016 (5)

N. Tsatrafyllis, B. Bergues, H. Schröder, L. Veisz, E. Skantzakis, D. Gray, B. Bodi, S. Kuhn, G. D. Tsakiris, D. Charalambidis, and P. Tzallas, “The ion microscope as a tool for quantitative measurements in the extreme ultraviolet,” Sci. Rep. 6, 21556 (2016).
[Crossref]

C. M. Heyl, H. Coudert-Alteirac, M. Miranda, M. Louisy, K. Kovacs, V. Tosa, E. Balogh, K. Varjú, A. L’Huillier, A. Couairon, and C. L. Arnold, “Scale-invariant nonlinear optics in gases,” Optica 3, 75–81 (2016).
[Crossref]

M. Ossiander, F. Siegrist, V. Shirvanyan, R. Pazourek, A. Sommer, T. Latka, A. Guggenmos, S. Nagele, J. Feist, J. Burgerdörfer, R. Kienberger, and M. Schultze, “Attosecond correlation dynamics,” Nat. Phys. 13, 280–285 (2016).
[Crossref]

Y. Nabekawa, Y. Furukawa, T. Okino, A. A. Eilanlou, E. J. Takahashi, K. Yamanouchi, and K. Midorikawa, “Sub-10-fs control of dissociation pathways in the hydrogen molecular ion with a few-pulse attosecond pulse train,” Nat. Commun. 7, 12835 (2016).
[Crossref]

B. Manschwetus, L. Rading, F. Campi, S. Maclot, H. Coudert-Alteirac, J. Lahl, H. Wikmark, P. Rudawski, C. M. Heyl, B. Farkas, T. Mohamed, A. L’Huillier, and P. Johnsson, “Two-photon double ionization of neon using an intense attosecond pulse train,” Phys. Rev. A 93, 061402 (2016).
[Crossref]

2015 (2)

Y.-J. Chen, S. Pabst, A. Karamatskou, and R. Santra, “Theoretical characterization of the collective resonance states underlying the xenon giant dipole resonance,” Phys. Rev. A 91, 032503 (2015).
[Crossref]

T. Mazza, A. Karamatskou, M. Ilchen, S. Bakhtiarzadeh, A. J. Rafipoor, P. O’Keeffe, T. J. Kelly, N. Walsh, T. Costello, M. Meyer, and R. Santra, “Sensitivity of nonlinear photoionization to resonance substructure in collective excitation,” Nat. Commun. 6, 6799 (2015).
[Crossref]

2014 (2)

W. Helml, A. R. Maier, W. Schweinberger, I. Grguras, P. Radcliffe, G. Doumy, C. Roedig, J. Gagnon, M. Messerschmidt, S. Schorb, C. Bostedt, F. Grüner, L. F. DiMauro, D. Cubaynes, J. D. Bozek, T. Tschentscher, J. T. Costello, M. Meyer, R. Coffee, S. Düsterer, A. L. Cavalieri, and R. Kienberger, “Measuring the temporal structure of few-femtosecond free-electron laser x-ray pulses directly in the time domain,” Nat. Photonics 8, 950–957 (2014).
[Crossref]

G. Kolliopoulos, B. Bergues, H. Schröder, P. A. Carpeggiani, L. Veisz, G. D. Tsakiris, D. Charalambidis, and P. Tzallas, “Revealing quantum path details in high-field physics,” Phys. Rev. A 90, 013822 (2014).
[Crossref]

2013 (3)

R. Guichard, M. Richter, J.-M. Rost, U. Saalmann, A. A. Sorokin, and K. Tiedtke, “Multiple ionization of neon by soft x-rays at ultrahigh intensity,” J. Phys. B 46, 164025 (2013).
[Crossref]

A. Guggenmos, R. Rauhut, M. Hofstetter, S. Hertrich, B. Nickel, J. Schmidt, E. M. Gullikson, M. Seibald, W. Schnick, and U. Kleineberg, “Aperiodic CrSc multilayer mirrors for attosecond water window pulses,” Opt. Express 21, 21728–21740 (2013).
[Crossref]

