Second harmonic generation (SHG) microscopy, involving the doubling of the frequency of light by a material, is a valuable characterization technique that is highly sensitive to local material symmetry at lengths scales close to the diffraction limit. The use of high-NA microscope objectives introduces an additional layer of complexity when performing quantitative analysis of SHG polarimetry data due to the appreciable effects that strong focusing has on the polarization of the probe beam. A systematic investigation of this problem is presented, producing analytical and numerical solutions of SHG polarimetry generated under high-NA lenses in a microscope setup. Modeling of a variety of standard samples, from single crystals to thin films, is performed and compared against experimental data.
Optical Second Harmonic Generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. The closed-form analytical solution of the nonlinear optical responses is essential for evaluating the optical responses of new materials whose optical properties are unknown a priori. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry (♯SHAARP) for single interface (si) and in multilayers (ml) for homogeneous crystals. The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes predicted from the package using standard materials. SHAARP.si and SHAARP.ml are available through GitHub https://github.com/Rui-Zu/SHAARP and https://github.com/bzw133/SHAARP.ml, respectively.
The development of CMOS-compatible nonlinear optical materials is essential for the continued growth of integrated photonics. This work investigates B-substituted AlN as a novel material platform with suitability towards UV light generation using second harmonic generation. The linear and nonlinear optical properties are characterized as a function of B composition. An enhancement of second harmonic generation coefficients with B substitution is observed, accompanied by a minor reduction in the bandgap. A waveguide structure is fabricated and used to measure loss in sputter-deposited films. A quasi-phase-matched ferroelectric domain pattern is produced and efficient second harmonic generation of UV light demonstrated.
Optical second harmonic generation (SHG) is a process that doubles the photon frequency and is widely used to detect broken inversion symmetry and local polar order. Analytical SHG modeling is essential to connect experimental results to material properties, such as point group symmetry and SHG susceptibilities. However, complexity builds up when the crystal exhibits low symmetry, absorption, and consists of multiple interfaces. Thus, the SHG model in the literature involves many approximations, leading to a scattered dataset of reported SHG properties. Here, we have developed an open-source package called ♯SHAARP which derives analytical solutions and performs numerical simulations of reflected SHG from crystals with arbitrary symmetry group, orientation, complex and anisotropic linear dielectric tensors with frequency dispersion, a general SHG tensor, and any polarization state of the incident and SHG light. ♯SHAARP enables accurate SHG analysis of a broad range of materials.
The correlated polar semimetal Ca3Ru2O7 exhibits a rich phase diagram including two magnetic transitions (TN =56 K and TC =48 K) with the appearance of an insulating-like pseudogap (at TC ). In addition, there is a crossover back to metallic behavior at T∗=30 K, the origin of which is still under debate. We utilized ultrafast optical pump optical probe spectroscopy to investigate quasi- particle dynamics as a function of temperature in this enigmatic quantum material. n conjunction with density functional theory, our experimental results synergistically reveal the origin of the T-dependent pseudogap. Further, our data and analysis indicate that the T∗ emerges as a natural consequence of T-dependent gapping out of carriers, and does not correspond to a separate electronic transition. Our results highlight the value of low fluence ultrafast optics as a sensitive probe of low energy electronic structure, thermodynamic parameters, and transport properties of Ruddlesden-Popper ruthenates.
Using time- and spatially-resolved hard X-ray diffraction microscopy, the striking structural and electrical dynamics upon optical excitation of a single crystal of BaTiO3 are simultaneously captured on sub-nanoseconds and nanoscale within individual ferroelectric domains and across walls. A large emergent photo-induced electric field of up to 20 million volts per meter is discovered in a surface layer of the crystal, which then drives polarization and lattice dynamics that are dramatically dis- tinct in a surface layer versus bulk regions. A dynamical phase-field modeling (DPFM) method is developed that reveals the microscopic origin of these dynamics, leading to GHz polarization and elastic waves travelling in the crystal with sonic speeds and spatially varying frequencies. The ad- vance of spatiotemporal imaging and dynamical modeling tools open opportunities of disentangling ultrafast processes in complex mesoscale structures such as ferroelectric domains
Phononic crystals and acoustic metamaterials enable the precise control of elastic properties, even in ranges inaccessible to traditional materials, making them useful for applications ranging from acoustic waveguiding to thermoelectrics. In particular, surface phononic crystals (SPCs) consisting of periodic nanolines on a semi-infinite substrate can be used to generate narrow bandwidth pseudosurface acoustic waves with exquisite sensitivity to the elastic properties of the underlying substrate. Tuning the period of the surface phononic crystal tunes the penetration depth of the pseudosurface wave, and thus selectively probes different depths of layered substrates. In our experiments, we use ultrafast near infrared laser pulses to excite these waves in the hypersonic frequency range by illuminating absorbing metallic nanolines fabricated on top of complex substrates. We probe the nanoscale dynamics launched by our SPCs via pump-probe spectroscopy where we monitor the diffraction of ultrafast pulses of extreme ultraviolet light generated via tabletop high harmonic generation. We then extract the mechanical properties of the substrate by comparing our measurements to quantitative finite element analysis. Utilizing this technique, we characterize the effective elastic and thermal transport properties of 3D periodic semiconductor metalattices.
