Optical Parametric Oscillator Laser Research Articles

Nanofabrication of Lithium Niobate Anti‐Reflective Subwavelength Structures for High Power Mid‐Infrared Lasers

AbstractLithium niobate (LN) crystal with anti‐reflective subwavelength structures (ASSs) has great applications in high‐power tunable optical parametric oscillator (OPO) lasers. However, it is still a great challenge to 3D nanofabrication of LN ASSs. Herein, a wet‐etching‐assisted laser polarization domain inversion (WE‐LPDI) technology is proposed to fabricate periodic cone arrays with a period from 200 nm to 4 µm on LN. Based on the optimized structural parameters, large‐area LN ASSs with a period of 1.3 µm and a height of 1.7 µm were fabricated on LN, which exhibits an average transmittance of 3–5 µm increasing from 78% to 85% and a highest transmittance of 88% at 5 µm. It has been demonstrated that the LN ASSs show high stability under high‐temperature and high‐power laser irradiation, which shows potential applications for high‐power mid‐IR lasers. The results indicate that the WE‐LPDI technology provides a novel way for 3D nanofabrication of LN.

Thin flexible photoacoustic endoscopic probe with a distal-driven micro-step motor for pump-probe-based high-specific molecular imaging.

Conventional photoacoustic endoscopy (PAE) is mostly for structural imaging, and its molecular imaging ability is quite limited. In this work, we address this issue and present the development of a flexible acoustic-resolution-based photoacoustic endoscopic (AR-PAE) probe with an outer diameter of 8 mm. This probe is driven by a micro-step motor at the distal end, enabling flexible and precise angular step control to synchronize with the optical parametric oscillator (OPO) lasers. This probe retains the high spatial resolution, high penetration depth, and spectroscopic imaging ability of conventional AR-PAE. Moreover, it is capable for background-free high-specific photoacoustic molecular imaging with a novel pump-probe detection technique, as demonstrated by the distribution visualizing of the FDA approved contrast agent methylene blue (MB) in an ex-vivo pig ileum. This proposed method represents an important technical advancement in multimodal PAE, and can potentially make considerable contributions across various biomedical fields.

Resonant Laser Induced Breakdown Spectroscopy for quantitative elemental depth profile analysis of WTa coating

This work reports on the procedure of Resonant-LIBS, in which ablation and subsequent excitation is achieved by fine-tuning an Optical Parametric Oscillator (OPO) laser to the resonant transition of tungsten (W I) at 255.14 nm and analyzing the optical emission spectroscopy results. Compared to conventional LIBS, the ablation rate is significantly reduced in the resonant regime, resulting in finer resolution of depth profiles. This reduction in ablation rate can be attributed to a process called Resonance Laser Ablation (RLA) where a part of the laser energy is employed for ablation, while the rest is dedicated to resonant excitation. The sample under consideration is a WTa-coated (7μm) Mo substrate prepared by a dual magnetron sputtering system. These efforts are motivated by the need for improvement in quantitative depth analysis of W-based Plasma-Facing Components (PFC). Particularly to target the undesirable surface modifications due to the interaction with H isotopes in fusion plasma, such as fuel retention or erosion/deposition.

A Low-Cost Test Method for Accurate Detection of Different Excited-State Species with a Lifetime Span over 5 Orders of Magnitude in One Time Window

Accurate quantification on the quantum yields (φ) of both the prompt fluorescence (PF) and the delayed fluorescence (DF) species is quite essential for the clarification of molecular design rationales for thermally activated delayed fluorescence (TADF) luminogens. Currently, most φPF and φDF data of TADF fluorophores were acquired through time-correlated single-photon counting (TCSPC) lifetime measurement systems. However, because of their equal-time-channel working manner, so far all the commercially available TCSPC systems cannot render accurate measurement on φPF of TADF materials due to the lack of enough valid data points in the faster decay region of the corresponding photoluminescence (PL) decay curves. Although an intensified charge coupled device (ICCD) system equipped with a streak camera or an optical parametric oscillation laser has been proven to be a powerful tool for accurate determination of φPF and φDF of TADF fluorophores, the ultrahigh cost of these ICCD systems makes them inaccessible to most users. Herein, by replacing the timing module of a commercial TCSPC system with a low-cost and versatile time-to-digital converter (TDC) module, we developed a modified TCSPC system that can work in an unequal-time-channel manner. The resultant TDC-TCSPC system can not only concurrently determine the accurate lifetime of PF and DF species whose lifetime span even exceeds 5 orders of magnitude in just one time window but also render accurate measurements on φPF and φDF of TADF fluorophores. The reliability of the TDC-TCSPC method was verified through TCSPC- and ICCD-based comparative experiments on ACMPS, a known TADF fluorophore. Our results not only can provide a low-cost and convenient test method for accurate determination of key experimental data of TADF materials but also will facilitate deeper understanding of the molecular design principles for high-performance TADF materials.

