High-harmonic spectroscopy of quantum phase transitions in a high-Tc superconductor.

We report on the nonlinear optical signatures of quantum phase transitions in the high-temperature superconductor YBCO, observed through high harmonic generation. While the linear optical response of the material is largely unchanged when cooling across the phase transitions, the nonlinear optical response sensitively imprints two critical points, one at the critical temperature of the cuprate with the exponential growth of the surface harmonic yield in the superconducting phase and another critical point, which marks the transition from strange metal to pseudogap phase. To reveal the underlying microscopic quantum dynamics, a strong-field quasi-Hubbard model was developed, which describes the measured optical response dependent on the formation of Cooper pairs. Further, the theory provides insight into the carrier scattering dynamics and allows us to differentiate between the superconducting, pseudogap, and strange metal phases. The direct connection between nonlinear optical response and microscopic dynamics provides a powerful methodology to study quantum phase transitions in correlated materials. Further implications are light wave control over intricate quantum phases, light-matter hybrids, and application for optical quantum computing.

Spectrally resolved ultrafast transient dynamics of a femtosecond fiber-feedback optical parametric oscillator.

We report on spectrotemporal transient dynamics in a femtosecond fiber-feedback optical parametric oscillator (FFOPO) system. Burst modulation of the pump beam in combination with dispersive Fourier transformation sampling allows to record single-pulse signal spectra at 41 MHz sampling rate. Therefore, each individual pulse of the signal transients can be spectrally resolved. We characterize the signal output behavior for anomalous as well as for normal intra-cavity dispersion. Amongst steady state output we observed period-doubling cycles and other attractors, which occured at higher intra-cavity nonlinearity levels. The experimental findings are supported by numerical simulations, in order to identify the linear and nonlinear effects, which govern the wavelength tuning behavior of this FFOPO system. We find that steady state operation is preferred and that the wavelength tuning stability of the FFOPO dramatically increases when using a normal dispersion feedback fiber.

Hybrid fiber-solid-state laser with 3D-printed intracavity lenses.

Microscale 3D-printing has revolutionized micro-optical applications ranging from endoscopy, imaging, to quantum technologies. In all these applications, miniaturization is key, and in combination with the nearly unlimited design space, it is opening novel, to the best of our knowledge, avenues. Here, we push the limits of miniaturization and durability by realizing the first fiber laser system with intra-cavity on-fiber 3D-printed optics. We demonstrate stable laser operation at over 20 mW output power at 1063.4 nm with a full width half maximum (FWHM) bandwidth of 0.11 nm and a maximum output power of 37 mW. Furthermore, we investigate the power stability and degradation of 3D-printed optics at Watt power levels. The intriguing possibilities afforded by free-form microscale 3D-printed optics allow us to combine the gain in a solid-state crystal with fiber guidance in a hybrid laser concept. Therefore, our novel ansatz enables the compact integration of a bulk active media in fiber platforms at substantial power levels.

Femtosecond tunable light source with variable repetition rate between 640 kHz and 41†MHz with a 130†dB temporal pulse contrast ratio.

We demonstrate a femtosecond tunable light source with a variable pulse repetition rate based on a synchronously pumped fiber-feedback optical parametric oscillator (FFOPO) that incorporates an extended-cavity design. The repetition rate can be reduced by an acousto-optical modulator in the FFOPO pump beam. The extended FFOPO cavity supports signal oscillation down to the 64th subharmonic. The high nonlinearity of the FFOPO threshold suppresses signal output for residual pump pulses that are transmitted by the pulse picker. We characterize the temporal pulse contrast ratio of the FFOPO signal output with a second-order cross-correlation measurement. This FFOPO system enables pulse picking with extraordinarily high values up to 111 dB suppression of adjacent pulses and exhibits a temporal contrast ratio that exceeds 130 dB. It generates fs-pulses with tunable wavelength from 1415-1750 nm and 2.5-3.8 µm and variable repetition rates ranging from 640 kHz to 41 MHz.

Sub-40 fs optical parametric oscillator beyond the gain bandwidth limit.

