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Sample records for harmonic generation materials

  1. Harmonic generation in optical fibers

    SciTech Connect

    Sherborn, H.P.

    1990-05-01

    This patent describes an apparatus for providing second harmonic generated radiation. It comprises: an optical fiber disposed in a laser cavity, the optical fiber having a substantially single-mode core which is doped with an active laser material, the laser material being self-organizable to produce radiation by second harmonic generation, the laser material further being substantially transparent to the second harmonic generated radiation; and means for pumping the core of the optical fiber to produce laser radiation therein and the laser cavity further comprising means for extracting at least a portion of the second harmonic generated radiation.

  2. Organic materials for second harmonic generation. Final report

    SciTech Connect

    Twieg, R.J.

    1985-03-31

    Materials were chosen by screening the Cambridge Crystallographic Index for new noncentrosymmetric crystalline compounds, by screening commercially available materials or by synthesis of unique new substances. Measurements were then made on the powder form of these materials. Langmuir-Blodgett films were deposited and studied. In addition to the above studies, a computer program was developed to calculate (hyper) polarizabilities of organic molecules and thus aid in the selection of materials for testing. The nonlinear molecules have been divided into three classes according to absorption cutoff: 400 to 500 nm, 300 to 400 nm, and 200 to 300 nm. 108 refs., 7 tabs. (WRF)

  3. Single sub-50-attosecond pulse generation from chirp-compensated harmonic radiation using material dispersion

    SciTech Connect

    Kim, Kyung Taec; Kim, Chul Min; Umesh, G.; Nam, Chang Hee; Baik, Moon-Gu

    2004-05-01

    A method for obtaining a single sub-50-attosecond pulse using harmonic radiation is proposed. For the generation of broad harmonic radiation during a single half-optical cycle, atoms are driven by a femtosecond laser pulse with intensity above the saturation intensity for optical field ionization and hence experience a large nonadiabatic increase of the laser electric field between optical cycles. Although the chirped structure of the harmonic radiation imposes a limit on the minimum achievable pulse duration, we demonstrate that its positive chirp can be compensated by the negative group delay dispersion of an appropriately selected x-ray filter material, used also for the spectral selection, resulting in a single attosecond pulse with a duration less than 50 as.

  4. Investigation of the Higher Harmonic Lamb Wave Generation in Hyperelastic Isotropic Material

    NASA Astrophysics Data System (ADS)

    Rauter, Natalie; Lammering, Rolf

    Micro-structural damages, such as micro-cracks and voids, give locally rise to stresses and may initiate subsequent failure of structural components. Therefore, the development of methods for the detection of microstructural damage and the observation of their growth is an important and ongoing area of research, especially for thin-walled structures. The proposed method for the detection is based on the nonlinearity caused by the micro-structural damages. Lamb waves are generated which induce simultaneously higher harmonic modes due the inherent nonlinearity. For detailed investigations, numerical simulations are essential. In this work, the nonlinearity is modeled by the material law, which is based on the Neo- Hookean and Mooney-Rivlin material models. In contrast to previous studies, which used third order elastic coefficients, these hyperelastic material models are widely accepted, frequently used, and implemented in commonly available FEM software. In the numerical investigations, Lamb waves are generated in a thin-walled aluminum plate with windowed sine burst signals. Due to the nonlinearity in the material law, the waves are not only observed at the excitation frequency, but also at higher harmonic frequencies. Excitation at especially selected frequencies evoke the cumulative effect, and thus gives rise to the amplitudes of the higher harmonics. Comparing the S1-S2 and S2-S4 mode pairs clearly show the higher sensitivity of the latter to the material nonlinearity. This matches with previous published experimental results. Finally, it is shown that the results obtained agree qualitatively well with numerical analyses, in which the micro-structural damages are modeled directly by a respective finite element discretization.

  5. Designing a deep-ultraviolet nonlinear optical material with a large second harmonic generation response.

    PubMed

    Wu, Hongping; Yu, Hongwei; Yang, Zhihua; Hou, Xueling; Su, Xin; Pan, Shilie; Poeppelmeier, Kenneth R; Rondinelli, James M

    2013-03-20

    The generation of intense coherent deep-UV light from nonlinear optical materials is crucial to applications ranging from semiconductor photolithography and laser micromachining to photochemical synthesis. However, few materials with large second harmonic generation (SHG) and a short UV-cutoff edge are effective down to 200 nm. A notable exception is KBe2BO3F2, which is obtained from a solid-state reaction of highly toxic beryllium oxide powders. We designed and synthesized a benign polar material, Ba4B11O20F, that satisfies these requirements and exhibits the largest SHG response in known borates containing neither lone-pair-active anions nor second-order Jahn-Teller-active transition metals. We developed a microscopic model to explain the enhancement, which is unexpected on the basis of conventional anionic group theory arguments. Crystal engineering of atomic displacements along the polar axis, which are difficult to attribute to or identify within unique anionic moieties, and greater cation polarizabilities are critical to the design of next-generation SHG materials. PMID:23448539

  6. Optical harmonic generator

    DOEpatents

    Summers, Mark A.; Eimerl, David; Boyd, Robert D.

    1985-01-01

    A pair of uniaxial birefringent crystal elements are fixed together to form a serially arranged, integral assembly which, alternatively, provides either a linearly or elliptically polarized second-harmonic output wave or a linearly polarized third-harmonic output wave. The "extraordinary" or "e" directions of the crystal elements are oriented in the integral assembly to be in quadrature (90.degree.). For a second-harmonic generation in the Type-II-Type-II angle tuned case, the input fundamental wave has equal amplitude "o" and "e" components. For a third-harmonic generation, the input fundamental wave has "o" and "e" components whose amplitudes are in a ratio of 2:1 ("o":"e" reference first crystal). In the typical case of a linearly polarized input fundamental wave this can be accomplished by simply rotating the crystal assembly about the input beam direction by 10.degree.. For both second and third harmonic generation input precise phase-matching is achieved by tilting the crystal assembly about its two sensitive axes ("o").

  7. Optical harmonic generator

    DOEpatents

    Summers, M.A.; Eimerl, D.; Boyd, R.D.

    1982-06-10

    A pair of uniaxial birefringent crystal elements are fixed together to form a serially arranged, integral assembly which, alternatively, provides either a linearly or elliptically polarized second-harmonic output wave or a linearly polarized third-harmonic output wave. The extraordinary or e directions of the crystal elements are oriented in the integral assembly to be in quadrature (90/sup 0/). For a second-harmonic generation in the Type-II-Type-II angle tuned case, the input fundamental wave has equal amplitude o and e components. For a third-harmonic generation, the input fundamental wave has o and e components whose amplitudes are in a ratio of 2:1 (o:e reference first crystal). In the typical case of a linearly polarized input fundamental wave this can be accomplished by simply rotating the crystal assembly about the input beam direction by 10/sup 0/. For both second and third harmonic generation input precise phase-matching is achieved by tilting the crystal assembly about its two sensitive axeses (o).

  8. Optical second-harmonic generation measurements of porous low-k dielectric materials

    NASA Astrophysics Data System (ADS)

    Atkin, Joanna; Shaw, Thomas; Laibowitz, Robert; Heinz, Tony

    2009-03-01

    Low-k dielectric materials based on porous carbon-doped oxides, with relative dielectric constants as low as 2.1, are widely used as thin insulating films in the microelectronics industry. Knowledge of these materials' basic electronic properties, such as energy gaps, barrier heights, and trap states, is essential for modeling their electrical leakage and stability characteristics. We use femtosecond laser pulses to probe the dynamics of charge-carrier transfer processes across Si/LKD interfacial barriers by optical second harmonic generation (SHG). Larger electric fields from multiphoton injection can be developed in Si/LKD systems compared to Si/SiO2, indicating a significantly higher density of traps in the LKD. This is consistent with previously reported measurements of trap density by photoinjection techniques^*. We will also discuss results on the dynamics of discharging and on the dependence of charging phenomena on layer thickness. ^*J. M. Atkin, D. Song, T. M. Shaw, E. Cartier, R. B. Laibowitz, and T. F. Heinz, J. Appl. Phys. 103, 094104 (2008).

  9. Next generation data harmonization

    NASA Astrophysics Data System (ADS)

    Armstrong, Chandler; Brown, Ryan M.; Chaves, Jillian; Czerniejewski, Adam; Del Vecchio, Justin; Perkins, Timothy K.; Rudnicki, Ron; Tauer, Greg

    2015-05-01

    Analysts are presented with a never ending stream of data sources. Often, subsets of data sources to solve problems are easily identified but the process to align data sets is time consuming. However, many semantic technologies do allow for fast harmonization of data to overcome these problems. These include ontologies that serve as alignment targets, visual tools and natural language processing that generate semantic graphs in terms of the ontologies, and analytics that leverage these graphs. This research reviews a developed prototype that employs all these approaches to perform analysis across disparate data sources documenting violent, extremist events.

  10. Organometallic Salts Generate Optical Second Harmonics

    NASA Technical Reports Server (NTRS)

    Marder, Seth R.; Perry, Joseph W.

    1991-01-01

    Series of organometallic salts exhibit large second-order dielectric susceptibilities, as evidenced by generation of second harmonics when illuminated at visible and near-infrared wavelengths. Investigations of these and related compounds continue with view toward development of materials for use as optical second-harmonic generators, electro-optical modulators, optical switches, piezoelectric sensors, and parametric crystals.

  11. Second harmonic generation and sum frequency generation

    SciTech Connect

    Pellin, M.J.; Biwer, B.M.; Schauer, M.W.; Frye, J.M.; Gruen, D.M.

    1990-01-01

    Second harmonic generation and sum frequency generation are increasingly being used as in situ surface probes. These techniques are coherent and inherently surface sensitive by the nature of the mediums response to intense laser light. Here we will review these two techniques using aqueous corrosion as an example problem. Aqueous corrosion of technologically important materials such as Fe, Ni and Cr proceeds from a reduced metal surface with layer by layer growth of oxide films mitigated by compositional changes in the chemical makeup of the growing film. Passivation of the metal surface is achieved after growth of only a few tens of atomic layers of metal oxide. Surface Second Harmonic Generation and a related nonlinear laser technique, Sum Frequency Generation have demonstrated an ability to probe the surface composition of growing films even in the presence of aqueous solutions. 96 refs., 4 figs.

  12. SURFACE ENHANCED SECOND HARMONIC GENERATION

    SciTech Connect

    Chen, C. K.; de Castro, A. R.B.; Shen, Y. R.

    1980-09-01

    Second harmonic generation at a silver-air interface was enhanced due to surface roughness by a factor of 10{sup 4}. The local field enhancement is believed to be responsible for the effect. An unusually broad luminescence background extending far beyond the antiStokes side of the second harmonic was also observed.

  13. Harmonic generation at high intensities

    SciTech Connect

    Schafer, K.J.; Krause, J.L.; Kulander, K.C.

    1993-06-01

    Atomic electrons subject to intense laser fields can absorb many photons, leading either to multiphoton ionization or the emission of a single, energetic photon which can be a high multiple of the laser frequency. The latter process, high-order harmonic generation, has been observed experimentally using a range of laser wavelengths and intensities over the past several years. Harmonic generation spectra have a generic form: a steep decline for the low order harmonics, followed by a plateau extending to high harmonic order, and finally an abrupt cutoff beyond which no harmonics are discernible. During the plateau the harmonic production is a very weak function of the process order. Harmonic generation is a promising source of coherent, tunable radiation in the XUV to soft X-ray range which could have a variety of scientific and possibly technological applications. Its conversion from an interesting multiphoton phenomenon to a useful laboratory radiation source requires a complete understanding of both its microscopic and macroscopic aspects. We present some recent results on the response of single atoms at intensities relevant to the short pulse experiments. The calculations employ time-dependent methods, which we briefly review in the next section. Following that we discuss the behavior of the harmonics as a function of laser intensity. Two features are notable: the slow scaling of the harmonic intensities with laser intensity, and the rapid variation in the phase of the individual harmonics with respect to harmonic order. We then give a simple empirical formula that predicts the extent of the plateau for a given ionization potential, wavelength and intensity.

  14. Spontaneous Polarization in Bio-organic Materials Studied by Scanning Pyroelectric Microscopy (SPEM) and Second Harmonic Generation Microscopy (SHGM)

    NASA Astrophysics Data System (ADS)

    Putzeys, T.; Wübbenhorst, M.; van der Veen, M. A.

    2015-06-01

    Bio-organic materials such as bones, teeth, and tendon generally show nonlinear optical (Masters and So in Handbook of Biomedical Nonlinear Optical Microscopy, 2008), pyro- and piezoelectric (Fukada and Yasuda in J Phys Soc Jpn 12:1158, 1957) properties, implying a permanent polarization, the presence of which can be rationalized by describing the growth of the sample and the creation of a polar axis according to Markov's theory of stochastic processes (Hulliger in Biophys J 84:3501, 2003; Batagiannis et al. in Curr Opin Solid State Mater Sci 17:107, 2010). Two proven, versatile techniques for probing spontaneous polarization distributions in solids are scanning pyroelectric microscopy (SPEM) and second harmonic generation microscopy (SHGM). The combination of pyroelectric scanning with SHG-microscopy in a single experimental setup leading to complementary pyroelectric and nonlinear optical data is demonstrated, providing us with a more complete image of the polarization in organic materials. Crystals consisting of a known polar and hyperpolarizable material, CNS (4-chloro-4-nitrostilbene) are used as a reference sample, to verify the functionality of the setup, with both SPEM and SHGM images revealing the same polarization domain information. In contrast, feline and human nails exhibit a pyroelectric response, but a second harmonic response is absent for both keratin containing materials, implying that there may be symmetry-allowed SHG, but with very inefficient second harmonophores. This new approach to polarity detection provides additional information on the polar and hyperpolar nature in a variety of (bio) materials.

  15. Echo-Enabled Harmonic Generation

    SciTech Connect

    Stupakov, Gennady; /SLAC

    2012-06-28

    A recently proposed concept of the Echo-Enabled Harmonic Generation (EEHG) FEL uses two laser modulators in combination with two dispersion sections to generate a high-harmonic density modulation in a relativistic beam. This seeding technique holds promise of a one-stage soft x-ray FEL that radiates not only transversely but also longitudinally coherent pulses. Currently, an experimental verification of the concept is being conducted at the SLAC National Accelerator Laboratory aimed at the demonstration of the EEHG.

  16. A comparative study of second-harmonic generation in plasmonic and dielectric gratings made of centrosymmetric materials (Presentation Recording)

    NASA Astrophysics Data System (ADS)

    Weismann, Martin; Gallagher, Dominic F. G.; Panoiu, Nicolae-Coriolan

    2015-09-01

    We present a new numerical method for the analysis of second-harmonic generation (SHG) in one- and two-dimensional (1D, 2D) diffraction gratings containing centrosymmetric quadratically nonlinear materials. Thus, the nonlinear optical properties of a material are determined by its symmetry properties: non-centrosymmetric materials lack inversion symmetry and therefore allow local even-order SHG in the bulk of the material, whereas this process is forbidden in centrosymmetric materials. The inversion symmetry of centrosymmetric materials is broken at their surface whence they allow local surface SHG. Additionally, centrosymmetric materials give rise to nonlocal (bulk) SHG. Our numerical method extends the linear generalized source method (GSM), which is an efficient numerical method for solving the problem of linear diffraction in periodic structures of arbitrary geometry. The nonlinear GSM is a three-step algorithm: for a given excitation at the fundamental frequency the linear field is computed using the linear GSM. This field gives rise to a nonlinear source polarization at the second harmonic (SH) frequency. This nonlinear polarization comprises surface and bulk polarizations as additional source terms and is subsequently used to compute the nonlinear near- and far-field optical response at the SH. We study the convergence characteristics of the nonlinear GSM for 1D and 2D periodic structures and emphasize the numerical intricacies caused by the surface SH polarization term specific to centrosymmetric materials. In order to illustrate the practical significance of our numerical method, we apply it to metallic gratings made of Au and Ag as well as dielectric grating structures made of silicon and investigate the relative contribution of the bulk and surface nonlinearity to the nonlinear optical response at the SH. Particular attention is paid to optical effects that have a competing influence to the nonlinear optical response of the grating structures, namely the

  17. High Harmonic Generation from Rotationally Excited Molecules

    NASA Astrophysics Data System (ADS)

    Lock, Robynne M.

    2011-12-01

    High harmonic generation (HHG) is understood through a three-step model. A strong laser field ionizes an atom or molecule. The free electron propagates in the laser field and may recombine with the atom or molecule leading to the generation of extreme ultraviolet or soft x-ray light at odd harmonics of the fundamental. Since the wavelength of the recombining electron is on the order of internuclear distances in molecules, HHG acts as a probe of molecular structure and dynamics. Conversely, control of the molecules leads to control of the properties (intensity, phase, and polarization) of the harmonic emission. Rotationally exciting molecules provides field-free molecular alignment at time intervals corresponding to fractions of the rotational period of the molecule. Alignment is necessary for understanding how the harmonic emission depends on molecular structure and alignment. Additionally, HHG acts as a probe of the rotational wavepackets. This thesis reports three experiments on HHG from rotationally excited molecules. Before we can use HHG as a probe of complex molecular dynamics or control harmonic properties through molecules, the harmonic emission from aligned, linear molecules must first be understood. To that end, the first experiment measures the intensity and phase of harmonics generated from N 2O and N2 near times of strong alignment revealing interferences during recombination. The second experiment demonstrates HHG as a sensitive probe of rotational wavepacket dynamics in CO2 and N2O, revealing new revival features not detected by any other probe. The final experiment focuses on understanding and controlling the polarization state of the harmonic emission. Generating elliptically polarized harmonics would be very useful for probing molecular and materials systems. We observe an elliptical dichroism in polarization-resolved measurements of the harmonic emission from aligned N2 and CO2 molecules, revealing evidence for electron-hole dynamics between the

  18. Diabatic Mechanisms of Higher-Order Harmonic Generation in Solid-State Materials under High-Intensity Electric Fields

    NASA Astrophysics Data System (ADS)

    Tamaya, T.; Ishikawa, A.; Ogawa, T.; Tanaka, K.

    2016-01-01

    We theoretically investigate mechanisms of higher-order harmonic generation in solid-state materials under a high-intensity ac electric field. A new theoretical framework presented in this Letter holds the legitimacy of Bloch's theorem even under the influence of the high-intensity electric field and provides an exact treatment of the diabatic processes of Bloch electrons. Utilizing this framework, we first discovered that the diabatic processes, namely, ac Zener tunneling and semimetallization of semiconductors, are key factors for nonperturbative mechanisms of HHG. These mechanisms are classified by the field intensity and could be understood by an extended simple man model based on an analogy between tunnel ionization in gaseous media and Zener tunneling in semiconductors. These conclusions would stimulate the universal understanding of HHG mechanisms in both atomic and solid cases.

  19. Materials and characterization using acoustic nonlinearity parameters and harmonic generation - Effects of crystalline and amorphous structures

    NASA Technical Reports Server (NTRS)

    Cantrell, John H.; Yost, William T.

    1990-01-01

    The effects of material structure on the nonlinearity parameters are reviewed. Problems discussed include definition of nonlinearity parameters, square-law nonlinearity and collinear beam-mixing, structure dependence of the nonlinearity parameters, negative nonlinearity parameters, and implications for materials characterization.

  20. Anomalies in high-order harmonic generation at relativistic intensities

    SciTech Connect

    Teubner, U.; Foerster, E.; Pretzler, G.; Eidmann, K.; Witte, K.; Schlegel, Th.

    2003-01-01

    High-order harmonic generation from a solid target surface has been investigated using femtosecond laser pulses focused to intensities greater than 10{sup 18} W/cm{sup 2}. The experiments show that the harmonics are very intense, with a conversion efficiency that is one or two orders of magnitude larger than that of harmonics generated in gases. Beside the observation of presently the shortest wavelength harmonics from femtosecond-laser solid target interaction, i.e., down to 22 nm, an anomaly has been observed in the harmonic spectrum. In contrast to the expected well-known continuous 'roll off' of the high-harmonic orders, the harmonic intensity decreases with the increase of harmonic order, but in between shows minima which are significantly less intense than the neighboring harmonics. Furthermore, the order of the harmonic minima depend on target material. Additional calculations using numerical kinetic particle simulations and a simpler oscillating mirror model show that the physical origin of these modulations is an intricate interplay of resonance absorption and ponderomotive force which leads to a complex electron density profile evolution. Furthermore, this is emphasized by a spectral line analysis of the harmonics. In agreement with the theory, broad lines have been observed and, in particular for the harmonics in the minima, a complex interference structure is present.

  1. Harmonic generation in free-electron lasers

    NASA Astrophysics Data System (ADS)

    Freund, H. P.; Chang, C. L.; Bluem, H.

    1987-10-01

    The question of harmonic generation in FELs is addressed by considering a relativistic electron beam propagating through a loss-free rectangular waveguide in the presence of a linearly polarized wiggler magnetic field. Substantial growth rates and efficiencies at the higher harmonics are shown to be obtainable at the cost of more stringent requirements on beam quality. It is also found that the harmonic emission is far more sensitive to the effect of the thermal spread than is the fundamental. It is suggested that the higher beam currents obtainable on the forthcoming super-ACO storage ring could lead to coherent harmonic generation.

  2. Generating Second Harmonics In Nonlinear Resonant Cavities

    NASA Technical Reports Server (NTRS)

    Kozlovsky, William J.; Nabors, C. David; Byer, Robert L.

    1990-01-01

    Single-axial-mode lasers pump very-low-loss doubling crystals. Important advance in making resonant generation of second harmonics possible for diode-laser-pumped solid-state lasers is recent development of monolithic nonplanar ring geometries in neodymium:yttrium aluminum garnet (Nd:YAG) lasers that produce frequency-stable single-mode outputs. Other advance is development of high-quality MgO:LiNbO3 as electro-optically nonlinear material. Series of experiments devised to improve doubling efficiency of low-power lasers, and particularly of diode-laser-pumped continuous-wave Nd:YAG lasers.

  3. Promoting Spontaneous Second Harmonic Generation through Organogelation.

    PubMed

    Marco, A Belén; Aparicio, Fátima; Faour, Lara; Iliopoulos, Konstantinos; Morille, Yohann; Allain, Magali; Franco, Santiago; Andreu, Raquel; Sahraoui, Bouchta; Gindre, Denis; Canevet, David; Sallé, Marc

    2016-07-27

    An organogelator based on the Disperse Red nonlinear optical chromophore was synthesized according to a simple and efficient three-step procedure. The supramolecular gel organization leads to xerogels which display a spontaneous second harmonic generation (SHG) response without any need for preprocessing, and this SHG activity appears to be stable over several months. These findings, based on an intrinsic structural approach, are supported by favorable intermolecular supramolecular interactions, which promote a locally non-centrosymmetric NLO-active organization. This is in sharp contrast with most materials designed for SHG purposes, which generally require the use of expensive or heavy-to-handle external techniques for managing the dipoles' alignment. PMID:27415660

  4. High order harmonic generation in rare gases

    SciTech Connect

    Budil, K.S.

