Limits of the detection of microplastics in fish tissue using stimulated Raman scattering microscopy.

We demonstrate the detection sensitivity of microplastic beads within fish tissue using stimulated Raman scattering (SRS) microscopy. The intrinsically provided chemical contrast distinguishes different types of plastic compounds within fish tissue. We study the size-dependent signal-to-noise ratio of the microplastic beads and determine a lower boundary for the detectable size. Our findings demonstrate how SRS microscopy can serve as a complementary modality to conventional Raman scattering imaging in order to detect and identify microplastic particles in fish tissue.

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.

3D stimulated Raman spectral imaging of water dynamics associated with pectin-glycocalyceal entanglement.

Pectin is a heteropolysaccharide responsible for the structural integrity of the cell walls of terrestrial plants. When applied to the surface of mammalian visceral organs, pectin films form a strong physical bond with the surface glycocalyx. A potential mechanism of pectin adhesion to the glycocalyx is the water-dependent entanglement of pectin polysaccharide chains with the glycocalyx. A better understanding of such fundamental mechanisms regarding the water transport dynamics in pectin hydrogels is of importance for medical applications, e.g., surgical wound sealing. We report on the water transport dynamics in hydrating glass-phase pectin films with particular emphasis on the water content at the pectin-glycocalyceal interface. We used label-free 3D stimulated Raman scattering (SRS) spectral imaging to provide insights into the pectin-tissue adhesive interface without the confounding effects of sample fixation, dehydration, shrinkage, or staining.

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.

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.

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.

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.

Electrically switchable metallic polymer nanoantennas.

Electrical switching of a metal-to-insulator transition would provide a building block for integrated electro-optically active plasmonics. In this work, we realize plasmonic nanoantennas from metallic polymers, which show well-pronounced localized plasmon resonances in their metallic state. As a result of the electrochemically driven optical metal-to-insulator transition of the polymer, the plasmonic resonances can be electrically switched fully off and back on at video-rate frequencies of up to 30 hertz by applying alternating voltages of only ±1 volt. With the use of this concept, we demonstrate electrically switchable beam-steering metasurfaces with a 100% contrast ratio in transmission. Our approach will help to realize ultrahigh efficiency plasmonic-based integrated active optical devices, including high-resolution augmented and virtual reality technologies.

High density molecular jets of complex neutral organic molecules with Tesla valves.

Supersonic jets of gas-phase atoms and small molecules have enabled a variety of ultrafast and ultracold chemical studies. However, extension to larger, more complex neutral molecules proves challenging for two reasons: (i) Complex molecules, such as cis-stilbene, exist in a liquid or solid phase at room temperature and ambient pressure and (ii) a unidirectional flow of high-density gaseous beams of such molecules to the interaction region is required. No delivery system currently exists that can deliver dense enough molecular jets of neutral complex molecules without ionizing or exciting the target for use in gas-phase structural dynamics studies. Here, we present a novel delivery system utilizing Tesla valves, which generates more than an order-of-magnitude denser gaseous beam of molecules compared to a bubbler without Tesla valves at the interaction region by ensuring a fast unidirectional flow of the gaseous sample. We present combined experimental and flow simulations of the Tesla valve setup. Our results open new possibilities of studying large complex neutral molecules in the gas-phase with low vapor pressures in future ultrafast and ultracold studies.

Access to 1'-Amino Carbocyclic Phosphoramidite to Enable Postsynthetic Functionalization of Oligonucleotides.

We report a synthesis of a carbocyclic, abasic RNA phosphoramidite decorated with an amino functionality. The building block was efficiently incorporated into an RNA oligonucleotide in a site-specific manner, followed by deprotection to a free amino group. The amino moiety could be further derivatized as exemplified with fluorescein N-hydroxysuccinimide ester. Hence, this convertible building block may provide access to a variety of RNA oligonucleotides via postsynthetic amino group functionalization. In particular, providing a vector toward nucleobase replacements.

Tunable s-SNOM for Nanoscale Infrared Optical Measurement of Electronic Properties of Bilayer Graphene.

Here we directly probe the electronic properties of bilayer graphene using s-SNOM measurements with a broadly tunable laser source over the energy range from 0.3 to 0.54 eV. We tune an OPO/OPA system around the interband resonance of Bernal stacked bilayer graphene (BLG) and extract amplitude and phase of the scattered light. This enables us to retrieve and reconstruct the complex optical conductivity resonance in BLG around 0.39 eV with nanoscale resolution. Our technique opens the door toward nanoscopic noncontact measurements of the electronic properties in complex hybrid 2D and van der Waals material systems, where scanning tunneling spectroscopy cannot access the decisive layers.

Serum Myo-Inositol, Dimethyl Sulfone, and Valine in Combination with Creatinine Allow Accurate Assessment of Renal Insufficiency-A Proof of Concept.

Evaluation of renal dysfunction includes estimation of glomerular filtration rate (eGFR) as the initial step and subsequent laboratory testing. We hypothesized that combined analysis of serum creatinine, myo-inositol, dimethyl sulfone, and valine would allow both assessment of renal dysfunction and precise GFR estimation. Bio-banked sera were analyzed using nuclear magnetic resonance spectroscopy (NMR). The metabolites were combined into a metabolite constellation (GFRNMR) using n = 95 training samples and tested in n = 189 independent samples. Tracer-measured GFR (mGFR) served as a reference. GFRNMR was compared to eGFR based on serum creatinine (eGFRCrea and eGFREKFC), cystatin C (eGFRCys-C), and their combination (eGFRCrea-Cys-C) when available. The renal biomarkers provided insights into individual renal and metabolic dysfunction profiles in selected mGFR-matched patients with otherwise homogenous clinical etiology. GFRNMR correlated better with mGFR (Pearson correlation coefficient r = 0.84 vs. 0.79 and 0.80). Overall percentages of eGFR values within 30% of mGFR for GFRNMR matched or exceeded those for eGFRCrea and eGFREKFC (81% vs. 64% and 74%), eGFRCys-C (81% vs. 72%), and eGFRCrea-Cys-C (81% vs. 81%). GFRNMR was independent of patients' age and sex. The metabolite-based NMR approach combined metabolic characterization of renal dysfunction with precise GFR estimation in pediatric and adult patients in a single analytical step.

Machine learning for laser-induced electron diffraction imaging of molecular structures.

Ultrafast diffraction imaging is a powerful tool to retrieve the geometric structure of gas-phase molecules with combined picometre spatial and attosecond temporal resolution. However, structural retrieval becomes progressively difficult with increasing structural complexity, given that a global extremum must be found in a multi-dimensional solution space. Worse, pre-calculating many thousands of molecular configurations for all orientations becomes simply intractable. As a remedy, here, we propose a machine learning algorithm with a convolutional neural network which can be trained with a limited set of molecular configurations. We demonstrate structural retrieval of a complex and large molecule, Fenchone (C10H16O), from laser-induced electron diffraction (LIED) data without fitting algorithms or ab initio calculations. Retrieval of such a large molecular structure is not possible with other variants of LIED or ultrafast electron diffraction. Combining electron diffraction with machine learning presents new opportunities to image complex and larger molecules in static and time-resolved studies.

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.

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.

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.

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.

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.

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.