Impulsive control of the atomic dipole response in the time and frequency domain

The dipole response of an excited quantum system gives direct insight into the electron dynamics triggered by the incoming light. Spectroscopy techniques such as (attosecond) transient absorption spectroscopy make use of the fact that the dipole response leaves its characteristic fingerprint on the transmitted light. In this work, a general and comprehensive model is introduced, which allows for an analytic description of dipole dynamics triggered and modified by two ultrashort light pulses in both time and frequency domains. Based on this description, a two-dimensional spectral representation of time delay–resolved absorption data is developed. The power of the method to separate different pathways of light–matter interaction, which allows for their individual investigation, is demonstrated experimentally by studying electronic wave packet dynamics in doubly excited helium and inner-valence excited xenon. Furthermore, an in situ technique for characterization of the intense dressing laser pulse that drives (nonlinear) quantum dynamics in time-resolved absorption experiments is derived from the same analytic model and demonstrated experimentally. The possibility to characterize these ultrashort strong-field laser pulses directly within the spectroscopy target enhances the scope of transient absorption spectroscopy as it allows for the precise measurement and control of electron dynamics and increases the comparability between experiment and theory

Reconstruction and control of a time-dependent two-electron wave packet

The concerted motion of two or more bound electrons governs atomic1 and molecular2,3 non-equilibrium processes including chemical reactions, and hence there is much interest in developing a detailed understanding of such electron dynamics in the quantum regime. However, there is no exact solution for the quantumthree-body problem, and as a result even the minimal system of two active electrons and a nucleus is analytically intractable4. This makes experimental measurements of the dynamics of two bound and correlated electrons, as found in the helium atom, an attractive prospect.However, although the motion of single active electrons and holes has been observed with attosecond time resolution5-7, comparable experiments on two-electron motion have so far remained out of reach. Here we showthat a correlated two-electron wave packet can be reconstructed froma 1.2-femtosecondquantumbeatamong low-lying doubly excited states in helium.The beat appears in attosecond transient-absorption spectra5,7-9 measured with unprecedentedly high spectral resolution and in the presence of an intensity-tunable visible laser field.Wetune the coupling10-12 between the two low-lying quantum states by adjusting the visible laser intensity, and use the Fano resonance as a phase-sensitive quantum interferometer13 to achieve coherent control of the two correlated electrons. Given the excellent agreement with large-scalequantum-mechanical calculations for thehelium atom, we anticipate thatmultidimensional spectroscopy experiments of the type we report here will provide benchmark data for testing fundamental few-body quantumdynamics theory in more complex systems. Theymight also provide a route to the site-specificmeasurement and control of metastable electronic transition states that are at the heart of fundamental chemical reactionsWe thank E. Lindroth for calculating the dipole moment (2p2|r|sp2,3+), and also A. Voitkiv, Z.-H. Loh, and R. Moshammer for helpful discussions. We acknowledge financial support by the Max-Planck Research Group Program of the Max-Planck Gesellschaft (MPG) and the European COST Action CM1204 XLIC. L. A. and F. M. acknowledge computer time from the CCC-UAM and Mare Nostrum supercomputer centers and financial support by the European Research Council under the ERC Advanced Grant no. 290853 XCHEM, the Ministerio de Economía y Competitividad projects FIS2010-15127, FIS2013-42002-R and ERA-Chemistry PIM2010EEC-00751, and the European grant MC-ITN CORIN

Imaging detection and classification of particulate contamination on structured surfaces

We present new imaging techniques for the detection and classification of particulate contamination on structured surfaces. This allows for cleanliness inspection directly on the sample. Classical imaging techniques for particle detection, such as dark-field imaging, are typically limited to flat surfaces because structures, scratches, or rough surfaces will give similar signals as particles. This problem is overcome using stimulated differential imaging. Stimulation of the sample, e.g. by air blasts, results in displacement of only the particles while sample structures remain in place. Thus, the difference of images before and after stimulation reveals the particles with high contrast. Cleanliness inspection systems also need to distinguish (often harmful) metallic particles from (often harmless) nonmetallic particles. A recognized classification method is measuring gloss. When illuminated with directed light, the glossy surface of metallic particles directly reflects most parts of the light. Non-metallic particles, in contrast, typically scatter most of the light uniformly. Here, we demonstrate a new imaging technique to measure gloss. For this purpose, several images of the sample with different angles of illumination are taken and analyzed for similarity

Probing ultrafast coherent dynamics in core-excited xenon by using attosecond XUV-NIR transient absorption spectroscopy

We investigate the capability of attosecond transient absorption spectroscopy to characterize the dynamics of inner-shell-excited systems. In the transient absorption spectroscopy setup considered, wave packets are prepared by an attosecond XUV pulse and probed by a femtosecond NIR pulse. By using this, we study coherent electron dynamics in core-excited xenon atoms. In particular, we clarify which aspects of the dynamics can be revealed when the wave packets are probed using an NIR pulse and analyze why the inner-shell hole dynamics is more difficult to probe than the dynamics of the excited electron. We perform a theoretical analysis of the transient absorption signal as a function of the time delay between the XUV pump and NIR probe pulses, treating the excitation pulse perturbatively and the probe pulse nonperturbatively. We also demonstrate that an additional NIR dressing field can dramatically influence the transient absorption spectrum. Our theoretical predictions are compared with experimental results, suggesting that a precise characterization of the NIR pulse is necessary for a qualitative and quantitative comparison

Watching the emergence of a Fano resonance in doubly excited helium

We report on the experimental observation of the buildup of the 2s2p Fano resonance in helium in the time domain, which has been under theoretical investigation for more than a decade. The emergence of the absorption line is temporally resolved by interrupting the natural decay of the excited state via saturated strong-field ionization at a variable time delay. We compare the experimental data with full ab-initio simulations to validate the time-gating by strong-field ionization and thereby confirm the recently developed theory for the formation of Fano line-profiles

Watching the emergence of a Fano resonance in doubly excited helium

We report on the experimental observation of the buildup of the 2s2p Fano resonance in helium in the time domain, which has been under theoretical investigation for more than a decade. The emergence of the absorption line is temporally resolved by interrupting the natural decay of the excited state via saturated strong-field ionization at a variable time delay. We compare the experimental data with full ab-initio simulations to validate the time-gating by strong-field ionization and thereby confirm the recently developed theory for the formation of Fano line-profiles