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This paper presents the first demonstration of a mid-infrared (MIR) Fe:ZnSe laser gain-switched by a non-critical phase-matched potassium titanyl arsenate optical parametric oscillator and amplifier at 3.47 μm. A novel improvement in slope efficiency was achieved by this new pump source, which significantly promoted the quantum efficiency compared to the conventional pump wavelength near 2.9 μm. The slope efficiency of 70.7% is a new record for Fe:ZnSe lasers with an output energy of 86 mJ and pulse width of 6.7 ns at 10 Hz. The output wavelength was tunable from 3.9 to 4.5 μm by changing the crystal’s temperature from 80 to 300 K. The influence of the pump beam size on transverse parasitic oscillation and crystal damage was investigated considering the dynamic absorption effect in Fe:ZnSe. This unique design provides an advancing and promising method of high-energy and short-pulse-width MIR lasers for extreme applications requiring both high-energy density and high-peak-power intensity.

Characterization of an isolated attosecond pulse (IAP) in the extreme ultraviolet (XUV) or soft x-ray (SXR) region is essential for its applications. Here we propose to retrieve an IAP in the time domain directly through the modulation of high-harmonic generation (HHG) spectra in the presence of a time-delayed intense few-cycle infrared or mid-infrared laser. The retrieval algorithm is derived based on the strong-field approximation and an extended quantitative rescattering model. We show that both isolated XUV pulses with a narrow spectral bandwidth and isolated SXR pulses with a broad bandwidth can be well characterized through the HHG streaking spectra. Such an all-optical method for characterizing the IAP differs from the commonly used approach based on the streaked photoelectron spectra that would require electron spectrometers. We check the robustness of the retrieval method by changing the dressing laser or by adjusting the steps of time delay. We also show that the XUV pulse can be accurately retrieved by treating the HHG streaking spectra calculated from solving the time-dependent Schrödinger equation for single atoms as the ‘experimental’ data.

Lignin monomers have attracted attention as functional materials for various industrial uses. However, it is challenging to obtain these monomers by degrading polymerized lignin due to the rigid ether linkage between the aromatic rings. Here, we propose a novel approach based on molecular vibrational excitation using infrared free electron laser (IR-FEL) for the degradation of lignin. The IR-FEL is an accelerator-based pico-second pulse laser, and commercially available powdered lignin was irradiated by the IR-FEL under atmospheric conditions. Synchrotron-radiation infrared microspectroscopy analysis showed that the absorption intensities at 1050 cm−1, 1140 cm−1, and 3400 cm−1 were largely decreased alongside decolorization. Electrospray ionization mass chromatography analysis showed that coumaryl alcohol was more abundant and a mass peak corresponding to hydrated coniferyl alcohol was detected after irradiation at 2.9 μm (νO-H) compared to the original lignin. Interestingly, a mass peak corresponding to vanillic acid appeared after irradiation at 7.1 μm (νC=C and νC-C), which was supported by our two-dimensional nuclear magnetic resonance spectroscopy analysis. Therefore, it seems that partial depolymerization of lignin can be induced by IR-FEL irradiation in a wavelength-dependent manner.

Photothermal therapy (PTT) is a fledgling therapeutic strategy for cancer treatment with minimal invasiveness but clinical adoption has been stifled by concerns such as insufficient biodegradability of the PTT agents and lack of an efficient delivery system. Here, black phosphorus (BP) nanosheets are incorporated with a thermosensitive hydrogel [poly(d,l‐lactide)‐poly(ethylene glycol)‐poly(d,l‐lactide) (PDLLA‐PEG‐PDLLA: PLEL)] to produce a new PTT system for postoperative treatment of cancer. The BP@PLEL hydrogel exhibits excellent near infrared (NIR) photothermal performance and a rapid NIR‐induced sol–gel transition as well as good biodegradability and biocompatibility in vitro and in vivo. Based on these merits, an in vivo PTT postoperative treatment strategy is established. Under NIR irradiation, the sprayed BP@PLEL hydrogel enables rapid gelation forming a gelled membrane on wounds and offers high PTT efficacy to eliminate residual tumor tissues after tumor removal surgery. Furthermore, the good photothermal antibacterial performance prevents infection and this efficient and biodegradable PTT system is very promising in postoperative treatment of cancer. A sprayable and biodegradable photothermal therapy (PTT) system composed of a thermosensitive hydrogel incorporated with black phosphorus (BP) nanosheets is presented for post‐surgical treatment of cancer. The obtained hydrogel enables rapid gelation and offers high PTT efficacy to eliminate residual tumor after surgery. This efficient and biodegradable PTT system is very promising in the postoperative treatment of cancer.

