Recoil-ion and electron momentum spectroscopy is a rapidly developing technique that allows one to measure the vector momenta of several ions and electrons resulting from atomic or molecular fragmentation. In a unique combination, large solid angles close to 4π and superior momentum resolutions around a few per cent of an atomic unit (a.u.) are typically reached in state-of-the art machines, so-called reaction-microscopes. Evolving from recoil-ion and cold target recoil-ion momentum spectroscopy (COLTRIMS), reaction-microscopes—the `bubble chambers of atomic physics'—mark the decisive step forward to investigate many-particle quantum-dynamics occurring when atomic and molecular systems or even surfaces and solids are exposed to time-dependent external electromagnetic fields. This paper concentrates on just these latest technical developments and on at least four new classes of fragmentation experiments that have emerged within about the last five years. First, multi-dimensional images in momentum space brought unprecedented information on the dynamics of single-photon induced fragmentation of fixed-in-space molecules and on their structure. Second, a break-through in the investigation of high-intensity short-pulse laser induced fragmentation of atoms and molecules has been achieved by using reaction-microscopes. Third, for electron and ion-impact, the investigation of two-electron reactions has matured to a state such that the first fully differential cross sections (FDCSs) are reported. Fourth, comprehensive sets of FDCSs for single ionization of atoms by ion-impact, the most basic atomic fragmentation reaction, brought new insight, a couple of surprises and unexpected challenges to theory at keV to GeV collision energies. In addition, a brief summary on the kinematics is provided at the beginning. Finally, the rich future potential of the method is briefly envisaged.

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Recoil-ion and electron momentum spectroscopy: reaction-microscopes

Atomic Spectra Database

The investigation of high-order harmonic generation (HHG) of femtosecond laser pulses by means of laser-produced plasmas is surveyed. This kind of harmonic generation is an alternative to the HHG in gases and shows significantly higher conversion efficiency. Furthermore, with plasma targets there is no limitation on applicable laser intensity and thus the generated harmonics can be much more intense. In principle, harmonic light may also be generated at relativistic laser intensity, in which case their harmonic intensities may even exceed that of the focused laser pulse by many orders of magnitude. This phenomenon presents new opportunities for applications such as nonlinear optics in the extreme ultraviolet region, photoelectron spectroscopy, and opacity measurements of high-density matter with high temporal and spatial resolution. On the other hand, HHG is strongly influenced by the laser-plasma interaction itself. In particular, recent results show a strong correlation with high-energy electrons generated during the interaction process. The harmonics are a promising tool for obtaining information not only on plasma parameters such as the local electron density, but also on the presence of large electric and magnetic fields, plasma waves, and the (electron) transport inside the target. This paper reviews the theoretical and experimental progress on HHGmore » via laser-plasma interactions and discusses the prospects for applying HHG as a short-wavelength, coherent optical tool.« less

High-order harmonics from laser-irradiated plasma surfaces

The observation of coherent dynamics ensuing from the excitation of molecular systems by femtosecond laser pulses is at the heart of femtochemistry. The time-dependent evolution of coherent superpositions of quantum states, the physical basis for the observation of coherent dynamics and their manipulation are of central importance to coherent control of physicochemical processes. In the early days of femtochemistry, there was significant skepticism regarding the type of information that could be learned from spectroscopic experiments using very short pulses. There were arguments that one could infer the dynamics from frequency-resolved experiments and that the femtosecond experiments did not offer new information. It was also assumed that experiments with very short pulses would smear the available spectroscopic information because of their broad bandwidths. Approximately two decades after the initial experiments, it has become clear that femtosecond experiments have opened an extremely valuable window into the dynamic behavior of atomic and molecular systems that is influencing how we think about physics, chemistry, and biology. In particular, we highlight the fact that some of the highest resolution spectroscopic measurements being carried out employ femtosecond laser pulses. These experiments, specifically those taking advantage of rotational coherence, provide resolution that rivals microwave spectroscopy. The reason spectroscopic information is not lost in femtochemistry experiments is coherence, a property that can be manipulated to control physicochemical processes by a number of different approaches, which will be reviewed here. This review presents a summary of some of the most salient contributions to the field of coherent laser control from an experimentalist’s perspective. While a number of theoretical papers have made key contributions to the field, it is from the experimental successes, as well as failures, that we can best learn how to implement new strategies and develop future applications. Coherent laser control, in the context of this review, encompasses experiments in which the coherent properties of the laser and/or the molecule are required for controlling a particular physicochemical process. We distinguish for each of the experiments between coherence in the laser field(s), * To whom correspondence should be addressed. Phone (517) 3559715 (ext-315). Fax (517) 353-1793. E-mail dantus@msu.edu. 1813 Chem. Rev. 2004, 104, 1813−1859

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Experimental coherent laser control of physicochemical processes.

