Ultrafast Photo-Ion Probing of the Relaxation Dynamics in 2-Thiouracil.

In this work, we investigate the relaxation processes of 2-thiouracil after UV photoexcitation to the S2 state through the use of ultrafast, single-colour, pump-probe UV/UV spectroscopy. We place focus on investigating the appearance and subsequent decay signals of ionized fragments. We complement this with VUV-induced dissociative photoionisation studies collected at a synchrotron, allowing us to better understand and assign the ionisation channels involved in the appearance of the fragments. We find that all fragments appear when single photons with energy > 11 eV are used in the VUV experiments and hence appear through 3+ photon-order processes when 266 nm light is used. We also observe three major decays for the fragment ions: a sub-autocorrelation decay (i.e., sub-370 fs), a secondary ultrafast decay on the order of 300-400 fs, and a long decay on the order of 220 to 400 ps (all fragment dependent). These decays agree well with the previously established S2 → S1 → Triplet → Ground decay process. Results from the VUV study also suggest that some of the fragments may be created by dynamics occurring in the excited cationic state.

Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser.

In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L1- and L2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster-Kronig and Auger-Meitner emission at the L1- and L2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.

Ultrafast Photo-ion Probing of the Ring-Opening Process in Trans-Stilbene Oxide.

The ultrafast photo-induced ring opening of the oxirane derivative trans-stilbene oxide has been studied through the use of ultrafast UV/UV pump-probe spectroscopy by using photo-ion detection. Single- and multiphoton probe paths and final states were identified through comparisons between UV power studies and synchrotron-based vacuum ultraviolet (VUV) single-photon ionization studies. Three major time-dependent features of the parent ion (sub-450 fs decay, (1.5±0.2) ps, and >100 ps) were observed. These decays are discussed in conjunction with the primary ring-opening mechanism of stilbene oxide, which occurs through C-C dissociation in the oxirane ring. The appearance of fragments relating to the masses of dehydrogenated diphenylmethane (167 amu) and dehydrogenated methylbenzene (90 amu) were also investigated. The appearance of the 167 amu fragment could suggest an alternative ultrafast ring-opening pathway via the dissociation of one of the C-O bonds within the oxirane ring.

Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction.

Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. Here we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S1→S0 internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule.

Phase measurement and far-field reconstruction on externally coupled laser diode arrays.

Passive coherent combination of several discrete low power laser diodes is a promising way to overcome the issue of degrading beam quality when scaling single emitters to > 10 W output power. Such systems would be an efficient alternative to current high power sources, yet they suffer from fatal coherence loss when operated well above threshold. We present a new way to obtain detailed coherence information for laser diode arrays using a spatial light modulator to help identify the underlying decoherence processes. Reconstruction tests of the emitted far-field distribution are conducted to evaluate the performance of our setup.

Mode stabilization of a laterally structured broad area diode laser using an external volume Bragg grating.

An external volume Bragg grating (VBG) is used for transverse and longitudinal mode stabilization of a broad area diode laser (BAL) with an on-chip transverse Bragg resonance (TBR) grating. The internal TBR grating defines a transverse low-loss mode at a specific propagation angle inside the BAL. Selection of the TBR mode was realized via the angular geometry of an external resonator assembly consisting of the TBR BAL and a feedback element. A feedback mirror provides near diffraction limited and spectral narrow output in the TBR mode albeit requiring an intricate alignment procedure. If feedback is provided via a VBG, adjustment proves to be far less critical and higher output powers were achieved. Moreover, additional modulation in the far field distribution became discernible allowing for a better study of the TBR concept.

Broad area diode laser with on-chip transverse Bragg grating stabilized in an off-axis external cavity.

The emission characteristics of a novel, specially designed broad area diode laser (BAL) with on-chip transversal Bragg resonance (TBR) grating in lateral direction were investigated in an off-axis external cavity setup. The internal TBR grating defines a low loss transversal mode at a specific angle of incidence and a certain wavelength. By providing feedback at this specific angle with an external mirror, it is possible to select this low loss transverse mode and stabilize the BAL. Near diffraction limited emission with an almost single lobed far field pattern could be realized, in contrast to the double lobed far field pattern of similar setups using standard BALs or phase-locked diode laser arrays. Furthermore, we could achieve a narrow bandwidth emission with a simplified setup without external frequency selective elements.