    1994-05-01

    The process of high order harmonic generation in atomic gases has shown great promise as a method of generating extremely short wavelength radiation, extending far into the extreme ultraviolet (XUV). The process is conceptually simple. A very intense laser pulse (I {approximately}10{sup 13}-10{sup 14} W/cm{sup 2}) is focused into a dense ({approximately}10{sup l7} particles/cm{sup 3}) atomic medium, causing the atoms to become polarized. These atomic dipoles are then coherently driven by the laser field and begin to radiate at odd harmonics of the laser field. This dissertation is a study of both the physical mechanism of harmonic generation as well as its development as a source of coherent XUV radiation. Recently, a semiclassical theory has been proposed which provides a simple, intuitive description of harmonic generation. In this picture the process is treated in two steps. The atom ionizes via tunneling after which its classical motion in the laser field is studied. Electron trajectories which return to the vicinity of the nucleus may recombine and emit a harmonic photon, while those which do not return will ionize. An experiment was performed to test the validity of this model wherein the trajectory of the electron as it orbits the nucleus or ion core is perturbed by driving the process with elliptically, rather than linearly, polarized laser radiation. The semiclassical theory predicts a rapid turn-off of harmonic production as the ellipticity of the driving field is increased. This decrease in harmonic production is observed experimentally and a simple quantum mechanical theory is used to model the data. The second major focus of this work was on development of the harmonic {open_quotes}source{close_quotes}. A series of experiments were performed examining the spatial profiles of the harmonics. The quality of the spatial profile is crucial if the harmonics are to be used as the source for experiments, particularly if they must be refocused.

  5. Imaging with Second-Harmonic Generation Nanoparticles

    NASA Astrophysics Data System (ADS)

    Hsieh, Chia-Lung

    Second-harmonic generation nanoparticles show promise as imaging probes due to their coherent and stable signal with a broad flexibility in the choice of excitation wavelength. In this thesis, we developed and demonstrated barium titanate nanoparticles as second-harmonic radiation imaging probes. We studied the absolute second-harmonic generation efficiency of the nanoparticles on single-particle level. The polarization dependent second-harmonic signal of single nanoparticles was studied in detail. From the measured polar response, we were able to find the orientation of the nanoparticle. We developed a biochemical interface for using the second-harmonic nanoprobes as biomarkers, including in vitro cellular imaging and in vivo live animal imaging. The nanoparticles were surface functionalized with primary amine groups for stable colloidal dispersion. We achieved specific labeling of the second-harmonic nanoprobes via immunostaining where the antibodies were covalently conjugated onto the nanoparticles. We observed no toxicity of the functionalized nanoparticles to biological cells. The coherent second-harmonic signal radiated from the nanoparticles offers opportunities for new imaging techniques. Using interferometric detection, namely harmonic holography, both amplitude and phase of the second-harmonic field can be captured. Through digital beam propagation, three-dimensional field distribution, reflecting three-dimensional distribution of the nanoparticles, can be reconstructed. We achieved a scan-free three-dimensional imaging of nanoparticles in biological cells with sub-micron spatial resolution by using the harmonic holographic microscope. We further exploited the coherent second-harmonic signal for imaging through scattering media by performing optical phase conjugation of the second-harmonic signal. We demonstrated an all-digital optical phase conjugation of the second-harmonic signal originated from a nanoparticle by combining harmonic holography and

  6. High-harmonic generation in cavitated plasmas

    SciTech Connect

    Schroeder, C. B.; Esarey, E.; Comier-Michel, E.; Leemans, W. P.

    2008-05-15

    A method is proposed for producing coherent x-rays via high-harmonic generation using ultraintense lasers interacting with highly stripped ions in cavitated plasmas. This method relies on plasma cavitation by the wake of an intense drive beam (laser or electron beam) to produce an ion cavity. An ultrashort pulse laser propagating in the plasma-electron-free ion cavity generates laser harmonics. The longitudinal electron motion, which inhibits high-harmonic generation at high laser intensities, can be suppressed by the space-charge field in the ion cavity or by using a counterpropagating laser pulse. Periodic suppression of the longitudinal electron motion may also be used to quasi-phase-match. This method enables harmonic generation to be extended to the sub-A regime.

  7. Effective ATI channels in high harmonic generation

    NASA Astrophysics Data System (ADS)

    Kuchiev, M. Yu; Ostrovsky, V. N.

    2001-02-01

    Harmonic generation by an atom in a laser field is described by the three-step mechanism as proceeding via above-threshold ionization (ATI) followed by electron propagation in the laser-dressed continuum and subsequent laser-assisted recombination (LAR). The amplitude of the harmonic production is given by the coherent sum of contributions from different intermediate ATI channels labelled by the number, m, of absorbed laser photons. The range of m-values that give a substantial contribution is explored and found to be rather broad for high harmonic generation. The coherence effects are of crucial importance as they are responsible for the characteristic pattern of harmonic intensities with a plateau domain followed by a cut-off region. Due to the multiphoton nature of the process, an efficient summation of m-contributions can be carried out within the framework of the saddle-point method. The saddle points correspond to some complex-valued labels m = mc associated with the intermediate effective ATI channels in the three-step harmonic generation process. The advantage of this approach stems from the fact that summation over a large number of conventional ATI m-channels is replaced by summation over a small number of effective mc-channels. The equation governing mc has a transparent physical meaning: the electron ejected from the atom on the first (ATI) stage should return to the core to make LAR possible. The effective channel labels m move along characteristic trajectories in the complex plane as the system parameters vary. In the cut-off region of the harmonic spectrum a single effective channel contributes. For lower harmonics, in the plateau domain, two effective ATI channels become essential. The interference of their contributions leads to an oscillatory pattern in the harmonic generation rates. The calculated rates are in good agreement with the results obtained by other approaches.

  8. Valley-selective harmonic generations in transition metal dichalcogenide monolayers

    NASA Astrophysics Data System (ADS)

    Cheng, Jingxin; Jiang, Tao; Shan, Yuwei; Li, Yingguo; Chen, Xianhui; Shen, Y. R.; Liu, Weitao; Wu, Shiwei

    Transition metal dichalcogenide monolayer has emerged as another star in the family of atomically thin two dimensional materials. Different from graphene, the two sublattices in its honeycomb-like structure are occupied by different atoms, leading to the reduced rotational symmetry from six fold to three fold. The reduced symmetry and dimension not only result in many intriguing physics such as valley and excitons, but also lead to rich nonlinear optical phenomena such as strong second harmonic generation. In this talk, we will present a systematic study on linearly and circularly polarized harmonic generations in this wonder material. We show that both the second and third harmonic generations follow the conservation of angular momentum and are valley-selective. Furthermore, these nonlinear optical processes could be used as a powerful imaging tool for studying transition metal dichalcogenide monolayers and other similar 2D materials.

  9. A Model for Generative Harmonic Dictation.

    ERIC Educational Resources Information Center

    Bales, W. Kenton

    This BASIC computer program designed to help music theory students practice harmonic dictation generates examples for students to use in a drill and practice approach in developing aural skills. To facilitate the implementation of effective generative algorithms, the author has used a non-linear analytical technique similar to the chord symbol…

  10. Nonlinear harmonic generation in the STARS FEL

    NASA Astrophysics Data System (ADS)

    Abo-Bakr, M.; Goldammer, K.; Kamps, T.; Knobloch, J.; Kuske, B.; Leitner, T.; Meseck, A.

    2008-08-01

    BESSY proposes to build STARS, an FEL to demonstrate cascaded High Gain Harmonic Generation (HGHG). In two HGHG stages, a laser source of 700-900 nm is converted down to a wavelength of 40-70 nm. The STARS facility consists of a normal-conducting RF photoinjector, three superconducting TESLA-type acceleration modules, a magnetic bunch compressor and two stages of HGHG, each consisting of a modulator, dispersive chicane and a radiator. At the entrance of the undulator section, the beam energy is 325 MeV and the peak current is about 500 A. With these parameters, the STARS FEL reaches saturation with a peak power of 100-350 MW. A superradiant mode is also foreseen which boosts the radiation power to the GW-level. Due to nonlinear harmonic generation (NHG), free electron lasers also radiate coherently at higher harmonics of the FEL resonant frequency. STARS can hence extend its output range to even shorter wavelengths. This paper presents studies of the STARS harmonic content in the wavelength range of 6-20 nm. Seeding with high harmonic generation pulses at 32 nm is also discussed.

  11. Microwave harmonic generation and nonlinearity in microplasmas

    NASA Astrophysics Data System (ADS)

    Gregório, José; Parsons, Stephen; Hopwood, Jeffrey

    2016-06-01

    Nonlinearities in microplasmas excited by microwaves are described both experimentally and through a 2D fluid model. A split-ring resonator generates a microplasma in a 150 μm discharge gap at 1 GHz. Nonlinearity generates both radiated and conducted harmonics which are measured from 0.2–760 Torr (Ar) for power levels between 0.5 and 3 W. Asymmetric electrode configurations produce the highest 3rd harmonic power (>10 mW) at an optimal pressure of the order of 0.3 Torr. The microplasma is also demonstrated as a mixer. The experimental results are explained with the aid of a fluid model of the microplasma. The model shows that the smaller electrode in an asymmetric device is forced to attain a large microwave potential that strongly modulates the sheath thickness and the local electron energy. The voltage-dependent sheath width gives rises to a nonlinear sheath capacitance as well as short pulses of hot electron flux to the electrode. The modeled 3rd harmonic current is converted to an extractable harmonic power by a microwave circuit model. Using this technique the modeled and measured harmonic production of the microplasma are found to compare favorably.

  12. Selection rules for harmonic generation in solids

    NASA Astrophysics Data System (ADS)

    Moiseyev, Nimrod

    2015-05-01

    High-order harmonic generation (HHG) in a bulk crystal was first observed in 2011 [S. Ghimire, A. D. DiChiara, E. Sistrunk, P. Agostini, L. F. DiMauro, and D. A. Reis, Nat. Phys. 7, 138 (2011), 10.1038/nphys1847]. Only odd-order harmonics were observed as expected on the basis of the selection rules in solids, which were derived when only the interband currents were taken into consideration. Here we study HHG in solids when the intraband currents are taken into consideration as well. We show that the dynamical selection rules are broken in solids and the possibility of generation of even-order harmonics cannot be excluded on the basis of the dynamical symmetry analysis. However, a simple analysis of the expression we obtained for the amplitude of the emitted high-order harmonics shows, without the need to carry out numerical calculations, that the even-order harmonics are suppressed due to the localization of the field-free one-electron density probability on the atoms in the solids.

  13. Harmonic generation with multiple wiggler schemes

    SciTech Connect

    Bonifacio, R.; De Salvo, L.; Pierini, P.

    1995-02-01

    In this paper the authors give a simple theoretical description of the basic physics of the single pass high gain free electron laser (FEL), describing in some detail the FEL bunching properties and the harmonic generation technique with a multiple-wiggler scheme or a high gain optical klystron configuration.

  14. Nonlinear harmonic generation in distributed optical klystrons

    SciTech Connect

    H.P. Freund; George R. Neil

    2001-12-01

    A distributed optical klystron has the potential for dramatically shortening the total interaction length in high-gain free-electron lasers (INP 77-59, Novosibirsk, 1977; Nucl. Instr. and Meth A 304 (1991) 463) in comparison to a single-wiggler-segment configuration. This shortening can be even more dramatic if a nonlinear harmonic generation mechanism is used to reach the desired wavelength. An example operating at a 4.5{angstrom} fundamental and a 1.5{angstrom} harmonic is discussed.

  15. Wavelength Scaling of High Harmonic Generation Efficiency

    SciTech Connect

    Shiner, A. D.; Trallero-Herrero, C.; Kajumba, N.; Corkum, P. B.; Villeneuve, D. M.; Bandulet, H.-C.; Comtois, D.; Legare, F.; Giguere, M.; Kieffer, J-C.

    2009-08-14

    Using longer wavelength laser drivers for high harmonic generation is desirable because the highest extreme ultraviolet frequency scales as the square of the wavelength. Recent numerical studies predict that high harmonic efficiency falls dramatically with increasing wavelength, with a very unfavorable lambda{sup -(5-6)} scaling. We performed an experimental study of the high harmonic yield over a wavelength range of 800-1850 nm. A thin gas jet was employed to minimize phase matching effects, and the laser intensity and focal spot size were kept constant as the wavelength was changed. Ion yield was simultaneously measured so that the total number of emitting atoms was known. We found that the scaling at constant laser intensity is lambda{sup -6.3+}-{sup 1.1} in Xe and lambda{sup -6.5+}-{sup 1.1} in Kr over the wavelength range of 800-1850 nm, somewhat worse than the theoretical predictions.

  16. Synthesis and Characterization of Electroresponsive Materials with Applications In: Part I. Second Harmonic Generation. Part II. Organic-Lanthanide Ion Complexes for Electroluminescence and Optical Amplifiers.

    NASA Astrophysics Data System (ADS)

    Claude, Charles

    1995-01-01

    Materials for optical waveguides were developed from two different approaches, inorganic-organic composites and soft gel polymers. Inorganic-organic composites were developed from alkoxysilane and organically modified silanes based on nonlinear optical chromophores. Organically modified silanes based on N-((3^' -trialkoxysilyl)propyl)-4-nitroaniline were synthesized and sol-gelled with trimethoxysilane. After a densification process at 190^circC with a corona discharge, the second harmonic of the film was measured with a Nd:YAG laser with a fundamental wavelength of 1064nm, d_{33} = 13pm/V. The decay of the second harmonic was expressed by a stretched bi-exponential equation. The decay time (tau _2) was equal to 3374 hours, and was comparable to nonlinear optical systems based on epoxy/Disperse Orange 1. The processing temperature of the organically modified silane was limited to 200^circC due to the decomposition of the organic chromophore. Soft gel polymers were synthesized and characterized for the development of optical waveguides with dc-electrical field assisted phase-matching. Polymers based on 4-nitroaniline terminated poly(ethylene oxide-co-propylene oxide) were shown to exhibit second harmonic generation that were optically phase-matched in an electrical field. The optical signals were stable and reproducible. Siloxane polymers modified with 1-mercapto-4-nitrobenzene and 1-mercapto-4-methylsulfonylstilbene nonlinear optical chromophores were synthesized. The physical and the linear and nonlinear optical properties of the polymers were characterized. Waveguides were developed from the polymers which were optically phase -matched and had an efficiency of 8.1%. The siloxane polymers exhibited optical phase-matching in an applied electrical field and can be used with a semiconductor laser. Organic lanthanide ion complexes for electroluminescence and optical amplifiers were synthesized and characterized. The complexes were characterized for their thermal and

  17. Fast interferometric second harmonic generation microscopy

    PubMed Central

    Bancelin, Stéphane; Couture, Charles-André; Légaré, Katherine; Pinsard, Maxime; Rivard, Maxime; Brown, Cameron; Légaré, François

    2016-01-01

    We report the implementation of fast Interferometric Second Harmonic Generation (I-SHG) microscopy to study the polarity of non-centrosymmetric structures in biological tissues. Using a sample quartz plate, we calibrate the spatially varying phase shift introduced by the laser scanning system. Compensating this phase shift allows us to retrieve the correct phase distribution in periodically poled lithium niobate, used as a model sample. Finally, we used fast interferometric second harmonic generation microscopy to acquire phase images in tendon. Our results show that the method exposed here, using a laser scanning system, allows to recover the polarity of collagen fibrils, similarly to standard I-SHG (using a sample scanning system), but with an imaging time about 40 times shorter. PMID:26977349

  18. Resonant second harmonic generation in a gallium nitride two-dimensional photonic crystal on silicon

    NASA Astrophysics Data System (ADS)

    Zeng, Y.; Roland, I.; Checoury, X.; Han, Z.; El Kurdi, M.; Sauvage, S.; Gayral, B.; Brimont, C.; Guillet, T.; Mexis, M.; Semond, F.; Boucaud, P.

    2015-02-01

    We demonstrate second harmonic generation in a gallium nitride photonic crystal cavity embedded in a two-dimensional free-standing photonic crystal platform on silicon. The photonic crystal nanocavity is optically pumped with a continuous-wave laser at telecom wavelengths in the transparency window of the nitride material. The harmonic generation is evidenced by the spectral range of the emitted signal, the quadratic power dependence vs. input power, and the spectral dependence of second harmonic signal. The harmonic emission pattern is correlated to the harmonic polarization generated by the second-order nonlinear susceptibilities χzxx (2 ), χzyy (2 ) and the electric fields of the fundamental cavity mode.

  19. High harmonic generation in undulators for FEL

    NASA Astrophysics Data System (ADS)

    Zhukovsky, K.

    2016-02-01

    The analytical study of the undulator radiation (UR), accounting for major sources of the spectral line broadening is presented. Analytical expressions for the UR spectrum and intensity are obtained. They demonstrate possibilities of the compensation of the divergency by the constant magnetic component. Some examples of single and double frequency undulators are considered. Generation of harmonics is studied with account for homogeneous and inhomogeneous broadening in real devices. The obtained results with account for all broadening sources are applied for evaluation of free electron laser (FEL) performance and compared with those, obtained with the ideal undulator.

  20. Monitoring microstructural evolution in irradiated steel with second harmonic generation

    SciTech Connect

    Matlack, Kathryn H.; Kim, Jin-Yeon; Jacobs, Laurence J.; Wall, James J.; Qu, Jianmin

    2015-03-31

    Material damage in structural components is driven by microstructural evolution that occurs at low length scales and begins early in component life. In metals, these microstructural features are known to cause measurable changes in the acoustic nonlinearity parameter. Physically, the interaction of a monochromatic ultrasonic wave with microstructural features such as dislocations, precipitates, and vacancies, generates a second harmonic wave that is proportional to the acoustic nonlinearity parameter. These nonlinear ultrasonic techniques thus have the capability to evaluate initial material damage, particularly before crack initiation and propagation occur. This paper discusses how the nonlinear ultrasonic technique of second harmonic generation can be used as a nondestructive evaluation tool to monitor microstructural changes in steel, focusing on characterizing neutron radiation embrittlement in nuclear reactor pressure vessel steels. Current experimental evidence and analytical models linking microstructural evolution with changes in the acoustic nonlinearity parameter are summarized.

  1. Limitations and improvements for harmonic generation measurements

    SciTech Connect

    Best, Steven; Croxford, Anthony; Neild, Simon

    2014-02-18

    A typical acoustic harmonic generation measurement comes with certain limitations. Firstly, the use of the plane wave-based analysis used to extract the nonlinear parameter, β, ignores the effects of diffraction, attenuation and receiver averaging which are common to most experiments, and may therefore limit the accuracy of a measurement. Secondly, the method usually requires data obtained from a through-transmission type setup, which may not be practical in a field measurement scenario where access to the component is limited. Thirdly, the technique lacks a means of pinpointing areas of damage in a component, as the measured nonlinearity represents an average over the length of signal propagation. Here we describe a three-dimensional model of harmonic generation in a sound beam, which is intended to provide a more realistic representation of a typical experiment. The presence of a reflecting boundary is then incorporated into the model to assess the feasibility of performing single-sided measurements. Experimental validation is provided where possible. Finally, a focusing acoustic source is modelled to provide a theoretical indication of the afforded advantages when the nonlinearity is localized.

  2. NIR-triggered drug delivery by collagen-mediated second harmonic generation.

    PubMed

    Barhoumi, Aoune; Salvador-Culla, Borja; Kohane, Daniel S

    2015-06-01

    Second harmonic generation is a process through which nonlinear materials such as collagen can absorb two photons and scatter one with twice the energy. Collagen upconverts 730 nm (near-IR) to 365 nm (UV) through second harmonic generation, which cleaves a molecule bound to collagen via a UV-sensitive linker. PMID:25728310

  3. Transient regime in second harmonic generation

    NASA Astrophysics Data System (ADS)

    Szeftel, Jacob; Sandeau, Laure; Sandeau, Nicolas; Delezoide, Camille; Khater, Antoine

    2013-09-01

    The time growth of the electromagnetic field at the fundamental and double frequencies is studied from the very onset of the second harmonic generation (SHG) process for a set of dipoles lacking a symmetry centre and exhibiting a nonresonant coupling with a classical electromagnetic field. This approach consists first of solving the Schrödinger equation by applying a generalised Rabi rotation to the Hamiltonian describing the light-dipole interaction. This rotation has been devised for the resulting Hamiltonian to show up time-independent for both components of the electromagnetic field at the fundamental frequency and the second harmonic one. Then an energy conservation argument, derived from the Poynting theorem, is introduced to work out an additional relationship between the electromagnetic field and its associated electric polarisation. Finally this analysis yields the full time behaviour of all physical quantities of interest. The calculated results reproduce accurately both the observed spatial oscillations of the SHG intensity (Maker's fringes) and its power law dependence on the intensity of the incoming light at the fundamental frequency.

  4. Diode end pumped laser and harmonic generator using same

    NASA Technical Reports Server (NTRS)

    Byer, Robert L. (Inventor); Dixon, George J. (Inventor); Kane, Thomas J. (Inventor)

    1988-01-01

    A second harmonic, optical generator is disclosed in which a laser diode produces an output pumping beam which is focused by means of a graded, refractive index rod lens into a rod of lasant material, such as Nd:YAG, disposed within an optical resonator to pump the lasant material and to excite the optical resonator at a fundamental wavelength. A non-linear electro-optic material such as MgO:LiNbO.sub.3 is coupled to the excited, fundamental mode of the optical resonator to produce a non-linear interaction with the fundamental wavelength producing a harmonic. In one embodiment, the gain medium and the non-linear material are disposed within an optical resonator defined by a pair of reflectors, one of which is formed on a face of the gain medium and the second of which is formed on a face of the non-linear medium. In another embodiment, the non-linear, electro-optic material is doped with the lasant ion such that the gain medium and the non-linear doubling material are co-extensive in volume. In another embodiment, a non-linear, doubling material is disposed in an optical resonator external of the laser gai medium for improved stability of the second harmonic generation process. In another embodiment, the laser gain medium andthe non-linear material are bonded together by means of an optically transparent cement to form a mechanically stable, monolithic structure. In another embodiment, the non-linear material has reflective faces formed thereon to define a ring resonator to decouple reflections from the non-linear medium back to the gain medium for improved stability.

  5. High-order harmonic generation and Fano resonances

    NASA Astrophysics Data System (ADS)

    Strelkov, V. V.; Khokhlova, M. A.; Shubin, N. Yu

    2014-05-01

    We present a high-order harmonic generation theory which generalizes the strong-field approximation to the resonant case when the harmonic frequency is close to that of the transition from the ground state to an autoionizing state of the generating system. We show that the line shape of the resonant harmonic is a product of the Fano-like factor and the harmonic line which would be emitted in the absence of the resonance. The theory predicts rapid variation of the harmonic phase in the vicinity of the resonance. The calculated resonant harmonic phase is in reasonable agreement with recent measurements. Predicting the phase locking of a group of resonantly enhanced harmonics, our theory allows us to study the perspectives of producing an attosecond pulse train using such harmonics.