Complex oxides and strongly correlated electron systems are at the forefront of science due to their exquisite potential for optical, spintronic, transducing/actuating, multiferroic, electrochemical, and superconducting property enhancements. Accordingly, at the nanoscale, engineering of complex oxide compounds is a promising route for discovery of novel quantum functionalities in a vast space of synthesis technique, calling for high-resolution control and visualization of physical properties and their structural basis. The advent of optical pulse techniques and related instrumentation advances is used to access dynamical separation of correlated orders that hide at equilibrium and also to create novel phases, not available via mainstream synthesis techniques. In this this talk, I will discuss resonant and non-resonant spectroscopic manipulation of phase transitions in nanoferroic oxides, focusing on ultrafast optical creation of artificial supercrystals in epitaxial superlattices. While table top nonlinear optical techniques are used to access the ferroic properties, synchrotron based time-resolved structural techniques, including diffraction and spectroscopy are decisive tools for revealing the nature of orderings in superstructures, their symmetries, phase quantification and spatial distribution with sub-micron resolution.
We capture the spatio-temporal oscillations within large individual ferroelectric domains and across domain walls upon optical excitation in a single crystal of BaTiO3 with ~350 nm lateral resolution and ~100 ps temporal resolution using synchrotron x-ray pulses as probes. Spatially resolved ultrafast mapping across domain walls reveals that the optical excitation pump can generate GHz acoustic standing waves of different frequencies between the surface and buried domain wall interfaces at different depths. Phase-field simulations reveal that a thermo-electro-acoustic mechanism can quantitatively explain the observed dynamics. The study reveals the importance of combined spatial and temporal resolution for understanding ultrafast dynamics in inhomogeneous microstructures.
ZnSe and other zinc chalcogenide semiconductor materials can be doped with divalent transition metal ions to create a
mid-IR laser gain medium with active function in the wavelength range 2 - 5 microns and potentially beyond using
frequency conversion. As a step towards fiberized laser devices, we have manufactured ZnSe semiconductor fiber
waveguides with low (less than 1dB/cm at 1550nm) optical losses, as well as more complex ternary alloys with
ZnSxSe(1-x) stoichiometry to potentially allow for annular heterostructures with effective and low order mode corecladding
waveguiding.
Integration of semiconductor and metal structures into optical fibers to enable fusion of semiconductor optoelectronic
function with glass optical fibers is discussed. A chemical vapor deposition (CVD)-like process, adapted for high pressure
flow within microstructured optical fibers allows for flexible fabrication of such structures. Integration of semiconductor
optoelectronic devices such as lasers, detectors, and modulators into fibers may now become possible.
We present spatial mapping of fluorescence and Raman spectra across grains and grain boundaries in a transparent Nd-YAG laser material with 5 at% Nd- doping using confocal scanning optical microscopy. These signals do not show any significant spectral shifts, indicating exceptional compositional uniformity in the bulk and grain boundaries. Changes in the intensity of Raman and fluorescent signals between grains and grain boundaries are observed, arising primarily from scattering at the grain boundaries both in the interior and the surface of the ceramic.
We have recently fabricated continuous semiconducting micro and nanowires within the empty spaces of highly ordered microstructured (e.g., photonic crystal or holey) optical fibers (MOF's). These systems contain the highest aspect ratio semiconductor micro- and nanowires yet produced by any method: centimeters long and ~100 nm in diameter. These structures combine the flexible light guiding capabilities of an optical fiber with the electronic and optical functionalities of semiconductors and have many potential applications for in-fiber sensing, including in-fiber detection, modulation, and generation of light.
