UV 30†fs laser pulse generation using a multi-pass cell.

Ultrashort ultraviolet (UV) pulses are pivotal for resolving ultrafast electron dynamics. However, their efficient generation is strongly impeded by material dispersion and two-photon absorption, in particular, if pulse durations around a few tens of femtoseconds or below are targeted. Here, we present a new (to our knowledge) approach to ultrashort UV pulse generation: using the fourth-harmonic generation output of a commercial ytterbium laser system delivering 220 fs UV pulses, we implement a multi-pass cell (MPC) providing 5.6 µJ pulses at 256 nm, compressed to 30.5 fs. Our results set a short-wavelength record for MPC post-compression while offering attractive options to navigate the trade-off between upconversion efficiency and acceptance bandwidth for UV pulse production.

Sub-Hz relative linewidths from an interferometrically stabilized mid-infrared frequency comb.

Frequency combs present a unique tool for high-precision and rapid molecular spectroscopy. Difference frequency generation (DFG) of near-infrared sources is a common approach to generate passively stabilized mid-infrared combs. However, only little attention has been paid so far to precisely measure the coherence properties of such sources. Here, we investigate these using a Raman-soliton based DFG source driven by an Yb:fiber frequency comb. A heterodyne beat between the second harmonic of the phase-locked DFG comb near 4 µm and a 2 µm Tm:fiber frequency comb locked to the same optical reference is performed. Using this method, we measure the relative phase noise power spectral density of both combs. This results in a sub-Hz relative linewidth between the DFG comb and the Tm:fiber comb. We also introduce a new pump/seed delay locking mechanism based on interferometry for long-term stable intensity noise suppression.

Few-cycle pulse generation by double-stage hybrid multi-pass multi-plate nonlinear pulse compression.

Few-cycle pulses present an essential tool to track ultrafast dynamics in matter and drive strong field effects. To address photon-hungry applications, high average power lasers are used which, however, cannot directly provide sub-100-fs pulse durations. Post-compression of laser pulses by spectral broadening and dispersion compensation is the most efficient method to overcome this limitation. We present a notably compact setup which turns a 0.1-GW peak power, picosecond burst-mode laser into a 2.9-GW peak power, 8.2-fs source. The 120-fold pulse duration shortening is accomplished in a two-stage hybrid multi-pass, multi-plate compression setup. To our knowledge, neither shorter pulses nor higher peak powers have been reported to-date from bulk multi-pass cells alone, manifesting the power of the hybrid approach. It puts, for instance, compact, cost-efficient, and high repetition rate attosecond sources within reach.

Multi-gigawatt peak power post-compression in a bulk multi-pass cell at a high repetition rate.

The output of a 200kHz, 34W, 300fs ytterbium amplifier is compressed to 31fs with >88% efficiency to reach a peak power of 2.5GW, which to date is a record for a single-stage bulk multi-pass cell. Despite operation 80 times above the critical power for self-focusing in bulk material, the setup demonstrates excellent preservation of the input beam quality. Extensive beam and pulse characterizations are performed to show that the compressed pulses are promising drivers for high harmonic generation and nonlinear optics in gases or solids.

Temporal pulse quality of a Yb:YAG burst-mode laser post-compressed in a multi-pass cell.

Nonlinear pulse post-compression represents an efficient method for ultrashort, high-quality laser pulse production. The temporal pulse quality is, however, limited by amplitude and phase modulations intrinsic to post-compression. We here characterize in frequency and time domain with high dynamic range individual post-compressed pulses within laser bursts comprising 100-kHz-rate pulse trains. We spectrally broaden 730 fs, 3.2 mJ pulses from a Yb:YAG laser in a gas-filled multi-pass cell and post-compress them to 56 fs. The pulses exhibit a nearly constant energy content of 78% in the main peak over the burst plateau, which is close to the theoretical limit. Our results demonstrate attractive pulse characteristics, making multi-pass post-compressed lasers very applicable for pump-probe spectroscopy at, e.g., free-electron lasers or as efficient drivers for secondary frequency conversion stages.

Large Enhancement of Ferromagnetism under a Collective Strong Coupling of YBCO Nanoparticles.

