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At least 37 records · Page 2

Waveguide Harmonic Generator for the SIM

A second-harmonic generator (SHG) serves as the source of the visible laser beam in an onboard calibration scheme for NASA's planned Space Interferometry Mission (SIM), which requires an infrared laser beam and a visible laser beam coherent with the infrared laser beam. The SHG includes quasi-phase-matched waveguides made of MgO-doped, periodically poled lithium niobate, pigtailed with polarization- maintaining optical fibers. Frequency doubling by use of such waveguides affords the required combination of coherence and sufficient conversion efficiency for the intended application. The spatial period of the poling is designed to obtain quasi-phase- matching at a nominal middle excitation wavelength of 1,319.28 nm. The SHG is designed to operate at a warm bias (ambient temperature between 20 and 25 C) that would be maintained in its cooler environment by use of electric heaters; the heater power would be adjusted to regulate the temperature precisely and thereby maintain the required precision of the spatial period. At the state of development at the time of this reporting, the SHG had been packaged and subjected to most of its planned space-qualification tests.

Chang, Daniel↗

Extreme-ultraviolet spatiotemporal vortices via high harmonic generation

Spatiotemporal optical vortices (STOVs) are space–time structured light pulses with a unique topology that couples spatial and temporal domains and carry transverse orbital angular momentum (OAM). Up to now, their generation has been limited to the visible and infrared regions of the spectrum. During the last decade, it was shown that through the process of high-order harmonic generation, it is possible to upconvert spatial optical vortices that carry longitudinal OAM from the near-infrared into the extreme-ultraviolet (EUV), thereby producing vortices with distinct femtosecond and attosecond structure. In this work, we demonstrate theoretically and experimentally the generation of EUV spatiotemporal and spatiospectral vortices using near-infrared STOV driving laser pulses. Here, we use analytical expressions for focused STOVs to perform macroscopic calculations of high-order harmonic generation that are directly compared to the experimental results. As STOV beams are not eigenmodes of propagation, we characterize the highly charged EUV STOVs in both the near and far fields to show that they represent conjugated spatiotemporal and spatiospectral vortex pairs. Our work provides high-frequency light beams topologically coupled at the nanometre/attosecond scales domains with transverse OAM that could be suitable to explore electronic dynamics in magnetic materials, chiral media and nanostructures.

High-harmonic generation↗

Enhanced Second and Third Harmonic Generations in Metasurfaces Enabled through Point Group Design and Accidental Bound States in the Continuum

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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High harmonic generation in Haldane model quantum dots

We study theoretically the nonlinear electron dynamics of Haldane model quantum dots placed in the field of an ultrashort optical pulse. One of the tuning parameters of the Haldane model is the phase accumulated by an electron during its transfer between the next nearest neighbor sites. We study how this parameter affect the nonlinear electron dynamics and the generation of high optical harmonics. With increasing the phase from its zero value to 90°, the low-energy electron states in the conduction and valence bands become more localized near the edges of the quantum dot resulting in suppression of the band gap, enhancement of the dipole inter-band coupling, and strong suppression of the average low-energy electron density of the states. As a result, the nonlinear response of the electron system of a Haldane model quantum dot is the strongest at intermediate values of the phase, ≈ 30− 40°. At these values of the phase, the electron dynamics is irreversible and a few first high-order harmonics have the largest intensities. Here, when the phase approaches 90° value the generation of high harmonics is strongly suppressed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Observation of seeded second harmonic generation in bulk germanosilicate fiber preforms

Simultaneous irradiation of a bulk fiber preform with molar concentrations of 3 pct Ge and 0.5 pct P doped silica core region resulted in self-organized second harmonic generation with an effective chi(2) of about 1.2 x 10 to the -16th m/V. The experiments revealed that the bulk preform requires the same critical IR intensity (10 GW/sq cm) as the drawn fibers to prepare. Attempts to self-prepare the preform field, indicating that self-preparation in fibers is most likely initiated by second harmonic generation associated with the core-cladding interface.

Lawandy, N. M.↗

Second Harmonic Generation Electric Field Triplet Interferometry for Absolute Phasing

We report second harmonic generation (SHG) electric field triplet interferometry performed using three mutually coherent ultrafast pulses in a common path with controllable relative phases, namely, the light fields of a sample signal (SI), a reference oscillator (RO), and a local oscillator (LO). The ROLO phase determined from the interference of the light fields produced by two quartz wafers is subtracted from the phase determined from the SIROLO interferogram to yield the signal phase, ϕ SI . The new method also calibrates the measured SHG intensity from a given sample internally by sending the fundamental light field reflected from the sample into one of the quartz wafers in the ROLO element. The approach avoids having to exchange the sample against a reference material with a known χ(2) value or known phase and accounts on-the-fly for situations where the reflected fundamental light field intensity changes with experimental conditions. The new method is successfully benchmarked against z-cut α-quartz, fused silica held at its point of zero charge, and hematite nanolayers in air, across three different interferometers. Furthermore, the approach should be applicable for other second-order nonlinear spectroscopies, such as vibrational or electronic sum-frequency generation.

Interfaces↗

Phase matching in second-harmonic generation using artificial periodic structures.

The use of artificial periodic structures, consisting of spatial modulations of the linear and nonlinear susceptibilities of a nonlinear optical medium, to achieve phase matching in second-harmonic generation is analyzed. Dispersion relations and approximate formulas for the second-harmonic fields generated under various conditions are obtained and used to evaluate the experimental situation.