  6. Third-harmonic UV generation in silicon nitride nanostructures.

    PubMed

    Ning, Tingyin; Hyvärinen, Outi; Pietarinen, Henna; Kaplas, Tommi; Kauranen, Martti; Genty, Göery

    2013-01-28

    We report on strong UV third-harmonic generation from silicon nitride films and resonant waveguide gratings. We determine the absolute value of third-order susceptibility of silicon nitride at wavelength of 1064 nm to be χ(³) (-3ω,ω,ω,ω) = (2.8 ± 0.6) × 10⁻²⁰m²/V², which is two orders of magnitude larger than that of fused silica. The third-harmonic generation is further enhanced by a factor of 2000 by fabricating a resonant waveguide grating onto a silicon nitride film. Our results extend the operating range of CMOS-compatible nonlinear materials to the UV spectral regime. PMID:23389182

  7. Phase-matched harmonic generation in lithium triborate (LBO)

    NASA Astrophysics Data System (ADS)

    Velsko, Stephan P.; Webb, Mark; Davis, Laura; Huang, Chaoen

    1991-09-01

    The authors present refractive index, thermo-optic, phase-matching angle, nonlinear coefficient, absorption, and scattering data on lithium triborate (LBO) crystals. They briefly discuss the material quality of the crystals, including the results of calorimetric absorption measurements in the infrared and ultraviolet. They present a new set of refractive index values with better than fourth decimal place precision, as well as measurements of the thermo-optic parameters. The nonlinear coefficients and other frequency conversion parameters of LBO were investigated by studying the phase-matched generation of Nd:YAG harmonics. These results are summarized. The authors discuss angular and thermal bandwidths for phase matching. Finally, they compare the efficiency of LBO with that of several other frequency conversion crystals for a common commercial application-the generation of Nd:YAG harmonics.

  8. Efficient second harmonic generation in internal asymmetric plasmonic slot waveguide.

    PubMed

    Huang, Tianye; Tagne, Patrick Moteng; Fu, Songnian

    2016-05-01

    We theoretically propose an internal asymmetric plasmonic slot waveguide (IAPSW), containing two different materials in the slot region. The IAPSW is used for second harmonic generation (SHG) at a wavelength of 1.55 μm. The required phase matching condition is satisfied between the 0th-order mode at the fundamental frequency and the 1st-order mode at the second harmonic frequency. By choosing appropriate slot geometry and materials, the mode field distribution is engineered to enhance the nonlinear coupling coefficient for SHG. With an 11 μm long IAPSW, a conversion efficiency of 24% (1.8 × 105 W-1cm-2 normalized conversion efficiency) is predicted. Furthermore, the SHG efficiency is more pronounced in IAPSW with thinner slot. PMID:27137584

  9. Application of organic compounds for high-order harmonic generation of ultrashort pulses

    NASA Astrophysics Data System (ADS)

    Ganeev, R. A.

    2016-02-01

    The studies of the high-order nonlinear optical properties of a few organic compounds (polyvinyl alcohol, polyethylene, sugar, coffee, and leaf) are reported. Harmonic generation in the laser-produced plasmas containing the molecules and large particles of above materials is demonstrated. These studies showed that the harmonic distributions and harmonic cutoffs from organic compound plasmas were similar to those from the graphite ablation. The characteristic feature of observed harmonic spectra was the presence of bluesided lobes near the lower-order harmonics.

  10. Extreme harmonic generation in electrically driven spin resonance.

    PubMed

    Stehlik, J; Schroer, M D; Maialle, M Z; Degani, M H; Petta, J R

    2014-06-01

    We report the observation of multiple harmonic generation in electric dipole spin resonance in an InAs nanowire double quantum dot. The harmonics display a remarkable detuning dependence: near the interdot charge transition as many as eight harmonics are observed, while at large detunings we only observe the fundamental spin resonance condition. The detuning dependence indicates that the observed harmonics may be due to Landau-Zener transition dynamics at anticrossings in the energy level spectrum. PMID:24949787

  11. Attosecond Probing of Vibrational Dynamics with High-Harmonic Generation

    NASA Astrophysics Data System (ADS)

    Lein, Manfred

    2005-02-01

    The numerical solution of the time-dependent Schrödinger equation for vibrating hydrogen molecules in few-cycle laser pulses shows that high-harmonic generation is sensitive to the laser-induced vibrational motion. More intense harmonics are generated in heavier isotopes, the difference increasing with the harmonic frequency. Analytical theory reveals a dependence of the harmonics on the vibrational autocorrelation function. With the help of a genetic algorithm, the nuclear motion can be reconstructed from the harmonic spectra with sub-fs time resolution.

  12. Harmonic generation by circularly polarized laser beams propagating in plasma

    SciTech Connect

    Agrawal, Ekta; Hemlata,; Jha, Pallavi

    2015-04-15

    An analytical theory is developed for studying the phenomenon of generation of harmonics by the propagation of an obliquely incident, circularly polarized laser beam in homogeneous, underdense plasma. The amplitudes of second and third harmonic radiation as well as detuning distance have been obtained and their variation with the angle of incidence is analyzed. The amplitude of harmonic radiation increases with the angle of incidence while the detuning distance decreases, for a given plasma electron density. It is observed that the generated second and third harmonic radiation is linearly and elliptically polarized, respectively. The harmonic radiation vanishes at normal incidence of the circularly polarized laser beam.

  13. Mechanisms of below-threshold harmonic generation in atoms.

    PubMed

    Xiong, Wei-Hao; Geng, Ji-Wei; Tang, Jing-Yi; Peng, Liang-You; Gong, Qihuang

    2014-06-13

    Most previous studies have focused on high-order harmonic generation beyond the ionization threshold; mechanisms of below-threshold harmonics are less understood. We schematically study the harmonic emission process in this region by numerically solving the time-dependent Schrödinger equation of an atom in laser fields. We show that, besides the quantum path interference mechanism recently identified, the effects induced by the Coulomb potential also have a critical impact on these harmonics. These mechanisms can be distinguished in the structure of harmonic spectra by changing the laser wavelength and peak intensity. We find that the long quantum orbits can influence lower-order harmonics at a higher laser intensity. In addition, we show that the intensity-dependent steps of harmonic yield can disappear for certain harmonic orders, due to the trapping in the Rydberg states before recombination, which can explain recent experimental observations. PMID:24972202

  14. Transmission second harmonic generation in CdTe at 1.064 μm

    NASA Astrophysics Data System (ADS)

    Petrovic, M. S.; Suchocki, A.; Powell, R. C.; Cantwell, G.

    1991-12-01

    Transmission geometry measurements of the efficiency of second harmonic generation in various thicknesses of CdTe samples were made to determine the conversion efficiency dependence on material thickness. Neglecting pump depletion, it is found that for samples of well-defined symmetry, the second harmonic conversion efficiency scales with film thickness, with no observed enhancement owing to coherence length effects. The angular dependence of the observed second harmonic light in films of well-defined symmetry is consistent with second harmonic generation originating in the bulk.

  15. Electric field induced second harmonic generation with and without fringes

    NASA Astrophysics Data System (ADS)

    Meshulam, G.; Berkovic, G.; Kotler, Z.; Sa'ar, A.

    2000-09-01

    Electric field induced second harmonic generation (EFISH) is a well-known technique to measure the first hyperpolarizability (β) of organic molecules in solution. The characteristic experimental output is observation of oscillatory fringes of second harmonic radiation as the solution path length is changed and evaluation of β from the fringe amplitude. We present two different cases where even in the absence of these characteristic fringes β may still be evaluated: first, when using absorbing materials, and second, when using broadband laser sources. The ability to determine β by EFISH under these conditions greatly enhances the ability of this technique to measure β values over a wide range of laser frequencies. Measurements of the same molecule's β values at different frequencies are reported, verifying the two-level model for the dispersion of β.

  16. Effects of spatial transverse correlations in second-harmonic generation

    SciTech Connect

    Ether, D. S.; Souto Ribeiro, P. H.; Matos Filho, R. L. de; Monken, C. H.

    2006-05-15

    Second-harmonic generation is studied for the case where the fundamental field is light produced in a spontaneous parametric down-conversion process. We show that second-harmonic generation is sensitive to the transverse correlations between signal and idler fields. In particular, when the fundamental is prepared in a state exhibitting spatial antibunching, the second-harmonic intensity may be zero, independent of the intensity of the fundamental field.

  17. Deep-subwavelength waveguiding via inhomogeneous second-harmonic generation.

    PubMed

    Roppo, Vito; Vincenti, Maria Antonietta; de Ceglia, Domenico; Scalora, Michael

    2012-08-01

    We theoretically investigate second-harmonic generation in extremely narrow, subwavelength semiconductor and dielectric waveguides. We discuss a guiding mechanism characterized by the inhibition of diffraction and the suppression of cutoff limits in the context of a light trapping phenomenon that sets in under conditions of general phase and group velocity mismatch between the fundamental and the generated harmonic. PMID:22859096

  18. Symmetry-selective third-harmonic generation from plasmonic metacrystals.

    PubMed

    Chen, Shumei; Li, Guixin; Zeuner, Franziska; Wong, Wing Han; Pun, Edwin Yue Bun; Zentgraf, Thomas; Cheah, Kok Wai; Zhang, Shuang

    2014-07-18

    Nonlinear processes are often governed by selection rules imposed by the symmetries of the molecular configurations. The most well-known examples include the role of centrosymmetry breaking for the generation of even harmonics, and the selection rule related to the rotational symmetry in harmonic generation for fundamental beams with circular polarizations. While the role of centrosymmetry breaking in second harmonic generation has been extensively studied in plasmonic systems, the investigation of selection rules pertaining to circular polarization states of harmonic generation is limited to crystals, i.e., symmetries at the atomic level. In this Letter we demonstrate the rotational symmetry dependent third harmonic generation from nonlinear plasmonic metacrystals. We show that the selection rule can be imposed by the rotational symmetry of metacrystals embedded into an isotropic organic nonlinear thin film. The results presented here may open new avenues for designing symmetry-dependent nonlinear optical responses with tailored plasmonic nanostructures. PMID:25083645

  19. Second harmonic generation polarization properties of myofilaments

    NASA Astrophysics Data System (ADS)

    Samim, Masood; Prent, Nicole; Dicenzo, Daniel; Stewart, Bryan; Barzda, Virginijus

    2014-05-01

    Second harmonic generation (SHG) polarization microscopy was used to investigate the organization of myosin nanomotors in myofilaments of muscle cells. The distribution of the second-order nonlinear susceptibility component ratio χzzz(2)/χzxx(2) along anisotropic bands of sarcomeres revealed differences between the headless and head-containing regions of myofilaments. The polarization-in polarization-out SHG measurements of headless myosin mutants of indirect flight muscle in Drosophila melanogaster confirmed a lower susceptibility component ratio compared to the head-containing myocytes with wild-type myosins. The increase in the ratio is assigned to the change in the deflection angle of the myosin S2 domain and possible contribution of myosin heads. The nonlinear susceptibility component ratio is a sensitive indicator of the myosin structure, and therefore, it can be used for conformational studies of myosin nanomotors. The measured ratio values can also be used as the reference for ab initio calculations of nonlinear optical properties of different parts of myosins.

  20. Waveguide Harmonic Generator for the SIM

    NASA Technical Reports Server (NTRS)

    Chang, Daniel; Poberezhskiy, Ilya; Mulder, Jerry

    2008-01-01

    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.

  1. Second harmonic generation from the 'centrosymmetric' crystals.

    PubMed

    Nalla, Venkatram; Medishetty, Raghavender; Wang, Yue; Bai, Zhaozhi; Sun, Handong; Wei, Ji; Vittal, Jagadese J

    2015-05-01

    Second harmonic generation (SHG) is a well known non-linear optical phenomena which can be observed only in non-centrosymmetric crystals due to non-zero hyperpolarizability. In the current work we observed SHG from a Zn(II) complex which was originally thought to have crystallized in the centrosymmetric space group C2/c. This has been attributed to the unequal antiparallel packing of the metal complexes in the non-symmetric space group Cc or residual non-centrosymmetry in C2/c giving rise to polarizability leading to strong SHG. The enhancement of SHG by UV light has been attributed to the increase in non-centrosymmetry and hence polarity of packing due to strain induced in the crystals. The SHG signals measured from these crystals were as large as potassium dihydrogen phosphate crystals, KH2PO4 (KDP), and showed temperature dependence. The highest SHG efficiency was observed at 50 K. The SHG phenomenon was observed at broad wavelengths ranging from visible to below-red in these crystals. PMID:25995840

  2. Powders Analysis by Second Harmonic Generation Microscopy.

    PubMed

    Chowdhury, Azhad U; Zhang, Shijie; Simpson, Garth J

    2016-04-01

    A microscopy approach is developed for quantifying second harmonic generation (SHG) activity of powders that largely decouples linear and nonlinear optical interactions. Decoupling the linear and nonlinear optical effects provides a means to independently evaluate and optimize the role of each in crystal engineering efforts and facilitates direct comparisons between experimental and computational predictions of lattice hyperpolarizabilities. In this respect, the microscopy-based approach nicely complements well-established Kurtz-Perry ( J. Appl. Phys. 1968 , 39 , 3798 ) and related methods, in which collimated sources are used for powders analysis. Using a focused fundamental beam places a controllable upper bound on the interaction length, given by the depth of field. Because measurements are performed on a per-particle basis, crystal size-dependent trends can be recovered from a single powdered sample. An analytical model that includes scattering losses of a focused Gaussian beam reliably predicted several experimental observations. Specifically, the measured scattering length for SHG was in excellent agreement with the value predicted based on the particle size distribution. Additionally, histograms of the SHG intensities as functions of particle size and orientation agreed nicely with predictions from the model. PMID:26929984

  3. Higher-Order Harmonic Generation from Fullerene by Means of the Plasma Harmonic Method

    SciTech Connect

    Ganeev, R. A.; Bom, L. B. Elouga; Abdul-Hadi, J.; Ozaki, T.; Wong, M. C. H.; Brichta, J. P.; Bhardwaj, V. R.

    2009-01-09

    We demonstrate, for the first time, high-order harmonic generation from C{sub 60} by an intense femtosecond Ti:sapphire laser. Laser-produced plasmas from C{sub 60}-rich epoxy and C{sub 60} films were used as the nonlinear media. Harmonics up to the 19th order were observed. The harmonic yield from fullerene-rich plasma is about 25 times larger compared with those produced from a bulk carbon target. Structural studies of plasma debris confirm the presence and integrity of fullerenes within the plasma plume, indicating fullerenes as the source of high-order harmonics.

  4. Generation of even harmonics in coupled quantum dots

    SciTech Connect

    Guo Shifang; Duan Suqing; Yang Ning; Chu Weidong; Zhang Wei

    2011-07-15

    Using the spatial-temporal symmetry principle we developed recently, we propose an effective scheme for even-harmonics generation in coupled quantum dots. The relative intensity of odd and even harmonic components in the emission spectrum can be controlled by tuning the dipole couplings among the dots, which can be realized in experiments by careful design of the nanostructures. In particular, pure 2nth harmonics and (2n+1)th harmonics (where n is an integer) can be generated simultaneously with polarizations in two mutual perpendicular directions in our systems. An experimental design of the coupled dots system is presented.

  5. Second-harmonic generation with Bessel beams

    NASA Astrophysics Data System (ADS)

    Shatrovoy, Oleg

    We present the results of a numerical simulation tool for modeling the second-harmonic generation (SHG) interaction experienced by a diffracting beam. This code is used to study the simultaneous frequency and spatial profile conversion of a truncated Bessel beam that closely resembles a higher-order mode (HOM) of an optical fiber. SHG with Bessel beams has been investigated in the past and was determined have limited value because it is less efficient than SHG with a Gaussian beam in the undepleted pump regime. This thesis considers, for the first time to the best of our knowledge, whether most of the power from a Bessel-like beam could be converted into a second-harmonic beam (full depletion), as is the case with a Gaussian beam. We study this problem because using HOMs for fiber lasers and amplifiers allows reduced optical intensities, which mitigates nonlinearities, and is one possible way to increase the available output powers of fiber laser systems. The chief disadvantage of using HOM fiber amplifiers is the spatial profile of the output, but this can be transformed as part of the SHG interaction, most notably to a quasi-Gaussian profile when the phase mismatch meets the noncollinear criteria. We predict, based on numerical simulation, that noncollinear SHG (NC-SHG) can simultaneously perform highly efficient (90%) wavelength conversion from 1064 nm to 532 nm, as well as concurrent mode transformation from a truncated Bessel beam to a Gaussian-like beam (94% overlap with a Gaussian) at modest input powers (250 W, peak power or continuous-wave operation). These simulated results reveal two attractive features -- the feasibility of efficiently converting HOMs of fibers into Gaussian-like beams, and the ability to simultaneously perform frequency conversion. Combining the high powers that are possible with HOM fiber amplifiers with access to non-traditional wavelengths may offer significant advantages over the state of the art for many important applications

  6. Efficient millimeter wave 1140 GHz/ diode for harmonic power generation

    NASA Technical Reports Server (NTRS)

    1967-01-01

    Epitaxial gallium arsenide diode junction formed in a crossed waveguide structure operates as a variable reactance harmonic generator. This varactor diode can generate power efficiently in the low-millimeter wavelength.

  7. SEVENTH HARMONIC 20 GHz CO-GENERATOR

    SciTech Connect

    Hirshfield, Jay L

    2014-04-08

    To satisfy the need for multi-MW rf sources in frequency ranges where commercial sources do not exist, a study was undertaken on a class of devices based on gyro-harmonic frequency multiplication. This mechanism relies upon adding energy in gyrating motion to a linear electron beam that traverses a rotating-mode TE111-mode drive cavity in a dc magnetic field. The beam then drifts along the magnetic field into a second cavity, operating in the TEn11-mode tuned to the nth harmonic of the drive cavity. Studies of this configuration have been carried out for 2 < n < 7. Results are given for multi-MW, efficient operation of a 7th harmonic device operating at 20 GHz, and a 2nd harmonic device operating at 22.4 GHz.

  8. Second harmonic generation in graphene-coated nanowires.

    PubMed

    Gao, Yixiao; Shadrivov, Ilya V

    2016-08-01

    We study second harmonic generation in a pair of graphene-coated nanowires. We show that the phase matching condition for harmonic generation can be engineered in a wide range of frequencies by tuning the spacing between graphene nanowires. We derive coupled mode equations describing the process of second harmonic generation using an unconjugated Lorentz reciprocity theorem. We show that the highest harmonic generation efficiency can be achieved by phase matching the fundamental mode with the two lowest order symmetric modes at the second harmonic frequency. Despite losses in graphene, we predict that the efficiency can be further enhanced by reducing the radius of nanowires due to larger mode overlap and lower propagation loss. PMID:27472634

  9. High-harmonic generation from an atomically thin semiconductor

    NASA Astrophysics Data System (ADS)

    Liu, Hanzhe; Li, Yilei; Ghimire, Shambhu; Heinz, Tony; Reis, David

    The process of high-harmonic generation (HHG) from ultrashort laser pulses has recently been observed in bulk solids, complementing the well-established process in the gas phase. HHG is of interest both as a source of ultrashort pulses in the attosecond regime that has photon energies extending up to the soft x-ray region and as a method of probing material response outside the regime of perturbative nonlinear optics. In this paper, we present the observation of HHG from a single atomic layer of MoS2 driven by a strong infrared pulse of 100 fs duration and 0.3 eV photon energy. We observe distinct harmonics up to the 13th order of the infrared excitation. The non-perturbative nature of the HHG process is demonstrated by the weak power dependence of the harmonic intensities. To gain further insight into the process, we have investigated the variation of the HHG signal with sample orientation and the ellipticity of pump excitation. We compare and contrast the process with that from the bulk MoS2 crystal. We find significant differences in the response for the monolayer and bulk crystal, which can be understood in terms of the distinct crystallographic symmetries in the two cases.

  10. Resonant second harmonic generation in a gallium nitride two-dimensional photonic crystal on silicon

    SciTech Connect

    Zeng, Y.; Roland, I.; Checoury, X.; Han, Z.; El Kurdi, M.; Sauvage, S.; Boucaud, P.; Gayral, B.; Brimont, C.; Guillet, T.; Mexis, M.; Semond, F.

    2015-02-23

    We demonstrate second harmonic generation in a gallium nitride photonic crystal cavity embedded in a two-dimensional free-standing photonic crystal platform on silicon. The photonic crystal nanocavity is optically pumped with a continuous-wave laser at telecom wavelengths in the transparency window of the nitride material. The harmonic generation is evidenced by the spectral range of the emitted signal, the quadratic power dependence vs. input power, and the spectral dependence of second harmonic signal. The harmonic emission pattern is correlated to the harmonic polarization generated by the second-order nonlinear susceptibilities χ{sub zxx}{sup (2)}, χ{sub zyy}{sup (2)} and the electric fields of the fundamental cavity mode.

  11. Harmonics Generation by Surface Plasmon Polaritons on Single Nanowires

    PubMed Central

    2016-01-01

    We present experimental observations of visible wavelength second- and third-harmonic generation on single plasmonic nanowires of variable widths. We identify that near-infrared surface plasmon polaritons, which are guided along the nanowire, act as the source of the harmonics generation. We discuss the underlying mechanism of this nonlinear process, using a combination of spatially resolved measurements and numerical simulations to show that the visible harmonics are generated via a combination of both local and propagating plasmonic modes. Our results provide the first demonstration of nanoscale nonlinear optics with guided, propagating plasmonic modes on a lithographically defined chip, opening up new routes toward integrated optical circuits for information processing. PMID:27563688

  12. Second-harmonic generation in substoichiometric silicon nitride layers

    NASA Astrophysics Data System (ADS)

    Pecora, Emanuele; Capretti, Antonio; Miano, Giovanni; Dal Negro, Luca

    2013-03-01

    Harmonic generation in optical circuits offers the possibility to integrate wavelength converters, light amplifiers, lasers, and multiple optical signal processing devices with electronic components. Bulk silicon has a negligible second-order nonlinear optical susceptibility owing to its crystal centrosymmetry. Silicon nitride has its place in the microelectronic industry as an insulator and chemical barrier. In this work, we propose to take advantage of silicon excess in silicon nitride to increase the Second Harmonic Generation (SHG) efficiency. Thin films have been grown by reactive magnetron sputtering and their nonlinear optical properties have been studied by femtosecond pumping over a wide range of excitation wavelengths, silicon nitride stoichiometry and thermal processes. We demonstrate SHG in the visible range (375 - 450 nm) using a tunable 150 fs Ti:sapphire laser, and we optimize the SH emission at a silicon excess of 46 at.% demonstrating a maximum SHG efficiency of 4x10-6 in optimized films. Polarization properties, generation efficiency, and the second order nonlinear optical susceptibility are measured for all the investigated samples and discussed in terms of an effective theoretical model. Our findings show that the large nonlinear optical response demonstrated in optimized Si-rich silicon nitride materials can be utilized for the engineering of nonlinear optical functions and devices on a Si chip.

  13. Spectrum of second-harmonic radiation generated from incoherent light

    SciTech Connect

    Stabinis, A.; Pyragaite, V.; Tamosauskas, G.; Piskarskas, A.

    2011-10-15

    We report on the development of the theory of second-harmonic generation by an incoherent pump with broad angular and frequency spectra. We show that spatial as well as temporal walk-off effects in a nonlinear crystal result in angular dispersion of the second-harmonic radiation. We demonstrate that the acceptance angle in second-harmonic generation by incoherent light is caused by the width of the pump angular spectrum and the resulting angular dispersion of second-harmonic radiation but does not depend on crystal length. In this case the frequency spectrum of second-harmonic radiation is determined by its angular dispersion and the pump angular spectrum. The theory is supported by an experiment in which a LiIO{sub 3} crystal was pumped by a tungsten halogen lamp.

