Coherent control of molecular dynamics deals with the steering of quantum mechanical systems
with suitably shaped ultrashort laser fields. The coherence properties of the laser field are
exploited to achieve constructive interference for a predefined target wave function via a phasecorrect
superposition of wave functions. The goal of coherent control, the selective preparation
of a target state, is an important prerequisite for mode-selective chemistry.
The laser pulse tailored to drive the system from the initial to the target state as a perturbation
can in general not be determined by a quantum-mechanical calculation, since usually even the
Hamiltonian of the system is unknown. A practical alternative is to determine the required
shape of the laser field in a feedback-controlled regulation loop which uses a signal derived from
the experiment as feedback. The loop is repeated until a pulse that suits the requirements is
obtained. Experiments in this area have until recently mostly been limited to the wavelength
regime of Ti:Sa lasers and their fundamentals.
This work deals with the fundamentals of feedback-controlled shaping of ultrashort laser pulses
with respect to both establishment of its technical prerequisites and its application to suitable
model systems. The feedback loop has been tested using a simple optimization experiment with
known outcome; then it was applied to experiments of progressively increasing complexity. From
the optimized pulses, physical insight into the optimization process has been gained.
In the first part of this work, the required technology has been implemented and standardized
such that control experiments might employ it as a standard tool. One of the technical prerequisites
was the frequency conversion of the 800 nm Ti:Sa laser pulses to a wavelength range
suited to the particular systems. To this end, non-collinear optical parametric amplifiers have
been built in different designs that routinely produce tunable sub-20 fs pulses in the visible. The
characterization techniques for ultrashort pulses have been implemented as well.
Pulse shapers with cylindrical instead of spherical mirrors have been implemented for the modulation
of broadband pulses, and their functionality has been explained both theoretically and
experimentally. A new liquid crystal device, the core of our pulse shapers, has been developed in
cooperation with the group of Thomas Feurer at the Universit¨at Jena and the Jenoptik GmbH
which allows for the generation of more complex pulse shapes than with other commercially
available devices to date.
Using a pulse shaper to modulate the white light continuum that serves as the seed for the
non-collinear optical parametric amplifier, generation of phase-locked two-color double pulses
has been achieved, with tunable wavelengths, delays, and relative carrier phases between the
single pulses. The basic principle, phase conservation during optical parametric amplification,
has been demonstrated. With this setup, control experiments which require pulses with the
above described attributes in electronically controllable form are possible for the first time.
An evolutionary strategy used as the optimization algorithm in the feedback loop has been
programmed and characterized both in simulation and experiment using a simple optimization
experiment, namely pulse recompression by phase compensation.
In the second part of this work, pulse recompression of ultra-broadband spectra in the sub-20fs
regime serves as an example of utility of feedback-controlled optimization. This experiment simultaneously
served as a further test of the feedback loop in the limit of a physically unreachable
optimization goal.
It has been demonstrated that a suitable parameterization of the electric field, implemented by
a mapping of the optimization parameters adjusted by the algorithm to the physical parameterscontrolling the liquid crystal mask affords a means of acquiring physical knowledge from the
retrieved optimal electr