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DOE OSTI2015

Resolution enhancement in nonlinear photoacoustic imaging

Nonlinear processes can be exploited to gain access to more information than is possible in the linear regime. Nonlinearity modifies the spectra of the excitation signals through harmonic generation, frequency mixing, and spectral shifting, so that features originally outside the detector range can be detected. Here, we present an experimental study of resolution enhancement for photoacoustic imaging of thin metal layers immersed in water. In this case, there is a threshold in the excitation below which no acoustic signal is detected. Above threshold, the nonlinearity reduces the width of the active area of the excitation beam, resulting in a narrower absorption region and thus improved spatial resolution. This gain is limited only by noise, as the active area of the excitation can be arbitrarily reduced when the fluence becomes closer to the threshold. Here, we demonstrate a two-fold improvement in resolution and quantify the image quality as the excitation fluence goes through threshold.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Nonlinear focusing of ultrasonic waves by an axisymmetric diffraction grating embedded in water

We report the nonlinear focusing of ultrasonic waves by an axisymmetric diffraction grating immersed in water. In the linear regime, the system presents high focal gain (32 dB), with a narrow beam-width and intense side lobes as it is common in focusing by Fresnel-like lenses. Activating the nonlinearity of the host medium by using high amplitude incident waves, the focusing properties of the lens dramatically change. Theoretical predictions show that the focal gain of the system extraordinary increases in the strongly nonlinear regime (Mach number of 6.1 × 10{sup −4}). Particularly, the harmonic generation is locally activated at the focal spot, and the second harmonic beam is characterized by strongly reduced side-lobes and an excellent beam profile as experiments show in agreement with theory. The results can motivate applications in medical therapy or second harmonic imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

A comparative numerical analysis of linear and nonlinear aerodynamic sound generation by vortex disturbances in homentropic constant shear flows

Aerodynamic sound generation in shear flows is investigated in the light of the breakthrough in hydrodynamics stability theory in the 1990s, where generic phenomena of non-normal shear flow systems were understood. By applying the thereby emerged short-time/non-modal approach, the sole linear mechanism of wave generation by vortices in shear flows was captured [G. D. Chagelishvili, A. Tevzadze, G. Bodo, and S. S. Moiseev, “Linear mechanism of wave emergence from vortices in smooth shear flows,” Phys. Rev. Lett. 79, 3178-3181 (1997); B. F. Farrell and P. J. Ioannou, “Transient and asymptotic growth of two-dimensional perturbations in viscous compressible shear flow,” Phys. Fluids 12, 3021-3028 (2000); N. A. Bakas, “Mechanism underlying transient growth of planar perturbations in unbounded compressible shear flow,” J. Fluid Mech. 639, 479-507 (2009); and G. Favraud and V. Pagneux, “Superadiabatic evolution of acoustic and vorticity perturbations in Couette flow,” Phys. Rev. E 89, 033012 (2014)]. Its source is the non-normality induced linear mode-coupling, which becomes efficient at moderate Mach numbers that is defined for each perturbation harmonic as the ratio of the shear rate to its characteristic frequency. Based on the results by the non-modal approach, we investigate a two-dimensional homentropic constant shear flow and focus on the dynamical characteristics in the wavenumber plane. This allows to separate from each other the participants of the dynamical processes — vortex and wave modes — and to estimate the efficacy of the process of linear wave-generation. This process is analyzed and visualized on the example of a packet of vortex modes, localized in both, spectral and physical, planes. Further, by employing direct numerical simulations, the wave generation by chaotically distributed vortex modes is analyzed and the involved linear and nonlinear processes are identified. The generated acoustic field is anisotropic in the wavenumber plane, which results in highly directional linear sound radiation, whereas the nonlinearly generated waves are almost omni-directional. As part of this analysis, we compare the effectiveness of the linear and nonlinear mechanisms of wave generation within the range of validity of the rapid distortion theory and show the dominance of the linear aerodynamic sound generation. Finally, topological differences between the linear source term of the acoustic analogy equation and of the anisotropic non-normality induced linear mechanism of wave generation are found.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Nonlinear optical sub-bandgap excitation of ZnO-based photonic resonators