Wavelength-Tuning of Nanosecond Pulses in Er-Doped Fluoride Fibre Amplifier

We investigate the gain bandwidth and wavelength-tuning range of an erbium-doped fluoride fibre amplifier. The presented experimental setup consisted of a widely wavelength-tunable optical parametric oscillator (OPO), which was amplified in a single-stage Er-doped fluoride fibre amplifier. The OPO laser provided seed pulses with a pulse width of 5.2 ns and a repetition rate of 10 kHz. The fibre section consisted of 2.2 m of double-clad, single-mode fibre with a doping concentration of 7 mol%. Wavelength-tuning was analysed at gain values of up to 26 dB and amplified pulse energies of up to 37.4 <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"><tex-math notation="LaTeX">$\mu \mathrm{J}$</tex-math></inline-formula> . Using this setup, we demonstrate continuous wavelength tuning of more than 100 nm, covering the wavelength range from 2712 nm to 2818 nm.

Measurement of dynamic atomic polarizabilities of Al at 19 wavelengths from 420 nm to 680 nm in electrical exploding wire experiments.

The dynamic polarizabilities of Al atom at 19 wavelengths from 420 nm to 680 nm are measured experimentally for the first time. A 15 µm diameter Al wire is heated to the gas/ microdrop stage using a 3 kA, 25 ns pulsed current, and the energy deposition when the resistive voltage reaches its peak is 4.7 eV·atom-1, which is higher than the atomization enthalpy of Al but much lower than its first ionization potential. Two laser interferometric images of the Al gas are obtained simultaneously using a 532 nm laser and an optical parametric oscillator laser. Then an integrated phase method is used to reconstruct the Al atomic linear density distribution based on the known atomic polarizability at 532 nm, which acts as a bridge between the two interferograms to obtain the relative atomic polarizability value at a specific wavelength with respect to the value at 532 nm. The measured dynamic polarizability of Al atom decreases from 13.5×10-24 cm3 to 9.4×10-24 cm3 as the wavelength increases from 420 nm to 680 nm with a measurement error of approximately ±10%. The experimental result fits well with an uncoupled Hartree-Fock approximation, and the reconstructed static polarizability of 8.13 ± 0.79×10-24 cm3 is well matched with reference measurement results.

Tropospheric NO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; measurements using a three-wavelength optical parametric oscillator differential absorption lidar

Abstract. The conventional two-wavelength differential absorption lidar (DIAL) has measured air pollutants such as nitrogen dioxide (NO2). However, high concentrations of aerosol within the planetary boundary layer (PBL) can cause significant retrieval errors using only a two-wavelength DIAL technique to measure NO2. We proposed a new technique to obtain more accurate measurements of NO2 using a three-wavelength DIAL technique based on an optical parametric oscillator (OPO) laser. This study derives the three-wavelength DIAL retrieval equations necessary to retrieve vertical profiles of NO2 in the troposphere. Additionally, two rules to obtain the optimum choice of the three wavelengths applied in the retrieval are designed to help increase the differences in the NO2 absorption cross-sections and reduce aerosol interference. NO2 retrieval relative uncertainties caused by aerosol extinction, molecular extinction, absorption of gases other than the gas of interest and backscattering are calculated using two-wavelength DIAL (438 and 439.5 nm) and three-wavelength DIAL (438, 439.5 and 441 nm) techniques. The retrieval uncertainties in aerosol extinction using the three-wavelength DIAL technique are reduced to less than 2 % of those when using the two-wavelength DIAL technique. Moreover, the retrieval uncertainty analysis indicates that the three-wavelength DIAL technique can reduce more fluctuation caused by aerosol backscattering than the two-wavelength DIAL technique. This study presents NO2 concentration profiles which were obtained using the HU (Hampton University) three-wavelength OPO DIAL. As a first step to assess the accuracy of the HU lidar NO2 profiles, we compared the NO2 profiles to simulated data from the Weather Research and Forecasting Chemistry (WRF-Chem) model. This comparison suggests that the NO2 profiles retrieved with the three-wavelength DIAL technique have similar vertical structure and magnitudes typically within ±0.1 ppb compared to modeled profiles.

