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

Deconvolution of complex G protein–coupled receptor signaling in live cells using dynamic mass redistribution measurements

Label-free biosensor technology based on dynamic mass redistribution (DMR) of cellular constituents promises to translate GPCR signaling into complex optical 'fingerprints' in real time in living cells. Here we present a strategy to map cellular mechanisms that define label-free responses, and we compare DMR technology with traditional second-messenger assays that are currently the state of the art in GPCR drug discovery. The holistic nature of DMR measurements enabled us to (i) probe GPCR functionality along all four G-protein signaling pathways, something presently beyond reach of most other assay platforms; (ii) dissect complex GPCR signaling patterns even in primary human cells with unprecedented accuracy; (iii) define heterotrimeric G proteins as triggers for the complex optical fingerprints; and (iv) disclose previously undetected features of GPCR behavior. Our results suggest that DMR technology will have a substantial impact on systems biology and systems pharmacology as well as for the discovery of drugs with novel mechanisms

Oscillator-based High-order Harmonic Generation at 4MHz for Applications in Time-of-Flight Photoemission Spectroscopy

We generate high-order harmonics at 4MHz by a long-cavity laser and demonstrate applications in time-of-flight photoemission spectroscopy. Our results suggest a straightforward, oscillator-only setup for HHG-based photoelectron spectroscopy and microscopy with high repetition rate

Strong-field-gated buildup of a Rydberg series

The femtosecond-timescale formation of a Fano resonance in doubly excited helium has been recently observed, enabling a time-domain view into two-electron correlation dynamics. Measuring the absorption spectral line shape, the buildup of the resonance is revealed by imposing a temporal gate on the dipole response using strong-field ionization. Here, we apply this approach to the Rydberg series of the doubly excited states in helium. This reveals the characteristic times of emergence of isolated two-electron resonances from the continuous single-ionization background absorption, as well as their time-dependent line-shape asymmetry and the time it takes to separate individual spectral absorption lines within the series. Furthermore, we time resolve the dynamics of the excited wave packet by reconstructing its dipole response in the time domain and thereby characterize the ionization gate to close as fast as only 1.2 fs. These results represent an approach to resolve on the femtosecond and attosecond timescale the strong-field-ionization dynamics of excited coherent wave packets

Extracting Phase and Amplitude Modifications of Laser-Coupled Fano Resonances

Fano line shapes observed in absorption spectra encode information on the amplitude and phase of the optical dipole response. A change in the Fano line shape, e.g., by interaction with short-pulsed laser fields, allows us to extract dynamical modifications of the amplitude and phase of the coupled excited quantum states. We introduce and apply this physical mechanism to near-resonantly coupled doubly excited states in helium. This general approach provides a physical understanding of the laser-induced spectral shift of absorption-line maxima on a sub-laser-cycle time scale as they are ubiquitously observed in attosecond transient-absorption measurements

XUV-beamline for attosecond transient absorption measurements featuring a broadband common beam-path time-delay unit and in situ reference spectrometer for high stability and sensitivity

Measuring bound-state quantum dynamics, excited and driven by strong fields, is achievable by time-resolved absorption spectroscopy. Here, a vacuum beamline for spectroscopy in the attosecond temporal and extreme ultraviolet (XUV) spectral range is presented, which is a tool for observing and controlling nonequilibrium electron dynamics. In particular, we introduce a technique to record an XUV absorption signal and the corresponding reference simultaneously, which greatly improves the signal quality. The apparatus is based on a common beam path design for XUV and near-infrared (NIR) laser light in a vacuum. This ensures minimal spatiotemporal fluctuations between the strong NIR laser and the XUV excitation and reference beams, while the grazing incidence optics enable broadband spectral coverage. The apparatus combines high spectral and temporal resolution together with an increase in sensitivity to weak absorption signatures by an order of magnitude. This opens up new possibilities for studying strong-field-driven electron dynamics in bound systems on their natural attosecond time scale

Attosecond transient absorption of a continuum threshold

The laser-field-modified dipole response of the first ionization threshold of helium is studied by means of attosecond transient absorption spectroscopy. We resolve light-induced time-dependent structures in the photoabsorption spectrum both below and above the ionization threshold. By comparing the measured results to a quantum-dynamical model, we isolate the contributions of the unbound electron to these structures. They originate from light-induced couplings of near-threshold bound and continuum states and light-induced energy shifts of the free electron. The ponderomotive energy, at low laser intensities, is identified as a good approximation for the perturbed continuum response