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Third harmonic generation detection for strongly absorbing media in reflection with neodymium-glass mode-locked laser, measuring nonlinear susceptibilities of semiconductors and metals
Third-harmonic generation microscopy is a powerful label-free nonlinear imaging technique, providing essential information about structural characteristics of cells and tissues without requiring external labelling agents. In this work, we integrated a recently developed compact adaptive optics module into a third-harmonic generation microscope, to measure and correct for optical aberrations in complex tissues. Taking advantage of the high sensitivity of the third-harmonic generation process to material interfaces and thin membranes, along with the 1,300-nm excitation wavelength used here, our adaptive optical third-harmonic generation microscope enabled high-resolution in vivo imaging within highly scattering biological model systems. Examples include imaging of myelinated axons and vascular structures within the mouse spinal cord and deep cortical layers of the mouse brain, along with imaging of key anatomical features in the roots of the model plant Brachypodium distachyon. In all instances, aberration correction led to enhancements in image quality.
Here, we investigate enhanced second‑ and third‑harmonic generation (SHG and THG) in GaAs metasurfaces by combining electromagnetic point‑group designs with accidental bound states in the continuum (BICs). Using group theory, we predict the existence, suppression, and polarization selection rules of SHG and THG for metasurfaces belonging to the D 2h and C 2v point groups. In D 2h metasurfaces, inversion symmetry suppresses SHG while enabling polarization‑selective THG, which is strongly enhanced near accidental BICs with ultrahigh Q‑factors approaching 107. By breaking inversion symmetry to form C 2v metasurfaces through the introduction of nanogaps, SHG is now allowed and is dramatically enhanced near accidental BICs. Importantly, accidental BICs preserve polarization selection rules while providing a robust parameter range for high‑Q resonances, in contrast to quasi‑BICs induced by symmetry breaking. Our results demonstrate that the combination of point‑group theory and accidental‑BIC engineering offers a predictive and robust route toward highly efficient nonlinear metasurfaces.
In this paper, we investigate second- and third-harmonic generation processes in Au nanorod systems using the real-time time-dependent density functional tight binding method. Our study focuses on the computation of nonlinear signals based on the time dependent dipole response induced by linearly polarized laser pulses interacting with nanoparticles. We systematically explore the influence of various laser parameters, including pump intensity, duration, frequency, and polarization directions, on harmonic generation. We demonstrate all the results using Au nanorod dimer systems arranged in end-to-end configurations, and disrupting the spatial symmetry of regular single nanorod systems is crucial for second-harmonic generation processes. Furthermore, we study the impact of nanorod lengths, which lead to variable plasmon energies, on harmonic generation, and estimates of polarizabilities and hyper-polarizabilities are provided.
A compact and high-pulse-energy Ti:Sapphire laser with its Third Harmonic Generation (THG) has been developed for an airborne ozone differential absorption lidar (DIAL) to study the distributions and concentrations of the ozone throughout the troposphere. The Ti:Sapphire laser, pumped by a frequency-doubled Nd:YAG laser and seeded by a single mode diode laser, is operated either at 867 nm or at 900 nm with a pulse repetition frequency of 20 Hz. High energy laser pulses (more than 110 mJ/pulse) at 867 nm or 900 nm with a desired beam quality have been achieved and utilized to generate its third harmonic at 289nm or 300nm, which are on-line and off-line wavelengths of an airborne ozone DIAL. After being experimentally compared with Beta-Barium Borate (beta - BaB2O4 or BBO) nonlinear crystals, two Lithium Triborate (LBO) crystals (5 x 5 x 20 cu mm) are selected for the Third Harmonic Generation (THG). In this paper, we report the Ti:Sapphire laser at 900 nm and its third harmonic at 300 nm. The desired high ultraviolet (UV) output pulse energy is more than 30 mJ at 300 nm and the energy conversion efficiency from 900 nm to 300 nm is 30%.
We report improvements in conversion efficiency for third harmonic generation in sodium and rubidium vapor. 30-psec pulses of radiation at 1.064 micron have been converted to 0.3547 micron with an energy conversion efficiency of 10%. Factors limiting conversion efficiency are discussed.