  14. DETECTION OF MOLECULAR MONOLAYERS BY OPTICAL. SECOND HARMONIC GENERATION

    SciTech Connect

    Chen, C. K.; Heinz, T. F.; Ricard, D.; Shen, Y. R.

    1980-12-01

    Second harmonic generation is shown to be sensitive enough to detect molecular monolayers adsorbed on a silver surface. Adsorption of AgCl and pyridine on silver during and after an electrolytic cycle can be easily observed,

  15. Frequency-resolved optical grating using third-harmonic generation

    SciTech Connect

    Tsang, T.; Krumbuegel, M.A.; Delong, K.W.

    1995-12-01

    We demonstrate the first frequency-resolved optical gating measurement of an laser oscillator without the time ambiguity using third-harmonic generation. The experiment agrees well with the phase-retrieved spectrograms.

  16. Unified approach to Čerenkov second harmonic generation.

    PubMed

    Roppo, Vito; Kalinowski, Ksawery; Sheng, Yan; Krolikowski, Wieslaw; Cojocaru, Crina; Trull, Jose

    2013-11-01

    We discuss the effect of second harmonic generation via the Čerenkov-like process in nonlinear bulk media and waveguides. We show that in both schemes the Čerenkov harmonic emission represents in fact a nonlinear Bragg diffraction process. It is therefore possible, for the first time, to describe the bulk and waveguide Čerenkov emission uniformly by considering the spatial modulation of the second-order nonlinear polarization. This is also experimentally illustrated by studying the Čerenkov second harmonic generation at the boundary of a nonlinear quadratic medium via the total internal reflection inside the nonlinear crystal. PMID:24216797

  17. High order harmonic generation in dual gas multi-jets

    SciTech Connect

    Tosa, Valer E-mail: calin.hojbota@itim-cj.ro; Hojbota, Calin E-mail: calin.hojbota@itim-cj.ro

    2013-11-13

    High order harmonic generation (HHG) in gas media suffers from a low conversion efficiency that has its origins in the interaction of the atom/molecule with the laser field. Phase matching is the main way to enhance the harmonic flux and several solutions have been designed to achieve it. Here we present numerical results modeling HHG in a system of multi-jets in which two gases alternate: the first gas jet (for example Ne) generates harmonics and the second one which ionizes easier, recover the phase matching condition. We obtain configurations which are experimentally feasible with respect to pressures and dimensions of the jets.

  18. High Harmonic Generation at Long Wavelengths

    SciTech Connect

    Sheehy, B.; Martin, J. D. D.; DiMauro, L. F.; Agostini, P.; Schafer, K. J.; Gaarde, M. B.; Department of Physics, Lund Institute of Technology, P.O. Box 118, S-22100 Lund, ; Kulander, K. C.

    1999-12-20

    High harmonic radiation spectra up to 19th order in alkali metal vapors excited by an intense, picosecond mid-infrared (3-4 {mu} m ) laser are reported and compared to theory. The strong-field dynamics in the alkali metal atoms exhibit significant differences from all previously studied systems due to the strong coupling between their ground and first excited states. (c) 1999 The American Physical Society.

  19. Multi-Orbital contributions in High Harmonic Generation

    NASA Astrophysics Data System (ADS)

    Guehr, Markus

    2009-05-01

    The high harmonic spectrum generated from atoms or molecules in a strong laser field contains information about the electronic structure of the generation medium. In the high harmonic generation (HHG) process, a free electron wave packet tunnel-ionizes from the molecular orbital in a strong laser field. After being accelerated by the laser electric field, the free electron wave packet coherently recombines to the orbital from which is was initially ionized, thereby emitting the harmonic spectrum. Interferences between the free electron wave packet and the molecular orbital will shape the spectrum in a characteristic way. These interferences have been used to tomographically image the highest occupied molecular orbital (HOMO) of N2 [1]. Molecular electronic states energetically below the HOMO should contribute to laser-driven high harmonic generation (HHG), but this behavior has not been observed previously. We have observed evidence of HHG from multiple orbitals in aligned N2 [2]. The tunneling ionization (and therefore the harmonic generation) is most efficient if the orbital has a large extension in the direction of the harmonic generation polarization. The HOMO with its σg symmetry therefore dominates the harmonic spectrum if the molecular axis is parallel to the harmonic generation polarization, the lower bound πu HOMO-1 dominates in the perpendicular case. The HOMO contributions appear as a regular plateau with a cutoff in the HHG spectrum. In contrast, the HOMO-1 signal is strongly peaked in the cutoff region. We explain this by semi-classical simulations of the recombination process that show constructive interferences between the HOMO-1 and the recombining wave packet in the cutoff region. The ability to monitor several orbitals opens the route to imaging coherent superpositions of electronic orbitals. [1] J. Itatani et al., Nature 432, 867 (2004)[2] B. K. McFarland, J. P. Farrell, P. H. Bucksbaum and M. Gühr, Science 322, 1232 (2008)

  20. Control of Laser High-Harmonic Generation with Counterpropagating Light

    NASA Astrophysics Data System (ADS)

    Voronov, S. L.; Kohl, I.; Madsen, J. B.; Simmons, J.; Terry, N.; Titensor, J.; Wang, Q.; Peatross, J.

    2001-09-01

    Relatively weak counterpropagating light is shown to disrupt the emission of laser high-harmonic generation. Harmonic orders ranging from the teens to the low thirties produced by a 30-femtosecond pulse in a narrow argon jet are ``shut down'' with a contrast as high as 2 orders of magnitude by a chirped 1-picosecond counterpropagating laser pulse (60 times less intense). Alternatively, under poor phase-matching conditions, the counterpropagating light boosts harmonic production by similar contrast through quasiphase matching where out-of-phase emission is suppressed.

  1. Electromagnetic study of second harmonic generation by a corrugated waveguide

    NASA Astrophysics Data System (ADS)

    Neviere, Michel; Popov, E.; Reinisch, Raymond

    1995-09-01

    When an incident plane wave with circular frequency (omega) falls on a grating coated by a layer of nonlinear material, it generates a nonlinear polarization PNL(2(omega) ) which acts as a source term and produces a second harmonic (SH) field called signal. The excitation of an electromagnetic resonance like surface plasmon or a guided wave increases the local field and thus the signal. The problem is to be able to compute and optimize the latter. We have developed a new theory which uses a coordinate transformation mapping the grating profile onto a plane. This simplifies the boundary conditions but complicates the propagation equation. Taking advantage of the psuedoperiodicity of the problem, the Fourier harmonics of the field are solution of a set of first order differential equations with constant coefficients. The resolution of this system via eigenvalue and eigenvector technique avoid numerical instabilities and lead to accurate results which agree perfectly with those found via the Rayleigh method or by the Differential method, when they work. A phenomenological approach is then developed to explain the unusual shape of the resonance lines at 2(omega) , which is based on the poles and zeros of the scattering operator S at (omega) and 2(omega) . It is shown that S(2(omega) ) presents 3 complex poles with 3 associated complex zeros. Their knowledge, plus the nonlinear reflectivity of the plane device allows predicting all the possible shapes of the 2(omega) signal as a function of angle of incidence. The phenomenological study explains an experimental result, found a few years ago, that if 2(omega) lies inside the absorption band of the guiding material instead of the transparent region, the enhanced second harmonic generation (SHG) is changed into a reduced one. It means that in the case phase matching can lead to a minimum instead of maximum. An algorithm is then proposed to maximize the signal intensity; with polyurethane as a guiding material a conversion

  2. Magnetic Second-Harmonic Generation from Interfaces and Nanostructures

    NASA Astrophysics Data System (ADS)

    McGilp, J. F.

    2012-08-01

    Magneto-optic techniques provide non-contact and non-destructive characterization of magnetic materials. This includes embedded magnetic nanostructures, which are accessible due to the large penetration depth of optical radiation. Nonlinear magnetic second-harmonic generation (MSHG) can measure the surface and interlace magnetism of centrosymmetric magnetic films and nanostructures with sub-monolayer sensitivity. MSHG is briefly reviewed and examples from high symmetry interlaces and nanostructures described. Low symmetry systems, such as aligned magnetic nanostructures grown by self-organization on vicinal substrates, are more difficult to characterize, however, because of the large number of tensor components that may contribute to the signal. Normal incidence geometry simplifies the problem and this new approach is shown to allow the determination of hysteresis loops and the temperature dependent magnetic response of Au-capped Fe nanostructures grown on vicinal W(110).

  3. Second harmonic generation double stokes Mueller polarimetric microscopy of myofilaments

    PubMed Central

    Kontenis, Lukas; Samim, Masood; Karunendiran, Abiramy; Krouglov, Serguei; Stewart, Bryan; Barzda, Virginijus

    2016-01-01

    The experimental implementation of double Stokes Mueller polarimetric microscopy is presented. This technique enables a model-independent and complete polarimetric characterization of second harmonic generating samples using 36 Stokes parameter measurements at different combinations of incoming and outgoing polarizations. The degree of second harmonic polarization and the molecular nonlinear susceptibility ratio are extracted for individual focal volumes of a fruit fly larva wall muscle. PMID:26977362

  4. Spectrally Resolved Maker Fringes in High-Order Harmonic Generation

    NASA Astrophysics Data System (ADS)

    Heyl, C. M.; Güdde, J.; Höfer, U.; L'Huillier, A.

    2011-07-01

    We investigate macroscopic interference effects in high-order harmonic generation using a Ti:sapphire laser operating at a 100 kHz repetition rate. The structure and behavior of spectral and spatial interference fringes are explained and analytically described by transient phase matching of the long electron trajectory contribution. Time-frequency mapping due to the temporal chirp of the harmonic emission allows us to observe Maker fringes directly in the spectral domain.

  5. Resonant high-order harmonic generation from plasma ablation: Laser intensity dependence of the harmonic intensity and phase

    SciTech Connect

    Milosevic, D. B.

    2010-02-15

    Experimentally observed strong enhancement of a single high-order harmonic in harmonic generation from low-ionized laser plasma ablation is explained as resonant harmonic generation. The resonant harmonic intensity increases regularly with the increase of the laser intensity, while the phase of the resonant harmonic is almost independent of the laser intensity. This is in sharp contrast with the usual plateau and cutoff harmonics, the intensity of which exhibits wild oscillations while its phase changes rapidly with the laser intensity. The temporal profile of a group of harmonics, which includes the resonant harmonic, has the form of a broad peak in each laser-field half cycle. These characteristics of resonant harmonics can have an important application in attoscience. We illustrate our results using examples of Sn and Sb plasmas.

  6. Second harmonic generation using nonlinear Rayleigh surface waves in stone

    NASA Astrophysics Data System (ADS)

    Smith, Margaret; Kim, Gun; Kim, Jin-Yeon; Kurtis, Kimberly; Jacobs, Laurence

    2015-03-01

    This research tests the potential application of the Second Harmonic Generation (SHG) method using nonlinear Rayleigh surface waves to nondestructively quantify surface microstructural changes in thin stone. The acoustic nonlinearity parameter (β) has been assessed as a meaningful indicator for characterizing the nonlinearity of civil engineering materials; additionally, Rayleigh waves offer the opportunity to isolate a material's near surface microstructural status. Sandstone was selected for testing due to its relative uniformity and small grain size compared to other stone types; the sample thickness was 2 inches to reflect the minimum panel thickness recommended by the Indiana Limestone Institute. For this research, initially fully non-contact generation and detection techniques are evaluated before a 100kHz wedge transmitter and a 200kHz air-coupled receiver are employed for generation and detection of nonlinear Rayleigh waves. Non-contact transmitters and receivers have advantages such as removing the irregularities associated with coupling as well as not leaving residues, which in stone applications can be considered aesthetically damaging. The experimental results show that the nonlinear parameter, β, can be effectively isolated using the wedge transmitter and non-contact set up and that too much of the signal strength is lost in the fully non-contact method to extract meaningful results for this stone and stones with slow wave speeds. This indicates that the proposed SHG technique is effective for evaluating the nonlinearity parameter, β, and can next be applied to characterize near surface microstructural changes in thin applications of dimensioned stone.

  7. Generation of higher odd harmonics in a defective photonic crystal

    NASA Astrophysics Data System (ADS)

    Ramanujam, N. R.; Wilson, K. S. Joseph

    2015-06-01

    A photonic crystal (AB)2(DB)(AB)2 with high refractive index medium as silicon and low refractive medium as air is considered. Using the transfer matrix method, the transmission properties as a function of wavelength with photonic band gaps has been obtained. We are able to demonstrate the generation of third, fifth, seventh and ninth harmonics in the present work. We show that if the air medium is removed in the defect, the defect modes are generated but not harmonics. It can be designed to have a frequency conversion, and have a potential for becoming the basis for the next generation of optical devices.

  8. Generation of higher odd harmonics in a defective photonic crystal

    SciTech Connect

    Ramanujam, N. R.; Wilson, K. S. Joseph

    2015-06-24

    A photonic crystal (AB){sup 2}(DB)(AB){sup 2} with high refractive index medium as silicon and low refractive medium as air is considered. Using the transfer matrix method, the transmission properties as a function of wavelength with photonic band gaps has been obtained. We are able to demonstrate the generation of third, fifth, seventh and ninth harmonics in the present work. We show that if the air medium is removed in the defect, the defect modes are generated but not harmonics. It can be designed to have a frequency conversion, and have a potential for becoming the basis for the next generation of optical devices.

  9. Single-shot fluctuations in waveguided high-harmonic generation.

    PubMed

    Goh, S J; Tao, Y; van der Slot, P J M; Bastiaens, H J M; Herek, J; Biedron, S G; Danailov, M B; Milton, S V; Boller, K-J

    2015-09-21

    For exploring the application potential of coherent soft x-ray (SXR) and extreme ultraviolet radiation (XUV) provided by high-harmonic generation, it is important to characterize the central output parameters. Of specific importance are pulse-to-pulse (shot-to-shot) fluctuations of the high-harmonic output energy, fluctuations of the direction of the emission (pointing instabilities), and fluctuations of the beam divergence and shape that reduce the spatial coherence. We present the first single-shot measurements of waveguided high-harmonic generation in a waveguided (capillary-based) geometry. Using a capillary waveguide filled with Argon gas as the nonlinear medium, we provide the first characterization of shot-to-shot fluctuations of the pulse energy, of the divergence and of the beam pointing. We record the strength of these fluctuations vs. two basic input parameters, which are the drive laser pulse energy and the gas pressure in the capillary waveguide. In correlation measurements between single-shot drive laser beam profiles and single-shot high-harmonic beam profiles we prove the absence of drive laser beam-pointing-induced fluctuations in the high-harmonic output. We attribute the main source of high-harmonic fluctuations to ionization-induced nonlinear mode mixing during propagation of the drive laser pulse inside the capillary waveguide. PMID:26406689

  10. Generation of laser-driven higher harmonics from grating targets.

    PubMed

    Cerchez, M; Giesecke, A L; Peth, C; Toncian, M; Albertazzi, B; Fuchs, J; Willi, O; Toncian, T

    2013-02-01

    The first experimental evidence of the higher-order harmonic radiation generated by periodically modulated targets (gratings) irradiated by relativistic, ultrashort (<30 fs), high intensity [Iλ(2)=10(20) (W/cm(2)) μm(2)] laser pulse is presented. The interference effects on the grating surface lead to the emission of high harmonics up to 45th order along the target surface when the laser beam is focused onto a grating target close to normal incidence (5°). By means of numerical simulations we demonstrate the possibility of controlling the composition of the higher harmonic spectrum and we prove the influence of the laser pulse parameters in the interaction area (laser focusing and wavefront curvature) on the emission angle of a certain high harmonic order. PMID:23432262

  11. Hyperbolic metamaterial antenna for second-harmonic generation tomography.

    PubMed

    Segovia, Paulina; Marino, Giuseppe; Krasavin, Alexey V; Olivier, Nicolas; Wurtz, Gregory A; Belov, Pavel A; Ginzburg, Pavel; Zayats, Anatoly V

    2015-11-30

    The detection and processing of information carried by evanescent field components are key elements for subwavelength optical microscopy as well as single molecule sensing applications. Here, we numerically demonstrate the potential of a hyperbolic medium in the design of an efficient metamaterial antenna enabling detection and tracking of a nonlinear object, with an otherwise hidden second-harmonic signature. The presence of the antenna provides 103-fold intensity enhancement of the second harmonic generation (SHG) from a nanoparticle through a metamaterial-assisted access to evanescent second-harmonic fields. Alternatively, the observation of SHG from the metamaterial itself can be used to detect and track a nanoparticle without a nonlinear response. The antenna allows an optical resolution of several nanometers in tracking the nanoparticle's location via observations of the far-field second-harmonic radiation pattern. PMID:26698705

  12. Nonlinearly coupled localized plasmon resonances: Resonant second-harmonic generation

    NASA Astrophysics Data System (ADS)

    Ginzburg, Pavel; Krasavin, Alexey; Sonnefraud, Yannick; Murphy, Antony; Pollard, Robert J.; Maier, Stefan A.; Zayats, Anatoly V.

    2012-08-01

    The efficient resonant nonlinear coupling between localized surface plasmon modes is demonstrated in a simple and intuitive way using boundary integral formulation and utilizing second-order optical nonlinearity. The nonlinearity is derived from the hydrodynamic description of electron plasma and originates from the presence of material interfaces in the case of small metal particles. The coupling between fundamental and second-harmonic modes is shown to be symmetry selective and proportional to the spatial overlap between polarization dipole density of the second-harmonic mode and the square of the polarization charge density of the fundamental mode. Particles with high geometrical symmetry will convert a far-field illumination into dark nonradiating second-harmonic modes, such as quadrupoles. Effective second-harmonic susceptibilities are proportional to the surface-to-volume ratio of a particle, emphasizing the nanoscale enhancement of the effect.

  13. Impact of third-harmonic generation on the filamentation process

    NASA Astrophysics Data System (ADS)

    Doussot, J.; Béjot, P.; Faucher, O.

    2016-03-01

    The impact of third-harmonic generation on the propagation dynamics of a filament is revisited in light of recent theoretical and experimental results [P. Béjot, G. Karras, F. Billard, E. Hertz, B. Lavorel, E. Cormier, and O. Faucher, Phys. Rev. Lett. 112, 203902 (2014), 10.1103/PhysRevLett.112.203902] showing the extreme sensitivity of ionization to a bichromatic field. By performing a thorough parametric study, it is shown that third-harmonic generation can deeply influence the propagation of filaments in realistic focusing and pressure conditions. Demonstrated in the case of third-harmonic generation for different gases, this result sheds light on the effect of secondary radiations emitted during the filamentation process.

  14. Continuous control of the nonlinearity phase for harmonic generations.

    PubMed

    Li, Guixin; Chen, Shumei; Pholchai, Nitipat; Reineke, Bernhard; Wong, Polis Wing Han; Pun, Edwin Yue Bun; Cheah, Kok Wai; Zentgraf, Thomas; Zhang, Shuang

    2015-06-01

    The capability of locally engineering the nonlinear optical properties of media is crucial in nonlinear optics. Although poling is the most widely employed technique for achieving locally controlled nonlinearity, it leads only to a binary nonlinear state, which is equivalent to a discrete phase change of π in the nonlinear polarizability. Here, inspired by the concept of spin-rotation coupling, we experimentally demonstrate nonlinear metasurfaces with homogeneous linear optical properties but spatially varying effective nonlinear polarizability with continuously controllable phase. The continuous phase control over the local nonlinearity is demonstrated for second and third harmonic generation by using nonlinear metasurfaces consisting of nanoantennas of C3 and C4 rotational symmetries, respectively. The continuous phase engineering of the effective nonlinear polarizability enables complete control over the propagation of harmonic generation signals. Therefore, this method seamlessly combines the generation and manipulation of harmonic waves, paving the way for highly compact nonlinear nanophotonic devices. PMID:25849530

  15. Efficient Forward Second-Harmonic Generation from Planar Archimedean Nanospirals

    SciTech Connect

    Davidson, Roderick B.; Ziegler, Jed I.; Vargas, Guillermo; Avanesyan, Sergey M.; Gong, Yu; Hess, Wayne P.; Haglund Jr., Richard F.

    2015-01-21

    The enhanced electric field at plasmonic resonances in nanoscale antennas can lead to efficient harmonic generation, especially when the plasmonic geometry is asymmetric on either inter-particle or intra-particle levels. The planar Archimedean nanospiral offers a unique geometrical asymmetry for second-harmonic generation (SHG) because the SHG results neither from arranging centrosymmetric nanoparticles in asymmetric groupings, nor from noncentrosymmetric nanoparticles that retain a local axis of symmetry. Here we report forward SHG from planar arrays of Archimedean nanospirals using 15 fs pulse from a Ti:sapphire oscillator tuned to 800 nm wavelength. The measured harmonic-generation efficiencies are 2.6•10-9, 8•10-9 and 1.3•10-8 for left-handed circular, linear, and right-handed circular polarizations, respectively.

  16. Second- and third-harmonic generation with vector Gaussian beams

    NASA Astrophysics Data System (ADS)

    Carrasco, Silvia; Saleh, Bahaa E. A.; Teich, Malvin C.; Fourkas, John T.

    2006-10-01

    We consider second-harmonic generation (SHG) and third-harmonic generation (THG) in a nonlinear optical crystal illuminated by a vector Gaussian beam, i.e., a Gaussian beam in which the axial component of the excitation field is considered. This component exhibits twice the Gouy phase shift of the transverse component and vanishes at points on the beam axis. Harmonic generation stemming from this component exhibits a unique dependence on geometrical factors associated with the location and focusing of the beam relative to the location of the crystal. Using the first Born approximation (undepleted fundamental beam), we derive analytical formulas for the quantities that characterize these geometrical factors for a nonlinear optical crystal described by an arbitrary nonlinear susceptibility tensor, for both SHG and THG and for all polarization components. We also determine the efficiencies of these processes as functions of the geometry of the experimental arrangement for phase-matched crystals as well as for crystals of infinite length.

  17. Second-Harmonic Generation of Electrically Poled Borophosphate Glasses: Effects of Introducing Niobium or Sodium Oxides

    NASA Astrophysics Data System (ADS)

    Nazabal, V.; Fargin, E.; Videau, J. J.; Le Flem, G.; Le Calvez, A.; Montant, S.; Freysz, E.; Ducasse, A.; Couzi, M.

    1997-11-01

    Second-harmonic generation in poled glasses opens new frontiers in optical material research. Within this context new borophosphate glasses of the Ca(PO3)2-CaB4O7-Na2B4O7-Nb2O5system were synthesized and their second-harmonic generation was evaluated after poling treatment. The enhancement of the second-harmonic signal with niobium oxide content is related to the presence of distorted NbO6octahedra in the former of the glasses and to the increase in third-order susceptibility. The intensity of the measured second-harmonic signal is not dependent on the amount of sodium (100-1000 ppm) introduced into the glass.