Light-Matter strong coupling in the vacuum limit has been shown, over the past decade, to enhance material properties. Oxide nanoparticles are known to exhibit weak ferromagnetism due to vacancies in the lattice. Here we report the 700-fold enhancement of the ferromagnetism of YBa2Cu3O7-x nanoparticles under a cooperative strong coupling at room temperature. The magnetic moment reaches 0.90 µB/mol, and with such a high value, it competes with YBa2Cu3O7-x superconductivity at low temperatures. This strong ferromagnetism at room temperature suggest that strong coupling is a new tool for the development of next-generation magnetic and spintronic nanodevices.

Large optical nonlinearity enhancement under electronic strong coupling.

Nonlinear optical responses provide a powerful way to understand the microscopic interactions between laser fields and matter. They are critical for plenty of applications, such as in lasers, integrated photonic circuits, biosensing and medical tools. However, most materials exhibit weak optical nonlinearities or long response times when they interact with intense optical fields. Here, we strongly couple the exciton of cyanine dye J-aggregates to an optical mode of a Fabry-Perot (FP) cavity, and achieve an enhancement of the complex nonlinear refractive index by two orders of magnitude compared with that of the uncoupled condition. Moreover, the coupled system shows an ultrafast response of ~120 fs that we extract from optical cross-correlation measurements. The ultrafast and large enhancement of the optical nonlinar coefficients in this work paves the way for exploring strong coupling effects on various third-order nonlinear optical phenomena and for technological applications.

Postcompression of picosecond pulses into the few-cycle regime.

In this work, we demonstrate postcompression of 1.2 ps laser pulses to 13 fs via gas-based multipass spectral broadening. Our results yield a single-stage compression factor of about 40 at 200 W in-burst average power and a total compression factor >90 at reduced power. The employed scheme represents a route toward compact few-cycle sources driven by industrial-grade Yb:YAG lasers at high average power.

Repertoire Sequencing of B Cells Elucidates the Role of UNG and Mismatch Repair Proteins in Somatic Hypermutation in Humans.

The generation of high-affinity antibodies depends on somatic hypermutation (SHM). SHM is initiated by the activation-induced cytidine deaminase (AID), which generates uracil (U) lesions in the B-cell receptor (BCR) encoding genes. Error-prone processing of U lesions creates a typical spectrum of point mutations during SHM. The aim of this study was to determine the molecular mechanism of SHM in humans; currently available knowledge is limited by the number of mutations analyzed per patient. We collected a unique cohort of 10 well-defined patients with bi-allelic mutations in genes involved in base excision repair (BER) (UNG) or mismatch repair (MMR) (MSH2, MSH6, or PMS2) and are the first to present next-generation sequencing (NGS) data of the BCR, allowing us to study SHM extensively in humans. Analysis using ARGalaxy revealed selective skewing of SHM mutation patterns specific for each genetic defect, which are in line with the five-pathway model of SHM that was recently proposed based on mice data. However, trans-species comparison revealed differences in the role of PMS2 and MSH2 in strand targeting between mice and man. In conclusion, our results indicate a role for UNG, MSH2, MSH6, and PMS2 in the generation of SHM in humans comparable to their function in mice. However, we observed differences in strand targeting between humans and mice, emphasizing the importance of studying molecular mechanisms in a human setting. The here developed method combining NGS and ARGalaxy analysis of BCR mutation data forms the basis for efficient SHM analyses of other immune deficiencies.

Modification of Enzyme Activity by Vibrational Strong Coupling of Water.

Vibrational strong coupling (VSC) has recently emerged as a completely new tool for influencing chemical reactivity. It harnesses electromagnetic vacuum fluctuations through the creation of hybrid states of light and matter, called polaritonic states, in an optical cavity resonant to a molecular absorption band. Here, we investigate the effect of vibrational strong coupling of water on the enzymatic activity of pepsin, where a water molecule is directly involved in the enzyme's chemical mechanism. We observe an approximately 4.5-fold decrease of the apparent second-order rate constant kcat /Km when coupling the water stretching vibration, whereas no effect was detected for the strong coupling of the bending vibration. The possibility of modifying enzymatic activity by coupling water demonstrates the potential of VSC as a new tool to study biochemical reactivity.

Multi-watt, multi-octave, mid-infrared femtosecond source.