In the mid to late 1970s there was considerable debate as to which laser technology should be pursued—glass lasers (1-μm wavelength) or CO 2 lasers (10 μm). Based on target-physics considerations, theorists were advocating for shorter wavelengths. The physics understanding was confirmed by exciting results from the group at the École Polytechnique, who observed close to 100% target absorption with just a few joules of fourth-harmonic energy. These results motivated the leadership at LLE to plan similar experiments at the third harmonic, with a few more joules. This presentation covers a small time period from 1979 to 1980 during which highly efficient Third-Harmonic Generation (THG) became understood theoretically and demonstrated experimentally, leading to the worldwide adoption of THG with glass lasers for fusion research.
Here we report the group theory-based inverse design of meta-atoms for a dielectric metasurface in GaAs with predictable optical linear response and third harmonic generation (THG). Six sharp Fano resonances have been observed with a corresponding polarization dependence as predicted by group theory and the meta-atom’s symmetry in the D2h point group. THG has been observed for two modes under x-polarization excitation and one mode for y-polarization, in agreement with theoretical symmetry predictions. The polarization-dependent THG aspect ratio was observed to reach as high as 108. Through strategic structural or symmetry-preserving perturbations, it was shown that the THG can be enhanced or reduced by a factor of 7. The highest THG conversion efficiency was estimated to be 3.1×10-7 at the pump intensity of 1.51 MW/cm2. This high THG conversion efficiency indicates that our group theory approach to modal engineering opens a new path towards optical nonlinearity tuning in dielectric metasurfaces.
Root biology is pivotal in addressing global challenges including sustainable agriculture and climate change. However, roots have been relatively understudied among plant organs, partly due to the difficulties in imaging root structures in their natural environment. Here we used microfabricated ecosystems (EcoFABs) to establish growing environments with optical access and employed nonlinear multimodal microscopy of third-harmonic generation (THG) and three-photon fluorescence (3PF) to achieve label-free, in situ imaging of live roots and microbes at high spatiotemporal resolution. THG enabled us to observe key plant root structures including the vasculature, Casparian strips, dividing meristematic cells, and root cap cells, as well as subcellular features including nuclear envelopes, nucleoli, starch granules, and putative stress granules. THG from the cell walls of bacteria and fungi also provides label-free contrast for visualizing these microbes in the root rhizosphere. With simultaneously recorded 3PF signal, we demonstrated our ability to investigate root-microbe interactions by achieving single-bacterium tracking and subcellular imaging of fungal spores and hyphae in the rhizosphere.
Effects of quantum mechanical interferences on third-order susceptibilities in molecules are studied. First principle calculations for molecular hydrogen are presented and shown to agree with results derived from experimental stimulated Raman gain and spontaneous Raman cross-section data. 10 percent third-harmonic conversion efficiency in H2 at 1 atm without phase matching should require a 150 MW per sq cm at 4.81 microns. As little as 5.9-MW power is sufficient when the beam is properly focused. Resonance Raman scattering (RRS) is proposed for experimentally investigating the interference effects, which tend to reduce the strength of third-order nonlinear susceptibilities.
The National Ignition Facility (NIF) uses crystal optics made from Potassium Di-Hydrogen Phosphate (KDP) for frequency conversion, changing the fundamental wavelength of 1053 nm to the third harmonic at 351 nm. The crystal optics are manufactured at a vendor and shipped to Lawrence Livermore National Laboratory (LLNL) where they are measured, mitigated, cleaned, coated, and placed into line replaceable units (LRUs) in the Optics Processing Facility (OPF) clean room and transported to the NIF where they are stored under Nitrogen purge until they are installed in the beamline. The KDP crystal optics are sensitive to humidity and temperature, so they are stored under Nitrogen purge providing a clean and dry environment. The sensitivity to the environment and the brittle nature of the crystals makes transportation and handling (T&H) challenging. Coupled with challenges in holding the crystal optics in the LRU to not distort the optic, there is a balance between T&H and fixturing the optic in the laser system. The purpose of the LRU is to make the optics interchangeable allowing for a relatively quick interchange. Kinematic mounts and ceramic frames aid in making this possible. Optics in the NIF that are frequently changed out have an established recycle loop. The loop for an optic can be complex depending on the amount of processing and rework necessary. Some optics can’t be reconditioned so they are replaced with new optics.
The generation of 0.3547-micron radiation was performed by tripling 1.064-micron radiation in a phase-matched mixture of rubidium vapor and xenon. A third-harmonic nonlinear susceptibility in Rb vapor is confirmed. It is about 100,000 times greater than that of He. This large susceptibility is due to the large oscillator strengths and resonant enhancements resulting from Rb transitions in the near infrared, visible, and UV.