  18. Cascaded Cerenkov third-harmonic generation in random quadratic media

    SciTech Connect

    Ayoub, Mousa; Roedig, Philip; Imbrock, Joerg; Denz, Cornelia

    2011-12-12

    We investigate experimentally and theoretically the conical emission of Cerenkov-type third-harmonic generation in strontium barium niobate of random 2D-{chi}{sup (2)} distribution. The azimuthal intensity distribution is explained by the polarization properties of the fundamental and Cerenkov second-harmonic waves, depending on the cascaded origin of the generation process. Moreover, we show the role of the individual domain shape in an additional modulation on the conical emission, controlled by the electrical switching of the spontaneous polarization of the ferroelectric medium.

  19. Confocal Imaging of Biological Tissues Using Second Harmonic Generation

    SciTech Connect

    Kim, B-M.; Stoller, P.; Reiser, K.; Eichler, J.; Yan, M.; Rubenchik, A.; Da Silva, L.

    2000-03-06

    A confocal microscopy imaging system was devised to selectively detect Second harmonic signals generated by biological tissues. Several types of biological tissues were examined using this imaging system, including human teeth, bovine blood vessels, and chicken skin. All these tissues generated strong second harmonic signals. There is considerable evidence that the source of these signals in tissue is collagen. Collagen, the predominant component of most tissues, is known to have second order nonlinear susceptibility. This technique may have diagnostic usefulness in pathophysiological conditions characterized by changes in collagen structure including malignant transformation of nevi, progression of diabetic complications, and abnormalities in wound healing.

  20. Sensing with multipolar second harmonic generation from spherical metallic nanoparticles.

    PubMed

    Butet, Jérémy; Russier-Antoine, Isabelle; Jonin, Christian; Lascoux, Noëlle; Benichou, Emmanuel; Brevet, Pierre-François

    2012-03-14

    We show that sensing in the nonlinear optical regime using multipolar surface plasmon resonances is more sensitive in comparison to sensing in the linear optical regime. Mie theory, and its extension to the second harmonic generation from a metallic nanosphere, is used to describe multipolar second harmonic generation from silver metallic nanoparticles. The standard figure of merit of a potential plasmonic sensor based on this principle is then calculated. We finally demonstrate that such a sensor is more sensitive to optical refraction index changes occurring in the vicinity of the metallic nanoparticle than its linear counterpart. PMID:22375818

  1. Optimization study of third harmonic generation in quantum cascade lasers.

    PubMed

    Mojibpour, Ali; Pourfath, Mahdi; Kosina, Hans

    2014-08-25

    A systematic optimization study of quantum cascade lasers with integrated nonlinearity for third-harmonic generation is performed. To model current transport the Pauli master equation is solved using a Monte Carlo approach. A multi-objective particle swarm optimization algorithm is applied to obtain the Pareto front. Our theoretical analysis indicates an optimized structure with five orders of magnitude increase in the generated third-harmonic power with respect to the reference design. This striking performance comes with a low threshold current density of about 1.6 kA/cm2 and is attributed to double resonant phonon scattering assisted extraction and injection scheme of the laser. PMID:25321265

  2. Even harmonic generation in isotropic media of dissociating homonuclear molecules

    PubMed Central

    Silva, R. E. F.; Rivière, P.; Morales, F.; Smirnova, O.; Ivanov, M.; Martín, F.

    2016-01-01

    Isotropic gases irradiated by long pulses of intense IR light can generate very high harmonics of the incident field. It is generally accepted that, due to the symmetry of the generating medium, be it an atomic or an isotropic molecular gas, only odd harmonics of the driving field can be produced. Here we show how the interplay of electronic and nuclear dynamics can lead to a marked breakdown of this standard picture: a substantial part of the harmonic spectrum can consist of even rather than odd harmonics. We demonstrate the effect using ab-initio solutions of the time-dependent Schrödinger equation for and its isotopes in full dimensionality. By means of a simple analytical model, we identify its physical origin, which is the appearance of a permanent dipole moment in dissociating homonuclear molecules, caused by light-induced localization of the electric charge during dissociation. The effect arises for sufficiently long laser pulses and the region of the spectrum where even harmonics are produced is controlled by pulse duration. Our results (i) show how the interplay of femtosecond nuclear and attosecond electronic dynamics, which affects the charge flow inside the dissociating molecule, is reflected in the nonlinear response, and (ii) force one to augment standard selection rules found in nonlinear optics textbooks by considering light-induced modifications of the medium during the generation process. PMID:27596609

  3. Generation of intense high-order vortex harmonics.

    PubMed

    Zhang, Xiaomei; Shen, Baifei; Shi, Yin; Wang, Xiaofeng; Zhang, Lingang; Wang, Wenpeng; Xu, Jiancai; Yi, Longqiong; Xu, Zhizhan

    2015-05-01

    This Letter presents for the first time a scheme to generate intense high-order optical vortices that carry orbital angular momentum in the extreme ultraviolet region based on relativistic harmonics from the surface of a solid target. In the three-dimensional particle-in-cell simulation, the high-order harmonics of the high-order vortex mode is generated in both reflected and transmitted light beams when a linearly polarized Laguerre-Gaussian laser pulse impinges on a solid foil. The azimuthal mode of the harmonics scales with its order. The intensity of the high-order vortex harmonics is close to the relativistic region, with the pulse duration down to attosecond scale. The obtained intense vortex beam possesses the combined properties of fine transversal structure due to the high-order mode and the fine longitudinal structure due to the short wavelength of the high-order harmonics. In addition to the application in high-resolution detection in both spatial and temporal scales, it also presents new opportunities in the intense vortex required fields, such as the inner shell ionization process and high energy twisted photons generation by Thomson scattering of such an intense vortex beam off relativistic electrons. PMID:25978234

  4. Even harmonic generation in isotropic media of dissociating homonuclear molecules.

    PubMed

    Silva, R E F; Rivière, P; Morales, F; Smirnova, O; Ivanov, M; Martín, F

    2016-01-01

    Isotropic gases irradiated by long pulses of intense IR light can generate very high harmonics of the incident field. It is generally accepted that, due to the symmetry of the generating medium, be it an atomic or an isotropic molecular gas, only odd harmonics of the driving field can be produced. Here we show how the interplay of electronic and nuclear dynamics can lead to a marked breakdown of this standard picture: a substantial part of the harmonic spectrum can consist of even rather than odd harmonics. We demonstrate the effect using ab-initio solutions of the time-dependent Schrödinger equation for and its isotopes in full dimensionality. By means of a simple analytical model, we identify its physical origin, which is the appearance of a permanent dipole moment in dissociating homonuclear molecules, caused by light-induced localization of the electric charge during dissociation. The effect arises for sufficiently long laser pulses and the region of the spectrum where even harmonics are produced is controlled by pulse duration. Our results (i) show how the interplay of femtosecond nuclear and attosecond electronic dynamics, which affects the charge flow inside the dissociating molecule, is reflected in the nonlinear response, and (ii) force one to augment standard selection rules found in nonlinear optics textbooks by considering light-induced modifications of the medium during the generation process. PMID:27596609

  5. Harmonic Generation from Solid Targets - Optmization of Source Parameters

    NASA Astrophysics Data System (ADS)

    Zepf, Matthew; Watts, I. F.; Dangor, A. E.; Norreys, P. A.; Chambers, D. M.; Machacek, A.; Wark, J. S.; Tsakiris, G. D.

    1998-11-01

    High harmonics from solid targets have received renewed interest over the last few years. Theoretical predictions using 1 1/2 D codes suggest that very high orders (>100 ) can be generated at conversion efficiencies in excess of 10-6 [1,2] at Iλ^2 > 10^19 W/cm^2. Experiments have since been performed with pulses varying from 100 fs to 2.5 ps in duration [3-6]. The steep density gradient necessary to generate the harmonics can be generated by either ponderomotive steepening or by using ultraclean pulses which preserve the initial solid vacuum boundary. The two regimes are compared in terms of their dependence on the laser parameters and the emitted harmonic radiation. Particular emphasis will be given to measurements of the holeboring velocity, the polarisation of the harmonics and the intensity scaling in the two regimes. This comparison enables us to find the ideal parameter range for the optimization of harmonic source. [1] R. Lichters et al., Physics of Plasmas 3, 3425, (1996). [2] P. Gibbon, IEEE J. of Q. Elec. 33, 1915 (1997). [3] S. Kohlweyer, et al., Optics Comm. 177, 431 (1995). [4] P. Norreys et al., Phys. Rev. Lett., 76, 1832 (1995). [5] D. von der Linde et al., Phys. Rev. A, 52, R25 (1995) [6] M. Zepf, et al., submitted for publication in Phys. Rev. Lett.

  6. Titanosilicates with Strong Phase-Matched Second Harmonic Generation Responses.

    PubMed

    Chao, Tzu-Ling; Chang, Wen-Jung; Wen, Shu-Han; Lin, Yu-Qing; Chang, Bor-Chen; Lii, Kwang-Hwa

    2016-07-27

    The search for new and efficient nonlinear optical (NLO) materials has been an active research because of their technological importance in laser applications. Although a large number of frequency-doubling oxides, phosphates, borates, and fluoride-containing borates were found, no transition-metal silicate with useful NLO properties has been reported. We have now synthesized and grown crystals of two new titanosilicates, Li2K4[(TiO)Si4O12] and Li2Rb4[(TiO)Si4O12], by using a flux and supercritical hydrothermal method. Their unique 3D framework structures contain highly compressed TiO5 square pyramids which are arranged one over the other to form infinite ···Ti-O···Ti-O straight chains with alternating short and long Ti-O distances. These two materials meet the requirements for efficient second harmonic generation including lack of center of inversion symmetry, large susceptibility, phase matching, transmitting at wavelengths of interest, resistant to laser damage, and thermally stable. These attributes make them very attractive for frequency-doubling materials. PMID:27416357

  7. Detecting and characterizing ferroelectric domain boundaries using nonphase-matched second harmonic generation

    SciTech Connect

    Gehr, R.J.; Alford, W.J.; Smith, A.V.

    1998-12-31

    We demonstrate that tilted planar ferroelectric domain boundaries create tilted second harmonic beams in nonphase-matched second harmonic generation, and that the tilt of the boundary can be deduced from the harmonic direction.

  8. Extreme Harmonic Generation in Electrically Driven Spin Resonance

    NASA Astrophysics Data System (ADS)

    Stehlik, Jiri

    2015-03-01

    InAs nanowire double quantum dots offer a rich platform for studying single spin physics in a material with large spin-orbit (SO) coupling. The large SO coupling allows all electrical control of the electron spin through electric dipole spin resonance (EDSR). Here an oscillating electric field of frequency f displaces the electron wave function, while a magnetic field with strength B is applied. Spin rotations occur when the resonance condition hf = gμB B is met. Here g is the electron g-factor, h is Planck's constant, and μB is the Bohr magneton. We find that near zero interdot detuning efficient spin rotations also occur when hf = ngμB B , with n being an integer as large as 8 in our system. The harmonics feature a striking odd/even dependence. While the odd harmonics show an enhancement of the leakage current, the even harmonics show a reduction. In contrast, we do not observe any measurable harmonics at large detuning. We link the presence of harmonics with additional anti-crossings present in the level diagram. This implies that harmonics are the result of Landau-Zener transitions occurring at multiple anti-crossings. Recent theoretical work supports this conclusion. Research performed in collaboration with M. D. Schroer, M. Z. Maialle, M. H. Degani, and J. R. Petta. Research was supported by the Sloan and Packard Foundations, Army Research Office, DARPA QuEST and the NSF.

  9. Observation of Electronic Structure Minima in High-Harmonic Generation

    SciTech Connect

    Woerner, Hans Jakob; Villeneuve, D. M.; Niikura, Hiromichi; Bertrand, Julien B.; Corkum, P. B.

    2009-03-13

    We report detailed measurements of the high-harmonic spectra generated from argon atoms. The spectra exhibit a deep minimum that is shown to be independent of the laser intensity, and is thus a clear measure of the electronic structure of the atom. We show that exact field-free continuum wave functions reproduce the minimum, but plane wave and Coulomb wave functions do not. This remarkable observation suggests that electronic structure can be accurately determined in high-harmonic experiments despite the presence of the strong laser field. Our results clarify the relation between high-harmonic generation and photoelectron spectroscopy. The use of exact continuum functions also resolves the ambiguity associated with the choice of the dispersion relation.

  10. Generation of harmonics and supercontinuum in nematic liquid crystals

    SciTech Connect

    Nyushkov, B N; Trashkeev, S I; Klementyev, Vasilii M; Pivtsov, V S; Kobtsev, Sergey M

    2013-02-28

    Nonlinear optical properties of nematic liquid crystals (NLC) have been investigated. A technique for efficient laser frequency conversion in a microscopic NLC volume deposited on an optical fibre end face is experimentally demonstrated. An efficient design of a compact NLC-based IR frequency converter with a fibre input and achromatic collimator is proposed and implemented. Simultaneous generation of the second and third harmonics is obtained for the first time under pumping NLC by a 1.56-mm femtosecond fibre laser. The second-harmonic generation efficiency is measured to be about 1 %, while the efficiency of third-harmonic generation is several tenths of percent. A strong polarisation dependence of the third-harmonic generation efficiency is revealed. When pumping NLC by a cw laser, generation of spectral supercontinua (covering the visible and near-IR spectral ranges) is observed. The nonlinear effects revealed can be due to the light-induced change in the orientational order in liquid crystals, which breaks the initial symmetry and leads to formation of disclination structures. The NLC optical nonlinearity is believed to be of mixed orientationalelectronic nature as a whole. (laser optics 2012)

  11. Theory of second harmonic generation in randomly oriented species

    NASA Astrophysics Data System (ADS)

    Andrews, David L.; Allcock, Philip; Demidov, Andrey A.

    1995-01-01

    It is well known that second harmonic generation (SHG) is a process forbidden within atomic and molecular fluids. Nonetheless recent experimental observations of second harmonic evolution in suspensions of randomly oriented Halobacterium halobium purple membranes have raised new questions about the precise criteria which determine prohibition of the second harmonic. To address the problem a theoretical framework for SHG is developed that specifically deals with molecular systems, and is therefore cast in terms of molecular properties with more regard to the influence of the local structure. This contrasts with the classical approach based on bulk susceptibilities, which has not proved adequate to explain the conflicting experimental results. By properly formulating the detailed procedure for dealing with the necessary orientational averages, the present theory discloses a relationship between the coherent process of second harmonic generation and a directed component of its incoherent counterpart, hyper-Rayleigh scattering. Inter alia, the theory explains the SHG detected in purple membrane suspensions. The polarisation features of the harmonic evolution are also considered more generally, and in particular it is shown that the SHG signal will persist under conditions of circularly polarised pumping. This specific polarisation feature will allow experimental validation of the theory.

  12. Enhancement of third harmonic generation by wave vector mismatch to counter phase-modulation

    NASA Astrophysics Data System (ADS)

    Trippenbach, M.; Matuszewski, M.; Infeld, E.; Long Van, Cao; Tasgal, R. S.; Band, Y. B.

    2004-01-01

    Recent experimental developments in material sciences have generated hope that it will be possible to devise optical media where the difference in group velocity between the fundamental and third harmonic may be strongly suppressed. Under these circumstances both pulses would travel together over a long distance. This would lead to an enhancement of the generation process, and hence strong focusing and/or using ultra-short pulses might not be crucial. If the perfect phase matching condition is assumed, the only remaining mechanisms to decrease efficiency are self and cross phase modulation. Here we suggest that, instead of exactly matching wave vectors, we admit a small mismatch and show how it can be tailored to compensate for the cross phase modulation of the third harmonic by the fundamental during the generation process. This is very beneficial for the efficiency of third harmonic generation, even increasing it by a factor of two or more.

  13. Second-harmonic generation microscopy of collagen-bearing structures

    NASA Astrophysics Data System (ADS)

    Vanbel, Maarten K.; Callewaert, Tom; Verbiest, Thierry

    2014-05-01

    Nonlinear optical phenomena cover a broad research area. The emphasis is mostly on the generation of higher harmonics to be used in laser designs or on the characterization capabilities of nonlinear optics. The latter ability of nonlinear optics is important when combined with a microscope to detect simultaneously multiphoton fluorescence and second-harmonic generation. Submicron size features can then be investigated separately and information on their structure can be revealed by second-harmonic generation. For example, the point group symmetry can be determined in situ and in vivo in complex media. Moreover, nonlinear optical microscopy has several additional advantages: the generation and detection of nonlinear signals is intrinsically confocal and degradation, if present, only occurs at a localized places in the structure. In biological structures, multiphoton fluorescence and second-harmonic generation do not necessarily occur in the same type of the structure. This can be exploited to visualize different structures in one sample by simultaneous detection of two-photon fluorescence and second-harmonic generation. Also, the incident beam can be tuned to fit in the biological window of biological structures, which gives second-harmonic generation microscopy a significant advantage over linear microscopy due to absorbance issues in the visible wavelength range. We exploit these advantages to characterize collagen-bearing biological structures. Collagen is the dominant structural protein in connective tissue in mammals. Being the most abundant protein in the mammal clade, it is essential for the very existence of it. Collagen is a protein with a very strict quaternary structure. The most simple Ramachandran model states that an amino-acid sequence of Glycine-prolin-hydroxyprolin leads to a right-handed helical structure. The inherent stability is such that a sole helix cannot exist for a prolonged period of time, it will therefore combine with 2 near identical

  14. High intensity direct third harmonic generation in BBO

    SciTech Connect

    Banks, P.S., LLNL

    1998-02-23

    The azimuthal dependence of second- and third-order coupling are used to measure the relative contributions of each to direct third harmonic generation with efficiencies up to 6%. The values of {xi}{sub ij}{sup (3)} are measured.

  15. Efficient forward second-harmonic generation from planar archimedean nanospirals

    NASA Astrophysics Data System (ADS)

    Davidson, Roderick B., II; Ziegler, Jed I.; Vargas, Guillermo; Avanesyan, Sergey M.; Gong, Yu; Hess, Wayne; Haglund, Richard F., Jr.

    2015-05-01

    The enhanced electric field at plasmonic resonances in nanoscale antennas can lead to efficient harmonic generation, especially when the plasmonic geometry is asymmetric on either inter-particle or intra-particle levels. The planar Archimedean nanospiral offers a unique geometrical asymmetry for second-harmonic generation (SHG) because the SHG results neither from arranging centrosymmetric nanoparticles in asymmetric groupings, nor from non-centrosymmetric nanoparticles that retain a local axis of symmetry. Here, we report forward SHG from planar arrays of Archimedean nanospirals using 15 fs pulses from a Ti:sapphire oscillator tuned to 800 nm wavelength. The measured harmonic-generation efficiencies are 2.6·10-9, 8·10-9 and 1.3·10-8 for left-handed circular, linear, and right-handed circular polarizations, respectively. The uncoated nanospirals are stable under average power loading of as much as 300 μWper nanoparticle. The nanospirals also exhibit selective conversion between polarization states. These experiments show that the intrinsic asymmetry of the nanospirals results in a highly efficient, two-dimensional harmonic generator that can be incorporated into metasurface optics.

  16. Digital Video Disc Recorder Using Second Harmonic Generation Green Laser

    NASA Astrophysics Data System (ADS)

    Seo, Joong Eon; Park, In Sik; Oh, Young Nam; Lee, Seung Hoon; Seong, Pyong Yong; Jang, Yoon Ki; Shin, Dong Ho

    1993-11-01

    A prototype of a digital video disc recorder (D-VDR) with laser-disc-quality video and compact-disc-quality audio is developed and demonstrated using a second harmonic generation (SHG) green laser, narrow-track magneto-optical disk (MOD), mark edge recording and data compression.

  17. Few recent experiments on surface studies by second harmonic generation

    SciTech Connect

    Shen, Y.R.

    1985-12-01

    Surface second harmonic generation (SHG) is used to monitor adsorption and desorption of molecules on metal and semiconductor surfaces in ultrahigh vacuum. Surface SHG has also been used to study monolayers of molecules at a liquid/air interface. 13 refs., 6 figs. (WRF)

  18. Resonance Thirring solitons in type II second-harmonic generation

    NASA Astrophysics Data System (ADS)

    Trillo, Stefano

    1996-11-01

    It is shown that second-harmonic generation in a grating allows one to cancel the group-velocity difference between two polarization components at fundamental by means of nonlinearly induced phase shifts. This occurs when a new type of cascading soliton propagates on resonance.

  19. Imaging Collagen Orientation Using Polarization-Modulated Second Harmonic Generation

    SciTech Connect

    Stoller, P; Celliers, P M; Reiser, K M; Rubenchik, A M

    2002-01-10

    We use polarization-modulated second harmonic generation to image fiber orientation in collagen tissues, with an axial resolution of about 10 {micro}m and a transverse resolution of up to 1 {micro}m. A linearly polarized ultra-short pulse (200 fs) Ti:Sapphire laser beam is modulated using an electro-optic modulator and quarter-wave plate combination and focused onto a translation stage mounted sample using a microscope objective. The generated second harmonic light is collected using a photomultiplier tube and demodulated using phase sensitive detection to obtain signal intensity and fiber orientation information. In order to obtain second harmonic generation images of different types of collagen organization, we analyze several different tissues, including rat-tail tendon, mouse aorta, mouse fibrotic liver, and porcine skin. We can use our technique to image fibrotic tissue in histological sections of damaged liver and to identify burned tissue in porcine skin to a depth of a few hundred microns. Polarization-modulated second harmonic generation potentially could be a useful clinical technique for diagnosing collagen related disease or damage, especially in the skin.

  20. Modulation compression for short wavelength harmonic generation

    SciTech Connect

    Qiang, J.

    2010-01-11

    Laser modulator is used to seed free electron lasers. In this paper, we propose a scheme to compress the initial laser modulation in the longitudinal phase space by using two opposite sign bunch compressors and two opposite sign energy chirpers. This scheme could potentially reduce the initial modulation wavelength by a factor of C and increase the energy modulation amplitude by a factor of C, where C is the compression factor of the first bunch compressor. Such a compressed energy modulation can be directly used to generate short wavelength current modulation with a large bunching factor.

  1. High-order harmonic generation in a capillary discharge

    DOEpatents

    Rocca, Jorge J.; Kapteyn, Henry C.; Mumane, Margaret M.; Gaudiosi, David; Grisham, Michael E.; Popmintchev, Tenio V.; Reagan, Brendan A.

    2010-06-01

    A pre-ionized medium created by a capillary discharge results in more efficient use of laser energy in high-order harmonic generation (HHG) from ions. It extends the cutoff photon energy, and reduces the distortion of the laser pulse as it propagates down the waveguide. The observed enhancements result from a combination of reduced ionization energy loss and reduced ionization-induced defocusing of the driving laser as well as waveguiding of the driving laser pulse. The discharge plasma also provides a means to spectrally tune the harmonics by tailoring the initial level of ionization of the medium.

  2. Effect of Structural Modification on Second Harmonic Generation in Collagen

    SciTech Connect

    Stoller, P C; Reiser, K M; Celliers, P M; Rubenchik, A M

    2003-04-04

    The effects of structural perturbation on second harmonic generation in collagen were investigated. Type I collagen fascicles obtained from rat tails were structurally modified by increasing nonenzymatic cross-linking, by thermal denaturation, by collagenase digestion, or by dehydration. Changes in polarization dependence were observed in the dehydrated samples. Surprisingly, no changes in polarization dependence were observed in highly crosslinked samples, despite significant alterations in packing structure. Complete thermal denaturation and collagenase digestion produced samples with no detectable second harmonic signal. Prior to loss of signal, no change in polarization dependence was observed in partially heated or digested collagen.

