Adaptive coherent control using the von Neumann basis.

Recently we introduced the von Neumann representation as a joint time-frequency description for femtosecond laser pulses. Here we show that the von Neumann basis can be implemented into an evolutionary algorithm for adaptive optimization in coherent control. We perform simulations that demonstrate the efficiency compared to other parametrizations in the frequency domain.

Molecular quantum control landscapes in von Neumann time-frequency phase space.

Recently we introduced the von Neumann representation as a joint time-frequency description for femtosecond laser pulses and suggested its use as a basis for pulse shaping experiments. Here we use the von Neumann basis to represent multidimensional molecular control landscapes, providing insight into the molecular dynamics. We present three kinds of time-frequency phase space scanning procedures based on the von Neumann formalism: variation of intensity, time-frequency phase space position, and/or the relative phase of single subpulses.

Spatiotemporal control of nanooptical excitations.

The most general investigation and exploitation of light-induced processes require simultaneous control over spatial and temporal properties of the electromagnetic field on a femtosecond time and nanometer length scale. Based on the combination of polarization pulse shaping and time-resolved two-photon photoemission electron microscopy, we demonstrate such control over nanoscale spatial and ultrafast temporal degrees of freedom of an electromagnetic excitation in the vicinity of a nanostructure. The time-resolved cross-correlation measurement of the local photoemission yield reveals the switching of the nanolocalized optical near-field distribution with a lateral resolution well below the diffraction limit and a temporal resolution on the femtosecond time scale.

Ultrafast photoconversion of the green fluorescent protein studied by accumulative femtosecond spectroscopy.

The irreversible photoconversion of T203V green fluorescent protein (GFP) via decarboxylation is studied under femtosecond excitation using an accumulative product detection method that allows us to measure small conversion efficiencies of down to DeltaOD = 10(-7) absorbance change per pulse. Power studies with 800- and 400-nm pulse excitation reveal that excitation to higher states of the neutral form of the GFP chromophore induces photoconversion very efficiently. The singly excited neutral chromophore is a resonant intermediate of the two-step excitation process that leads to efficient photoconversion.

Inherently phase-stable coherent two-dimensional spectroscopy using only conventional optics.

We introduce an inherently phase-stable setup for coherent two-dimensional femtosecond spectroscopy in noncollinear box geometry using only conventional beam splitters, mirrors, and delay stages. Avoiding diffractive optics, pulse shapers, and active phase-locking loops, our spectroscopy setup is simple, robust, and works for ultrabroad bandwidths in all spectral regimes (infrared, visible, and ultraviolet).

Generation of polarization-shaped ultraviolet femtosecond pulses.

We experimentally demonstrate the generation and characterization of polarization-shaped femtosecond laser pulses in the ultraviolet at a central wavelength of 400 nm. Near-infrared laser pulses are first polarization shaped and then frequency doubled in an interferometrically stable setup that employs two perpendicularly oriented nonlinear crystals. A new pulse shaper design involving volume phase holographic gratings reduces losses and hence leads to an increase in pulse energy.

Product accumulation for ultrasensitive femtochemistry.

We present a novel experimental method for studying photochemical reactions that involve permanent products. The accumulation of photoproducts facilitates the measurement of extremely small product yields. A calibration of the setup accounts for diffusion effects, and the experimental results can be expressed in terms of single-pulse photochemical efficiencies.

The von Neumann picture: a new representation for ultrashort laser pulses.

In recent years, the use of joint time-frequency representations to characterize and interpret shaped femtosecond laser pulses has proven to be very useful. However, the number of points in a joint time-frequency representation is daunting as compared with those in either the frequency or time representation. In this article we introduce the use of the von Neumann representation, in which a femtosecond pulse is represented on a discrete lattice of evenly spaced time-frequency points using a non-orthogonal Gaussian basis.

Towards optimal control with shaped soft-x-ray light.

We demonstrate the first example of a closed-loop adaptive control experiment in the soft-x-ray spectral region. The branching ratio of the dissociative photoionization of sulfur hexafluoride (SF(6)) can be maximized and minimized by applying tailored soft-x-ray femtosecond light fields. The spectrally shaped coherent soft-x-ray pulses are produced by high-harmonic generation driven by phase-shaped femtosecond laser pulses.