P. Rudawski, C. M. Heyl, F. Brizuela, J. Schwenke, A. Persson, E. Mansten, R. Rakowski, L. Rading, F. Campi, B. Kim, P. Johnsson, and A. L’Huillier, “A high-flux high-order harmonic source,” Rev. Sci. Instrum. 84, 073103 (2013).
[Crossref]

2012 (1)

J. Ullrich, A. Rudenko, and R. Moshammer, “Free-electron lasers: new avenues in molecular physics and photochemistry,” Annu. Rev. Phys. Chem. 63, 635–660 (2012).
[Crossref]

2011 (4)

G. Sansone, L. Poletto, and M. Nisoli, “High-energy attosecond light sources,” Nat. Photonics 5, 655–663 (2011).
[Crossref]

P. Lambropoulos, K. G. Papamihail, and P. Decleva, “Theory of multiple ionization of xenon under strong XUV radiation and the role of the giant resonance,” J. Phys. B 44, 175402 (2011).
[Crossref]

P. Tzallas, E. Skantzakis, L. A. A. Nikolopoulos, G. D. Tsakiris, and D. Charalambidis, “Extreme-ultraviolet pump-probe studies of one femtosecond scale electron dynamics,” Nat. Phys. 7, 781–784 (2011).
[Crossref]

M. Schultze, B. Bergues, H. Schröder, F. Krausz, and K. L. Kompa, “Spatially resolved measurement of ionization yields in the focus of an intense laser pulse,” New J. Phys. 13, 033001 (2011).
[Crossref]

2010 (3)

F. Ferrari, F. Calegari, M. Lucchini, C. Vozzi, S. Stagira, G. Sansone, and M. Nisoli, “High-energy isolated attosecond pulses generated by above-saturation few-cycle fields,” Nat. Photonics 4, 875–879 (2010).
[Crossref]

V. Richardson, J. T. Costello, D. Cubaynes, S. Düsterer, J. Feldhaus, H. W. van der Hart, P. Juranic, W. B. Li, M. Meyer, M. Richter, A. A. Sorokin, and K. Tiedke, “Two-photon inner-shell ionization in the extreme ultraviolet,” Phys. Rev. Lett. 105, 013001 (2010).
[Crossref]

L.-W. Pi and A. F. Starace, “Potential barrier effects in two-photon ionization processes,” Phys. Rev. A 82, 053414 (2010).
[Crossref]

2009 (2)

M. G. Makris, P. Lambropoulos, and A. Mihelic, “Theory of multiphoton multielectron ionization of xenon under strong 93-eV radiation,” Phys. Rev. Lett. 102, 033002 (2009).
[Crossref]

Y. Nomura, R. Hörlein, P. Tzallas, B. Dromey, S. Rykovanov, Z. Major, J. Osterhoff, S. Karsch, L. Veisz, M. Zepf, D. Charalambidis, F. Krausz, and G. D. Tsakiris, “Attosecond phase locking of harmonics emitted from laser-produced plasmas,” Nat. Phys. 5, 124–128 (2009).
[Crossref]

2008 (2)

C. Sternemann, H. Sternemann, S. Huotari, F. Lehmkühler, M. Tolan, and J. S. Tse, “The barium giant dipole resonance in barite: a study of soft x-ray absorption edges using hard x-rays,” J. Anal. At. Spectrom. 23, 807–881 (2008).
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D. E. Rivas, A. Borot, D. E. Cardenas, G. Marcus, X. Gu, D. Herrmann, J. Xu, J. Tan, D. Kormin, G. Ma, W. Dallari, G. D. Tsakiris, I. B. Földes, S.-W. Chou, M. Weidman, B. Bergues, T. Wittmann, H. Schröder, P. Tzallas, D. Charalambidis, O. Razskazovskaya, V. Pervak, F. Krausz, and L. Veisz, “Next generation driver for attosecond and laser-plasma physics,” Sci. Rep. 7, 5224 (2017).
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K. C. Kulander, K. J. Schafer, and J. K. Krause, “Ionization and harmonic conversion,” in Super Intense Laser Atom Physics (Springer, 1993).