Zinc oxide (ZnO) is a versatile candidate for photonic devices due to its highly efficient optical emission. However, for pumping of ZnO photonic devices UV-sources are required. Here, we investigate the alternative usage of widely available pulsed near-infrared (NIR)-sources and compare the efficiency of linear and nonlinear excitation processes. We found that bulk ZnO, ZnO thin films grown by molecular beam epitaxy, and ZnO/SiO{sub 2} microdisk devices exhibit strong nonlinear response when excited with NIR pulses (λ ≈ 1060 nm). In addition, we show that the ZnO/SiO{sub 2} microdisks exhibit sharp whispering gallery modes over the blue-yellow part of the visible spectrum for both excitation conditions and high Q-factors up to Q = 4700. The results demonstrate that nonlinear excitation is an efficient way to pump ZnO photonic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Second order optical nonlinearity in silicon by symmetry breaking

Although silicon does not possess a dipolar bulk second order nonlinear susceptibility due to its centro-symmetric crystal structure, in recent years several attempts were undertaken to create such a property in silicon. This review presents the different sources of a second order susceptibility (χ{sup (2)}) in silicon and the connected second order nonlinear effects which were investigated up to now. After an introduction, a theoretical overview discusses the second order nonlinearity in general and distinguishes between the dipolar contribution—which is usually dominating in non-centrosymmetric structures—and the quadrupolar contribution, which even exists in centro-symmetric materials. Afterwards, the classic work on second harmonic generation from silicon surfaces in reflection measurements is reviewed. Due to the abrupt symmetry breaking at surfaces and interfaces locally a dipolar second order susceptibility appears, resulting in, e.g., second harmonic generation. Since the bulk contribution is usually small, the study of this second harmonic signal allows a sensitive observation of the surface/interface conditions. The impact of covering films, strain, electric fields, and defect states at the interfaces was already investigated in this way. With the advent of silicon photonics and the search for ever faster electrooptic modulators, the interest turned to the creation of a dipolar bulk χ{sup (2)} in silicon. These efforts have been focussing on several experiments applying an inhomogeneous strain to the silicon lattice to break its centro-symmetry. Recent results suggesting the impact of electric fields which are exerted from fixed charges in adjacent covering layers are also included. After a subsequent summary on “competing” concepts using not Si but Si-related materials, the paper will end with some final conclusions, suggesting possible future research direction in this dynamically developing field.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

The second– and third– order nonlinear optical properties and electronic transition of a NLO chromophore: A DFT study

It is well known that the practical applications of second-order and third-order nonlinear optical (NLO) materials have been reported in modern technology, such as optical data processing, transmission and storage, etc. In this respect, the linear and nonlinear optical parameters (the molecular static polarizability (α), and the first–order static hyperpolarizability (β{sub 0}), the second–order static hyperpolarizability (γ)), UV-vis spectra and HOMO and LUMO energies of 2-(1′-(4’’’-Methoxyphenyl)-5′-(thien-2″-yl)pyrrol-2′-yl)-1,3-benzothiazole were investigated by using the HSEh1PBE/6–311G(d,p) level of density functional theory. The UV–vis spectra were simulated using TD/HSEh1PBE/6– 311G(d,p) level, and the major contributions to the electronic transitions were obtained. The molecular hardness (η) and electronegativity (χ) parameters were also obtained by using molecular frontier orbital energies. The NLO parameters of the title compound were calculated, and obtained data were compared with that of para-Nitroaniline (pNA) which is a typical NLO material and the corresponding experimental data. Obtained data of the chromosphere display significant molecular second-and third-nonlinearity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Linear and nonlinear instability in vertical counter-current laminar gas-liquid flows