Optical Parametric Oscillation with Ultra-Low Power Threshold in a Dimer of Active-Passive Cavities

Optical parametric oscillation can convert the input laser into a couple of coherent optical output with signal and idler frequencies. It is an important method for the realization of the broadband middle infrared tunable lasers. The optical parametric oscillation process depends on the ultra-fast non-linear response of matter to light with a certain pump power. Therefore, reducing the pump threshold of the optical parametric oscillation process and improving the energy conversion efficiency are of great significance to the study of non-linear optics. In this paper, we construct a dimer system that couples a passive non-linear resonator to an active resonator. Based on the dimer system, an ultra-low threshold optical parametric oscillation generation method is proposed. By coupling the gain pump mode, the non-linear effect is effectively enhanced, the pump power threshold is reduced to half of when there is no gain, and the energy conversion efficiency is increased. We believe this research provides a feasible method for a low-threshold tunable and easy-to-integrate optical parametric oscillation laser source.

Fiber-coupling optical system for high-power and multi-wavelength diode laser bars oriented to integrated biomedical imaging systems

The use of pulsed high-power diode lasers (HPDLs) in the near infrared (NIR) range as multispectral sources has attracted much interest in biomedical applications due to their relatively low cost and small size compared to nanosecond Nd:YAG optical parametric oscillator (OPO) lasers. One of the main limitations of these sources is the availability to combine different wavelengths with high power density in the same beam. Various works have shown that the use of linear arrays of emitters as diode laser bars (DLBs) or stacked arrays of emitters as diode laser stacks (DLSs) allows the combination of multiple wavelengths while maintaining high power densities. Nevertheless, the highly asymmetric beam profile emitted by such laser sources between fast and slow axes implies the need for suitable beam shaping for efficient fiber coupling. In this work, we investigate a novel beam shaping technique to homogenize the beam quality of six DLBs in the wavelength range between 790 nm and 980 nm.We consider fast-axis collimating lenses (FAC) and beam twisters to reduce the beam asymmetry of the individual bars. The beams from the DLBs are then combined into a single multispectral beam using reflective mirrors, dichroic mirrors, and a polarizing beam splitter cube (PBC), and effectively coupled into a 400 µm core-diameter/N.A. = 0.22 optical fiber using a pair of cylindrical lenses. Simulation shows high coupled power densities with ~ 1.8 MW/cm2 at the output of the fiber. The coupling efficiency reaches 89.4%. The use of submillimeter fiber optic probes is particularly promising for photoacoustic endoscopy (PAE) applications requiring minimally invasive examination of internal organs.

Analysis of Fixed and Live Single Cells Using Optical Photothermal Infrared with Concomitant Raman Spectroscopy.

This paper reports the first use of a novel completely optically based photothermal method (O-PTIR) for obtaining infrared spectra of both fixed and living cells using a quantum cascade laser (QCL) and optical parametric oscillator (OPO) laser as excitation sources, thus enabling all biologically relevant vibrations to be analyzed at submicron spatial resolution. In addition, infrared data acquisition is combined with concomitant Raman spectra from exactly the same excitation location, meaning the full vibrational profile of the cell can be obtained. The pancreatic cancer cell line MIA PaCa-2 and the breast cancer cell line MDA-MB-231 are used as model cells to demonstrate the capabilities of the new instrumentation. These combined modalities can be used to analyze subcellular structures in both fixed and, more importantly, live cells under aqueous conditions. We show that the protein secondary structure and lipid-rich bodies can be identified on the submicron scale.