Supplementary Material (1)

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Figures (3)

Fig. 1.
Fig. 1. Experimental setup. The LWS-20 laser system that drives the HHG delivers sub-two-cycle laser pulses with a central wavelength around 740 nm at a repetition rate of 10 Hz. The pulses propagate in a 35-m-long evacuated beamline where they are focused into the generation chamber to a focal spot of 365 μm FWHM using an f=17  m spherical mirror. The XUV pulses are generated in a gas cell filled with a few mbar of neon. Optimum XUV pulses are typically generated with 35 mJ to 40 mJ laser pulse energy on target, providing a peak intensity of 13×1015  W/cm2. After HHG, the XUV and laser pulses propagate collinearly to the entrance of the experimental chamber. There, one or two 150-nm-thick Zr filters can be inserted into the beam to block photons with an energy below 65 eV, including the driving laser radiation. A multilayer XUV mirror is used to focus the beam on axis onto a xenon gas jet located in the object plane of an ion microscope. The latter records the spatial distribution of ions produced in the XUV focus via photoionization of the target gas. The chamber is equipped with different single-shot XUV diagnostic devices (an XUV CCD camera, an XUV flat-field grating spectrometer, and an absolutely calibrated XUV photodiode), which are used to characterize the generated radiation. (b) 100-shot average of the spectral energy density S(Eph) as a function of the photon energy Eph after generation (light grey area), and after a 150-nm-thick Zr filter (dark grey area). The normalized XUV spectrum on target after reflection from the 93-eV (115-eV) XUV focusing mirror is indicated by the blue (red) area. For visual convenience, the maximum of the blue and red spectra have been normalized to the value 0.1. (c) XUV beam profile measured at the XUV mirror position and averaged over 100 shots.
Fig. 2.
Fig. 2. TOF spectra of Xe at 93 eV. Measured mass spectra of the xenon charge states Xeq+ (q=1,,5) generated by photoionization of xenon atoms in the focus of the 93-eV XUV beam. The signal corresponds to the number of ions per unit mass-to-charge ratio m detected in a field of view of 395 μm in diameter. The number Nionq+ in the right upper corner of each graph corresponds to the number of ions Xeq+ generated per shot in the field of view of the IM, taking into account the 50% detection efficiency. The blue markers indicate the expected positions and frequencies of the seven stable xenon isotopes. The relative photoionization yields of all the measured charge states are shown in the lower right panel.
Fig. 3.
Fig. 3. Spatial dependence of the linear and nonlinear photoionization yields along the propagation axis z at a photon energy of (a) 93 eV and (b) 115 eV. Each of the images shown in the upper two panels in (a) and (b) correspond to an ion microscope image of the charge state indicated in the upper right corner. The maximum signal in each image is normalized to 1. The yield ratios R(z)=YXe4+(z)/YXe2+(z) and R(z)=YXe4+(z)/YXe3+(z) are shown in the lower panel of (a) and (b), respectively, where YXe2+(z), YXe3+(z) and YXe4+(z) are obtained by integrating the corresponding images along x (grey data points). The black line is obtained from the grey data points by a 65-point smoothing. The red line, from which we obtain the Rayleigh range zR, is a fit of the function k×(1+z2/zR2)1 to the data with fit parameters k and zR.

Tables (1)

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Table 1. Measured Xe4+ Two-Photon Ionization Cross Sections at 93 eV and 115 eV Determined Using Eqs. (1) and (2)a

Equations (2)

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σ˜(2)=λπ×M2Nph2×Ntot(2)ρa,
σ˜(2)=πσ2ln(2)×d02×R(0)Nph.

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