On-target temporal characterization of optical pulses at relativistic intensity.

High-field experiments are very sensitive to the exact value of the peak intensity of an optical pulse due to the nonlinearity of the underlying processes. Therefore, precise knowledge of the pulse intensity, which is mainly limited by the accuracy of the temporal characterization, is a key prerequisite for the correct interpretation of experimental data. While the detection of energy and spatial profile is well established, the unambiguous temporal characterization of intense optical pulses, another important parameter required for intensity evaluation, remains a challenge, especially at relativistic intensities and a few-cycle pulse duration.

Carrier-envelope phase dependence of the directional fragmentation and hydrogen migration in toluene in few-cycle laser fields.

The dissociative ionization of toluene initiated by a few-cycle laser pulse as a function of the carrier envelope phase (CEP) is investigated using single-shot velocity map imaging. Several ionic fragments, CH3 (+), H2 (+), and H3 (+), originating from multiply charged toluene ions present a CEP-dependent directional emission. The formation of H2 (+) and H3 (+) involves breaking C-H bonds and forming new bonds between the hydrogen atoms within the transient structure of the multiply charged precursor.

Generation of multi-octave spanning high-energy pulses by cascaded nonlinear processes in BBO.

We present the generation of optical pulses with a spectral range of 500-2400 nm and energies up to 10 µJ at 1 kHz repetition rate by cascaded second-order nonlinear interaction of few-cycle pulses in beta-barium borate (BBO). Numerical simulations with a 1D+time split-step model are performed to explain the experimental findings. The large bandwidth and smooth spectral amplitude of the resulting pulses make them an ideal seed for ultra-broadband optical parametric chirped pulse amplification and an attractive source for spectroscopic applications.

Broadband amplification by picosecond OPCPA in DKDP pumped at 515 nm.

On the quest towards reaching petawatt-scale peak power light pulses with few-cycle duration, optical parametric chirped pulse amplification (OPCPA) pumped on a time scale of a few picoseconds represents a very promising route. Here we present an experimental demonstration of few-ps OPCPA in DKDP, in order to experimentally verify the feasibility of the scheme. Broadband amplification was observed in the wavelength range of 830-1310 nm.

Experimental and theoretical investigation of timing jitter inside a stretcher-compressor setup.

In an optically synchronized short-pulse optical-parametric chirped-pulse amplification (OPCPA) system, we observe a few-100 fs-scale timing jitter. With an active timing stabilization system slow fluctuations are removed and the timing jitter can be reduced to 100 fs standard deviation (Std). As the main source for the timing fluctuations we could identify air turbulence in the stretcher-compressor setup inside the chirped pulse amplification (CPA) pump chain.

High energy picosecond Yb:YAG CPA system at 10 Hz repetition rate for pumping optical parametric amplifiers.

We present a chirped pulse amplification (CPA) system based on diode-pumped Yb:YAG. The stretched ns-pulses are amplified and have been compressed to less than 900 fs with an energy of 200 mJ and a repetition rate of 10 Hz. This system is optically synchronized with a broadband seed laser and therefore ideally suited for pumping optical parametric chirped pulse amplification (OPCPA) stages on a ps-timescale.

Photodissociation of group-6 hexacarbonyls: observation of coherent oscillations in an antisymmetric (pseudorotation) vibration in Mo(CO)(5) and W(CO)(5).

On dissociation of M(CO)(6), M = Cr, Mo and W, by a femtosecond UV laser (<270 to 360 nm), pronounced coherent oscillations are observed in the pentacarbonyl products on probing by long-wavelength (810 nm) ionization in the gas phase. They are vibrations in the ground state, driven by the slope from a conical intersection on relaxation from the initially formed excited state (S(1)). Surprisingly, with M = Mo and W we also find a fundamental of an antisymmetric (b(2) in C(4v)) vibration.

Time-resolved electron diffraction from selectively aligned molecules.

