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Research Area B.2

Potential energy surfaces of diphenylmethylchloride with the conical intersec-tion for 80-fs bond cleavage to the radical pair.

Molecular processes

The study and the control of electron correlation, light-driven electron dynamics and photoinduced chemistry require even shorter, more elaborately shaped and waveform-controlled light pulses. Capitalising on advances of MAP's state-of-the-art ultrashort-pulse sources from the first funding period and future developments (see Research Area A.1 (Broadband and intense coherent light sources) we pursue the real-time exploration of the fastest processes in molecular systems such as coupled electronic-nuclear dynamics and coupled electron / proton transfer and extend studies to ever more complex systems.

We will advance UV photoelectron spectroscopy towards 10-fs resolution and develop novel multi-dimensional multi-pulse coherent VIS / UV spectroscopies with tunable, shaped sub-10-fs pulses and combine themwith efficient computational methods for the analysis of the spectroscopic signals. Optimised strategies for the manipulation of electronic / nuclear dynamics in a wide range of systems will be developed by the concerted work of the theory groups to support and guide experimental research towards new frontiers. 

X-ray diffraction / transmission will allow us to record ultrafast structural changes in chemical and biological systems with atomic spatial resolution. Whilst a sub-picosecond laser-driven X-ray plasma source developed in the first funding period will serve as a workhorse for these studies, CALA's sub-10-fs laser-driven undulator X-ray source, LUX will allow us to advance X-ray diffraction to few-femtosecond temporal resolution for the first time, affording promise for unprecedented insight into structural dynamics of complex biological samples. Last but not least, with CALA's unique synchronised fs-pulsed ion and laser / X-ray beams we will push the frontiers of ultrafast radiation biology by addressing elementary processes induced in particle cancer therapy within 1 ps of the ion impact.

Main objectives for 2012-2017:

a) Development of sub-20-fs pump-probe photoelectron spectroscopy and exploration of ultrafast photoinduced chemical transformations in complex molecular systems

b) Studying fastest molecular processes, induced by fundamental couplings in multi-chromophoric systems, with sub-10-fs VIS / UV multi-pulse coherent spectroscopy

c) Advancing time-resolved X-ray diffraction / transmission to sub-10-fs resolution and exploring structural transformations in complex biological molecules

d) Furnishing time-resolved radiation biology with fs ion-beam pump and fs laser / X-ray probe pulses and use the novel tools for capturing primary (sub-ps) dynamics, e.g., radical generation, induced by ion impact in biological matter

e) Development and application – via theoretical analysis – of novel control strategies for the detection and steering of electronic motion and ultrafast chemical dynamics

f) Extension of the theory of coherent N-wave-mixing spectroscopy beyond the perturbative regime of nonlinear optics

g) Development of the “virtual spectroscopic laboratory” for the calculation of time- and frequency-resolved optical signals in spectroscopy

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