Sub-50 fs temporal resolution in an FEL-optical laser pump-probe experiment at FLASH2.

High temporal resolution is essential for ultra-fast pump-probe experiments. Arrival time jitter and drift measurements, as well as their control, become critical especially when combining XUV or X-ray free-electron lasers (FELs) with optical lasers due to the large scale of such facilities and their distinct pulse generation processes. This paper presents the application of a laser pulse arrival time monitor that actively corrects the arrival time of an optical laser relative to the FEL's main optical clock. Combined with post-analysis single pulse jitter correction this new approach improves the temporal resolution for pump-probe experiments significantly. Benchmark measurements on photo-ionization of xenon atoms performed at FLASH beamline FL26, demonstrate a sub-50 fs FWHM overall temporal resolution.

Laser-Induced Graphitization of Diamond Under 30 fs Laser Pulse Irradiation.

The degree of laser-induced graphitization from a sp3-bonded to a sp2-bonded carbon fraction in a single crystal chemical vapor deposited (CVD) diamond under varying fluence of an ultrashort pulsed laser (30 fs, 800 nm, 1 kHz) irradiation has been studied. The tetrahedral CVD sp3 phase is found to transition to primarily an sp2 aromatic crystalline graphitic fraction below the critical fluence of 3.9 J/cm2, above which predominantly an amorphous carbon is formed. A fractional increase of fluence from 3.3 to 3.9 J/cm2 (∼20%) results in a substantially (∼3-fold) increased depth of the sp2 graphitized areas owing to the nonlinear interactions associated with a fs laser irradiation. Additionally, formation of a C═O carbonyl group is observed below the critical threshold fluence; the C═O cleavage occurrs gradually with the increase of irradiation fluence of 30 fs laser light. The implications for these findings on enhancement of fs driven processing of diamonds are discussed.

Charge resonance enhanced ionization of CO2 probed by laser Coulomb explosion imaging.

The process by which a molecule in an intense laser field ionizes more efficiently as its bond length increases towards a critical distance R(c) is known as charge resonance enhanced ionization (CREI). We make a series of measurements of this process for CO(2), by varying pulse duration from 7 to 200 fs, in order to identify the charge states and time scales involved. We find that for the 4+ and higher charge states, 100 fs is the time scale required to reach the critical geometry ≈ 2.1 Å and <θ(OCO)> ≈ 163° (equilibrium CO(2) geometry is ≈ 1.16 Å and <θ(OCO)> ≈ 172°). The CO(2)(3+) molecule, however, appears always to begin dissociation from closer than 1.7 Å indicating that dynamics on charge states lower than 3+ is not sufficient to initiate CREI. Finally, we make quantum ab initio calculations of ionization rates for CO(2) and identify the electronic states responsible for CREI.