Torsten Siebert

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The coupling of specific nuclear and electronic degrees of freedom of a molecular system during non-radiative electronic transitions plays a central role in photochemistry and photobiology. This breakdown of the Born-Oppenheimer approximation during processes such as internal conversion determines the mechanism and product distribution of photochemical(More)
In an earlier publication we demonstrated that by using pairs of pulses of different colors (e.g., red and blue) it is possible to excite a dilute ensemble of molecules such that lasing and/or gain-swept superradiance is realized in a direction toward the observer. This approach is a conceptual step toward spectroscopic probing at a distance, also known as(More)
We use time-resolved coherent Raman spectroscopy to obtain molecule-specific signals from dipicolinic acid (DPA), which is a marker molecule for bacterial spores. We use femtosecond laser pulses in both visible and UV spectral regions and compare experimental results with theoretical predictions. By exciting vibrational coherence on more than one mode(More)
The vibrational modes of the deoxyribose-phosphodiester backbone moiety of DNA and their interactions with the interfacial aqueous environment are addressed with two-dimensional (2D) infrared spectroscopy on a femto- to picosecond time scale. Beyond the current understanding in the harmonic approximation, the anharmonic character and delocalization of the(More)
DNA oligomers are studied at 0% and 92% relative humidity, corresponding to N < 2 and N > 20 water molecules per base pair. Two-dimensional (2D) infrared spectroscopy of DNA backbone modes between 920 and 1120 cm(-1) maps fluctuating interactions at the DNA surface. At both hydration levels, a frequency fluctuation correlation function with a 300 fs decay(More)
Range and magnitude of electric fields at biomolecular interfaces and their fluctuations in a time window down to the subpicosecond regime have remained controversial, calling for electric-field mapping in space and time. Here, we trace fluctuating electric fields at the surface of native salmon DNA via their interactions with backbone vibrations in a wide(More)
The anionic V4O11 cluster is presented as a gas-phase system of low dimensionality for modeling surface activation of molecular oxygen and the reactivity toward unsaturated hydrocarbons. Together with the charged cluster aggregates and fragments taking part in the reaction, neutral reactant and product species are monitored via multiphoton ionization for(More)
An experimental methodology for a mechanistic analysis of gas phase chemical reactions is presented in the context of structure-reactivity relationships of metal oxide clusters relevant to photocatalysis. The spectroscopic approach is demonstrated with the investigation of the photoinduced oxygenation of propene on the V(4)O(11)(-) cluster, where the(More)
A practicable and economic method for the generation and full characterization of laser pulses ranging down to sub 7 fs duration with energies spanning the full microJ domain is presented. The method utilizes a self-induced and self-guiding filamentation of titanium-sapphire based, amplified pulses in air for spectral broadening, a standard chirp mirror(More)
Optically writable, thermally erasable surface relief gratings in thin Disperse Red 1 polymethyl methacrylate azopolymer films were used to demonstrate an arbitrarily reconfigurable fiber Bragg filter. Gratings were optically written on azopolymer-coated side-polished fiber blocks, and a write-erase-write cycle was demonstrated. Finite difference time(More)