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Research Area B.1

Schematic top-view of the world’s first UHV attosecond apparatus: the AS-3 beamline at MPQ. The back plate of the preparation chamber is rotatable so that the manipulator with the sample can be moved to different ports for target preparation and characterisation before the sample is inserted into the measurement chamber.

Electronic structure & dynamics

The dynamics of atomic, molecular, solid-state and biological systems are driven by elementary electronic processes. Over the last decade tools have been developed to investigate electronic motions on their native scale in the attosecond regime (1 as = 1018 s). They have provided real-time insight into fundamental electronic phenomena such as photoemission, optical-field-induced tunneling, charge transport and valence electron wavepacket dynamics. Several of these breakthroughs have been achieved in the framework of MAP.

Studies of electronic and molecular phenomena with state-of-the-art femto- and attosecond tools and techniques have been focused - both in MAP and elsewhere - mainly on simple systems so far. Meanwhile, the new metrologies are becoming matue enough to be applied to scrutinising increasingly more complex systems, ranging from organic molecules and biological macromolecules to organic-inorganic hybrid systems, functional materials and nano-structures.

We shall capitalise on the synergistic cooperation of theory and experiment and cutting-edge instrumentation, which have been created during the first funding period and will be further advanced along with computational modeling and theoretical description to explore and control electron phenomena in complex molecular systems and sophisticated artificial architectures. With synthesised fields, as-pulses and frequency combs, we shall capture electron correlations, the creation, motion and decay of electonic coherence in multi-electron systems, electronic-vibrational coupling, charge transfer / transport in molecular assemblies and solid-state structures in real time. Attosecond metrology will also provide insight into the fastest processes in condensed-matter systems such as the build-up of electronic band structure and screening effects.

Main objectives for 2012-2017:

a) Development of multi-dimensional frequency-comb spectroscopy for metrology of high-rate ultrashort-pulsed fields and nonlinear molecular frequency-comb spectroscopy

b) Studying strong-field ionisation, electron correlations and valence electron wavepacket formation and subsequent dynamics in multi-electron systems

c) Understanding and controlling of molecular organisation, energy level alignment and charge transfer in organic-inorganic hybrid systems

d) Observing in real time with attosecond resolution photoemission from surfaces and thin films, offering insight into dynamics of the build-up of band structure and screening effects, as well as state-resolved electron transport dynamics in solids and interfaces

e) Establishing a nonlinear attosecond science by demonstrating attosecond XUV-pump / XUV-probe spectroscopy of inner-shell electron dynamics

f) Development of a user-friendly code library for the simulation of correlated electron dynamics

g) Development of localised short-time electron wave-packet propagation methods including the many-body environment in a solid

h) Enhancement of established electronic structure codes for treatment of strong-field quantum dynamics of electrons