Article

Generation of 2.5 μJ vacuum ultraviolet pulses with sub-50 fs duration by noncollinear four-wave mixing in argon.

Max-Born-Institute for Nonlinear Optics and Ultrafast Spectroscopy, 2A Max-Born-Strasse, D-12489 Berlin, Germany. mghotbi@mbi‑berlin.de
Optics Letters (Impact Factor: 3.18). 10/2010; 35(20):3492-4. DOI: 10.1364/OL.35.003492
Source: PubMed

ABSTRACT Generation of sub-50fs vacuum UV pulses with more than 2.5μJ energy at a 1kHz repetition rate is reported. The pulses at 160nm are produced using noncollinear difference-frequency four-wave mixing between the fundamental and third harmonics of an amplified Ti:sapphire laser in argon. While the pulse duration is maintained by increasing the phase-matching pressure, noncollinear interaction improves the conversion efficiency by 1 order of magnitude in comparison with the previous results in collinear geometry.

0 Followers
 · 
111 Views
  • [Show abstract] [Hide abstract]
    ABSTRACT: The sixth harmonic (6ω, 133 nm) of a Ti:sapphire laser is generated using cascaded four-wave mixing in filamentation propagation of the fundamental (ω) and the second harmonic (2ω) pulses through Ne gas. The method provides the 6ω pulse energy higher than 5 nJ/pulse at 1 kHz and a pulse duration shorter than 17 fs without dispersion compensation.
    Optics Letters 10/2014; 39(20). DOI:10.1364/OL.39.006021 · 3.18 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: We investigate non-adiabatic dynamics of NO molecules that are photo-excited in the vacuum ultraviolet photon energy range using time-resolved velocity map imaging. Highly excited valence and Rydberg states are populated with a tunable (147–151 nm) femtosecond laser pulse and then ionized by a time-delayed near-IR laser pulse. Three main contributions are observed in the photoelectron kinetic spectra with corresponding electron yields that show pronounced oscillations. Two oscillations are assigned to ro-vibronic coupling in the valence-Rydberg mixture of the B and 4dδ N2Δ(v = 0) states and the B2Π(v = 25) and 4pπ K2Π(v = 1) states, respectively. We assign a third oscillation to originate from a coupling between two Rydberg states.
    Journal of Physics B Atomic Molecular and Optical Physics 06/2014; 47(12):124016. DOI:10.1088/0953-4075/47/12/124016 · 1.92 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: Two-dimensional (2D) resonance Raman spectroscopies hold great potential for uncovering photoinduced relaxation processes in molecules but are not yet widely applied because of technical challenges. Here, we describe a newly developed 2D resonance Raman experiment operational at the third-harmonic of a Titanium-Sapphire laser. High-sensitivity and rapid data acquisition are achieved by combining spectral interferometry with a background-free (six-pulse) laser beam geometry. The third-harmonic laser pulses are generated in a filament produced by the fundamental and second-harmonic pulses in neon gas at pressures up to 35 atm. The capabilities of the setup are demonstrated by probing ground-state wavepacket motions in triiodide. The information provided by the experiment is explored with two different representations of the signal. In one representation, Fourier transforms are carried out with respect to the two experimentally controlled delay times to obtain a 2D Raman spectrum. Further insights are derived in a second representation by dispersing the signal pulse in a spectrometer. It is shown that, as in traditional pump-probe experiments, the six-wave mixing signal spectrum encodes the wavepacket's position by way of the (time-evolving) emission frequency. Anharmonicity additionally induces dynamics in the vibrational resonance frequency. In all cases, the experimental signals are compared to model calculations based on a cumulant expansion approach. This study suggests that multi-dimensional resonance Raman spectroscopies conducted on systems with Franck-Condon active modes are fairly immune to many of the technical issues that challenge off-resonant 2D Raman spectroscopies (e.g., third-order cascades) and photon-echo experiments in the deep UV (e.g., coherence spikes). The development of higher-order nonlinear spectroscopies operational in the deep UV is motivated by studies of biological systems and elementary organic photochemistries.
    The Journal of Chemical Physics 09/2014; 141(11):114202. DOI:10.1063/1.4894846 · 3.12 Impact Factor