We experimentally demonstrate ultrafast electron diffraction from transiently aligned molecules in the absence of external (aligning) fields. A sample of aligned molecules is generated through photodissociation with femtosecond laser pulses, and the diffraction pattern is captured by probing the sample with picosecond electron pulses shortly after dissociation-before molecular rotation causes the alignment to vanish. In our experiments the alignment decays with a time constant of 2.

Vacuum ultraviolet pulses of 11 fs from fifth-harmonic generation of a Ti:sapphire laser.

We demonstrate that in a short Ar cell, generation of the fifth harmonic from 12 fs pulses at 810 nm directly results in ultrashort vacuum UV pulses at 162 nm. They have a spectral width of approximately 5 nm and a duration of 11+/-1 fs (1.4 times the transform limit), as measured by cross correlation with the fundamental pulses.

Sub-10-fs supercontinuum radiation generated by filamentation of few-cycle 800 nm pulses in argon.

Focusing 12 fs pulses of 800 nm with moderate energy (0.35 mJ) into atmospheric-pressure argon (Ar) gives rise to filamentation (self-focusing) and a supercontinuum with a very broad pedestal, extending to 250 nm. According to the present understanding, the short wavelengths are produced by self-phase modulation in the self-steepened trailing edge of the pulse.

Ultrafast relaxation and coherent oscillations in aminobenzonitriles in the gas phase probed by intense-field ionization.

4-Aminobenzonitrile derivatives have two excited states of similar energy: besides the benzene-like L(b) state (also termed "locally excited" or LE state) one with charge-transfer (CT) character that is slightly higher in the isolated molecules. The CT state can be lowered by solvents of suitable polarity, so that dual fluorescence can be observed in them. It is controversial along which coordinate this state is displaced, although the amino-group twist is a wide-spread assumption.

Forward and backward pericyclic photochemical reactions have intermediates in common, yet cyclobutenes break the rules.

Photochemical pericyclic reactions are believed to proceed via a so-called pericyclic minimum on the lowest excited potential surface (S(1)), which is common to both the forward and backward reactions. Such a common intermediate has never been directly detected. The photointerconversion of 1,3-butadiene and cyclobutene is the prevailing prototype for such reactions, yet only diene ring closure proceeds with the stereospecificity that the Woodward-Hoffmann rules predict.

Coherent oscillation and ultrafast internal conversion of tetrafluoroethene after excitation at 197 nm.

C2F4 was excited by using a 150 fs pulse in its longest-wavelength band to the Rydberg (3 s) state and then probed by photoionization techniques at 810 nm. The molecule relaxes in two consecutive steps (time constants 29 and 118 fs), probably via the pipi* state, which is lowered in energy by stretching and twisting the C=C bond. A coherent oscillation (350 fs) was found, which we assign to an overtone of the twist vibration (47.

Ultrafast temporary charge transfer in pyrrolidinyl-benzonitrile and pyrrolyl-benzonitrile in the gas phase.

4-(N-pyrrolidinyl)benzonitrile and 4-(N-pyrrolyl)benzonitrile were excited by an ultrashort pulse at 270 nm to their La (S2) states and then probed by ionization at long wavelengths. Parent and fragment ion signals show components with time constants < 100 fs which we attribute to ultrafast relaxation to the Lb (S1) state. From this short time we infer a conical intersection between the Lb and La surfaces.

Ultrafast charge transfer via a conical intersection in dimethylaminobenzonitrile.

The L(a)-like S2 state (2A) of 4-(dimethylamino)benzonitrile was pumped at 267 nm in the gas phase at 130 degrees C. Nonresonant multiphoton ionization at 800 nm with mass-selective detection then probed the subsequent processes. Whereas ionization at the Franck-Condon geometry only gave rise to the parent ion, fragmentation increased on motion towards the charge-transfer (CT) state.

Ultrafast [2 + 2]-cycloaddition in norbornadiene.

Excitation of norbornadiene (bicyclo[2.2.1]hepta-2,5-diene) at 200 nm populates two states in parallel, the second pi(pi*) state and a Rydberg state.