  3. Microscopic approach to second harmonic generation in quantum cascade lasers.

    PubMed

    Winge, David O; Lindskog, Martin; Wacker, Andreas

    2014-07-28

    Second harmonic generation is analyzed from a microscopical point of view using a non-equilibrium Green's function formalism. Through this approach the complete on-state of the laser can be modeled and results are compared to experiment with good agreement. In addition, higher order current response is extracted from the calculations and together with waveguide properties, these currents provide the intensity of the second harmonic in the structure considered. This power is compared to experimental results, also with good agreement. Furthermore, our results, which contain all coherences in the system, allow to check the validity of common simplified expressions. PMID:25089458

  4. Two-color pump of laser plasmas for harmonic generation

    NASA Astrophysics Data System (ADS)

    Ganeev, R. A.

    2016-05-01

    Various laser-produced metal plasmas were used for high-order sum and difference harmonic generation using the mixing of tunable mid-infrared pulses from optical parametric amplifier and 810 nm ultrashort pulses. We show that, regardless of non-optimal spatio-temporal overlap of two sources of radiation in the plasmas, the application of proposed technique allows a significant growth of harmonic yield and broadening of the number of different combinations of interacting waves in the extreme ultraviolet region, which could be useful for observation of the resonance induced enhancement of some frequency components.

  5. High harmonic generation by novel fiber amplifier based sources.

    PubMed

    Hädrich, S; Rothhardt, J; Krebs, M; Tavella, F; Willner, A; Limpert, J; Tünnermann, A

    2010-09-13

    Significant progress in high repetition rate ultrashort pulse sources based on fiber technology is presented. These systems enable operation at a high repetition rate of up to 500 kHz and high average power in the extreme ultraviolet wavelength range via high harmonic generation in a gas jet. High average power few-cycle pulses of a fiber amplifier pumped optical parametric chirped pulse amplifier are used to produce µW level average power for the strongest harmonic at 42.9 nm at a repetition rate of 96 kHz. PMID:20940915

  6. Polarization of high harmonic generated spectra in H+2ion

    NASA Astrophysics Data System (ADS)

    Castiglia, Giuseppe; Corso, Pietro Paolo; Daniele, Rosalba; Fiordilino, Emilio; Morales, Francesca

    2013-10-01

    We study the polarization of the harmonics generated by a homonuclear diatomic molecule in the presence of an intense, linearly polarized laser field. The polarization parameters of the emitted radiation are investigated as a function of the angle ? between the laser electric field and the molecular axis. The calculations are carried out by assuming a single active electron model with fixed nuclei; a two-dimensional model of the system is used. We find a different dependence of the parameters of the harmonics vs ? in the first or second half of the emitted spectrum. In particular, the differences are accentuated for ?, while for higher angles, until the perpendicular orientation, almost all the harmonics present similar characteristics.

  7. Theory of Harmonic Generation on a Traveling Wave Tube

    NASA Astrophysics Data System (ADS)

    Dong, C. F.; Zhang, P.; Chernin, D.; Lau, Y. Y.; Simon, D. H.; Wong, P.; Greening, G.; Gilgenbach, R. M.

    2015-11-01

    In a klystron, charge overtaking of electrons leads to an infinity of AC current. The harmonic content therein has been calculated accurately, with or without space charge effects. This paper extends the klystron theory to a traveling wave tube (TWT). We calculate the harmonic content on the beam current on a TWT that results from an input signal of a single frequency. We assume that the electron motion is described by linear theory, which is generally accurate over 85 percent of the tube length. These linear orbits may lead to charge overtaking and therefore harmonic generation, as in a klystron. We calculate the buildup of harmonic content as a function of distance from the input, and compare these analytic results with the CHRISTINE code. Reasonable agreement was found. A dimensionless ``bunching parameter'' for TWT, X = sqrt[(Pi/Pb)/C], is identified, which characterizes the harmonic content in the AC current, where Pi is the input power of the signal, Pb is the DC beam power, and C is Pierce's gain parameter. Supported by AFOSR FA9550-14-1-0309, FA9550-15-1-0097, ONR N00014-13-1-0566, and L-3 Communications.

  8. Monitoring photoaging by use of multiphoton fluorescence and second harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Lin, Sung-Jan; Jee, Shiou-Hwa; Chan, Jung-Yi; Wu, Ruei-Jr; Lo, Wen; Tan, Hsin-Yuan; Lin, Wei-Chou; Chen, Jau-Shiuh; Young, Tai-Horng; Hsu, Chih-Jung; Dong, Chen-Yuan

    2006-02-01

    It is a field of great interest to develop therapies to rejuvenate photoaged skin. However, the treatment response can not be ideally determined due to lack of a reliable non-invasive method to quantify photoaging. In this study, the photoaging process of skin is investigated by use of a multiphoton fluorescence and second harmonic generation microscopy. We obtain the autofluorescence and second harmonic generation images of superficial dermis from facial skin of individuals of different ages. The results show that autofluorescence signals increase with age while second harmonic generation signals decrease with age. The results are consistent with the histological findings in which collagen is progressively replaced by elastic fibers. In the case of severe photoaging, solar elastosis can be clearly demonstrated by the presence of thick curvy autofluorescent materials in the superficial dermis. We propose a second harmonic generation to autofluorescence aging index of dermis to quantify the photoaging changes. This index is shown to be a good indicator of photoaging. Our results suggest that multiphoton fluorescence and second harmonic generation microscopy can be developed into a non-invasive imaging modelity for the clinical evaluation of photoaging.

  9. Evidence of High Harmonics from Echo-Enabled Harmonic Generation for Seeding X-ray Free Electron Lasers

    SciTech Connect

    Xiang, D.; Colby, E.; Dunning, M.; Gilevich, S.; Hast, C.; Jobe, K.; McCormick, D.; Nelson, J.; Raubenheimer, T.O.; Soong, K.; Stupakov, G.; Szalata, Z.; Walz, D.; Weathersby, S.; Woodle, M.; /SLAC

    2012-02-15

    Echo-enabled harmonic generation free electron lasers hold great promise for the generation of fully coherent radiation in x-ray wavelengths. Here we report the first evidence of high harmonics from the echo-enabled harmonic generation technique in the realistic scenario where the laser energy modulation is comparable to the beam slice energy spread. In this experiment, coherent radiation at the seventh harmonic of the second seed laser is generated when the energy modulation amplitude is about 2-3 times the slice energy spread. The experiment confirms the underlying physics of echo-enabled harmonic generation and may have a strong impact on emerging seeded x-ray free electron lasers that are capable of generating laserlike x rays which will advance many areas of science.

  10. Predicting bulk damage in NIF triple harmonic generators

    SciTech Connect

    De Yoreo, J; Runkel, M; Williams, W

    1998-09-18

    Recently reported experiments have investigated the statistics of laser damage in KDP and KD*P. Automated damage tests have allowed cumulative failure and damage probability distributions to be constructed. Large area tests have investigated the feasibility of on-line laser conditioning and damage evolution for tripler harmonic generation (THG) crystals on the National Ignition Facility (NIF). These tests have shown that there is a nonzero probability of damage at NIF redline fluence (14.3 J/cm2, 351 nm, 3 ns) and that the damage pinpoint density evolves exponentially with fluence. In this paper, the results of these tests are used in conjunction with model spatial profiles of the NIP beam to predict the level of damage created in the THG crystal. A probabilistic calculation based on the overlap of the beam fluence and damage probabiity distribution shows that the overall damage probability is less than 3% for well-conditioned, high quality KDP/KD*P crystals of conventional or rapid growth. The number density of generated pinpoints has been calculated by mapping the damage evolution curves onto the NlF model profile. This shows that the number of damage pinpoints generated in high fluence portions of the NIF beam will be low for well-conditioned THG crystals. In contrast, unconditioned triplers of the same material will exhibit an increase in pinpoint density of greater than 20x. To test the validity of these calculations a 37 cm, conventionally grown KD*P tripler from the Beamlet laser was scatter mapped for bulk damage. The tripler had been exposed to NE-like fluences during its operational lifetime on Beamlet and exhibited very low levels of bulk pinpoint damage, essentially supporting the predictions based on tests and modeling.

  11. New Molecular Ferroelectrics Accompanied by Ultrahigh Second-Harmonic Generation.

    PubMed

    Liu, Chuang; Gao, Kaige; Cui, Zepeng; Gao, Linsong; Fu, Da-Wei; Cai, Hong-Ling; Wu, X S

    2016-05-19

    Second-harmonic generation (SHG) is one of the outstanding properties for practical applications. However, the great majority of molecular ferroelectric materials have very low nonlinear optical coefficients, attenuating their attractive performance. Here we synthesized (4-amino-2-bromopyridinium)(4-amino-2-bromopyridine)tetrafluoroborate (1), whose second-order nonlinear optical coefficient reaches up to 2.56 pm V(-1), 2.67 times of that of KDP, and (4-amino-2-bromopyridinium)tetrafluoroborate (2), possessing a more incredible large second-order nonlinear optical coefficient as high as 10.24 pm V(-1), 10.67 times that of KDP. The compound 1 undergoes two reversible phase transitions at around T1 = 244.1 K and T2 = 154.6 K, caused by dramatic changes of the protonated cations and order-disorder of anions, which was disclosed by differential scanning calorimetry, heat capacity, dielectric anomalies, SHG, and single-crystal X-ray diffraction analysis. The pyroelectric measurements reveal that compound 1 is a Rochelle salt type ferroelectric, which has a large spontaneous polarization of about 3 μC/cm(2). PMID:27111056

  12. 78 FR 8431 - Hazardous Materials: Harmonization with International Standards (RRR)

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-02-06

    ... From the Federal Register Online via the Government Publishing Office DEPARTMENT OF TRANSPORTATION Pipeline and Hazardous Materials Safety Administration 49 CFR Part 172 RIN 2137-AE87 Hazardous Materials: Harmonization with International Standards (RRR) Correction In rule document 2012-31243 appearing on pages...

  13. Dependence of high-order-harmonic generation on dipole moment in Si O2 crystals

    NASA Astrophysics Data System (ADS)

    Yu, Chao; Zhang, Xirui; Jiang, Shicheng; Cao, Xu; Yuan, Guanglu; Wu, Tong; Bai, Lihua; Lu, Ruifeng

    2016-07-01

    High-order-harmonic generation in α-quartz Si O2 is theoretically investigated under a strong laser field by solving the extended semiconductor Bloch equations. The accurate band structures as well as dipole moments between different bands are obtained from state-of-the-art first-principles calculations. We find that the shapes of k -space-dependent dipole moments play an important role in harmonic generation. The calculated results show that harmonic conversion efficiency is significantly enhanced and the cutoff energy is distinctly increased when the dipole moments change greatly along a valley in the k direction in the solid. Based on that dependence on the dipole moment, we also show that symmetry groups greatly affect the harmonic spectra from the solid materials. Moreover, a two-color synthesized field is used to achieve a supercontinuum harmonic spectrum near the cutoff region, and isolated attosecond pulses can be obtained directly by filtering out the harmonic radiation. We hope the contribution presented in this work provides a useful reference for future studies on laser-crystal interactions.

  14. Reexamining the high-order harmonic generation of HD molecule in non-Born-Oppenheimer approximation

    NASA Astrophysics Data System (ADS)

    Du, Hongchuan; Yue, Shengjun; Wang, Huiqiao; Wu, Hongmei; Hu, Bitao

    2016-03-01

    The high-order harmonic generation of the HD molecule is studied in non-Born-Oppenheimer approximation. It is found that there are only the odd harmonics in the harmonic spectrum of the HD molecule though the generation of even harmonics is possible in principle. Theoretical analysis [T. Kreibich et al., Phys. Rev. Lett. 87, 103901 (2001)] reveals that the nuclear dipole moment can contribute to the generation of the even harmonics, but the acceleration of the nucleus is about three orders of magnitude less than that of the electron. Hence, the even harmonics cannot be observed in the harmonic spectrum of the HD molecule.

  15. Creation and doubling of vortices in intracavity second harmonic generation

    NASA Astrophysics Data System (ADS)

    Lim, Oo-Kaw; Boland, Brian; Saffman, Mark; Krolikowski, Wieslaw

    2004-05-01

    Optical vortices are topological objects whose transformation properties under propagation in linear and nonlinear optical media have been the subject of much recent interest. In this work we demonstrate generation and frequency doubling of unit charge vortices in a linear astigmatic resonator. By appropriate alignment of a near confocal cavity we couple a fundamental laser beam at 860nm to a vortical resonator mode. With a nonlinear crystal in the resonator a doubly charged vortex at the second harmonic frequency is generated. Topological instability of the double charge harmonic vortices leads to well separated vortex cores that are shown to rotate and become anisotropic, as the resonator is tuned across resonance. A simple theory that accounts for crystal induced astigmatism agrees well with the experimental measurements.

  16. Corneal imaging by second and third harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Brocas, Arnaud; Jay, Louis; Mottay, Eric; Brunette, Isabelle; Ozaki, Tsuneyuki

    2008-02-01

    Advanced imaging methods are essential tools for improved outcome of refractive surgery. Second harmonic generation (SHG) and third harmonic generation (THG) microscopy are noninvasive high-resolution imaging methods, which can discriminate the different layers of the cornea, thus having strong impact on the outcome of laser surgery. In this work, we use an Ytterbium femtosecond laser as the laser source, the longer wavelength of which reduces scattering, and allows simultaneous SHG and THG imaging. We present SHG and THG images and profiles of pig corneas that clearly show the anterior surface of the cornea, the entry in the stroma and its end, and the posterior surface of the cornea. These observations allow localizing the epithelium, the stroma and the endothelium. Other experiments give information about the structure and cytology of the corneal layers.

  17. Enhanced Harmonic Generation via Breaking of Phase-Matching Symmetry

    NASA Astrophysics Data System (ADS)

    Sergan, Ekaterina; Gibson, George

    2016-05-01

    We discuss experimental results of third harmonic generation (THG) with a focused Gaussian beam in the semi-infinite limit, using two methods. The first method involves placing a metal septum at the waist such that the laser drills a small pinhole, which in turn disrupts the beam after the waist. The second method uses a very thin septum as a separator for two gasses: one with a large third order susceptibility (before the focus), and the other with a small susceptibility (after the focus). Both methods inhibit harmonic generation immediately after the beam waist, leading to increased conversion efficiency and better mode quality. Our work involves studies of conversion efficiency with varying septum thickness and gas pressure, and the results are compared to computer simulations. We would like to acknowledge support from the NSF under Grant No. PHY-1306845.

  18. Second harmonic generation and enhancement in microfibers and loop resonators

    NASA Astrophysics Data System (ADS)

    Gouveia, Marcelo A.; Lee, Timothy; Ismaeel, Rand; Ding, Ming; Broderick, Neil G. R.; Cordeiro, Cristiano M. B.; Brambilla, Gilberto

    2013-05-01

    We model and experimentally investigate second harmonic generation in silica microfibers and loop resonators, in which the second order nonlinearity arises from the glass-air surface dipole and bulk multipole contributions. In the loop resonator, the recirculation of the pump light on resonance is used to increase the conversion. The effect of the loop parameters, such as coupling and loss, is theoretically studied to determine their influence on the resonance enhancement. Experimentally, microfibers were fabricated with diameters around 0.7 μm to generate the intermodally phase matched second harmonic with an efficiency up to 4.2 × 10-8 when pumped with 5 ns 1.55 μm pulses with a peak power of 90 W. After reconfiguring the microfiber into a 1 mm diameter loop, the efficiency was resonantly enhanced by 5.7 times.

  19. Continuous third harmonic generation in a terahertz driven modulated nanowire

    SciTech Connect

    Hamilton, Kathleen E. De, Amrit; Pryadko, Leonid P.; Kovalev, Alexey A.

    2015-06-07

    We consider the possibility of observing continuous third-harmonic generation using a strongly driven, single-band one-dimensional metal. In the absence of scattering, the quantum efficiency of frequency tripling for such a system can be as high as 93%. Combining the Floquet quasi-energy spectrum with the Keldysh Green's function technique, we derive a semiclassical master equation for a one-dimensional band of strongly and rapidly driven electrons in the presence of weak scattering by phonons. The power absorbed from the driving field is continuously dissipated by phonon modes, leading to a quasi-equilibrium in the electron distribution. We use the Kronig-Penney model with varying effective mass to establish the growth parameters of an InAs/InP nanowire near optimal for third harmonic generation at terahertz frequency range.

  20. Enhanced second harmonic generation from coupled asymmetric plasmonic metal nanostructures

    NASA Astrophysics Data System (ADS)

    Yildiz, Bilge Can; Emre Tasgin, Mehmet; Kurtulus Abak, Musa; Coskun, Sahin; Emrah Unalan, Husnu; Bek, Alpan

    2015-12-01

    We experimentally demonstrate that two coupled metal nanostructures (MNSs), a silver nanowire and bipyramid, can produce ∼30 times enhanced second harmonic generation compared to the particles alone. We develop a simple theoretical model, presenting the path interference effects in the nonlinear response of coupled MNSs. We show that the reason for such an enhancement can be the occurrence of a Fano resonance due to the coupling of the converter MNS to the long-lived mode of the attached MNS.

  1. Second-harmonic generation in KNbO3 crystals

    NASA Astrophysics Data System (ADS)

    Lu, Yutian; Zhao, Quingchun; Li, Yongchun; He, Huijuan; Zou, Qun; Lu, Zheng; Zhaohua, Geng

    1993-04-01

    Efficient second-harmonic generation from a pulsed parametric laser to 427 to 470 nm has been obtained in a KNbO3 crystal only 1.5 mm in length by angular tuning at room temperature. The energy conversion efficiency is over 40%. Single pulse blue light output reaches 60 kW in peak power. The angular dependence of a phase matching wavelength, the relation between conversion efficiency and fundamental intensity, and acceptable angular phase mismatch are studied and discussed.

  2. Role of Many-Electron Dynamics in High Harmonic Generation

    SciTech Connect

    Gordon, Ariel; Kaertner, Franz X.; Rohringer, Nina; Santra, Robin

    2006-06-09

    High harmonic generation (HHG) in many-electron atoms is studied theoretically. The breakdown of the frozen-core single active electron approximation is demonstrated, as it predicts roughly the same radiation amplitude in all noble gases. This is in contradiction with experiments, where heavier noble gases are known to emit much stronger HHG radiation than lighter ones. This experimental behavior of the noble gases can be qualitatively reproduced when many-electron dynamics, within a simple approximation, is taken into account.

  3. Second-harmonic generation with magnetic-field controllability.

    PubMed

    Ju, Sheng; Cai, Tian-Yi; Wei, Chi-I; Guo, Guang-Yu

    2009-12-15

    Based on density functional theory with the generalized gradient approximation plus on-site Coulomb repulsion method, we study the magnetic-ordering dependence of second-harmonic generation (SHG) in a polar magnet BiCoO(3). The large second-order optical susceptibility, which can reach 3.7x10(-7) esu, exhibits a strong magnetic-ordering dependence, giving rise to magnetic-field controllable SHG response in polar magnets. PMID:20016638

  4. High gain amplifiers: Power oscillations and harmonic generation

    SciTech Connect

    Dattoli, G.; Ottaviani, P. L.; Pagnutti, S.

    2007-08-01

    We discuss the power oscillations in saturated high gain free electron laser amplifiers and show that the relevant period can be written in terms of the gain length. We use simple arguments following from the solution of the pendulum equation in terms of Jacobi elliptic functions. Nontrivial effects due to nonlinear harmonic generation and inhomogeneous broadening are discussed too, as well as the saturated dynamics of short pulses.

  5. Effect of localized microstructural evolution on higher harmonic generation of guided wave modes

    NASA Astrophysics Data System (ADS)

    Choi, Gloria; Liu, Yang; Yao, Xiaochu; Lissenden, Cliff J.

    2015-03-01

    Higher harmonic generation of ultrasonic waves has the potential to be used to detect precursors to macroscale damage of phenomenon like fatigue due to microstructural evolution contributing to nonlinear material behavior. Aluminum plates having various plastic zone sizes were plastically deformed to different levels. The fundamental shear horizontal mode was then generated in the plate samples via a magnetostrictive transducer. After propagating through the plastic zone the primary wave mode (SH0) and its third harmonic (sh0) were received by a second transducer. Results of a parallel numerical study using the S1-s2 Lamb mode pair, where sensitivity to changes in third order elastic constants were investigated, are described within the context of the experimental results. Specimens used within both studies are geometrically similar and have double edge notches for dog bone samples that introduce localized plastic deformation. Through both studies, the size of the plastic zone with respect to the propagation distance and damage intensity influence the higher harmonics.

  6. Second-harmonic generation of electrically poled borophosphate glasses: Effects of introducing niobium or sodium oxides

    SciTech Connect

    Nazabal, V.; Fargin, E.; Videau, J.J.

    1997-11-01

    Second-harmonic generation in poled glasses opens new frontiers in optical material research. Within this context new boro-phosphate glasses of the Ca(PO{sub 3})2-CaB{sub 4}O{sub 7}-Na{sub 2}B{sub 4}O{sub 7}-Nb{sub 2}O{sub 5} system were synthesized and their second-barmonic generation was evaluated after poling treatment. The enhancement of the second-harmonic signal with niobium oxide content is related to the presence of distorted NbO{sub 6} octahedra in the former of the glasses and to the increase in third-order susceptibility. The intensity of the measured second-harmonic signal is not dependent on the amount of sodium (100-1000 ppm) introduced into the glass.

  7. Optical Third Harmonic Generation from Isotropic Multilayer Media.

    NASA Astrophysics Data System (ADS)

    Kaatz, Philip Gerald

    Optical third harmonic generation, THG, has been used to characterize the nonlinear optical response in several types of isotropic multilayer media at fundamental wavelengths of 1064, 1542, and 1907 nm. The boundary conditions and the interaction of the optical waves produced by intense electromagnetic fields are presented and solved for the case of an isotropic slab, a polymeric film deposited onto an optical flat, and an optical glass cuvette filled with an organic liquid. The third harmonic from fused silica and BK7 optical glasses has been measured on optically flat samples of these glasses. The relative nonlinear susceptibility, chi^{(3)} , of BK7 optical glass to fused silica as measured by the intensity of the THG interference pattern and known refractive index data for these glasses varies from 1.28 at 1907 nm to 1.33 at 1542 nm and 1.42 at 1064 nm. The nonlinear wave interactions in bilayer media were analyzed and characterized for two polymeric materials deposited by spin casting from solutions onto fused silica optical flats. Poly(methylmethacrylate), PMMA films were used for the THG measurement. Refractive indices were measured by quasiwaveguiding onto PMMA films deposited onto heavy flint glass prisms for the visible wavelengths and by UV-VIS-NIR spectroscopy in the infrared. Poly(di-n-hexylsilylene) films of thicknesses ranging from.37 to 1.44 mu were also characterized by the preceding methods. These films exhibit a reversible thermochromism at 42^circ C, where the wavelength at the absorption maximum increases by ~60 nm to 374 nm below the thermochromic transition temperature. The third order nonlinear susceptibility, chi^{(3) }, relative to fused silica ranges from ~11 at 50^circC to ~55 below the thermochromic transition at 23^circC. An empirical relationship for chi^{(3) } as a function of the wavelength at maximum absorption was proposed and applied to polymeric media. The nonlinear optical response of several organic liquids was characterized

  8. Surface lattice resonances in second-harmonic generation from metasurfaces.

    PubMed

    Czaplicki, Robert; Kiviniemi, Antti; Laukkanen, Janne; Lehtolahti, Joonas; Kuittinen, Markku; Kauranen, Martti

    2016-06-15

    We investigate the role of surface-lattice resonances (SLRs) in second-harmonic generation (SHG) from arrays of metal nanoparticles. The SLRs affect the generated signal when the sample is rotated away from normal incidence. The adjustment of the incident angle tunes the SLRs to the fundamental wavelength for SHG and improves the quality of the resonance for better resonance enhancement of SHG. Compared to normal incidence, an enhancement by a factor of 10 is observed. However, at certain incident angles, the enhancement is interrupted by diffraction anomalies, which redirect light into the substrate, increasing radiation damping and compromising the quality of the resonance. PMID:27304263

  9. Seventh Harmonic Co-Generation by Cyclotron Resonance Acceleration

    NASA Astrophysics Data System (ADS)

    Wang, Changbiao; Hirshfield, J. L.; Ganguly, Achintya K.

