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At least 91 records · Page 5

Nonlinear optical processing with Fabry-Perot interferometers containing phase recording media

New techniques in nonlinear optical processing are explored, based on the operation of intensity level selection as performed by a Fabry-Perot interferometer containing a phase object. The image being processed is recorded on a medium between the mirrors as a spatially varying phase shift less than pi. The interferometer only transmits light through those portions of the object that corresponds to a single value of the phase and hence to a single intensity level in the input. More complicated operations such as thresholding and analog-to-digital conversion are performed by modulating the light source as the different levels are selected. Photoresist and lithium niobate have been used as phase objects, and experimental data for both are presented. Three kinds of Fabry-Perot interferometers have been used to demonstrate nonlinear processing using coherent and incoherent light. Color images have been produced with black and white inputs and white light illumination.

Bartholomew, B. J.↗

Nonlinear optics from hybrid dispersive orbits

In this paper we expand the technique of characterizing nonlinear optics from off-energy closed orbits (NOECO) to cover harmonic sextupoles in storage rings. The existing NOECO technique has been successfully used to correct the chromatic sextupole errors on the MAX-IV machine [Olsson et al., Phys. Rev. Accel. Beams 23, 102803], however, it does not account for harmonic sextupoles, which are still widely used on many other machines. By generating vertical dispersion with chromatic skew quadrupoles, a measurable chromatic function dependence on harmonic sextupoles can be observed on hybrid dispersive orbits. Proof of concept of this technique was accomplished by simulations and beam measurements on the National Synchrotron Light Source II (NSLS-II) storage ring.

43 PARTICLE ACCELERATORS↗

Nonlinear optics from hybrid dispersive orbits

Here in this paper we expand the technique of characterizing nonlinear optics from off-energy closed orbits (NOECO) to cover harmonic sextupoles in storage rings. The existing NOECO technique has been successfully used to correct the chromatic sextupole errors on the MAX-IV machine (Olsson et al., 2020), however, it does not account for harmonic sextupoles, which are still widely used on many other machines. By generating vertical dispersion with chromatic skew quadrupoles, a measurable chromatic function dependence on harmonic sextupoles can be observed on hybrid dispersive orbits. Proof of concept of this technique was accomplished by simulations and beam measurements on the National Synchrotron Light Source II (NSLS-II) storage ring.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS 2 : Insight from First-Principles Exciton-State Coupling Formalism and Calculations

Excitons are vital in the photophysics of materials, especially in low-dimensional systems. The conceptual and quantitative understanding of excitonic effects in nonlinear optical (NLO) processes is more challenging compared to linear ones. Here, we present an ab initio approach to second-order NLO responses, incorporating excitonic effects, that employs an exciton-state coupling formalism and allows for a detailed analysis of the role of individual excitonic states. Taking monolayer h-BN and MoS 2 as two prototype 2D materials, we calculate their second harmonic generation (SHG) susceptibility and shift current conductivity tensor. We find strong excitonic enhancement in the NLO responses requires that the resonant excitons are not only optically bright themselves but also able to couple strongly to other bright excitons. Our results explain the occurrence of two strong peaks in the SHG of monolayer h-BN and why the A and B excitons of MoS 2 unexpectedly exhibit minimal excitonic enhancement in both SHG and shift current generation.

36 MATERIALS SCIENCE↗

Polar coupling enabled nonlinear optical filtering at MoS 2 /ferroelectric heterointerfaces

Complex oxide heterointerfaces and van der Waals heterostructures present two versatile but intrinsically different platforms for exploring emergent quantum phenomena and designing new functionalities. The rich opportunity offered by the synergy between these two classes of materials, however, is yet to be charted. Here, we report an unconventional nonlinear optical filtering effect resulting from the interfacial polar alignment between monolayer MoS 2 and a neighboring ferroelectric oxide thin film. The second harmonic generation response at the heterointerface is either substantially enhanced or almost entirely quenched by an underlying ferroelectric domain wall depending on its chirality, and can be further tailored by the polar domains. Unlike the extensively studied coupling mechanisms driven by charge, spin, and lattice, the interfacial tailoring effect is solely mediated by the polar symmetry, as well explained via our density functional theory calculations, pointing to a new material strategy for the functional design of nanoscale reconfigurable optical applications.

36 MATERIALS SCIENCE↗

Encoding the complete electric field of an ultraviolet ultrashort laser pulse in a near-infrared nonlinear-optical signal

We introduce a variation on the cross-correlation frequency-resolved optical gating (XFROG) technique that uses a near-infrared (NIR) nonlinear-optical signal to characterize pulses in the ultraviolet (UV). Using a transient-grating XFROG beam geometry, we create a grating using two copies of the unknown UV pulse and diffract a NIR reference pulse from it. We show that, by varying the delay between the UV pulses creating the grating, the UV pulse intensity-and-phase information can be encoded into a NIR signal. We also implemented a modified generalized-projections phase-retrieval algorithm for retrieving the UV pulses from these spectrograms. We performed proof-of-principle measurements of chirped pulses and double pulses, all at 400 nm. This approach should be extendable deeper into the UV and potentially even into the extreme UV or x-ray range.