Abstract The traditional manual analysis of microplastics has been criticized for its labor-intensive, inaccurate identification of small microplastics, and the lack of uniformity. There are already three automated analysis strategies for microplastics based on vibrational spectroscopy: laser direct infrared (LDIR)–based particle analysis, Raman-based particle analysis, and focal plane array-Fourier transform infrared (FPA-FTIR) imaging. We compared their performances in terms of quantification, detection limit, size measurement, and material identification accuracy and speed by analyzing the same standard and environmental samples. LDIR-based particle analysis provides the fastest analysis speed, but potentially questionable material identification and quantification results. The number of particles smaller than 60 μm recognized by LDIR-based particle analysis is much less than that recognized by Raman-based particle analysis. Misidentification could occur due to the narrow tuning range from 1800 to 975 cm−1 and dispersive artifact distortion of infrared spectra collected in reflection mode. Raman-based particle analysis has a submicrometer detection limit but should be cautiously used in the automated analysis of microplastics in environmental samples because of the strong fluorescence interference. FPA-FTIR imaging provides relatively reliable quantification and material identification for microplastics in environmental samples greater than 20 μm but might provide an imprecise description of the particle shapes. Optical photothermal infrared (O-PTIR) spectroscopy can detect submicron-sized environmental microplastics (0.5–5 μm) intermingled with a substantial amount of biological matrix; the resulting spectra are searchable in infrared databases without the influence of fluorescence interference, but the process would need to be fully automated.

A high-throughput approach to detecting, quantifying, and characterizing microplastics (MPs) by shape, size, and polymer type using laser direct infrared (LDIR) spectroscopy in surface water samples is demonstrated. Three urban creeks were sampled for their MP content near Cincinnati, OH. A simple Fenton reaction was used to oxidize the surface water samples, and the water samples were filtered onto a gold-coated polyester membrane. Infrared (IR) analysis for polymer identification was conducted, with recoveries of 88.3% ± 1.2%. This method was able to quantify MPs down to a diameter of 20 µm, a size comparable to that of MPs quantified by other techniques such as Fourier transform infrared spectroscopy (FTIR) and Raman spectroscopy. A shape-classifying algorithm was designed using the aspect ratio values of particles to categorize MPs as fibers, fibrous fragments, fragments, spherical fragments, or spheres. Cut-off values were identified from measurements of known sphere, fragment, and fibrous particles. About half of all environmental samples were classified as fragments while the other shapes accounted for the other half. A cut-off hit quality index (HQI) value of 0.7 was used to classify known and unidentified particles based on spectral matches to a reference library. Center for Marine Debris Research Polymer Kit 1.0 standards were analyzed by LDIR and compared to the given FTIR spectra by HQI, showing that LDIR obtains similar identifications as FTIR analysis. The simplicity and automation of the LDIR allows for quick, reproducible particle analysis, making LDIR attractive for high-throughput analysis of MPs.