We consider the genesis and dynamics of interfacial instability in vertical gas-liquid flows, using as a model the two-dimensional channel flow of a thin falling film sheared by counter-current gas. The methodology is linear stability theory (Orr-Sommerfeld analysis) together with direct numerical simulation of the two-phase flow in the case of nonlinear disturbances. We investigate the influence of two main flow parameters on the interfacial dynamics, namely the film thickness and pressure drop applied to drive the gas stream. To make contact with existing studies in the literature, the effect of various density contrasts is also examined. Energy budget analyses based on the Orr-Sommerfeld theory reveal various coexisting unstable modes (interfacial, shear, internal) in the case of high density contrasts, which results in mode coalescence and mode competition, but only one dynamically relevant unstable interfacial mode for low density contrast. A study of absolute and convective instability for low density contrast shows that the system is absolutely unstable for all but two narrow regions of the investigated parameter space. Direct numerical simulations of the same system (low density contrast) show that linear theory holds up remarkably well upon the onset of large-amplitude waves as well as the existence of weakly nonlinear waves. For high density contrasts, corresponding more closely to an air-water-type system, linear stability theory is also successful at determining the most-dominant features in the interfacial wave dynamics at early-to-intermediate times. Nevertheless, the short waves selected by the linear theory undergo secondary instability and the wave train is no longer regular but rather exhibits chaotic motion. The same linear stability theory predicts when the direction of travel of the waves changes — from downwards to upwards. We outline the practical implications of this change in terms of loading and flooding. The change in direction of the wave propagation is represented graphically in terms of a flow map based on the liquid and gas flow rates and the prediction carries over to the nonlinear regime with only a small deviation.

42 ENGINEERING↗
DOE OSTI2016

Experimental implementation of a nonlinear beamsplitter based on a phase-sensitive parametric amplifier

Beamsplitters have played an important role in quantum optics experiments. They are often used to split and combine two beams, especially in the construct of an interferometer. In this letter, we experimentally implement a nonlinear beamsplitter using a phase-sensitive parametric amplifier, which is based on four-wave mixing in hot rubidium vapor. Here we show that, despite the different frequencies of the two input beams, the output ports of the nonlinear beamsplitter exhibit interference phenomena. We make measurements of the interference fringe visibility and study how various parameters, such as the intensity gain of the amplifier, the intensity ratio of the two input beams, and the one and two photon detunings, affect the behavior of the nonlinear beamsplitter. It may find potential applications in quantum metrology and quantum information processing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Thermally stimulated nonlinear refraction in gelatin stabilized Cu-PVP nanocomposite thin films

This article illustrates investigations on thermally stimulated third order nonlinear refraction of Cu-PVP nanocomposite thin films. Cu nanoparticles have been synthesized using chemical reduction method and thin films in PVP matrix have been obtained using spin coating technique. Thin films have been characterized by X-ray diffraction (XRD) and Ultraviolet-visible (UV-vis) spectroscopyfor structural and linear optical studies. Third order nonlinear refraction studies have been performed using closed aperture z-scan technique under continuous wave (CW) He-Ne laser. Cu-PVP nanocomposites are found to exhibit strong nonlinear refractive index stimulated by thermal lensing effect.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Orbit-based analysis of nonlinear energetic ion dynamics in tokamaks. II. Mechanisms for rapid chirping and convective amplification

The nonlinear interactions between shear Alfvén modes and tangentially injected beam ions in the 150–400 keV range are studied numerically in realistic geometry for a JT-60U tokamak scenario. In Paper I, which was reported in the companion paper, the recently developed orbit-based resonance analysis method was used to track the resonant frequency of fast ions during their nonlinear evolution subject to large magnetic and electric drifts. Here, that method is applied to map the wave-particle power transfer from the canonical guiding center phase space into the frequency-radius plane, where it can be directly compared with the evolution of the fluctuation spectra of fast-ion-driven modes. Using this technique, we study the nonlinear dynamics of strongly driven shear Alfvén modes with low toroidal mode numbers n = 1 and n = 3. In the n = 3 case, both chirping and convective amplification can be attributed to the mode following the resonant frequency of the radially displaced particles, i.e., the usual one-dimensional phase locking process. In the n = 1 case, a new chirping mechanism is found, which involves multiple dimensions, namely, wave-particle trapping in the radial direction and phase mixing across velocity coordinates.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Edge localized mode rotation and the nonlinear dynamics of filaments