47 OTHER INSTRUMENTATION↗

Direct Observation of Circularly Polarized Nonlinear Optical Activities in Chiral Hybrid Lead Halides

Circularly polarized light emission is a crucial application in imaging, sensing, and photonics. However, utilizing low-energy photons to excite materials, as opposed to high-energy light excitation, can facilitate deep-tissue imaging and sensing applications. The challenge lies in finding materials capable of directly generating circularly polarized nonlinear optical effects. In this study, we introduce a chiral hybrid lead halide (CHLH) material system, R/S-DPEDPb 3 Br 8 ·H 2 O (DPED = 1,2-diphenylethylenediammonium), which can directly produce circularly polarized second harmonic generation (CP-SHG) through linearly polarized infrared light excitation, exhibiting a polarization efficiency as high as 37% at room temperature. To understand the spin relaxation mechanisms behind the high polarization efficiency, we utilized two models, so-called D’yakonov–Perel’ (DP) and Bir–Aronov–Pikus (BAP) mechanisms. The unique zigzag inorganic frameworks within the hybrid structure are believed to reduce the dielectric confinement and exciton binding energy, thus enhancing spin polarization, especially in regions with a high excitation pump fluence based on the DP mechanism. In the case of low excitation pump fluence, the BAP mechanism dominates, as evidenced by the observed decrease in the polarization ratio from CP-SHG measurement. Using density functional theory analysis, we elucidate how the distinctive 8-coordination environment of lead bromide building blocks effectively suppresses spin–orbit coupling at the conduction band minimum. This suppression significantly diminishes spin-splitting, thereby slowing the spin relaxation rate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Melt Growth of a Nonlinear Optical Crystal Triethylphosphine Sulfide using Modified Bridgman-Stockbarger Technique

Bulk single crystals of triethylphosphine sulfide (C2H5)3P(S), a potential nonlinear optical organic material has been grown from melt using Bridgman- Stockbarger method. Commercially available material triethylphosphine sulfide procured from Johnson Matthey was purified by physical vapor transport using low pressure sublimaton (about 30 mTorr). Modified Bridgman-Stockbarger technique is characterized by the smallest possible quantity of product in the melt for a short period of time. The temperature gradient was chosen to be about 10 C/cm and the ampoule was lowering rate was chosen to be 0.2-0.3 mm/h. For various growth conditions, several single crystal of triethylphosphine sulfide have been grown with sizes 10X10X15mm(exp 3). The second harmonic generation (SHG) efficiency was measured and has been found to be comparable to phase matched potassium dihydrogen phosphate crystals. Further characterization of the grown single crystals is in progress and the results will be presented at the symposium.

Curry, K.↗

Nonlinear Optical Image Processing with Bacteriorhodopsin Films

The transmission properties of some bacteriorhodopsin film spatial light modulators are uniquely suited to allow nonlinear optical image processing operations to be applied to images with multiplicative noise characteristics. A logarithmic amplitude transmission feature of the film permits the conversion of multiplicative noise to additive noise, which may then be linearly filtered out in the Fourier plane of the transformed image. The bacteriorhodopsin film displays the logarithmic amplitude response for write beam intensities spanning a dynamic range greater than 2.0 orders of magnitude. We present experimental results demonstrating the principle and capability for several different image and noise situations, including deterministic noise and speckle. Using the bacteriorhodopsin film, we successfully filter out image noise from the transformed image that cannot be removed from the original image.

Downie, John D.↗

Compositional dependence of linear and nonlinear optical response in crystalline hafnium zirconium oxide thin films

Composition dependence of second harmonic generation, refractive index, extinction coefficient, and optical bandgap in 20 nm thick crystalline Hf 1– x Zr x O 2 (0 ≤ x ≤ 1) thin films is reported here. The refractive index exhibits a general increase with increasing ZrO 2 content with all values within the range of 1.98–2.14 from 880 nm to 400 nm wavelengths. A composition dependence of the indirect optical bandgap is observed, decreasing from 5.81 eV for HfO 2 to 5.17 eV for Hf 0.4 Zr 0.6 O 2 . The bandgap increases for compositions with x > 0.6, reaching 5.31 eV for Hf 0.1 Zr 0.9 O 2 . Second harmonic signals are measured for 880 nm incident light. The magnitude of the second harmonic signal scales with the magnitude of the remanant polarization in the composition series. Film compositions that display near zero remanent polarizations exhibit minimal second harmonic generation while those with maximum remanent polarization also display the largest second harmonic signal. The results are discussed in the context of ferroelectric phase assemblage in the hafnium zirconium oxide films and demonstrate a path toward a silicon-compatible integrated nonlinear optical material.

36 MATERIALS SCIENCE↗

Nonlinear Optical Properties and Applications of Polydiacetylene

Recently, we have demonstrated a picosecond all-optical switch, which also functions as a partial all-optical NAND logic gate using a novel polydiacetylene that is synthesized in our laboratory. The nonlinear optical properties of the polydiacetylene material are measured using the Z-scan technique. A theoretical model based on a three level system is investigated and the rate equations of the system are solved. The theoretical calculations are proven to match nicely with the experimental results. The absorption cross-sections for both the first and higher excited states are estimated. The analyses also show that the material suffers a photochemical change beyond a certain level of the laser power and its physical properties suffer radical changes. These changes are the cause for the partial NAND gate function and the switching mechanism.