Amyloidosis is known to be caused by the deposition of amyloid fibrils into various biological tissues; effective treatments for the disease are little established today. An infrared free‐electron laser (IR‐FEL) is an accelerator‐based picosecond‐pulse laser having tunable infrared wavelengths. In the current study, the irradiation effect of an IR‐FEL was tested on an 11‐residue peptide (NFLNCYVSGFH) fibril from β2‐microglobulin (β2M) with the aim of applying IR‐FELs to amyloidosis therapy. Infrared microspectroscopy (IRM) and scanning electron microscopy showed that a fibril of β2M peptide was clearly dissociated by IR‐FEL at 6.1 µm (amide I) accompanied by a decrease of the β‐sheet and an increase of the α‐helix. No dissociative process was recognized at 6.5 µm (amide II) as well as at 5.0 µm (non‐specific wavelength). Equilibrium molecular dynamics simulations indicated that the α‐helix can exist stably and the probability of forming interchain hydrogen bonds associated with the internal asparagine residue (N4) is notably reduced compared with other amino acids after the β‐sheet is dissociated by amide I specific irradiation. This result implies that N4 plays a key role for recombination of hydrogen bonds in the dissociation of the β2M fibril. In addition, the β‐sheet was disrupted at temperatures higher than 340 K while the α‐helix did not appear even though the fibril was heated up to 363 K as revealed by IRM. The current study gives solid evidence for the laser‐mediated conversion from β‐sheet to α‐helix in amyloid fibrils at the molecular level. An infrared free‐electron laser was applied to dissociate amyloid fibrils of a peptide as a goal of the development of a novel therapeutic strategy for amyloidosis. Solid evidence for β‐sheet to α‐helix conversion in the peptide fibril by vibrational excitation of amide bonds was obtained by both experiment and molecular dynamics simulation.

A nanosecond infrared laser (NIRL) was investigated in cutting dental roots. The focus of the investigation was defining the preparation accuracy and registration of thermal effects during laser application. Ten teeth were processed in the root area using a NIRL in several horizontal, parallel incisions to achieve tooth root ablation as in an apicoectomy. Temperature change was monitored during ablation and the quality of the cutting edges in the roots were studied by means of micro-CT, optical coherence tomography, and histology of decalcified and undecalcified specimens. NIRL produced clearly defined cut surfaces in dental hard tissues. The automated guidance of the laser beam created regular, narrow dentin defects that tapered in a V-shape towards the ablation plane. A biologically significant increase in the temperature of the object and its surroundings did not occur during the laser application. Thermal dentin damage was not detected in histological preparations of treated teeth. Defined areas of the tooth root may be ablated using a NIRL. For clinical translation of NIRL in apicoectomy, it would be necessary to increase energy delivered to hard tissue and develop beam application facilitating beam steering for oral treatment.

By employing a graded-interfaces model based on a generalized formalism for interface-roughness (IFR) scattering that was modified for mid-infrared emitting quantum cascade lasers (QCLs), we have accurately reproduced the electro-optical characteristics of published record-performance 4.9 µm- and 8.3 µm-emitting QCLs. The IFR-scattering parameters at various interfaces were obtained from measured values and trends found via atom-probe tomography analysis of one of our 4.6 μm-emitting QCL structures with variable barrier heights. Those values and trends, when used for designing a graded-interface, 4.6 μm-emitting QCL, led to experimental device characteristics in very good agreement with calculated ones. We find that the published record-high performance values are mainly due to both injection from a prior-stage low-energy (active-region) state into the upper-laser ( ) level, thus at low field-strength values, as well as to strong photon-induced carrier transport. However, the normalized leakage-current density is found to be quite high: 26–28 % and 23.3 %, respectively, mainly because of IFR-triggered shunt-type leakage through high-energy active-region states, in the presence of high average electron temperatures in the laser level and an energy state adjacent to it: 1060 K and 466 K for 4.9 µm- and 8.3 µm-emitting QCLs, respectively. Then, modeling with graded interfaces becomes a tool for designing devices of performances superior to the best reported to date, thus closing in on fundamental limits. The model is employed to design a graded-interface 8.1 µm-emitting QCL with suppressed carrier leakage via conduction-band engineering, which reaches a maximum front-facet wall-plug efficiency value of 22.2 %, significantly higher than the current record (17 %); thus, a value close to the fundamental front-facet, upper limit (i.e., 25 %) for ∼8 µm-emitting QCLs.