Tang, C. L.↗

Second harmonic generation in topological insulators under quantizing magnetic fields

We theoretically investigate the second harmonic generation (SHG) of topological insulator surface states in a perpendicular magnetic field. Our theory is based on the microscopic expression of the second-order magneto-optical conductivity developed from the density matrix formalism, taking into account hexagonal warping effects on the surface states' band structure. Using numerically exact Landau-level energies and wave functions including hexagonal warping, we calculate the spectrum of SHG conductivities under normal incidence for different values of magnetic field and chemical potential. The imaginary parts of the SHG conductivities show prominent resonant peaks corresponding to one-photon and two-photon inter-Landau-level transitions. Treating the hexagonal warping term perturbatively, these transitions are clarified analytically within a perturbation theory from which approximate selection rules for the allowable optical transitions for SHG are determined. Furthermore, our results show extremely high SHG susceptibility that is easily tunable by magnetic field and doping level for topological surface states in the far-infrared regime, exceeding that of many conventional nonlinear materials. This work highlights the key role of hexagonal warping effects in generating second-order optical responses and provides insights into the nonlinear magneto-optical properties of the topological insulators.

Landau levels↗

Insulating moiré homobilayers lack a threefold symmetric second-harmonic generation

Atoms within moiré bilayers relax in plane to minimize elastic energy; such relaxation brings their space group symmetries down to P1. Here, the ab initio second harmonic generation (SHG) of twisted and atomistically optimized hBN bilayers was determined at four twist angles (θ = 38.21°, 60.00°, 73.17°, and 98.21°) and for three displacements τ measured away from the ground state AA' configuration. All moiré bilayers have a P1 space symmetry after structural optimization. This situation is quite different to monolayers with hexagonal lattices, which retain a threefold symmetry. We point out that the actual symmetries of the SHG reported for hBN bilayers on two experimental works do not coincide with the sixfold symmetric theoretical profiles they provide [either sin 2 ⁡(3⁢Φ) or cos 2 ⁡(3⁢Φ)], and show that the intrinsic low structural symmetry of (atomically optimized) hBN bilayer moirés can in fact be read out from experimental SHG intensity profiles—which are tunable by θ and by the frequency of light ω: The SHG is most definitely not sixfold symmetric because moirés do not retain a threefold symmetry. Furthermore, an extrinsic twofold symmetry of the SHG emission is realized by tilting the pump by an angle α away from the 2D material's normal, regardless of θ and ω. Furthermore, the design of in-plane and ultrathin sources of SHG with low symmetry could be useful for the eventual creation of entanglement sources from 2D materials.

2-dimensional systems↗

Phonon second harmonic generation in NaBr studied by inelastic neutron scattering and computer simulation

The phenomenon of second harmonic generation (SHG) was found for phonons in anharmonic NaBr by inelastic neutron scattering. The temperature dependence of this phonon SHG was measured from 300 K to 650 K. At 300 K the second harmonic (SH) is seen as a high-energy branch around 33 meV, nearly independent of $\overrightarrow{Q}$. The temperature effective potential (TDEP) method and classical molecular dynamics (MD) simulation with machine learning interatomic potential were able to reproduce the SH, and showed that SHG occurs with the flat transverse optical (TO) phonon branch. A classical model of a nonlinear medium explains the intensity and lifetime of the SH, compared to those of the TO modes. Also successful was a quantum model based on the Heisenberg-Langevin equation for interacting phonons coupled to a thermal bath, which also predicts a spectral distribution of the SH. In conclusion, the measured temperature dependence of the intensity of the second harmonic showed that it follows the Planck distribution of a one-phonon quasiparticle, and not two TO phonons.

36 MATERIALS SCIENCE↗

Limitations on squeezing and formation of the superposition of two macroscopically distinguishable states at fundamental frequency in the process of second harmonic generation

The results of numerical simulations of quantum state evolution in the process of second harmonic generation (SHG) are discussed. It is shown that at a particular moment of time in the fundamental mode initially coherent state turns into a superposition of two macroscopically distinguished states. The question of whether this superposition exhibits quantum interference is analyzed.

Nikitin, S. P.↗

Large Non‐Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP 2 Se 6

2D van der Waals (vdW) materials have emerged as a highly promising candidates for nonlinear optical (NLO) applications. This study presents the synthesis, comprehensive linear optical, and optical second harmonic generation (SHG) characterization of a novel 2D vdW semiconductor SnP2Se6 in its bulk single crystal form. It exhibits an indirect bandgap of ≈1.47 eV and an exceptional non-resonant SHG coefficient of d 33 ∼ −222 ± 30 pm V −1 at a fundamental wavelength of 2 µm, which is ≈7 times larger than that of the commercial AgGaSe 2 with a comparable bandgap. Density functional theory (DFT) calculations of the linear and nonlinear optical properties exhibit reasonable agreement with the experimental measurements, revealing the chemical origin of the enhanced properties. Moreover, SnP 2 Se 6 can exhibit both type-I and type-II phase matching over a wide spectral range, fulfilling one of the key criteria for an ideal NLO crystal. These exceptional properties position SnP 2 Se 6 as a highly promising candidate for NLO applications.

36 MATERIALS SCIENCE↗