A change in the Li/(Li+Ta) ratio in LiTaO3 crystals from 0.485 (congruent) to ~0.5 (stoichiometric) results in a up to 130 times reduction in coercive fields for domain reversal and an elimination of the internal fields and domain backswitching. Dramatic differences in the fatigue behavior are also observed, that results in an electro-optic effect that is very sensitive to electrodes in stoichiometric compositions and rather insensitive in congruent compositions.
We report on several recently demonstrated microphotonic devices based in ferroelectric single crystals. The device concept is to micro-pattern ferroelectric domains in the shape of lenses and prisms whose refractive index is electric field tunable through the electro-optic effect. Two different devices have been fabricated and tested. The performance of an integrated lens and scanner device is demonstrated with electric field tunable focusing power and a scanning range of 14.6°. A 2-stage cascaded horn-shaped scanner is demonstrated with a scanning range of 25.4° at 5 kHz. Ferroelectric materials offer a unique platform for integrating several optical functions, like focusing, scanning, and frequency conversion, all in the same device.
We report theoretical and experimental studies of 1-D and 2-d tunable nonlinear photonic crystals made of liquid crystal or liquid crystal infiltrated periodic structures. Theoretical modeling shows that such structures exhibit tunable bandgap, and sugar-prism effect. Experimentally, we have demonstrated the possibility of writing dynamic or permanent [but switchable] index gratings to dye-doped LC films that act as planar waveguides.
Dynamic scanning and focusing of a laser beam using a robust integrated solid state platform is desirable for many space-based applications including free-space optical communications, target tracking, and optical data storage/processing. Electro-optic devices offer promise as an ideal platform for such applications. However, the relatively low focal powers and scan angles of existing electro-optic devices have limited their use in these areas. Recently, we have applied state of the art fabrication techniques and design optimization to achieve the first integrated lens and scanner device capable of collimating and focusing beams with input diameters of a few microns, then scanning the beam through a large angular range (nearly 20 degrees). The device, fabricated in a bulk LiTaO3 crystal, is deal for coupling light into or out of channel waveguide or fiber optic systems. We will discuss the expected performance of the existing device in a radiation environment for space-based applications. In addition, we will discuss the expected performance of similarly optimized devices fabricated in other ferroelectric materials, radiation hardened and otherwise.
We demonstrate two high-speed electro-optic devices: an integrated lens/scanner and a variable radius collimating lens stack fabricated on a single crystal of Z-cut LiTaO3. The lens and scanner components consist of lithographically defined domain-inverted regions extending through the thickness of the crystal. A lens power of 0.233 cm-1kV-1, a deflection angle of 12.68 mrad kV-1, and a scan rate of 225 kHz at 375 V were observed. The collimating lens stack is theoretically capable of collimating the output from 2 - 10 micron diameter channel waveguides.
An in-built internal field of 5 KV/mm was measured in Z-cut LiTaO3 single crystals in the direction of the original polarization. This was reflected in the asymmetry (along the field axis) in the polarization hysteresis curve as a function of external electric field. Measurement of internal field as a function of crystal thickness revealed that the internal field is a volume effect. Using infrared absorption measurements, the spectrum of the hydroxl ions (OH-) present in these crystals was measured at room temperature. The shape of the spectrum changes with polarization reversal in these crystals indicating a strong correlation with the direction of internal field with respect to the polarization direction. It suggests that the origin of internal field lies in point defect complexes involving OH- ions.
The coercive field for domain reversal in a 0.5 mm Z-cut LiTaO3 was measured to be 21 KV/mm. However, if the polarization of the crystal is reversed using an electric field of 21 KV/mm, the coercive field for a second reversal is found to be 11 KV/mm. This asymmetry is due to the presence of an in-built internal field of 5 KV/mm in the virgin crystal. If the electron beam writing is done on the new C-face of the polarization reversed region of the crystal, (1) no cracking was observed, (2) the writing required less charge for domain inversion because of the reduced coercive field, thereby facilitating shorter scan times. We have obtained uniform 3.6 micrometers period domain inversion grating using this technique.
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