High-harmonic generation provides an attractive light source of coherent radiation in the extreme-ultraviolet (XUV) and soft-x-ray regions of the spectrum and allows for the production of single attosecond pulses or pulse trains. This Colloquium covers the control of high-harmonic spectra by temporal and spatial pulse shaping of the driving laser pulses and its implications on time-resolved XUV spectroscopy and attosecond pulse shaping. It summarizes important steps for extending existing pulse shaping techniques and control schemes from the near-infrared or visible part to shorter wavelengths. Using adaptive pulse shaping of the driving laser pulses, several groups have demonstrated control of the high-harmonic spectrum, including the author's work on the complete control over the XUV spectrum of high-order harmonics, generated in a gas-filled hollow fiber. It is possible to achieve both the enhancement and the suppression of single or several selected harmonic orders. These arbitrarily shaped soft-x-ray spectra will allow for important modifications of the resulting harmonic pulses in the temporal domain. This constitutes first steps towards direct attosecond pulse shaping in the soft-x-ray domain. Moreover, high-harmonic generation in a hollow-core fiber can be enhanced by coupling into a single fiber mode using a feedback-controlled adaptive two-dimensional spatial light modulator.

Colloquium : Optimal control of high-harmonic generation

Interferences of free electron wave packets generated by a pair of identical, time-delayed, femtosecond laser pulses which ionize excited atomic potassium have been observed. Two different schemes are investigated: threshold electrons produced by one-photon ionization with parallel laser polarization and above threshold ionization electrons produced by a two-photon transition with crossed laser polarization. Our results show that the temporal coherence of light pulses is transferred to free electron wave packets, thus opening the door to a whole variety of exciting experiments.

Interferences of ultrashort free electron wave packets.

This work studied the emission of XUV radiation from water microdroplets under excitation with either a single or a pair of intense femtosecond laser pulses (Ti:Sa, 80 fs, ∼1014 W/cm2 , 800 nm, 1 kHz). When varying the delay between the two pulses a transition from pure incoherent plasma emission to coherent high-harmonic generation was observed. Under optimized conditions high-harmonic radiation up to the 27th order was obtained.

High-harmonic generation and plasma radiation from water microdroplets

High harmonic generation is compared in the dependence on the ellipticity of the fundamental laser radiation for an atomic and a molecular system. In particular argon and nitrogen are compared employing molecular beams and intense ( 3×1014 W/cm2) and ultrashort (80 fs) 800 nm laser pulses. It turns out that for all the harmonics under investigation (H5, H13 and H21) the harmonic yield decreases slower with the ellipticity for the molecule than for the atom. This indicates differences in atomic and molecular high harmonic generation.

Ellipticity dependence of atomic and molecular high harmonic generation

High harmonic generation at 1 kHz repetition rate is reported. A piezoelectric pulsed valve together with a femtosecond Ti:Sapphire laser both operating at 1 kHz are employed to generate high harmonic radiation in xenon and argon. The characteristics of the valve have been analyzed by using a fast ion gauge and a time-of-flight mass-spectrometer.

High harmonic generation at 1 kHz repetition rate with a pulsed valve

We compare high-harmonic generation (HHG) for an atomic and a diatomic molecular system This is done by studying the cllipticity dependence for the generation process in the two representative gases Ar and N2 as they have almost identical ionization potential and average static polarizabilities The experiment was carried out by changing the initial polarization state of an 800 nm, 80 fs laser pulse, which was focused to an intensity of 3 × 1014 W cm−2 We report an overall weaker dependence on ellipticity for the molecular system In addition, a simulation based on the three-step model is presented, which is then used to discuss the experimental results We point out that to explain molecular HHG fully, a theory which goes beyond the three-step model has to be established

A. Flettner

Papers

Interferences of ultrashort free electron wave packets.

High-harmonic generation and plasma radiation from water microdroplets

Ellipticity dependence of atomic and molecular high harmonic generation

High harmonic generation at 1 kHz repetition rate with a pulsed valve

Atomic and molecular high-harmonic generation: a comparison of ellipticity dependence based on the three-step model