Structure and photochemistry of a potential precursor of circumstellar dust: The optical spectrum of Si4C2+

Mixed silicon carbide clusters are important components of circumstellar shells and their optical properties are fundamental for modelling the chemistry involved in the evolution of dust particles. Herein, we report the ultraviolet photodissociation (UVPD) spectrum of mass-selected Si4C2+ cations obtained in the 208–330 nm range (3.8–6.0 eV) in a quadrupole/time-of-flight tandem mass spectrometer coupled to a laser desorption source operating with a SiC rod and a broadly tuneable optical parametric oscillator laser. The UVPD spectrum is observed in the two lowest-energy fragment channels, corresponding to dominant loss of atomic Si at low energy and the rather stable Si2C molecule at high energy. The UVPD spectrum is analyzed by quantum chemical calculations at two levels of density functional theory (CAM-B3LYP, M11) to determine the structures, energies, electronic spectra, and fragmentation energies of the lowest-energy isomers. To locate these isomers on the multidimensional potential energy surface, basin hopping is employed as global optimization approach. The UVPD spectrum is consistent with the optical absorption spectrum computed for the two lowest-energy isomers, one of which is reported for the first time.

Compact long-working-distance laser-diode-based photoacoustic microscopy with a reflective objective

Photoacoustic microscopy (PAM) has quickly developed into a noninvasive biomedical imaging technique to achieve detection, diagnosis, and monitoring. Compared with Q-switched neodymium-doped yttrium aluminum garnet or optical parametric oscillator lasers, a low-cost and small-size laser diode (LD) used as an alternative light source is conducive to achieving the miniaturization and integration for preclinical transformation. However, the LD’s low peak output power needs the high numerical aperture objective to attain tight focus, which limits the working distance (WD) of the system in only 2–3 mm, resulting in not achieving the backward coaxial confocal mode. Here, we present a compact visible LD-based PAM system with a reflective objective to achieve a 22 mm long WD and a 10 µm lateral resolution. Different depth subcutaneous microvascular networks in label-free mouse ears have successfully reappeared in vivo with a signal-to-noise ratio up to 14 dB by a confocal alignment. It will be a promising tool to develop into a handy tool for subcutaneous blood vessel imaging.

Stimulated Raman Microscopy Implemented by Three Femtosecond Laser Sources

In this work, the implementation of a femtosecond Stimulated Raman Scattering microscope, equipped with three femtosecond laser sources: a Titanium-Sapphire (Ti:Sa), an optical parametric oscillator (OPO), and a second harmonic generator (SHG); is presented. Our microscope is designed so that it can cover all the regions of Raman spectra, taking advantage of two possible laser combinations. The first, Ti:Sa and OPO laser beams, which cover the C-H region (&gt;2800 cm-1 ) in stimulated Raman gain (SRG) modality, whereas the second, Ti:Sa and SHG laser beams, covering the C-H region and the fingerprint region in stimulated Raman losses (SRL) modality. The successful realization of the microscope is demonstrated, reporting images of polystyrene beads using both SRL and SRG modalities.

Infrared multiple photon dissociation action spectroscopy of protonated unsymmetrical dimethylhydrazine and proton-bound dimers of hydrazine and unsymmetrical dimethylhydrazine.

The gas-phase structures of protonated unsymmetrical 1,1-dimethylhydrazine (UDMH) and the proton-bound dimers of UDMH and hydrazine are examined by infrared multiple photon dissociation (IRMPD) action spectroscopy utilizing light generated by a free electron laser and an optical parametric oscillator laser system. To identify the structures present in the experimental studies, the measured IRMPD spectra are compared to spectra calculated at the B3LYP-GD3BJ/6-311+G(d,p) level of theory. These comparisons show that protonated UDMH binds the proton at the methylated nitrogen atom (α) with two low-lying α conformers probably being populated. For (UDMH)2H+, the proton is shared between the methylated nitrogen atoms with several low-lying α conformers likely to be populated. Higher-lying conformers of (UDMH)2H+ in which the proton is shared between α and β (unmethylated) nitrogen atoms cannot be ruled out on the basis of the IRPMD spectrum. For (N2H4)2H+, there are four low-lying conformers that all reproduce the IRMPD spectrum reasonably well. As hydrazine and UDMH see usage as fuels for rocket engines, such spectra are potentially useful as a means of remotely monitoring rocket launches, especially in cases of unsuccessful launches where environmental hazards need to be assessed.

