High-harmonic spectroscopy provides a unique insight into the electronic structure of atoms and molecules 1-5. Although attosecond science holds the promise of accessing the timescale of electron-electron interactions, until now, their signature has not been seen in high-harmonic spectroscopy. We have recorded high-harmonic spectra of atoms to beyond 160 eV, using a new, almost ideal laser source with a wavelength of 1.8 µm and a pulse duration of less than two optical cycles. We show that we can relate these spectra to differential photoionization cross-sections measured with synchrotron sources. In addition, we show that the highharmonic spectra contain features due to collective multielectron effects involving inner-shell electrons, in particular the giant resonance in xenon. We develop a new theoretical model based on the strong-field approximation and show that it is in agreement with the experimental observations. Measuring and understanding the electronic structure and correlated dynamics of matter on its natural timescale represents the main thrust of ultrafast laser science. Electron correlations affect essential properties of complex systems ranging from configuration interactions in molecules to cooperative phenomena in solids, such as superconductivity. Our knowledge of the electronic structure of matter originates from several decades of research on photoionization and photoelectron spectroscopy 6-8 , mainly driven by the development of synchrotron-based sources. Recent advances in strong-field physics have opened an alternative approach to probing both the electronic structure 1,9 and the dynamics 10-12 of molecules using table-top laser sources. These new methods rely on the recollision of an electron, removed from the molecule by a strong laser field, with its parent ion 13 , as illustrated in Fig. 1a. The electronic structure of the molecule is encoded in the emitted high-harmonic spectrum through the amplitude and phase of the photorecombination matrix elements 4,11,14,15. We use high-harmonic spectroscopy to investigate a new class of collective electronic dynamics-induced and probed by the recombining electron. The kinetic energy of the returning electron is usually much larger than the difference between electronic energy levels of the parent ion. Consequently, inelastic scattering followed by recombination is energetically possible, as illustrated in Fig. 1b. Using the xenon atom as an example, we demonstrate that such processes indeed occur and that they can locally enhance the efficiency of high-harmonic generation (HHG) by more than one order of magnitude. We show that such a seemingly complex pathway contributes significantly to the phase-matched process. This observation uncovers a new

Wavelength scaling of high harmonic generation efficiencyUsing longer wavelength laser drivers for high harmonic generation is desirable because the highest extreme ultraviolet frequency scales as the square of the wavelength. Recent numerical studies predict that high harmonic efficiency falls dramatically with increasing wavelength, with a very unfavorable Àð5À6Þ scaling. We performed an experimental study of the high harmonic yield over a wavelength range of 800-1850 nm. A thin gas jet was employed to minimize phase matching effects, and the laser intensity and focal spot size were kept constant as the wavelength was changed. Ion yield was simultaneously measured so that the total number of emitting atoms was known. We found that the scaling at constant laser intensity is À6:3AE1:1 in Xe and À6:5AE1:1 in Kr over the wavelength range of 800-1850 nm, somewhat worse than the theoretical predictions.

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