Edge Localized Modes (ELMs) rotating precursors were reported few milliseconds before an ELM crash in several tokamak experiments. Also, the reversal of the filaments rotation at the ELM crash is commonly observed. In this article, we present a mathematical model that reproduces the rotation of the ELM precursors as well as the reversal of the filaments rotation at the ELM crash. Linear ballooning theory is used to establish a formula estimating the rotation velocity of ELM precursors. The linear study together with nonlinear magnetohydrodynamic simulations give an explanation to the rotations observed experimentally. Unstable ballooning modes, localized at the pedestal, grow and rotate in the electron diamagnetic direction in the laboratory reference frame. Approaching the ELM crash, this rotation decreases corresponding to the moment when the magnetic reconnection occurs. During the highly nonlinear ELM crash, the ELM filaments are cut from the main plasma due to the strong sheared mean flow that is nonlinearly generated via the Maxwell stress tensor.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Nonlinear optical characterization of graphite oxide thin film by open aperture Z-scan technique

In this paper we explore the structural characterization of graphite oxide powder prepared from graphite powder by oxidation via modified Hummers method. The nonlinear optical properties of the spin coated graphite oxide thin film is also explored by open aperture Z-Scan technique. Structural and physiochemical properties of the samples were investigated with the help of Fourier Transform Infrared Spectroscopy (FTIR) and Raman Spectroscopy (Raman).The results of FT-IR and Raman spectroscopy showed that the graphite is oxidized by strong oxidants and the oxygen atoms are introduced into the graphite layers forming C=C, O-H and –C-H groups. The synthesized sample has good crystalline nature with lesser defects. The nonlinear optical property of GO thin film was studied by open aperture Z-Scan technique using Q-switched Nd-Yag Laser at 532 nm. The Z-scan plot showed that the investigated GO thin film has saturable absorption behavior. The nonlinear absorption coefficient and saturation intensity were also estimated to explore its applications in Q switched mode locking laser systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Nonlinear negative refraction by difference frequency generation

Negative refraction has attracted much interest for its promising capability in imaging applications. Such an effect can be implemented by negative index meta-materials, however, which are usually accompanied by high loss and demanding fabrication processes. Recently, alternative nonlinear approaches like phase conjugation and four wave mixing have shown advantages of low-loss and easy-to-implement, but associated problems like narrow accepting angles can still halt their practical applications. Here, we demonstrate theoretically and experimentally a scheme to realize negative refraction by nonlinear difference frequency generation with wide tunability, where a thin Beta barium borate slice serves as a negative refraction layer bending the input signal beam to the idler beam at a negative angle. Furthermore, we realize optical focusing effect using such nonlinear negative refraction, which may enable many potential applications in imaging science.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Oscillating plasma bubble and its associated nonlinear studies in presence of low magnetic field

Oscillating plasma bubbles have been created around a cylindrical mesh grid of 75% optical transparency in a DC plasma system with a low magnetic field. Plasma bubbles are created by developing ion density gradient around a cylindrical grid of 20 cm in diameter and 25 cm in height, inserted into the plasma. Relaxation and contraction of the plasma bubbles in the presence of external conditions, such as magnetic field and pressure, have been studied. A Langmuir probe has been used to detect the plasma floating potential fluctuations at different imposed experimental conditions. Nonlinear behavior of the system has been characterized by adopting nonlinear techniques such as Fast Fourier Transform, Phase Space Plot, and Recurrence Plot. It shows that the system creates highly nonlinear phenomena associated with the plasma bubble under the imposed experimental conditions. A theoretical and numerical model has also been developed to satisfy the observed experimental analysis. Moreover, observations are extended further to study the growth of instability associated with the plasma bubbles. The intention of the present work is to correlate the findings about plasma bubbles and their related instability with the one existing in the equatorial F-region of the ionosphere.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Magnetoplasmonic RF mixing and nonlinear frequency generation