Spectroscopy in the wavelength range from 2 to 11 µm (900 to 5000 cm-1) implies a multitude of applications in fundamental physics, chemistry, as well as environmental and life sciences. The related vibrational transitions, which all infrared-active small molecules, the most common functional groups, as well as biomolecules like proteins, lipids, nucleic acids, and carbohydrates exhibit, reveal information about molecular structure and composition. However, light sources and detectors in the mid-infrared have been inferior to those in the visible or near-infrared, in terms of power, bandwidth, and sensitivity, severely limiting the performance of infrared experimental techniques. This article demonstrates the generation of femtosecond radiation with up to 5 W at 4.1 µm and 1.3 W at 8.5 µm, corresponding to an order-of-magnitude average power increase for ultrafast light sources operating at wavelengths longer than 5 µm. The presented concept is based on power-scalable near-infrared lasers emitting at a wavelength near 1 µm, which pump optical parametric amplifiers. In addition, both wavelength tunability and supercontinuum generation are reported, resulting in spectral coverage from 1.6 to 10.2 µm with power densities exceeding state-of-the-art synchrotron sources over the entire range. The flexible frequency conversion scheme is highly attractive for both up-conversion and frequency comb spectroscopy, as well as for a variety of time-domain applications.

Multi-mW, few-cycle mid-infrared continuum spanning from 500 to 2250 cm-1.

The demand for and usage of broadband coherent mid-infrared sources, such as those provided by synchrotron facilities, are growing. Since most organic molecules exhibit characteristic vibrational modes in the wavelength range between 500 and 4000 cm-1, such broadband coherent sources enable micro- or even nano-spectroscopic applications at or below the diffraction limit with a high signal-to-noise ratio1, 2, 3. These techniques have been applied in diverse fields ranging from life sciences, material analysis, and time-resolved spectroscopy. Here we demonstrate a broadband, coherent and intrinsically carrier-envelope-phase-stable source with a spectrum spanning from 500 to 2250 cm-1 (-30 dB) at an average power of 24 mW and a repetition rate of 77 MHz. This performance is enabled by the first mode-locked thin-disk oscillator operating at 2 µm wavelength, providing a tenfold increase in average power over femtosecond oscillators previously demonstrated in this wavelength range4. Multi-octave spectral coverage from this compact and power-scalable system opens up a range of time- and frequency-domain spectroscopic applications.

Efficient High-Power Ultrashort Pulse Compression in Self-Defocusing Bulk Media.

Peak and average power scalability is the key feature of advancing femtosecond laser technology. Today, near-infrared light sources are capable of providing hundreds of Watts of average power. These sources, however, scarcely deliver pulses shorter than 100 fs which are, for instance, highly beneficial for frequency conversion to the extreme ultraviolet or to the mid- infrared. Therefore, the development of power scalable pulse compression schemes is still an ongoing quest. This article presents the compression of 90 W average power, 190 fs pulses to 70 W, 30 fs. An increase in peak power from 18 MW to 60 MW is achieved. The compression scheme is based on cascaded phase-mismatched quadratic nonlinearities in BBO crystals. In addition to the experimental results, simulations are presented which compare spatially resolved spectra of pulses spectrally broadened in self-focusing and self-defocusing media, respectively. It is demonstrated that balancing self- defocusing and Gaussian beam convergence results in an efficient, power-scalable spectral broadening mechanism in bulk material.

All solid-state spectral broadening: an average and peak power scalable method for compression of ultrashort pulses.

Spectral broadening in bulk material is a simple, robust and low-cost method to extend the bandwidth of a laser source. Consequently, it enables ultrashort pulse compression. Experiments with a 38 MHz repetition rate, 50 W average power Kerr-lens mode-locked thin-disk oscillator were performed. The initially 1.2 µJ, 250 fs pulses are compressed to 43 fs by means of self-phase modulation in a single 15 mm thick quartz crystal and subsequent chirped-mirror compression. The losses due to spatial nonlinear effects are only about 40 %. A second broadening stage reduced the Fourier transform limit to 15 fs. It is shown that the intensity noise of the oscillator is preserved independent of the broadening factor. Simulations manifest the peak power scalability of the concept and show that it is applicable to a wide range of input pulse durations and energies.

Carrier-envelope-phase stabilization via dual wavelength pumping.

A power-scalable concept for carrier-envelope-phase stabilization is presented. It takes advantage of simultaneous pumping of the zero- and first-phonon absorption line of Yb:YAG at 969 and 940 nm. The concept was implemented to lock the carrier-envelope-offset frequency of a 45 W average power Kerr-lens mode-locked thin-disk oscillator. The lock performance is compared to previous experiments where carrier-envelope-stabilization was realized by means of cavity loss modulation.