Abstract
The dream of physico-chemists to control molecular reactions with light beyond electronic excitations pushes the development of laser pulse shaping capabilities in the mid-infrared (MIR) spectral range. Here, we present a compact optical parametric amplifier platform for the generation and shaping of MIR laser pulses in the wavelength range between 8 μm and 15 μm. Opportunities for judiciously tailoring the electromagnetic waveform are investigated, demonstrating light field control with a spectral resolution of 59 GHz at a total spectral bandwidth of 5 THz. In experiments focusing on spectral amplitude manipulation these parameters result in a time window of 1.8 ps available for shaping the temporal pulse envelope and a phase modulation resolution of 100 mrad for several picosecond delays.
Highlights
Microscopic understanding of chemical dynamics on a molecular level is of fundamental importance in many science disciplines
The dream of physico-chemists to control molecular reactions with light beyond electronic excitations pushes the development of laser pulse shaping capabilities in the midinfrared (MIR) spectral range
Molecular function manifests itself in time-dependent changes of geometric structure, i. e. bond distances and bond angles describing the molecular dynamics of the system
Summary
Microscopic understanding of chemical dynamics on a molecular level is of fundamental importance in many science disciplines. Ultrashort deliberately shaped mid-infrared (MIR) laser pulses are suitable for a systematic investigation of these reactions, because they provide three key properties [6, 8] Their interaction takes place on the immanent time scales of molecular dynamics. Thereby a vibrational mode can be excited in a step-wise fashion, in which the laser pulse provides always a matching quantum of the energy needed to excite the higher vibrational level in the anharmonic potential This approach of vibrational ladder climbing populates high lying vibrational states creating non-thermal vibrational ensembles [9, 10]. We demonstrate AOM-technique with its advantages of spectral amplitude and phase shaping and with very high spectral resolution by using an acousto-optic modulator (AOM) mask in a 4 f configuration to wavelengths beyond 10 μm In the following it will be discussed, what capabilities are at hand to stretch and manipulate laser pulses.
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