Label-free imaging of lipid-rich biological tissues by mid-infrared photoacoustic microscopy.

.Significance: Mid-infrared (IR) imaging based on the vibrational transition of biomolecules provides good chemical-specific contrast in label-free imaging of biology tissues, making it a popular tool in both biomedical studies and clinical applications. However, the current technology typically requires thin and dried or extremely flat samples, whose complicated processing limits this technology’s broader translation.Aim: To address this issue, we report mid-IR photoacoustic microscopy (PAM), which can readily work with fresh and thick tissue samples, even when they have rough surfaces.Approach: We developed a transmission-mode mid-IR PAM system employing an optical parametric oscillation laser operating in the wavelength range from 2.5 to . Due to its high sensitivity to optical absorption and the low ultrasonic attenuation of tissue, our PAM achieved greater probing depth than Fourier transform IR spectroscopy, thus enabling imaging fresh and thick tissue samples with rough surfaces.Results: In our spectroscopy study, the symmetric stretching at (3508 nm) was found to be an excellent source of endogenous contrast for lipids. At this wavenumber, we demonstrated label-free imaging of the lipid composition in fresh, manually cut, and unprocessed tissue sections of up to 3-mm thickness.Conclusions: Our technology requires no time-consuming sample preparation procedure and has great potential in both fast clinical histological analysis and fundamental biological studies.

Threshold Photodetachment Spectroscopy of the Positronium Negative Ion.

Threshold photodetachment spectroscopy of the positronium negative ion has been accomplished for the first time employing an efficient source of the ions and photodetachment techniques combined with a tunable optical parametric oscillator and amplifier laser. The photodetachment threshold, corresponding to the electron affinity of positronium (1^{3}S_{1}), was determined to be 326.88±0.09(stat)±0.10(syst) meV by laser photodetachment threshold measurements. This result is consistent with a variational calculation corrected for leading relativistic and quantum electrodynamical effects.

Detailed Characterization of the Postionization Efficiencies in MALDI-2 as a Function of Relevant Input Parameters.

A recently introduced technique based on MALDI with laser-induced postionization (PI), also named MALDI-2, increases the ion yields for numerous classes of lipids, metabolites, and carbohydrates in MALDI-MS imaging experiments under certain experimental conditions. Here, we used a semiautomatic LabVIEW-based protocol to investigate and optimize the efficiency of the PI process dependent on four relevant input parameters and a dense parameter grid: pulse energies of the two lasers, delay between the laser pulses, and buffer gas pressure in the ion source. All experiments were conducted with a modified MALDI-2 Synapt G2-S mass spectrometer (Waters) and use of a focal spot size on the sample of 15-17 μm. A wavelength-tunable optical parametric oscillator (OPO) laser served for PI at 260 or 280 nm. The investigated MALDI matrices were: 2,5-dihydroxybenzoic acid (positive ion mode, +), 2,5-dihydroxyacetophenone (+), α-cyano-4-hydroxycinnamic acid (+), norharmane (negative-ion mode, -), and 1,5-diaminonapthalene (-). A porcine brain extract served as lipid standard. In the positive-ion mode, a maximum boost for the generated [M + H]+ species was found with a N2 buffer gas pressure of ∼2 mbar and a delay between the laser emissions of ∼10 μs. Higher optimal delay settings of several 10 μs were registered for the two studied matrices in negative-ion mode. With regard to the laser fluences, best PI efficiencies were reached using maximum available ablation and PI laser pulse energies of up to 25 and 160 μJ, respectively. For analytes not profiting from MALDI-2, best ion signal yields were recorded for ablation laser pulse energies of around 7 μJ, depending on the MALDI matrix. At higher laser pulse energies, sizable fragmentation is observed for these ions. The PI laser pulse energy did not have any influence on the ion signals of these species. For optimal ion yield of all analyte species, best results were obtained with an ablation laser pulse energy of ∼7 μJ and a PI laser pulse energy of ∼160 μJ. Our comprehensive data set provides valuable insight into the mechanisms underlying the MALDI-2 processes and could help to further optimize this emerging technique.