The characterization of atmospheric winds on a global basis is a key parameter required for accurate weather prediction. The use of a space based lidar system for remote measurement of wind speed would provide detailed and highly accurate data for future weather prediction models. This paper reports the demonstration of efficient third harmonic conversion of a 1 micrometer laser to provide an ultraviolet (UV) source suitable for a wind lidar system based on atmospheric molecular scattering. Although infrared based lidars using aerosol scattering have been demonstrated to provide accurate wind measurement, a UV based system using molecular or Rayleigh scattering will provide accurate global wind measurements, even in those areas of the atmosphere where the aerosol density is too low to yield good infrared backscatter signals. The overall objective of this work is to demonstrate the maturity of the laser technology and its suitability for a near term flight aboard the space shuttle. The laser source is based on diode-pumped solid-state laser technology which has been extensively demonstrated at TRW in a variety of programs and internal development efforts. The pump laser used for the third harmonic demonstration is a breadboard system, designated the Laser for Risk Reduction Experiments (LARRE), which has been operating regularly for over 5 years. The laser technology has been further refined in an engineering model designated as the Compact Advanced Pulsed Solid-State Laser (CAPSSL), in which the laser head was packaged into an 8 x 8 x 18 inch volume with a weight of approximately 61 pounds. The CAPSSL system is a ruggedized configuration suitable for typical military applications. The LARRE and CAPSSL systems are based on Nd:YAG with an output wavelength of 1064 nm. The current work proves the viability of converting the Nd:YAG fundamental to the third harmonic wavelength at 355 nm for use in a direct detection wind lidar based on atmospheric Rayleigh scattering.
The potential efficiency of using nonlinear up-conversion techniques for the high efficiency type lasers (CO,CO2, and chemical) is assessed. Results indicate that: the small pump photon energy necessitates the use of molecular media for conversion if resonance enhancement is to be used and that molecular systems present several problems. These difficulties include: their levels are complex; their transition probabilities are often unknown; and the oscillator strengths among vibrational levels in the ground electronic state of a molecule are much smaller than those among electronic states of an atom, thus limiting the magnitude of nonlinear interactions. It is shown that this problem can be eliminated by making use of vibronic transitions which, being primarily electronic transitions have much larger matrix elements and efficient conversion can be achieved with molecular systems.
Phase matching for frequency tripling of 1.06 microns is demonstrated in a homogeneous mixture of sodium and magnesium vapor. The ratio of Mg to Na vapor pressures required for phase matching is 2:1. This ratio is about 1/75 of that required to phase match Na with Xe.
The second- and third-order nonlinear optical properties of acridine yellow-doped lead-tin fluorophosphate (LTF) glass have been directly studied by measurement of surface enhanced second harmonic generation and third harmonic generation. The three photon excitation fluorescence is also observed. Based on these results, the large nonlinearities of the acridine LTF system which is a new nonlinear optical material are experimentally demonstrated.
Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow the optical response of a material to be tailored far beyond its natural properties. Therefore, metasurfaces are highly appealing for enabling the engineering of nonlinear optical interactions. Current studies of nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlocking a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior by considering the polarization degree of freedom. We establish an effective nonlinear medium model that serves as a design toolbox for developing amorphous silicon-based geometric metasurfaces with customizable features for third-harmonic generation. We further extract quantitative values of the artificial nonlinear susceptibility tensor elements related to the investigated nonlinear process and geometry. The implemented functional devices demonstrate the versatility of dielectric metasurfaces in shaping the emitted light in terms of amplitude, phase, and polarization for the precise engineering of advanced nonlinear architectures targeting applications in nonlinear imaging and complex light generation.
The effect that fluorine and chlorine substitution has on the nonlinear optical properties of porphyrin, tetramethylporphyrin and tetraphenylporphyrin has been theoretically studied. The calculations of nonlinear optical properties have been obtained by performing finite-field calculations on structures determined by semiempirical methods. In addition, tetra(p-chlorophenyl)porphyrin and tetra(p-bromophenyl)porphyrin were synthesized by the condensation of pyrrol and the appropriate aldehyde. Thin films of polymethylmethacrylate were obtained containing these materials, by spin coating onto glass substrates. The films were characterized by third-harmonic generation. It was determined that the experimental conditions enhance the third-order polarizability of the tetraphenylporphyrins by a factor of about 1.6.