We present the design of a magnetoplasmonic Mach-Zehnder interferometer (MZI) modulator facilitating radio-frequency (RF) mixing and nonlinear frequency generation. This is achieved by forming the MZI arms from long-range dielectric-loaded plasmonic waveguides containing bismuth-substituted yttrium iron garnet (Bi:YIG). The magnetization of the Bi:YIG can be driven in the nonlinear regime by RF magnetic fields produced around adjacent transmission lines. Correspondingly, the nonlinear temporal dynamics of the transverse magnetization component are mapped onto the nonreciprocal phase shift in the MZI arms, and onto the output optical intensity signal. We show that this tunable mechanism can generate harmonics, frequency splitting, and frequency down-conversion with a single RF excitation, as well as RF mixing when driven by two RF signals. This magnetoplasmonic component can reduce the number of electrical sources required to generate distinct optical modulation frequencies and is anticipated to satisfy important applications in integrated optics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Entropic and gradient flow formulations for nonlinear diffusion

Nonlinear diffusion ∂{sub t}ρ = Δ(Φ(ρ)) is considered for a class of nonlinearities Φ. It is shown that for suitable choices of Φ, an associated Lyapunov functional can be interpreted as thermodynamic entropy. This information is used to derive an associated metric, here called thermodynamic metric. The analysis is confined to nonlinear diffusion obtainable as hydrodynamic limit of a zero range process. The thermodynamic setting is linked to a large deviation principle for the underlying zero range process and the corresponding equation of fluctuating hydrodynamics. For the latter connections, the thermodynamic metric plays a central role.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

A force-level theory of the rheology of entangled rod and chain polymer liquids. I. Tube deformation, microscopic yielding, and the nonlinear elastic limit

In this paper, we employ a first-principles-based, force-level approach to construct the anharmonic tube confinement field for entangled fluids of rigid needles, and also for chains described at the primitive-path (PP) level in two limiting situations where chain stretch is assumed to either be completely equilibrated or unrelaxed. The influence of shear and extensional deformation and polymer orientation is determined in a nonlinear elastic limit where dissipative relaxation processes are intentionally neglected. For needles and PP-level chains, a self-consistent analysis of transverse polymer harmonic dynamical fluctuations predicts that deformation-induced orientation leads to tube weakening or widening. In contrast, for deformed polymers in which chain stretch does not relax, we find tube strengthening or compression. For all three systems, a finite maximum transverse entanglement force localizing the polymers in effective tubes is predicted. The conditions when this entanglement force can be overcome by an externally applied force associated with macroscopic deformation can be crisply defined in the nonlinear elastic limit, and the possibility of a “microscopic absolute yielding” event destroying the tube confinement can be analyzed. For needles and contour-relaxed PP chains, this force imbalance occurs at a stress of order the equilibrium shear modulus and a strain of order unity, corresponding to a mechanically fragile entanglement tube field. However, for unrelaxed stretched chains, tube compression stabilizes transverse polymer confinement, and there appears to be no force imbalance. These results collectively suggest that the crossover from elastic to irreversible viscous response requires chain retraction to initiate disentanglement. Finally, we qualitatively discuss comparisons with existing phenomenological models for nonlinear startup shear, step strain, and creep rheology experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Nonlinear saturation of the Weibel instability

The growth and saturation of magnetic fields due to the Weibel instability (WI) have important implications for laboratory and astrophysical plasmas, and this has drawn significant interest recently. Since the WI can generate a large magnetic field from no initial field, the maximum magnitudes achieved can have significant consequences for a number of applications. Hence, an understanding of the detailed dynamics driving the nonlinear saturation of the WI is important. This work considers the nonlinear saturation of the WI when counter-streaming populations of initially unmagnetized electrons are perturbed by a magnetic field oriented perpendicular to the direction of streaming. Previous works have found magnetic trapping to be important and connected electron skin depth spatial scales to the nonlinear saturation of the WI. The results presented in this work are consistent with these findings for a high-temperature case. However, using a high-order continuum kinetic simulation tool, this work demonstrates that when the electron populations are colder, a significant electrostatic potential develops that works with the magnetic field to create potential wells. The electrostatic field develops due to transverse flows induced by the WI and in some cases is strengthened by a secondary instability. This field plays a key role in saturation of the WI for colder populations. In conclusion, the role of the electrostatic potential in Weibel instability saturation has not been studied in detail previously.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