    1997-05-01

    The TE_72 mode in cylindrical waveguide has group velocity nearly equal to that of the TE_11 mode if the operating frequency of TE_72 is seven times of that of TE_11.(C. Wang, J. L. Hirshfield, and A. K. Ganguly, Phys. Rev. Lett. 77), 3819 (1996). This allows coherent radiation to be generated at the seventh harmonic while the TE_11 mode interacts with an electron beam via cyclotron autoresonance.(C. Wang and J. L. Hirshfield, Phys. Rev. E 51), 2456 (1995); M. A. LaPointe, R. B. Yoder, C. Wang, A. K. Ganguly, and J. L. Hirshfield, Phys. Rev. Lett. 76, 2718 (1996). For a 300 kV, 30 A warm beam pumped by 20 MW rf power at 2.856 GHz, simulations indicate that careful choice of the magnetic field profile and suppression of TE_11 mode after it is completely depleted can increase the seventh harmonic output up to 10 MW at 20 GHz. It is furthermore shown that injection can also benefit co-generation, both increasing harmonic output up to 16 MW and improving spent beam quality, which is helpful to beam energy recovery for efficiency enhancement.

  10. High harmonic generation from impulsively aligned SO2

    NASA Astrophysics Data System (ADS)

    Devin, Julien; Wang, Song; Kaldun, Andreas; Bucksbaum, Phil

    2016-05-01

    Previous work in high harmonics generation (HHG) in aligned molecular gases has mainly focused on rotational dynamics in order to determine the contributions of different orbitals to the ionization step. In our experiment, we focus on the shorter timescale of vibrational dynamics. We generate high harmonics from impulsively aligned SO2 molecules in a gas jet and record the emitted attosecond pulse trains in a home-built high resolution vacuum ultra violet (VUV) spectrometer. Using the high temporal resolution of our setup, we are able to map out the effects of vibrational wavepackets with a sub-femtosecond resolution. The target molecule, SO2 gas, is impulsively aligned by a near-infrared laser pulse and has accessible vibrations on the timescale of the short laser pulse used. We present first experimental results for the response to this excitation in high-harmonics. We observe both fast oscillations in the time domain as well as shifts of the VUV photon energy outside of the pulse overlaps. Research supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Chemical Sciences, Geosciences, and Biosciences Division and by the National Science Foundation Graduate Research Fellowship.

  11. Higher harmonics generation in relativistic electron beam with virtual cathode

    SciTech Connect

    Kurkin, S. A. Badarin, A. A.; Koronovskii, A. A.; Hramov, A. E.

    2014-09-15

    The study of the microwave generation regimes with intense higher harmonics taking place in a high-power vircator consisting of a relativistic electron beam with a virtual cathode has been made. The characteristics of these regimes, in particular, the typical spectra and their variations with the change of the system parameters (beam current, the induction of external magnetic field) as well as physical processes occurring in the system have been analyzed by means of 3D electromagnetic simulation. It has been shown that the system under study demonstrates the tendency to the sufficient growth of the amplitudes of higher harmonics in the spectrum of current oscillations in the VC region with the increase of beam current. The obtained results allow us to consider virtual cathode oscillators as promising high power mmw-to-THz sources.

  12. Second harmonic generation of chemical oxygen-iodine laser

    NASA Astrophysics Data System (ADS)

    Miura, Noriaki; Mese, Norimichi; Yoshino, Satoru; Uchiyama, Taro

    1993-05-01

    Intracavity second harmonic generation of chemical oxygen iodine laser utilizing LiB3O5 crystal has been studied. A chemical oxygen iodine laser of which the fundamental maximum output power is 3 W in TEM00 mode with the Cl2 flow rate of 300 mmol/min is used. Obtained total second harmonic power is a maximum of about 6 W. Therefore, we could estimate that the effective extraction efficiency is 200%. It is thought that the latter is above 100% due to the condition that the output coupling for the fundamental beam is not optimum. And applying the result of a fundamental laser power measurement, the internal conversion efficiency is estimated at 0.29%.

  13. Semiclassical-wave-function perspective on high-harmonic generation

    NASA Astrophysics Data System (ADS)

    Mauger, François; Abanador, Paul M.; Lopata, Kenneth; Schafer, Kenneth J.; Gaarde, Mette B.

    2016-04-01

    We introduce a semiclassical-wave-function (SCWF) model for strong-field physics and attosecond science. When applied to high-harmonic generation (HHG), this formalism allows one to show that the natural time-domain separation of the contribution of ionization, propagation, and recollisions to the HHG process leads to a frequency-domain factorization of the harmonic yield into these same contributions, for any choice of atomic or molecular potential. We first derive the factorization from the natural expression of the dipole signal in the temporal domain by using a reference system, as in the quantitative rescattering (QRS) formalism [J. Phys. B 43, 122001 (2010), 10.1088/0953-4075/43/12/122001]. Alternatively, we show how the trajectory component of the SCWF can be used to express the factorization, which also allows one to attribute individual contributions to the spectrum to the underlying trajectories.

  14. Higher harmonics generation in relativistic electron beam with virtual cathode

    NASA Astrophysics Data System (ADS)

    Kurkin, S. A.; Badarin, A. A.; Koronovskii, A. A.; Hramov, A. E.

    2014-09-01

    The study of the microwave generation regimes with intense higher harmonics taking place in a high-power vircator consisting of a relativistic electron beam with a virtual cathode has been made. The characteristics of these regimes, in particular, the typical spectra and their variations with the change of the system parameters (beam current, the induction of external magnetic field) as well as physical processes occurring in the system have been analyzed by means of 3D electromagnetic simulation. It has been shown that the system under study demonstrates the tendency to the sufficient growth of the amplitudes of higher harmonics in the spectrum of current oscillations in the VC region with the increase of beam current. The obtained results allow us to consider virtual cathode oscillators as promising high power mmw-to-THz sources.

  15. Emission times in high-order harmonic generation

    SciTech Connect

    Chirila, C. C.; Dreissigacker, I.; Lein, M.; Zwan, E. V. van der

    2010-03-15

    We calculate the emission times of the radiation in high-order harmonic generation using the Gabor transform of numerical data obtained from solving the time-dependent Schroedinger equation in one, two, and three dimensions. Both atomic and molecular systems, including nuclear motion, are investigated. Lewenstein model calculations are used to gauge the performance of the Gabor method. The resulting emission times are compared against the classical simple man's model as well as against the more accurate quantum orbit model based on complex trajectories. The influence of the range of the binding potential (long or short) on the level of agreement is assessed. Our analysis reveals that the short-trajectory harmonics are emitted slightly earlier than predicted by the quantum orbit model. This partially explains recent experimental observations for atoms and molecules. Furthermore, we observe a distinct signature of two-center interference in the emission times for H{sub 2} and D{sub 2}.

  16. High-order harmonic generation in carbon-nanotube-containing plasma plumes

    SciTech Connect

    Ganeev, R. A.; Naik, P. A.; Singhal, H.; Chakera, J. A.; Kumar, M.; Joshi, M. P.; Srivastava, A. K.; Gupta, P. D.

    2011-01-15

    High-order harmonic generation (HHG) in carbon-nanotube (CNT)-containing plasma plumes has been demonstrated. Various targets were ablated to produce the plasma plumes containing nanotubes for the HHG in these media. Harmonics up to the 29th order were generated. Odd and even harmonics were generated using a two-color pump. The integrity of CNTs within the plasma plume, indicating nanotubes as the source of high-order harmonics, was confirmed by structural studies of plasma debris.

  17. Inorganic materis for anomalous-dispersion phase-matched second harmonic generation: Rubidium titanyl arsenate isomorphs, Rb[Ti{sub 1-2x}Ln{sub x}Nb{sub x}]OAsO{sub 4}

    SciTech Connect

    Anderson, M.T.; Phillips, M.L.F.; Stucky, G.D.

    1993-12-31

    We report the synthesis and optical properties of Rb[Ti{sub 1-2x}Ln{sub x}Nb{sub x}]OAsO{sub 4}. The solid solubility of lanthanide ions in the materials decreases exponentially as the size of the lanthanide ion increases. The materials exhibit absorption spectra characteristic of the particular lanthanide ion in the structure. The spectral regions between absorption peaks are transparent and will allow the transmission of fundamental and second-harmonic radiation. The charge transfer band is red-shifted 0 to 27 nm relative to RbTiOAsO{sub 4} (midpoint 331 nm). Second-harmonic intensities measured at 532 nm decrease exponentially as lanthanide ion concentration increases.

  18. Optical bistability and second-harmonic generation in thin film coupled cavity photonic crystal structures

    NASA Astrophysics Data System (ADS)

    Diao, Liyong

    This thesis deals with design, fabrication and modeling of bistable and multi-stable switching dynamics and second-harmonic generation in two groups of thin film coupled cavity photonic crystal structures. The first component studies optical bistability and multistability in such structures. Optical bistability and multistability are modelled by a nonlinear transfer matrix method. The second component is focused on the modelling and experimental measurement of second-harmonic generation in such structures. It is found that coupled cavity structures can reduce the threshold and index change for bistable operation, but single cavity structures can do the same. However, there is a clear advantage in using coupled cavity structures for multistability in that the threshold for multistability can be reduced. Second-harmonic generation is enhanced by field localization due to the resonant effect at the fundamental wavelength in single and coupled cavity structures by simulated and measured results. The work in this thesis makes three significant contributions. First, in the successful fabrication of thin film coupled cavity structures, the simulated linear transmissions of such structures match those of the fabricated structures almost exactly. Second, the newly defined figure of merit at the maximum transmission point on the bistable curve can be used to compare the material damage tolerance to any other Kerr effect nonlinear gate. Third, the simulated second-harmonic generation agrees excellently with experimental results. More generally optical thin film fabrication has commercial applications in many industry sections, such as electronics, opto-electronics, optical coating, solar cell and MEMS.

  19. Echo-Enabled Harmonic Generation for Seeded FELs

    SciTech Connect

    Stupakov, G.; /SLAC

    2011-05-19

    In the x-ray wavelengths, the two leading FEL concepts are the self-amplified spontaneous emission (SASE) configuration and the high-gain harmonic generation (HGHG) scheme. While the radiation from a SASE FEL is coherent transversely, it typically has rather limited temporal coherence. Alternatively, the HGHG scheme allows generation of fully coherent radiation by up-converting the frequency of a high-power seed laser. However, due to the relatively low up-frequency conversion efficiency, multiple stages of HGHG FEL are needed in order to generate x-rays from a UV laser. The up-frequency conversion efficiency can be greatly improved with the recently proposed echo-enabled harmonic generation (EEHG) technique. In this work we will present the concept of EEHG, and address some practically important issues that affect the performance of the seeding. We show how the EEHG can be incorporated in the FEL scheme and what is the expected performance of the EEHG seeded FEL. We will then briefly describe the first proof-of-principle EEHG experiment carried out at the Next Linear Collider Test Accelerator (NLCTA) at SLAC. We will also discuss latest advances in the echo-scheme approach, and refer to subsequent modifications of the original concept.

  20. High harmonic generation from Bloch electron in Solids

    NASA Astrophysics Data System (ADS)

    Wu, Mengxi; Ghimire, Shambhu; Reis, David; Schafer, Kenneth; Gaarde, Mette

    2015-05-01

    We study the generation of high harmonic radiation by Bloch electrons in a model solid driven by a strong mid-infrared laser field. We solve the single-electron time-dependent Schrödinger equation (TDSE) using a velocity-gauge method [New J. Phys. 15, 013006 (2013)]. The resulting harmonic spectrum exhibits a primary plateau due to the coupling of the valence band to the first conduction band, with a cutoff energy that scales linearly with field strength and laser wavelength. We also find a weaker second plateau due to coupling to higher-lying conduction bands, with a cutoff that is also approximately linear in the field strength. To facilitate the analysis of the time-frequency characteristics of the emitted harmonics, we also solve the TDSE in the Houston states [Phys. Rev. B 33, 5494 (1986)], which allows us to separate inter- and intra-band contributions to the current. We find that the inter- and intra-band contributions display very different time-frequency characteristics. We show that solutions in these two bases are equivalent under an unitary transformation but that, unlike the velocity gauge method, the Houston state treatment is numerically unstable when more than a few low lying energy bands are used.

  1. Vacuum high-harmonic generation and electromagnetic shock

    NASA Astrophysics Data System (ADS)

    Böhl, P.; King, B.; Ruhl, H.

    2016-04-01

    > When one takes into account the presence of virtual charged states in the quantum vacuum, a nonlinear self-interaction can arise in the propagation of electromagnetic fields. This self-interaction is often referred to as `real photon-photon scattering'. When the centre-of-mass energy of colliding photons is much lower than the rest energy of an electron-positron pair, this quantum effect can be included in the classical field equations of motion as a vacuum current and charge density using the Heisenberg-Euler Lagrangian. Using analytical and numerical methods for subcritical fields, the intrinsic solution to Maxwell's equations has been found for counterpropagating probe and pump plane waves in the presence of vacuum four- and six-wave mixing. In the corresponding all-order solution for the scattered probe, a route to vacuum high-harmonic generation is identified in which a long phase length can compensate for the weakness of interacting fields. The resulting shocks in the probe carrier wave and envelope are studied for different parameter regimes and polarisation set-ups. In this special issue, we study two additional set-ups: that of a slowly varying single-cycle background to highlight the effect of an oscillating background on the probe harmonic spectrum, and that of a few-cycle probe to highlight the smoothing of the harmonic peaks produced by a wider spectrum of probe photons. We also correct sign errors in an earlier publication.

  2. STARS A Two Stage High Gain Harmonic Generation FEL Demonstrator

    SciTech Connect

    M. Abo-Bakr; W. Anders; J. Bahrdt; P. Budz; K.B. Buerkmann-Gehrlein; O. Dressler; H.A. Duerr; V. Duerr; W. Eberhardt; S. Eisebitt; J. Feikes; R. Follath; A. Gaupp; R. Goergen; K. Goldammer; S.C. Hessler; K. Holldack; E. Jaeschke; Thorsten Kamps; S. Klauke; J. Knobloch; O. Kugeler; B.C. Kuske; P. Kuske; A. Meseck; R. Mitzner; R. Mueller; M. Neeb; A. Neumann; K. Ott; D. Pfluckhahn; T. Quast; M. Scheer; Th. Schroeter; M. Schuster; F. Senf; G. Wuestefeld; D. Kramer; Frank Marhauser

    2007-08-01

    BESSY is proposing a demonstration facility, called STARS, for a two-stage high-gain harmonic generation free electron laser (HGHG FEL). STARS is planned for lasing in the wavelength range 40 to 70 nm, requiring a beam energy of 325 MeV. The facility consists of a normal conducting gun, three superconducting TESLA-type acceleration modules modified for CW operation, a single stage bunch compressor and finally a two-stage HGHG cascaded FEL. This paper describes the faciliy layout and the rationale behind the operation parameters.

  3. Second harmonic generation from multilayers of oriented metal bisphosphonates

    SciTech Connect

    Neff, G.A.; Mahon, T.M.; Abshere, T.A.; Page, C.J.

    1996-12-31

    Second order nonlinear optical properties (NLO) require the presence of a polarizable moiety situated in an anharmonic potential. The approach to incorporating such properties into self-assembled multilayers involves use of asymmetric {alpha},{omega} bisphosphonates which meet this requirement by virtue of their chemical structure and binding properties. The authors have developed and optimized protection and deprotection schemes to allow for oriented layering of these molecules. Characterization by optical ellipsometry and grazing angle X-ray diffraction provides insight on average layer thicknesses and bulk film densities. Second harmonic generation (SHG) intensity from the bulk film is measured to verify NLO activity.

  4. High Harmonic Generation from Multiple Orbitals in N2

    SciTech Connect

    McFarland, B.; Farrell, Joseph P.; Bucksbaum, Philip H.; Guehr, Markus; /SLAC, Pulse /Stanford U., Phys. Dept.

    2009-03-05

    Molecular electronic states energetically below the highest occupied molecular orbital (HOMO) should contribute to laser-driven high harmonic generation (HHG), but this behavior has not been observed previously. Our measurements of the HHG spectrum of N{sub 2} molecules aligned perpendicular to the laser polarization showed a maximum at the rotational half-revival. This feature indicates the influence of electrons occupying the orbital just below the N{sub 2} HOMO, referred to as the HOMO-1. Such observations of lower-lying orbitals are essential to understanding subfemtosecond/subangstrom electronic motion in laser-excited molecules.

  5. Quantitative Modeling of Single Atom High Harmonic Generation

    SciTech Connect

    Gordon, Ariel; Kaertner, Franz X.

    2005-11-25

    It is shown by comparison with numerical solutions of the Schroedinger equation that the three step model (TSM) of high harmonic generation (HHG) can be improved to give a quantitatively reliable description of the process. Excellent agreement is demonstrated for the H atom and the H{sub 2}{sup +} molecular ion. It is shown that the standard TSM heavily distorts the HHG spectra, especially of H{sub 2}{sup +}, and an explanation is presented for this behavior. Key to the improvement is the use of the Ehrenfest theorem in the TSM.

  6. Stokes vector formalism based second harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Qiu, Jianjun; Mazumder, Nirmal; Tsai, Han-Ruei; Hu, Chih-Wei; Kao, Fu-Jen

    2012-02-01

    In this study, we have developed a four-channel Stokes vector formalism based second harmonic generation (SHG) microscopy to map and analyze SHG signal. A four-channel Stokesmeter setup is calibrated and integrated into a laser scanning microscope to measure and characterize the SH's corresponding Stokes parameters. We are demonstrating the use of SH and its Stokes parameters to visualize the birefringence and crystalline orientation of KDP and collagen. We believe the developed method can reveal unprecedented information for biomedical and biomaterial studies.

  7. Second harmonic generation microscopy reveals hidden polar organization in fluoride doped MIL-53(Fe).

    PubMed

    Markey, Karen; Putzeys, Tristan; Horcajada, Patricia; Devic, Thomas; Guillou, Nathalie; Wübbenhorst, Michael; Cleuvenbergen, Stijn Van; Verbiest, Thierry; De Vos, Dirk E; van der Veen, Monique A

    2016-03-01

    Polar metal-organic frameworks have potential applications as functional non-linear optical, piezoelectric, pyroelectric and ferroelectric materials. Using second harmonic generation microscopy we found that fluoride doping of the microporous iron(iii) terephthalate MOF MIL-53(Fe) induces a polar organization in its structure, which was not previously detected with XRD. The polar order is only observed when both fluoride and guest molecules are present, and may be related to a complex interplay between the adsorbates and the framework, leading to a modification of the positioning of fluoride in the inorganic Fe-chains. Combined polarized second harmonic generation microscopy and scanning pyroelectric microscopy show that the polar axis is unidirectional and of the same sense over the whole crystal, extending up to 100 micrometers. This finding shows how MOF materials can be endowed with useful properties by doping MOFs with fluoride. PMID:26812223

  8. Polarization gating of high harmonic generation in the water window

    NASA Astrophysics Data System (ADS)

    Li, Jie; Ren, Xiaoming; Yin, Yanchun; Cheng, Yan; Cunningham, Eric; Wu, Yi; Chang, Zenghu

    2016-06-01

    We implement the polarization gating (PG) technique with a two-cycle, 1.7 μm driving field to generate an attosecond supercontinuum extending to the water window spectral region. The ellipticity dependence of the high harmonic yield over a photon energy range much broader than previous work is measured and compared with a semi-classical model. When PG is applied, the carrier-envelope phase (CEP) is swept to study its influence on the continuum generation. PG with one-cycle (5.7 fs) and two-cycle (11.3 fs) delay are tested, and both give continuous spectra spanning from 50 to 450 eV under certain CEP values, strongly indicating the generation of isolated attosecond pulses in the water window region.

  9. Designs and numerical calculations for echo-enabled harmonic generation at very high harmonics

    NASA Astrophysics Data System (ADS)

    Penn, G.; Reinsch, M.

    2011-09-01

    The echo-enabled harmonic generation (EEHG) scheme for driving an FEL using two seeded energy modulations at much longer wavelengths than the output wavelength is a promising concept for future seeded FELs. There are many competing requirements in the design of an EEHG beamline which need careful optimization. Furthermore, revised simulation tools and methods are necessary because of both the high harmonic numbers simulated and the complicated nature of the phase space manipulations which are intrinsic to the scheme. This paper explores the constraints on performance and the required tolerances for reaching wavelengths well below 1/100th of that of the seed lasers, and describes some of the methodology for designing such a beamline. Numerical tools, developed both for the GENESIS and GINGER FEL codes, are presented and used here for more accurate study of the scheme beyond a time-averaged model. In particular, the impact of the local structure in peak current and bunching, which is an inherent part of the EEHG scheme, is evaluated.

  10. Pencil lead plasma for generating multimicrojoule high-order harmonics with a broad spectrum

    SciTech Connect

    Pertot, Y.; Elouga Bom, L. B.; Ozaki, T.; Bhardwaj, V. R.

    2011-03-07

    Using the plasma harmonic method, we show the generation of efficient and intense high-order harmonics from plasma of pencil lead. We demonstrate multimicrojoule energy in each harmonic order for the 11th to the 17th order of a Ti:sapphire laser. By analyzing the target morphology and the plasma composition, we conclude that these intense harmonics are generated from nanoparticles of graphitic carbon.

