Ultrafast dynamics of fluorene initiated by highly intense laser fields.

We present an investigation of the ultrafast dynamics of the polycyclic aromatic hydrocarbon fluorene initiated by an intense femtosecond near-infrared laser pulse (810 nm) and probed by a weak visible pulse (405 nm). Using a multichannel detection scheme (mass spectra, electron and ion velocity-map imaging), we provide a full disentanglement of the complex dynamics of the vibronically excited parent molecule, its excited ionic states, and fragments. We observed various channels resulting from the strong-field ionization regime. In particular, we observed the formation of the unstable tetracation of fluorene, above-threshold ionization features in the photoelectron spectra, and evidence of ubiquitous secondary fragmentation. We produced a global fit of all observed time-dependent photoelectron and photoion channels. This global fit includes four parent ions extracted from the mass spectra, 15 kinetic-energy-resolved ionic fragments extracted from ion velocity map imaging, and five photoelectron channels obtained from electron velocity map imaging. The fit allowed for the extraction of 60 lifetimes of various metastable photoinduced intermediates.

Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy.

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+ state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

Third and fifth order nonlinear susceptibilities in thin HfO2 layers.

Third harmonic generation (THG) from dielectric layers is investigated. By forming a thin gradient of HfO2 with continuously increasing thickness, we are able to study this process in detail. This technique allows us to elucidate the influence of the substrate and to quantify the layered materials third χ(3)(3ω: ω, ω, ω) and even fifth order χ(5)(3ω: ω, ω, ω, ω, - ω) nonlinear susceptibility at the fundamental wavelength of 1030 nm. This is to the best of our knowledge the first measurement of the fifth order nonlinear susceptibility in thin dielectric layers.

Below-threshold harmonic generation in gas-jets for Th-229 nuclear spectroscopy.

The generation of below-threshold harmonics in gas-jets constitutes a promising path towards optical frequency combs in the vacuum ultra-violet (VUV) spectral range. Of particular interest is the 150 nm range, which can be exploited to probe the nuclear isomeric transition of the Thorium-229 isotope. Using widely available high-power, high-repetition-rate Ytterbium-based laser sources, VUV frequency combs can be generated through the process of below-threshold harmonic generation, in particular 7th harmonic generation of 1030 nm. Knowledge about the achievable efficiencies of the harmonic generation process is crucial for the development of suitable VUV sources. In this work, we measure the total output pulse energies and conversion efficiencies of below-threshold harmonics in gas-jets in a phase-mismatched generation scheme using Argon and Krypton as nonlinear media. Using a 220 fs, 1030 nm source, we reach a maximum conversion efficiency of 1.1 × 10-5 for the 7th harmonic (147 nm) and 0.78 × 10-4 for the 5th harmonic (206 nm). In addition, we characterize the 3rd harmonic of a 178 fs, 515 nm source with a maximum efficiency of 0.3%.

Generating Ultrabroadband Deep-UV Radiation and Sub-10 nm Gap by Hybrid-Morphology Gold Antennas.

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

Full characterization of 8 fs deep UV pulses via a dispersion scan.

We report on, to the best of our knowledge, the first characterization of deep ultraviolet (UV) pulses by the dispersion scan (d-scan) technique. Negatively chirped 8 fs deep UV pulses are generated via the phase transfer of shaped few-cycle near-infrared pulses in a sum frequency generation process with narrowband second harmonic. The pulses are characterized by a d-scan technique incorporating a cross-polarized wave (XPW) generation nonlinearity. Being a single-beam degenerate four-wave mixing process, XPW does not acquire frequency conversion and, thus, is ideally suited for characterizing pulses in the UV, where the material dispersion severely limits phase matching. The characterization method is benchmarked by measuring the dispersion effect of a known fused silica plate on the pulses.

Rapid phase retrieval of ultrashort pulses from dispersion scan traces using deep neural networks.

The knowledge of the temporal shape of femtosecond pulses is of major interest for all their applications. The reconstruction of the temporal shape of these pulses is an inverse problem for characterization techniques, which benefit from an inherent redundancy in the measurement. Conventionally, time-consuming optimization algorithms are used to solve the inverse problems. Here, we demonstrate the reconstruction of ultrashort pulses from dispersion scan traces employing a deep neural network. The network is trained with a multitude of artificial and noisy dispersion scan traces from randomly shaped pulses. The retrieval takes only 16 ms enabling video-rate reconstructions. This approach reveals a great tolerance against noisy conditions, delivering reliable retrievals from traces with signal-to-noise ratios down to 5.

Simple route toward efficient frequency conversion for generation of fully coherent supercontinua in the mid-IR and UV range.

Fiber supercontinua represent light sources of pivotal importance for a wide range of applications, ranging from optical communications to frequency metrology. Although spectra encompassing more than three octaves can be produced, the applicability of such spectra is strongly hampered due to coherence degradation during spectral broadening. Assuming pulse parameters at the cutting edge of currently available laser technology, we demonstrate the possibility of strongly coherent supercontinuum generation. In a fiber with two zero-dispersion wavelengths a higher-order soliton experiences a temporal breakdown, without any compression or splitting behavior, which leads to nearly complete conversion of input solitonic radiation into resonant nonsolitonic radiation in the dispersive wave regime. As the process is completely deterministic and shows little sensitivity to input noise, the resulting pulses appear to be compressible down to the sub-cycle level and may thus hold a new opportunity for direct generation of attosecond pulses in the visible to near ultraviolet wavelength range.

Few-cycle optical pulse characterization via cross-polarized wave generation dispersion scan technique.

We demonstrate a dispersion scan (d-scan) pulse characterization scheme employing cross-polarized wave (XPW) generation as a nonlinear optical process. XPW generation is a degenerate four-wave mixing process with no phase-matching limitations. Therefore, its implementation in the d-scan method is a good choice for the characterization of few-cycle pulses in remote spectral regions. We fully characterize 5-10 fs pulses delivered through a hollow-core fiber in the near-IR region and compare the results with the second-harmonic generation (SHG) frequency-resolved optical gating and SHG d-scan characterization methods.

Spatio-temporal focusing of an ultrafast pulse through a multiply scattering medium.

Pulses of light propagating through multiply scattering media undergo complex spatial and temporal distortions to form the familiar speckle pattern. There is much current interest in both the fundamental properties of speckles and the challenge of spatially and temporally refocusing behind scattering media. Here we report on the spatially and temporally resolved measurement of a speckle field produced by the propagation of an ultrafast optical pulse through a thick strongly scattering medium. By shaping the temporal profile of the pulse using a spectral phase filter, we demonstrate the spatially localized temporal recompression of the output speckle to the Fourier-limit duration, offering an optical analogue to time-reversal experiments in the acoustic regime. This approach shows that a multiply scattering medium can be put to profit for light manipulation at the femtosecond scale, and has a diverse range of potential applications that includes quantum control, biological imaging and photonics.