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2 Ultrafast and Nonlinear Phenomena:
   Atoms, Molecules, Clusters, and Plasma
Group coordinator: U. Eichmann
Overview

This research focus is devoted to ultrafast and nonlinear processes in atoms, molecules, clusters and plasmas induced by short laser pulses. It covers a broad range of intensities from ultra-strong fields where the external field is the dominant interaction down to light-matter interaction at perturbative field strengths.

Few-particle interactions are typically investigated with novel spectroscopic methods yielding comprehensive kinematical information, and allowing for detailed comparison with elaborate theories. The detailed understanding of few-particle and plasma dynamics in ultrafast and strong laser pulses has proven to be one of the keys to novel applications in nonlinear optics.

Fundamental processes in strong fields presently focus on multi-electron dynamics and correlations in atoms, molecules and clusters, including multiple ionisation, harmonic generation and strong field reaction control. Processes in ultra-strong fields focus on relativistic effects in multi-electron ionisation of atoms and ions, and on relativistic plasma dynamics including the generation and application of laser accelerated protons (proton imaging) and coherent EUV radiation (“X-ray lasers (XRL)”)

Studies of ultrafast processes and structural changes are concerned with the investigation of nuclear and electronic dynamics, as well as ultrafast chemical reactions. The work focuses on molecular clusters and biologically relevant molecules in the gas phase, molecular liquids and polyatomic molecules in the condensed phase using novel methods of multidimensional spectroscopy.

Present activities are grouped in four projects, focusing on the dynamics of fully ionised matter (plasmas), on the transitions between neutral and ionised matter, and on the light-induced dynamics of molecular motion and fragmentation.

Fully ionised matter

Investigations involve both the internal dynamics of plasmas created by relativistic laser intensities, and the creation and control of secondary radiation, specifically protons and EUV-radiation. After implementation of the unique possibility to synchronize two separate high-power lasers the medium term research strategy involves shaping the energy spectrum of accelerated protons while simultaneously searching for methods to reduce the energy required for a repetitive production of MeV ion beams. Optimisation of proton emittance and energy will be studied through variation of laser pulse parameters, using micro-structured, multi-layered or spherical targets. Once the proton imaging technique is established it will be used to study field structures in relativistic plasmas, such as the predicted mechanisms of electron flow, soliton structures, laser filamentation and strong magnetic fields. Main activities in 2-01, close collaboration with 2-02, 1-02 and 4-2. The sub-project “table-top X-ray laser” focuses on the optimisation of coherent EUV-emission from laser-created plasmas. The next steps towards the long-term vision (stable saturated lasing around 13 nm with microjoule pulse energies, high beam brilliance and high repetition rate between 10 Hz and 1 kHz) involve the investigation of seeded amplification, using seed pulses generated by high harmonics (HHG), in a saturated 10 Hz operation pumped by shaped pulses from the MBI Ti:sapphire laser. After that, the step towards higher repetition rates will depend on research towards novel pump lasers, providing shaped ps pulses with energies on the order of Joule and repetition rates up to 1 kHz. Applications for interferometric studies (including plasma diagnostics) are foreseen as well as in diagnostics and component characterization in the industrially relevant spectral region around 13 nm. Main activities in 2-01, close collaboration with 3-04.

Strong field ionisation dynamics

The general goal is to understand the interplay between electron-electron correlation and dynamics in ultra-strong fields. The prevailing experimental method is detailed fragment spectroscopy, co-pioneered by MBI research groups, which will in the mid-term future be applied to new targets and in new intensity regimes in order to explore the limits of existing theoretical models. Specifically, this includes the study of the influence of molecular structure on the multi-electron dynamics, the yet unexplored transition regime between multi-photon and single photon double ionisation, the electron dynamics on the single- and sub-single-optical cycle time scale as well as multiple ionisation of atoms and ions at relativistic light intensities. Tools to realise these objectives will be few-cycle pulses with stabilized and adjustable carrier-envelope phase, ultra-short high-order harmonic light pulses, relativistic laser intensities, and ionic trapped targets. Medium term applications will include the absolute in-situ determination of ultra-high laser intensities through relativistic field ionisation of atoms and ions (“atomic intensity probe”), trying to solve a long-lasting problem in ultra-high intensity laser research. The experimental work will be accompanied and augmented by in-house theory. Main activity in 2-02, close collaboration with 1-02 , 2-03 and 4-1

Large finite systems

For atomic and molecular clusters and extended organic molecules both strong and weak laser pulses are exploited. Excitation, (multiple) ionisation, fragmentation and reaction dynamics are studied in an intensity regime up to 10 16 W/cm2, corresponding to electric field strengths which are very strong from the perspective of controlling and manipulating intra- and intermolecular potentials and reaction pathways. Model systems are C60, (H2O)n and (NH3)n but also biochromophores, aminoacids and peptides for which recent studies indicate substantial analytic potential in multi-dimensional (laser field controlled) mass spectroscopy. Key tools are temporally (and possibly polarisation) shaped, broad band laser pulses with optimal control feedback loops, dynamic imaging in combination with photoelectron – photo-ion coincidence techniques as well as multi colour time resolved pump-probe spectroscopy. Complementary studies on doped helium droplets allow to investigate laser induced photochemistry in an ultracold and superfluid environment and thus offer additional degrees of freedom for specific control schemes. Main activity in 2-03, close collaboration with 1-01 and 2-02. At low laser pulse intensities, photochemical elementary reactions in biologically relevant systems are studied, such as hydrogen or electron transfer or internal conversion by time-resolved mass- , electron- and coincidence spectroscopy. A detailed understanding of reaction pathways in isolated biomolecules is obtained by close collaborations with theoretical groups. Micro-solvated clusters mimic solvation and environmental effects and connect our detailed understanding of isolated molecules with the complex structures relevant to biology. Increasingly complex molecules and aggregates will provide a bottom-up description of photo-chemical processes in biological systems. A pioneering combination of hole-burning methods, impulsive alignment and pump-probe spectroscopy will allow a structure–selective characterization of excited state dynamics in isolated clusters. Main activities in 2-03, close collaboration with 2-02 and 2-04.

Vibrational and reaction dynamics in the condensed phase: General goal is the real-time elucidation of ultrafast structural and relaxation (energy flow) dynamics of molecular and biomolecular systems, either for equilibrium-state structures subject to fluctuating surroundings (such as solvent shells or protein backbones), or structural changes induced by optically triggered chemical reactions. The methodology encompasses the advancement of nonlinear ultrafast spectroscopy, ranging from (multidimensional) photon echo techniques to pump-probe methods and time-resolved emission studies. In the future, the quantitative measurements of microscopic molecular couplings in liquids and polyatomic molecules determining structural and relaxation dynamics will be a major topic, both for electronic ground and excited states. Here, multidimensional spectroscopy as well as IR-pump IR/Raman-probe measurements will play a key role. In addition, complementary studies of vibrational spectroscopy and X-ray techniques to resolve transient molecular structures will be of interest. In addition to liquids and polyatomic molecules, ultrafast dynamics of biological systems such as proteins in their natural condensed phase environment constitute a major research topic. Main activities in 2-04, close collaboration with 2.03.