We report a compact and passively stable optical parametric oscillator for direct generation of sub-40 fs pulses, five times shorter than the 200 fs pump oscillator. By employing an intracavity all normal dispersion feedback fiber, we achieved low-noise and coherent broadening beyond the parametric gain bandwidth limitation. We demonstrate spectral coverage from 1.1 to 2.0 µm with excellent passive power and spectral stability below 0.1% rms and a footprint smaller than 14 × 14 cm2.

Burst-mode femtosecond fiber-feedback optical parametric oscillator.

In multiphoton 3D direct laser writing and stimulated Raman scattering applications, rapid and arbitrary pulse modulation with an extremely high contrast ratio would be very beneficial. Here, we demonstrate a femtosecond fiber-feedback optical parametric oscillator (FFOPO) system in combination with pulse picking in the pump beam. This allows tunable signal output at variable burst rates from DC all the way up to 5 MHz. Furthermore, arbitrary pulse sequences can be generated. The rapid signal buildup dynamics provide individual full-power pulses with only two prepulses. This is possible without the requirement for additional injection seeding. Hereby, the intrinsically high intra-cavity losses of the FFOPO system are found to beneficial, as they enable rapid off-switching of the output as signal ring-down is efficiently suppressed. Possible applications are the reduction of the average power while maintaining a high peak power level, as well as tunable arbitrary pulse sequence generation.

Imaging the Renner-Teller effect using laser-induced electron diffraction.

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS2) in the [Formula: see text] excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS2 molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the [Formula: see text] excited state in neutral CS2, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS2, which is known to appear as a two-center scatterer.

Compact harmonic cavity optical parametric oscillator for optical parametric amplifier seeding.

We present a broadly tunable highly efficient frequency conversion scheme, based on a low-threshold harmonic cavity optical parametric oscillator (OPO) followed by an idler-seeded power amplifier. By choosing the cavity length of the OPO equal to the 10th harmonic of its 41 MHz Yb:KGW solid-state pump laser, a very compact optical setup is achieved. A singly-resonant cavity without output coupler results in a low oscillation threshold of only 28-100 mW in the entire signal tuning range of 1.37-1.8 µm. The 2.4-4.15 µm idler radiation is coupled out at the 41 MHz pump frequency and employed to seed a post amplifier with nearly Watt-level output power. In addition, the seeder plus power amplifier concept results in clean signal and idler pulses at the fundamental repetition rate of 41 MHz with a time-bandwidth product below 0.4 and a relative intensity noise 10 dB lower compared to the solid-state pump laser.

Alignment-free difference frequency light source tunable from 5 to 20†µm by mixing two independently tunable OPOs.

Tunable mid-infrared ultrashort lasers have become an essential tool in vibrational spectroscopy in recent years. They enabled and pushed a variety of spectroscopic applications due to their high brilliance, beam quality, low noise, and accessible wavelength range up to 20 µm. Many state-of-the-art devices apply difference frequency generation (DFG) to reach the mid-infrared spectral region. Here, birefringent phase-matching is typically employed, resulting in a significant crystal rotation during wavelength tuning. This causes a beam offset, which needs to be compensated to maintain stable beam pointing. This is crucial for any application. In this work, we present a DFG concept, which avoids crystal rotation and eliminates beam pointing variations over a broad wavelength range. It is based on two independently tunable input beams, provided by synchronously pumped parametric seeding units. We compare our concept to the more common DFG approach of mixing the signal and idler beams from a single optical parametric amplifier (OPA) or oscillator (OPO). In comparison, our concept enhances the photon efficiency of wavelengths exceeding 11 µm more than a factor of 10 and we still achieve milliwatts of output power up to 20 µm. This concept enhances DFG setups for beam-pointing-sensitive spectroscopic applications and can enable research at the border between the mid- and far-IR range due to its highly efficient performance.

Few-cycle mid-infrared pulses from BaGa2GeSe6.