The bond dissociation energy of VO measured by resonant three-photon ionization spectroscopy.

The predissociation threshold of VO has been measured using resonant three-photon ionization (R3PI) spectroscopy. Given the high density of electronic states in the molecule, it is argued that the molecule dissociates rapidly as soon as the thermochemical bond dissociation energy (BDE) is exceeded, allowing the measured predissociation threshold to be assigned as the BDE. This is the first time a BDE has been measured using the R3PI method. The first photon is provided by an optical parametric oscillator (OPO) laser that promotes VO into a high-energy, discrete vibronic state. A tunable dye laser then excites the molecule further to a resonant state close to the dissociation limit where there is a quasi-continuum of states. A second photon from the same dye laser pulse ionizes the molecule, generating VO+ ions. The dye laser is then scanned to higher energies, and when the energy of one OPO photon plus one dye photon exceeds the BDE, the molecule dissociates before another dye photon can be absorbed to induce ionization. The combined photon energy at the sharp drop in the ion signal is assigned as the BDE. The experiment has been repeated using four different intermediate states, all yielding the same BDE, D0(VO) = 6.545(2) eV. Using thermochemical cycles, a revised value for the BDE of cationic VO is obtained, D0(V+-O) = 6.053(2) eV. The 0 K enthalpy of formation for VO(g) is also derived as ΔfH0K 0VO(g) = 128.6(1.0) kJ mol-1. Previous spectroscopic and thermochemical studies of VO are reviewed.

In Vivo Dual-Modal Photoacoustic and Ultrasound Imaging of Sentinel Lymph Nodes Using a Solid-State Dye Laser System.

Photoacoustic imaging (PAI) is being actively investigated as a non-invasive and non-radioactive imaging technique for sentinel lymph node (SLN) biopsy. By taking advantage of optical and ultrasound imaging, PAI probes SLNs non-invasively with methylene blue (MB) in both live animals and breast cancer patients. However, these PAI systems have limitations for widespread use in clinics and commercial marketplaces because the lasers used by the PAI systems, e.g., tunable liquid dye laser systems and optical parametric oscillator (OPO) lasers, are bulky in size, not economical, and use risky flammable and toxic liquid dyes. To overcome these limitations, we are proposing a novel dual-modal photoacoustic and ultrasound imaging system based on a solid-state dye laser (SD-PAUSI), which is compact, convenient, and carries far less risk of flammability and toxicity. Using a solid-state dye handpiece that generates 650-nm wavelength, we successfully imaged the MB tube positioned deeply (~3.9 cm) in chicken breast tissue. The SLNs were also photoacoustically detected in the in vivo rats beneath a 2.2-cm-thick layer of chicken breast, which is deeper than the typical depth of SLNs in humans (1.2 ± 0.5 cm). Furthermore, we showed the multispectral capability of the PAI by switching the dye handpiece, in which the MB-dyed SLN was selectively highlighted from the surrounding vasculature. These results demonstrated the great potential of the SD-PAUSI as an easy but effective modality for SLN detection.

Wavelength-Dependent Ultraviolet Photodissociation of Protonated Tryptamine.

Ultraviolet photodissociation (UVPD) experiments of protonated tryptamine ([Tryp+H]+) have been implemented by a Fourier transform ion cyclotron resonance (FTICR) mass spectrometer combined with a wavelength-tunable optical parametric oscillator (OPO) laser. UVPD mass spectra under different laser wavelengths have been obtained, in which the dependence of the yield of fragment ions on the laser wavelength was observed. The UVPD spectrum of [Tryp+H]+ has been obtained in the range of 210-310 nm. Besides the previously reported two competitive channels of H loss and NH3 loss, two important channels of losing CH2NH and CH2NH2 units were observed and further studied by UV-UV tandem mass spectrometry and theoretical calculations. Interestingly, results show that the pair of competitive channels of CH2NH loss and CH2NH2 loss are both from the McLafferty-type rearrangement caused by ππ* electronic excited states. After the excitation, the two different dissociation pathways produce two different ion-neutral complexes, respectively. The wavelength-dependent dissociation and the existing competitive channels shown in this study reflect the diversity of UVPD processes of such organic molecules.