Abdeldayem, Hossin↗

Diagrammatic evaluation of the density operator for nonlinear optical calculations

Time-ordered diagrammatic representations are shown to precisely define and to simplify calculations of radiative perturbations to the density matrix. Nonlinear optical susceptibilities, here exemplified by that of CARS, can be obtained by simple propagator rules. An interpretation of transient Raman scattering in terms of time-ordered contributions is also discussed.

Yee, S. Y.↗

Using naturally occurring polysaccharides to align molecules with nonlinear optical activity

The Biophysics and Advanced Materials Branch of the Microgravity Science and Applications Division at Marshall Space Flight Center has been investigating polymers with the potential for nonlinear optical (NLO) applications for a number of years. Some of the potential applications for NLO materials include optical communications, computing, and switching. To this point the branch's research has involved polydiacetylenes, phthalocyanins, and other synthetic polymers which have inherent NLO properties. The aim of the present research is to investigate the possibility of using naturally occurring polymers such as polysaccharides or proteins to trap and align small organic molecules with useful NLO properties. Ordering molecules with NLO properties enhances 3rd order nonlinear effects and is required for 2nd order nonlinear effects. Potential advantages of such a system are the flexibility to use different small molecules with varying chemical and optical properties, the stability and cost of the polymers, and the ability to form thin, optically transparent films. Since the quality of any polymer films depends on optimizing ordering and minimizing defects, this work is particularly well suited for microgravity experiments. Polysaccharide and protein polymers form microscopic crystallites which must align to form ordered arrays. The ordered association of crystallites is disrupted by gravity effects and NASA research on protein crystal growth has demonstrated that low gravity conditions can improve crystal quality.

Prasthofer, Thomas↗

Implementing nonlinear optics from Off-Energy closed orbit at NSLS-II

To characterize the second-order (chromatic sextupole) magnet lattice with high precision, we implemented nonlinear optics from off-energy closed orbit (NOECO) tool based on the linear optics from closed orbit modulation (LOCOM) method, named LOCOM-NOECO. The preliminary numerical study indicates that 1–2% precision can be achieved for the calibration of chromatic sextupoles. Further, this accuracy could potentially help in resolving some long-standing challenges of NSLS-II (e.g., the discrepancy between the designed and measured dynamic apertures) if such high precision can be fulfilled. As an independent crosscheck, we also implemented NOECO based on the independent component analysis (ICA) method using turn-by-turn (TBT) BPM data, named ICA-NOECO. Both ICA-NOECO and LOCOM-NOECO have been successfully applied to identify the pre-dialed random errors of a chromatic sextupole family including five power supplies, and achieved the root mean square (RMS) residual error of 1% and peak error less than 2%. Moreover, to mitigate the chromatic sextupole error effect, we applied the correction and achieved significant improvements in the injection efficiency as well as the dynamic apertures.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A versatile low-cost Czochralski crystal growth system for nonlinear optical organic materials

A versatile low-cost Czochralski system for pulling crystals from melt has been described. It is designed for low melting, transparent, and nonlinear optical materials. One of the most important novel feature of this crystal growth system is that the entire growth process including the solid-liquid interface can be viewed from any direction. Another is the use of an after-heater to reduce excess heat loss from the surface of the melt.

Aggarwal, M. D.↗

Stationary and non-stationary nonlinear optical spectroscopy on surface polaritons

A phenomenological theory is given for non-stationary electromagnetic surface waves propagating along the boundary plane between two homogeneous isotropic media. The description of nonlinear optical effects using shortened wave equations is demonstrated for spontaneous and simulated Raman scattering processes on surface polaritons.

Ponath, H. E.↗

Strong ultrafast nonlinear optical response from megaelectronvolt electrons in semiconductors

Understanding radiation–matter interactions on ultrafast timescales is essential for radiation detection technologies, particularly those requiring precise timing, such as plasma monitoring, synchrotron diagnostics and medical imaging. However, the detection of highly ionizing radiation is challenging due to the stochastic nature of the interactions, resulting in dispersed energy deposition. Here we show a nonlinear optical response in semiconductors induced by 150-fs, 4.2-MeV electrons that generate highly localized charge carriers. The induced sub-10-ps optical modulation reached up to 24.5%, accompanied by a blueshift in the absorption edge consistent with band filling and carrier densities of 10 18 cm −3 . These carrier densities are 100-fold higher than expected from the deposited energy, indicating the extreme spatial localization of carriers at inelastic collisions along the ionization trajectories, thereby leading to the observed modulation. The strong nonlinearity of the MeV-electron-induced optical response enables the precise spatiotemporal detection of ionizing radiation at room temperature using common semiconductors and laser systems.

Jeong, D. [Stanford Univ., CA (United States)] (OR↗