BaGa2GeSe6 (BGGSe) is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold. A numerical study shows the material's capacity for octave-spanning mid-infrared pulse generation up to 18 µm. In a first experiment, we show that a long crystal length of 2.6 mm yields a pulse energy of 21 pJ at 100 MHz with a spectral bandwidth covering 5.8 to 8.5 µm. The electric field of the carrier-envelope-phase stable pulse is directly measured with electro-optical sampling and reveals a pulse duration of 91 fs, which corresponds to sub-four optical cycles, thus confirming some of the prospects of the material for ultrashort pulse generation and mid-infrared spectroscopy.

Coherently broadened, high-repetition-rate laser for stimulated Raman scattering-spectroscopic optical coherence tomography.

We present a novel light source specifically tailored for stimulated Raman scattering-spectroscopic optical coherence tomography (SRS-SOCT), which is, to the best of our knowledge, a novel molecular imaging method that combines the molecular sensitivity of SRS with the spatial and spectral multiplexing capabilities of SOCT. The novel laser consists of an 8 W, 450 fs Yb:KGW oscillator, with a repetition rate of 40 MHz, which delivers the Stokes beam for SRS-SOCT and also pumps and amplifies an optical parametric oscillator (OPO). The output of the amplified OPO is then frequency doubled and coherently broadened using a custom-made tapered fiber that generates bandwidth pulses >40 nm, compressible to <50 fs, with the average power over 150 mW, near the shot-noise limit above 250 kHz. The broadened and compressed pulse simultaneously serves as the pump beam and SOCT light source for SRS-SOCT. This light source is assessed for SRS-SOCT, and its implications for other imaging methods are discussed.

Imaging an isolated water molecule using a single electron wave packet.

Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of H2O+ with picometer and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched H2O+ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O-H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of H2O+ is altered in the presence of an external field.

Nanoscale Hydrogenography on Single Magnesium Nanoparticles.

Active plasmonics is enabling novel devices such as switchable metasurfaces for active beam steering or dynamic holography. Magnesium with its particle plasmon resonances in the visible spectral range is an ideal material for this technology. Upon hydrogenation, metallic magnesium switches reversibly into dielectric magnesium hydride (MgH2), turning the plasmonic resonances off and on. However, up until now, it has been unknown how exactly the hydrogenation process progresses in the individual plasmonic nanoparticles. Here, we introduce a new method, namely nanoscale hydrogenography, that combines near-field scattering microscopy, atomic force microscopy, and single-particle far-field spectroscopy to visualize the hydrogen absorption process in single Mg nanodisks. Using this method, we reveal that hydrogen progresses along individual single-crystalline nanocrystallites within the nanostructure. We are able to monitor the spatially resolved forward and backward switching of the phase transitions of several individual nanoparticles, demonstrating differences and similarities of that process. Our method lays the foundations for gaining a better understanding of hydrogen diffusion in metal nanoparticles and for improving future active nano-optical switching devices.

Narrowband cw injection seeded high power femtosecond double-pass optical parametric generator at 43 MHz: Gain and noise dynamics.

We demonstrate narrowband cw injection seeding of a femtosecond double-pass optical parametric generator at 43 MHz repetition rate with a simple, low power external cavity diode laser. Up to 2.5 W of near-IR radiation (1.5 - 1.66 µm) as well as 800 mW of tunable mid-IR radiation (2.75 - 3.15 µm) with pulse durations below 300 fs are generated with a remarkable pulse-to-pulse and long term power stability. Compared to conventional, vacuum noise seeded optical parametric generators, the presented frequency conversion scheme does not only exhibit superior gain and noise dynamics, but also a high degree of flexibility upon control parameters such as pump power, seed power, or spectral position of the seed.

Low drift cw-seeded high-repetition-rate optical parametric amplifier for fingerprint coherent Raman spectroscopy.

We introduce a broadly tunable robust source for fingerprint (170 - 1620 cm-1) Raman spectroscopy. A cw thulium-doped fiber laser seeds an optical parametric amplifier, which is pumped by a 7-W, 450-fs Yb:KGW bulk mode-locked oscillator with 41 MHz repetition rate. The output radiation is frequency doubled in a MgO:PPLN crystal and generates 0.7 - 1.3-ps-long narrowband pump pulses that are tunable between 885 and 1015 nm with >80 mW average power. The Stokes beam is delivered by a part of the oscillator output, which is sent through an etalon to create pulses with 1.7 ps duration. We demonstrate a stimulated Raman gain measurement of toluene in the fingerprint spectral range. The cw seeding intrinsically ensures low spectral drift.

