Unveiling second harmonic generation from femtosecond-laser microstructured Nd:YAG crystal.

In this work we apply second harmonic microscopy to the analysis of damage tracks inscribed by femtosecond laser irradiation in a Nd:YAG crystal. While second harmonic generation is not expected in the bulk of this centrosymmetric material, the 2D and 3D images obtained via second harmonic microscopy show that the induced micro-modification of the crystal structure leads to a localized generation of the nonlinear signal. The nature of this modification and its dependence on irradiation and detection parameters is discussed. These findings demonstrate the capability of second harmonic microscopy for the morphological analysis of written structures in Nd:YAG and open the door for the design and fabrication of new nonlinear structures to be integrated in novel photonic devices.

High efficiency diode-pumped Pr:LiLuF4 visible lasers in femtosecond-laser-written waveguides.

In this work we investigate the power scaling of diode-pumped Pr:LiLuF4 waveguide lasers produced by direct femtosecond writing. The waveguides studied consisted in depressed cladding waveguides with different geometries. We observed laser emission at 604 nm, achieving a maximum output power of 275 mW and a slope efficiency of 40%, and 721 nm, demonstrating 310 mW of output power and a slope efficiency of 50%. Moreover, we obtained, what we believe is for the first time in a diode-pumped waveguide, laser emission at 523 nm, with a maximum output power of 65 mW and a slope efficiency of 11%. In the end, we also demonstrated the first diode-pumped operation of a single-transverse-mode waveguide laser at 721 nm, reaching a maximum output power of 28 mW and maintaining a high quality beam with an M2 of 1.1.

Diode-pumped visible lasing in femtosecond-laser-written Pr:LiLuF4 waveguide.

In this Letter we report the realization of a femtosecond-laser-written diode-pumped Pr:LiLuF4 visible waveguide laser. The waveguide studied in this work consisted of a depressed-index cladding, whose design and fabrication were optimized to minimize the propagation loss. Laser emission has been achieved at 604 nm and 721 nm, with output power of 86 mW and 60 mW, respectively, and slope efficiencies of 16% and 14%. In addition, we obtained, for the first time in a praseodymium-based waveguide laser, stable continuous-wave laser operation at 698 nm (3 mW of output power and 0.46% of slope efficiency), corresponding to the wavelength necessary for the clock transition of the strontium-based atomic clock. The waveguide laser emission at this wavelength is mainly in the fundamental mode (i.e., the larger propagation constant mode) showing a nearly Gaussian intensity profile.

Faster chiral versus collinear magnetic order recovery after optical excitation revealed by femtosecond XUV scattering.

While chiral spin structures stabilized by Dzyaloshinskii-Moriya interaction (DMI) are candidates as novel information carriers, their dynamics on the fs-ps timescale is little known. Since with the bulk Heisenberg exchange and the interfacial DMI two distinct exchange mechanisms are at play, the ultrafast dynamics of the chiral order needs to be ascertained and compared to the dynamics of the conventional collinear order. Using an XUV free-electron laser we determine the fs-ps temporal evolution of the chiral order in domain walls in a magnetic thin film sample by an IR pump - X-ray magnetic scattering probe experiment. Upon demagnetization we observe that the dichroic (CL-CR) signal connected with the chiral order correlator mzmx in the domain walls recovers significantly faster than the (CL + CR) sum signal representing the average collinear domain magnetization mz2 + mx2. We explore possible explanations based on spin structure dynamics and reduced transversal magnetization fluctuations inside the domain walls and find that the latter can explain the experimental data leading to different dynamics for collinear magnetic order and chiral magnetic order.

Femtosecond Double-Pulse Laser Ablation and Deposition of Co-Doped ZnS Thin Films.

Nanostructured thin films of Co-doped zinc sulfide were synthesized through femtosecond pulsed laser deposition. The scheme involved ablation of physically mixed Co and ZnS with pairs of ultrashort pulses separated in time in the 0-300 ps range. In situ monitorization of the deposition process was carried out through a simultaneous reflectivity measurement. The crystallinity of generated nanoparticles and the inclusion of Co in the ZnS lattice is demonstrated by transmission electron microscopy and energy dispersive X-ray microanalysis (TEM-EDX) characterization. Surface morphology, Raman response, and photoluminescence of the films have also been assessed. The role of interpulse temporal separation is most visible in the thickness of the films obtained at the same total fluence, with much thicker films deposited with short delays than with individual uncoupled pulses. The proportion of Co in the synthesized doped ZnS nanoparticles is found to be substantially lower than the original proportion, and practically independent on interpulse delay.

Simultaneous two-color snapshot view on ultrafast charge and spin dynamics in a Fe-Cu-Ni tri-layer.

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here, we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M-shell resonances of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. We furthermore observe that the electronic dynamics of Ni and Fe show pronounced differences when probed at their resonance, while the demagnetization dynamics are similar. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

Ablation dynamics of Co/ZnS targets under double pulse femtosecond laser irradiation.

Femtosecond lasers, used as tools to investigate the ablation dynamics of solids, can help to develop strategies to control the deposition of nanomaterials by pulsed laser ablation. In this work, Co/ZnS targets, potential candidates for the synthesis of diluted magnetic semiconductor materials, are irradiated by sequences of two femtosecond laser pulses delayed in the picosecond time scale. The ionic composition of the ablation plasma and the dependence of the ion signals on the interpulse delay and relative fluence are determined by time-of-flight mass spectrometry. The results show that, when pulses of different fluence are used, highly asymmetric ion yields are obtained, with more intense ion signals detected when the lower fluence pulse is temporally ahead. The comparison between asymmetric and equal fluence double pulse ablation dynamics provides some understanding of the different processes that modify the properties of the layer irradiated by the first pulse and of the mechanisms affecting the coupling of the delayed pulse into the material. The final outcome of the double pulse irradiation is characterized through the analysis of the deposits produced upon ablation.

Comparison of high-order harmonic generation in uracil and thymine ablation plumes.

We present studies of high-order harmonic generation (HHG) in laser ablation plumes of the ribonucleic acid nucleobase uracil and its deoxyribonucleic acid counterpart thymine. Harmonics were generated using 780 nm, 30 fs and 1300 nm, 40 fs radiation upon ablation with 1064 nm, 10 ns or 780 nm, 160 ps pulses. Strong HHG signals were observed from uracil plumes with harmonics emitted with photon energies >55 eV. Results obtained in uracil plumes were compared with those from thymine, which did not yield signs of harmonic generation. The ablation plumes of the two compounds were examined by collection of the ablation debris on a silicon substrate placed in close proximity to the target and by time-of-flight mass spectrometry. From this evidence we conclude that the differences in HHG signal are due to the different fragmentation dynamics of the molecules in the plasma plume. These studies constitute the first attempt to analyse differences in structural properties of complex molecules through plasma ablation-induced HHG spectroscopy.