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Biomedical subjects

Tobias Brixner

Publications and source records attributed to Tobias Brixner.

3 recordsLinked to original sources

Femtosecond shaping of transverse and longitudinal light polarization.

Femtosecond laser pulse shaping techniques have been restricted to propagating transverse electromagnetic waves. We present a scheme for pulse shaping of optical near fields based on the excitation of longitudinal electromagnetic fields with polarization-shaped light pulses. By solving Maxwell's equations for a model nanostructure, i.e., a scanning tunneling microscope tip, with help from the boundary-element method, we demonstrate that the electric field vector oscillates in a complex yet controllable fashion in three dimensions. Many applications are envisioned because literally another dimension in the optimal control of light-matter interaction is accessible.

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Phase-stabilized two-dimensional electronic spectroscopy.

Two-dimensional (2D) spectroscopy is a powerful technique to study nuclear and electronic correlations between different transitions or initial and final states. Here we describe in detail our development of inherently phase-stabilized 2D Fourier-transform spectroscopy for electronic transitions. A diffractive-optic setup is used to realize heterodyne-detected femtosecond four-wave mixing in a phase-matched box geometry. Wavelength tunability in the visible range is accomplished by means of a 3 kHz repetition-rate laser system and optical parametric amplification. Nonlinear signals are fully characterized by spectral interferometry. Starting from fundamental principles, we discuss the origin of phase stability and the precise calibration of excitation-pulse time delays using movable glass wedges. Automated subtraction of undesired scattering terms removes experimental artifacts. On the theoretical side, the response-function formalism is extended to describe molecules with three electronic levels, and the shape of 2D spectral features is discussed. As an example for this technique, experimental 2D spectra are shown for the dye molecule Nile Blue in acetonitrile at 595 nm, recorded for a series of population times. Simulations explore the influence of different model parameters and qualitatively reproduce the experimental results. We show that correlations between different electronically excited states can be determined from the spectra. The technique described here can be used to measure the third-order response function of complex systems covering several electronic transitions.

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Quantum control of gas-phase and liquid-phase femtochemistry.

Active control of chemical reactions on a microscopic (molecular) level, that is, the selective breaking or making of chemical bonds, is an old dream. However, conventional control agents used in chemical synthesis are macroscopic variables such as temperature, pressure or concentration, which gives no direct access to the quantum-mechanical reaction pathway. In quantum control, by contrast, molecular dynamics are guided with specifically designed light fields. Thus it is possible to efficiently and selectively reach user-defined reaction channels. In the last years, experimental techniques were developed by which many breakthroughs in this field were achieved. Femtosecond laser pulses are manipulated in so-called pulse shapers to generate electric field profiles which are specifically adapted to a given quantum system and control objective. The search for optimal fields is guided by an automated learning loop, which employs direct feedback from experimental output. Thereby quantum control over gas-phase as well as liquid-phase femtochemical processes has become possible. In this review, we first discuss the theoretical and experimental background for many of the recent experiments treated in the literature. Examples from our own research are then used to illustrate several fundamental and practical aspects in gas-phase as well as liquid-phase quantum control. Some additional technological applications and developments are also described, such as the automated optimization of the output from commercial femtosecond laser systems, or the control over the polarization state of light on an ultrashort timescale. The increasing number of successful implementations of adaptive learning techniques points at the great versatility of computer-guided optimization methods. The general approach to active control of light-matter interaction has also applications in many other areas of modern physics and related disciplines.

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