Ultra-stable high average power femtosecond laser system tunable from 1.33 to 20 µm.

A highly stable 350 fs laser system with a gap-free tunability from 1.33 to 2.0 µm and 2.13 to 20 µm is demonstrated. Nanojoule-level pulse energy is achieved in the mid-infrared at a 43 MHz repetition rate. The system utilizes a post-amplified fiber-feedback optical parametric oscillator followed by difference frequency generation between the signal and idler. No locking or synchronization electronics are required to achieve outstanding free-running output power and spectral stability of the whole system. Ultra-low intensity noise, close to the pump laser's noise figure, enables shot-noise limited measurements.

Multi-Watt femtosecond optical parametric master oscillator power amplifier at 43 MHz.

We present a high repetition rate mid-infrared optical parametric master oscillator power amplifier (MOPA) scheme, which is tunable from 1370 to 4120nm. Up to 4.3W average output power are generated at 1370nm, corresponding to a photon conversion efficiency of 78%. Bandwidths of 6 to 12nm with pulse durations between 250 and 400fs have been measured. Strong conversion saturation over the whole signal range is observed, resulting in excellent power stability. The system consists of a fiber-feedback optical parametric oscillator that seeds an optical parametric power amplifier. Both systems are pumped by the same Yb:KGW femtosecond oscillator.

High-power mid-infrared high repetition-rate supercontinuum source based on a chalcogenide step-index fiber.

We demonstrate a tunable and robust femtosecond supercontinuum source with a maximum output power of 550 mW and a maximum spectral width of up to 2.0 µm, which can cover the mid-infrared region from 2.3 µm up to 4.9 µm by tuning the pump wavelength. As2S3 chalcogenide step-index fibers with core diameters of 7 and 9 µm are pumped at different wavelengths from 2.5 µm up to 4.1 µm with femtosecond pulses by means of a post-amplified optical parametric oscillator pumped by an Yb:KGW laser. The spectral behavior of the supercontinuum is investigated by changing the pump wavelength, core diameter, fiber length, and pump power. Self-phase modulation is identified as the main broadening mechanism in the normal dispersion regime. This source promises to be an excellent laboratory tool for infrared spectroscopy owing to its high brilliance as demonstrated for the CS2-absorption bands around 3.5 µm.

Compact, low-noise, all-solid-state laser system for stimulated Raman scattering microscopy.

We present a highly stable and compact laser source for stimulated Raman scattering (SRS) microscopy. cw-seeding of an optical parametric amplifier pumped by a bulk femtosecond Yb-oscillator and self-phase modulation in a tapered fiber allow for broad tunability without any optical or electronic synchronization. The source features noise levels of the Stokes beam close to the shot-noise limit at MHz modulation frequencies. We demonstrate the superior performance of our system by SRS imaging of micrometer-sized polymer beads.

Watt-level optical parametric amplifier at 42 MHz tunable from 1.35 to 4.5 µm coherently seeded with solitons.

We report on an optical parametric amplifier at high repetition rate of 41.7 MHz seeded by an optical soliton from a tapered fiber. Gap-free signal tuning from 1.35 µm to 1.95 µm with corresponding idler wavelengths from 2.2 µm to 4.5 µm is demonstrated. The system provides up to 1.8 W average power at 1.4 µm, more than 1.1 W up to 1.7 µm, and more than 400 mW up to 4.0 µm with a signal pulse duration of 200 to 300 fs. It is directly pumped by a solid-state oscillator providing up to 7.4 W at 1.04 µm wavelength with 425 fs pulse duration. Soliton-seeding is shown to lead to excellent pulse-to-pulse stability, but it introduces a timing-jitter on the millisecond timescale. Using a two-stage concept the timing-jitter is efficiently suppressed due to the passive synchronization of both conversion stages.