  11. Bright high-order harmonic generation with controllable polarization from a relativistic plasma mirror.

    PubMed

    Chen, Zi-Yu; Pukhov, Alexander

    2016-01-01

    Ultrafast extreme ultraviolet (XUV) sources with a controllable polarization state are powerful tools for investigating the structural and electronic as well as the magnetic properties of materials. However, such light sources are still limited to only a few free-electron laser facilities and, very recently, to high-order harmonic generation from noble gases. Here we propose and numerically demonstrate a laser-plasma scheme to generate bright XUV pulses with fully controlled polarization. In this scheme, an elliptically polarized laser pulse is obliquely incident on a plasma surface, and the reflected radiation contains pulse trains and isolated circularly or highly elliptically polarized attosecond XUV pulses. The harmonic polarization state is fully controlled by the laser-plasma parameters. The mechanism can be explained within the relativistically oscillating mirror model. This scheme opens a practical and promising route to generate bright attosecond XUV pulses with desirable ellipticities in a straightforward and efficient way for a number of applications. PMID:27531047

  12. Bright high-order harmonic generation with controllable polarization from a relativistic plasma mirror

    PubMed Central

    Chen, Zi-Yu; Pukhov, Alexander

    2016-01-01

    Ultrafast extreme ultraviolet (XUV) sources with a controllable polarization state are powerful tools for investigating the structural and electronic as well as the magnetic properties of materials. However, such light sources are still limited to only a few free-electron laser facilities and, very recently, to high-order harmonic generation from noble gases. Here we propose and numerically demonstrate a laser–plasma scheme to generate bright XUV pulses with fully controlled polarization. In this scheme, an elliptically polarized laser pulse is obliquely incident on a plasma surface, and the reflected radiation contains pulse trains and isolated circularly or highly elliptically polarized attosecond XUV pulses. The harmonic polarization state is fully controlled by the laser–plasma parameters. The mechanism can be explained within the relativistically oscillating mirror model. This scheme opens a practical and promising route to generate bright attosecond XUV pulses with desirable ellipticities in a straightforward and efficient way for a number of applications. PMID:27531047

  13. Intense sub-2 optical cycle laser pulses at 1.8 micron for high harmonic generation

    NASA Astrophysics Data System (ADS)

    Legare, Francois; Schmidt, Bruno E.; Béejot, Pierre; Giguère, Mathieu; Shiner, Andrew D.; Trallero-Herrero, Carlos; Bisson, Éric; Kasparian, Jerome; Wolf, Jean-Pierre; Villeneuve, David M.; Kieffer, Jean-Claude; Corkum, Paul B.

    2010-03-01

    Shortening of attosecond pulse duration utilizing high harmonic generation (HHG) requires access to few cycle pulses in the infrared spectral range because the cut-off shifts towards higher photon energies proportional to the square of the driving field wavelength. Furthermore, the ability of performing time-resolved molecular orbital tomography of polyatomic molecules will benefit from longer wavelengths compared to 800 nm because of their low ionization potential. A simple scheme for generating 0.4 mJ 11.5 fs pulses at 1.8 μm is presented. Optical parametric amplified pulses were spectrally broadened in a hollow-core fiber and subsequently compressed by utilizing linear propagation through bulk material. The physical origin of the pulse compression scheme will be confirmed with numerical simulations of nonlinear propagation in the hollow-core fiber. Finally, high harmonic generation of noble gas atoms will be reported.

  14. Whispering-gallery-mode analysis of phase-matched doubly resonant second-harmonic generation

    NASA Astrophysics Data System (ADS)

    Dumeige, Yannick; Féron, Patrice

    2006-12-01

    We propose a coupled modes analysis of second-harmonic generation in microdisk resonators. We demonstrate that whispering gallery modes can be used to obtain a combination of modal and geometrical quasi-phase-matching (without domain inversion) to obtain efficient conversion in isotropic and nonferroelectric materials such as III-V semiconductor compounds. Finally we use an analytical model to describe the coupling between a bus waveguide and the nonlinear microdisk to achieve an optimization scheme for practical configuration.

  15. Background-free electric field-induced second harmonic generation with interdigitated combs of electrodes.

    PubMed

    Jašinskas, Vidmantas; Gedvilas, Mindaugas; Račiukaitis, Gediminas; Gulbinas, Vidmantas

    2016-06-15

    The electric field-induced second harmonic (EFISH) generation is a powerful tool for the investigation of optical nonlinearities, material polarization, internal electric fields, and other properties of photonic materials and devices. A conventional generation of the second harmonics (SH) in materials with the disturbed centrosymmetry causes a field-independent background to EFISH and limits its applications. Here we suggest and analyze the application of the interdigitated combs of electrodes for EFISH generation in thin films. Interdigitated electrodes form an optical transmission amplitude diffraction grating. Phase matching of the EFISH radiation creates unusual diffraction fringes with the zero intensity along the zeroth order direction and with the diffraction angles different from diffraction angles of incident fundamental laser radiation and its second harmonics. It enables a simple geometrical separation of the EFISH signal from a conventional SH background, simplifies the sample preparation, and provides additional experimental possibilities. We demonstrate applicability of the suggested technique for characterization of submicrometer thickness organic films of transparent and resonantly interacting polymers and of their mixtures. PMID:27304282

  16. Singularity-driven second- and third-harmonic generation at {epsilon}-near-zero crossing points

    SciTech Connect

    Vincenti, M. A.; Ceglia, D. de; Ciattoni, A.; Scalora, M.

    2011-12-15

    We show an alternative path to efficient second- and third-harmonic generation in proximity of the zero crossing points of the dielectric permittivity in conjunction with low absorption. Under these circumstances, any material, either natural or artificial, will show similar degrees of field enhancement followed by strong harmonic generation, without resorting to any resonant mechanism. The results presented in this paper provide a general demonstration of the potential that the zero-crossing-point condition holds for nonlinear optical phenomena. We investigate a generic Lorentz medium and demonstrate that a singularity-driven enhancement of the electric field may be achieved even in extremely thin layers of material. We also discuss the role of nonlinear surface sources in a realistic scenario where a 20-nm layer of CaF{sub 2} is excited at 21 {mu}m, where {epsilon}{approx} 0. Finally, we show similar behavior in an artificial composite material that includes absorbing dyes in the visible range, provide a general tool for the improvement of harmonic generation using the {epsilon}{approx} 0 condition, and illustrate that this singularity-driven enhancement of the field lowers the thresholds for a plethora of nonlinear optical phenomena.

  17. High-harmonic generation in aligned water molecules

    NASA Astrophysics Data System (ADS)

    Wang, Song; Devin, Julien; Hoffmann, Matthias; Cryan, James; Kaldun, Andreas; Bucksbaum, Philip

    2016-05-01

    In recent years, the use of high harmonic generation (HHG) in aligned molecular vapors has become a powerful tool to study ultrafast dynamics of electronic and nuclear wave packets. In our new experimental setup, we are able to orient H2 O and D2 O molecules using a single cycle terahertz (THz) pulse. Aligning water is especially interesting as the highest occupied molecular orbital (HOMO) of water contains a node in the xz plane of the molecular frame, allowing us to perform HHG from second highest occupied molecular orbital (HOMO-1) only, by setting the polarization of the fundamental laser along the z-axis of the aligned water molecules. We are particularly interested in the HOMO-1 state, as there is fast motion of the H-O-H angle leading to sub-wavelength dynamics. On this poster we present our all-optical alignment setup where HHG and single-cycle THz generation take place in high-vacuum, where measurements with arbitrary polarization angles between the two are possible. In addition, we discuss the effects of the molecular orientation on HHG, including symmetry breaking that could produce even harmonics and isotope effects between H2 O and D2 O due to different vibrational energies. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.

  18. Third Harmonic Generation from Aligned Single-Wall Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Morris, Darius T., Jr.

    Optical properties of single-wall carbon nanotubes (SWCNTs) have been extensively studied during the last decade, and much basic knowledge has been accumulated on how light emission, scattering, and absorption occur in the realm of linear optics. However, their nonlinear optical properties remain largely unexplored. Here, we have observed strong third harmonic generation from highly aligned SWCNTs with intense mid-infrared radiation. Through power dependent experiments, we have determined the absolute value of the third-order nonlinear optical susceptibility, chi(3), of our SWCNT film to be 6.92 x 10--12 esu, which is three orders of magnitude larger than that of the fused silica reference sample we used. Furthermore, through polarization-dependent third harmonic generation experiments, all the nonzero tensor elements of chi(3) have also been extracted. The contribution of the weaker tensor elements to the overall chi (3) signal has been calculated to be approximately 1/6 of that of the dominant c3z zzz component. These results open up new possibilities for application of carbon nanotubes in optoelectronics.

  19. Second Harmonic Generation Mediated by Aligned Water in Starch Granules.

    PubMed

    Cisek, Richard; Tokarz, Danielle; Krouglov, Serguei; Steup, Martin; Emes, Michael J; Tetlow, Ian J; Barzda, Virginijus

    2014-12-26

    The origin of second harmonic generation (SHG) in starch granules was investigated using ab initio quantum mechanical modeling and experimentally examined using polarization-in, polarization-out (PIPO) second harmonic generation microscopy. Ab initio calculations revealed that the largest contribution to the SHG signal from A- and B-type allomorphs of starch originates from the anisotropic organization of hydroxide and hydrogen bonds mediated by aligned water found in the polymers. The hypothesis was experimentally tested by imaging maize starch granules under various hydration and heat treatment conditions that alter the hydrogen bond network. The highest SHG intensity was found in fully hydrated starch granules, and heat treatment diminished the SHG intensity. The PIPO SHG imaging showed that dried starch granules have a much higher nonlinear optical susceptibility component ratio than fully hydrated granules. In contrast, deuterated starch granules showed a smaller susceptibility component ratio demonstrating that SHG is highly sensitive to the organization of the hydroxyl and hydrogen bond network. The polarization SHG imaging results of potato starch granules, representing starch allomorph B, were compared to those of maize starch granules representing allomorph A. The results showed that the amount of aligned water was higher in the maize granules. Nonlinear microscopy of starch granules provides evidence that varying hydration conditions leads to significant changes in the nonlinear susceptibility ratio as well as the SHG intensity, supporting the hypothesis from ab initio calculations that the dominant contribution to SHG is due to the ordered hydroxide and hydrogen bond network. PMID:25427055

  20. Automated cardiac sarcomere analysis from second harmonic generation images

    NASA Astrophysics Data System (ADS)

    Garcia-Canadilla, Patricia; Gonzalez-Tendero, Anna; Iruretagoyena, Igor; Crispi, Fatima; Torre, Iratxe; Amat-Roldan, Ivan; Bijnens, Bart H.; Gratacos, Eduard

    2014-05-01

    Automatic quantification of cardiac muscle properties in tissue sections might provide important information related to different types of diseases. Second harmonic generation (SHG) imaging provides a stain-free microscopy approach to image cardiac fibers that, combined with our methodology of the automated measurement of the ultrastructure of muscle fibers, computes a reliable set of quantitative image features (sarcomere length, A-band length, thick-thin interaction length, and fiber orientation). We evaluated the performance of our methodology in computer-generated muscle fibers modeling some artifacts that are present during the image acquisition. Then, we also evaluated it by comparing it to manual measurements in SHG images from cardiac tissue of fetal and adult rabbits. The results showed a good performance of our methodology at high signal-to-noise ratio of 20 dB. We conclude that our automated measurements enable reliable characterization of cardiac fiber tissues to systematically study cardiac tissue in a wide range of conditions.

  1. Beam Conditioning and Harmonic Generation in Free ElectronLasers

    SciTech Connect

    Charman, A.E.; Penn, G.; Wolski, A.; Wurtele, J.S.

    2004-07-05

    The next generation of large-scale free-electron lasers (FELs) such as Euro-XFEL and LCLS are to be devices which produce coherent X-rays using Self-Amplified Spontaneous Emission (SASE). The performance of these devices is limited by the spread in longitudinal velocities of the beam. In the case where this spread arises primarily from large transverse oscillation amplitudes, beam conditioning can significantly enhance FEL performance. Future X-ray sources may also exploit harmonic generation starting from laser-seeded modulation. Preliminary analysis of such devices is discussed, based on a novel trial-function/variational-principle approach, which shows good agreement with more lengthy numerical simulations.

  2. Time-resolved phase-sensitive second harmonic generation spectroscopy

    NASA Astrophysics Data System (ADS)

    Nowakowski, Paweł J.; Woods, David A.; Bain, Colin D.; Verlet, Jan R. R.

    2015-02-01

    A methodology based on time-resolved, phase-sensitive second harmonic generation (SHG) for probing the excited state dynamics of species at interfaces is presented. It is based on an interference measurement between the SHG from the sample and a local oscillator generated at a reference together with a lock-in measurement to remove the large constant offset from the interference. The technique is characterized by measuring the phase and excited state dynamics of the dye malachite green at the water/air interface. The key attributes of the technique are that the observed signal is directly proportional to sample concentration, in contrast to the quadratic dependence from non-phase sensitive SHG, and that the real and imaginary parts of the 2nd order non-linear susceptibility can be determined independently. We show that the method is highly sensitive and can provide high quality excited state dynamics in short data acquisition times.

  3. High-harmonic generation from Bloch electrons in solids

    NASA Astrophysics Data System (ADS)

    Wu, Mengxi; Ghimire, Shambhu; Reis, David A.; Schafer, Kenneth J.; Gaarde, Mette B.

    2015-04-01

    We study the generation of high-harmonic radiation by Bloch electrons in a model transparent solid driven by a strong midinfrared laser field. We solve the single-electron time-dependent Schrödinger equation (TDSE) using a velocity-gauge method [M. Korbman et al., New J. Phys. 15, 013006 (2013), 10.1088/1367-2630/15/1/013006] that is numerically stable as the laser intensity and number of energy bands are increased. The resulting harmonic spectrum exhibits a primary plateau due to the coupling of the valence band to the first conduction band, with a cutoff energy that scales linearly with field strength and laser wavelength. We also find a weaker second plateau due to coupling to higher-lying conduction bands, with a cutoff that is also approximately linear in the field strength. To facilitate the analysis of the time-frequency characteristics of the emitted harmonics, we also solve the TDSE in a time-dependent basis set, the Houston states [J. B. Krieger and G. J. Iafrate, Phys. Rev. B 33, 5494 (1986), 10.1103/PhysRevB.33.5494], which allows us to separate interband and intraband contributions to the time-dependent current. We find that the interband and intraband contributions display very different time-frequency characteristics. We show that solutions in these two bases are equivalent under a unitary transformation but that, unlike the velocity-gauge method, the Houston state treatment is numerically unstable when more than a few low-lying energy bands are used.

  4. Radially polarized annular beam generated through a second-harmonic-generation process.

    PubMed

    Sato, Shunichi; Kozawa, Yuichi

    2009-10-15

    A radially polarized beam with an annular intensity pattern was generated through a second-harmonic-generation process by focusing an azimuthally polarized Ti:sapphire pulsed laser beam to a c-cut beta-barium borate (BBO) crystal. The annular intensity pattern of the second-harmonic wave had a nearly sixfold symmetry as a result of the nonlinear susceptibility tensor of the BBO crystal. The width of the annulus was as narrow as less than 1/40th of its radius. PMID:19838261

  5. Mode matching in multiresonant plasmonic nanoantennas for enhanced second harmonic generation

    NASA Astrophysics Data System (ADS)

    Celebrano, Michele; Wu, Xiaofei; Baselli, Milena; Großmann, Swen; Biagioni, Paolo; Locatelli, Andrea; de Angelis, Costantino; Cerullo, Giulio; Osellame, Roberto; Hecht, Bert; Duò, Lamberto; Ciccacci, Franco; Finazzi, Marco

    2015-05-01

    Boosting nonlinear frequency conversion in extremely confined volumes remains a challenge in nano-optics research, but can enable applications in nanomedicine, photocatalysis and background-free biosensing. To obtain brighter nonlinear nanoscale sources, approaches that enhance the electromagnetic field intensity and counter the lack of phase matching in nanoplasmonic systems are often employed. However, the high degree of symmetry in the crystalline structure of plasmonic materials (metals in particular) and in nanoantenna designs strongly quenches second harmonic generation. Here, we describe doubly-resonant single-crystalline gold nanostructures with no axial symmetry displaying spatial mode overlap at both the excitation and second harmonic wavelengths. The combination of these features allows the attainment of a nonlinear coefficient for second harmonic generation of ˜5 × 10-10 W-1, enabling a second harmonic photon yield higher than 3 × 106 photons per second. Theoretical estimations point toward the use of our nonlinear plasmonic nanoantennas as efficient platforms for label-free molecular sensing.

  6. Mode matching in multiresonant plasmonic nanoantennas for enhanced second harmonic generation.

    PubMed

    Celebrano, Michele; Wu, Xiaofei; Baselli, Milena; Großmann, Swen; Biagioni, Paolo; Locatelli, Andrea; De Angelis, Costantino; Cerullo, Giulio; Osellame, Roberto; Hecht, Bert; Duò, Lamberto; Ciccacci, Franco; Finazzi, Marco

    2015-05-01

    Boosting nonlinear frequency conversion in extremely confined volumes remains a challenge in nano-optics research, but can enable applications in nanomedicine, photocatalysis and background-free biosensing. To obtain brighter nonlinear nanoscale sources, approaches that enhance the electromagnetic field intensity and counter the lack of phase matching in nanoplasmonic systems are often employed. However, the high degree of symmetry in the crystalline structure of plasmonic materials (metals in particular) and in nanoantenna designs strongly quenches second harmonic generation. Here, we describe doubly-resonant single-crystalline gold nanostructures with no axial symmetry displaying spatial mode overlap at both the excitation and second harmonic wavelengths. The combination of these features allows the attainment of a nonlinear coefficient for second harmonic generation of ∼5 × 10(-10) W(-1), enabling a second harmonic photon yield higher than 3 × 10(6) photons per second. Theoretical estimations point toward the use of our nonlinear plasmonic nanoantennas as efficient platforms for label-free molecular sensing. PMID:25895003

  7. Harmonic Generation in the Multifrequency Recirculating Planar Magnetron

    NASA Astrophysics Data System (ADS)

    Exelby, S. C.; Greening, G. B.; Jordan, N. M.; Simon, D.; Zhang, P.; Lau, Y. Y.; Gilgenbach, R. M.

    2015-11-01

    The Multifrequency Recirculating Planar Magnetron (MFRPM) is a high power microwave source adapted from the Recirculating Planar Magnetrona, currently under investigation at the University of Michigan. The device features 2 dissimilar periodic structures allowing for the generation of (L-band) 1- and (S-band) 2-GHz high power microwave pulses simultaneously. These distinct frequencies offer the potential for variable coupling for defense applications, such as counter-IED. Experiments have been performed on the RPM, driven by the Michigan Electron Long Beam Accelerator with a Ceramic insulator (MELBA-C) using a -300kV, 1-10 kA, 0.3-1.0 us pulse applied to the cathode. Using the Mode Control Cathodeb and a coax-to-waveguide extraction system, the MFRPM has demonstrated simultaneous production of 20 MW at 1 GHz and 10 MW at 2 GHz. The L-band oscillator also produced both 2- and 4-GHz oscillations when the S-band oscillator turns on. These harmonics persist after the S-band oscillator turns off. Ongoing work will attempt to isolate these harmonics to measure the power accurately and confirm these observations. Supported by the Office of Naval Research grant no. N00014-13-1-0566 and L-3 Communications.

  8. Harmonic Generation in InAs Nanowire Double Quantum Dots

    NASA Astrophysics Data System (ADS)

    Schroer, M. D.; Jung, M.; Petersson, K. D.; Petta, J. R.

    2012-02-01

    InAs nanowires provide a useful platform for investigating the physics of confined electrons subjected to strong spin-orbit coupling. Using tunable, bottom-gated double quantum dots, we demonstrate electrical driving of single spin resonance.ootnotetextS. Nadj-Perge et al., Nature 468, 1084 (2010)^,ootnotetextM.D. Schroer et al., Phys. Rev. Lett. 107, 176811 (2011) We observe a standard spin response when the applied microwave frequency equals the Larmour frequency f0. However, we also observe an anomalous signal at frequencies fn= f0/ n for integer n up to n ˜5. This is equivalent to generation of harmonics of the spin resonance field. While a f0/2 signal has observed,ootnotetextE.A. Laird et al., Phys. Rev. Lett. 99, 246601 (2007) we believe this is the first observation of higher harmonics in spin resonance. Possible mechanisms will be discussed.ootnotetextE.I. Rashba, arXiv:1110.6569 (2011) Acknowledgements: Research supported by the Sloan and Packard Foundations, the NSF, and Army Research Office.

  9. Multiple layer optical memory system using second-harmonic-generation readout

    DOEpatents

    Boyd, Gary T.; Shen, Yuen-Ron

    1989-01-01

    A novel optical read and write information storage system is described which comprises a radiation source such as a laser for writing and illumination, the radiation source being capable of radiating a preselected first frequency; a storage medium including at least one layer of material for receiving radiation from the radiation source and capable of being surface modified in response to said radiation source when operated in a writing mode and capable of generating a pattern of radiation of the second harmonic of the preselected frequency when illuminated by the radiation source at the preselected frequency corresponding to the surface modifications on the storage medium; and a detector to receive the pattern of second harmonic frequency generated.

  10. Second-harmonic generation from bimetal composites doped with metal nanoparticles

    NASA Astrophysics Data System (ADS)

    Daneshfar, Nader

    2016-05-01

    In the present paper, we study the nonlinear optical response of the bimetal composites doped with metal nanoparticles in the framework of nonlinear Mie theory combined with the Maxwell-Garnett model. We concentrate on the second-order harmonic generation from bimetal nanocomposites including silver and gold particles, since sometimes the nonlinear optical response is sensitive to the more accurate of material structure than linear optical response. We show that optical second harmonic generation is strongly sensitive to temperature as an environmental parameter, interparticle plasmon coupling between Au and Ag nanoparticles (the filling factor of inclusions), the particle size and the surrounding medium. However, this work shows good potential of bimetal composites for nonlinear optics at the nanoscale.

  11. Second- and third-harmonic generation in metal-based structures

    SciTech Connect

    Scalora, M.; Akozbek, N.; Bloemer, M. J.; Vincenti, M. A.; Ceglia, D. de; Roppo, V.; Centini, M.

    2010-10-15

    We present a theoretical approach to the study of second- and third-harmonic generation from metallic structures and nanocavities filled with a nonlinear material in the ultrashort pulse regime. We model the metal as a two-component medium, using the hydrodynamic model to describe free electrons and Lorentz oscillators to account for core electron contributions to both the linear dielectric constant and harmonic generation. The active nonlinear medium that may fill a metallic nanocavity, or be positioned between metallic layers in a stack, is also modeled using Lorentz oscillators and surface phenomena due to symmetry breaking are taken into account. We study the effects of incident TE- and TM-polarized fields and show that a simple reexamination of the basic equations reveals additional, exploitable dynamical features of nonlinear frequency conversion in plasmonic nanostructures.

  12. Resonant second harmonic generation of a Gaussian electromagnetic beam in a collisional magnetoplasma

    SciTech Connect

    Kaur, Sukhdeep; Sharma, A. K.; Salih, Hyder A.

    2009-04-15

    Second harmonic generation of a right circularly polarized Gaussian electromagnetic beam in a magnetized plasma is investigated. The beam causes Ohmic heating of electrons and subsequent redistribution of the plasma, leading to self-defocusing. The radial density gradient, in conjunction with the oscillatory electron velocity, produces density oscillation at the wave frequency. The density oscillation beats with the oscillatory velocity to produce second harmonic current density, giving rise to resonant second harmonic radiation when the wave frequency is one-third of electron cyclotron frequency. The second harmonic field has azimuthal dependence as exp(i{theta}). The self-defocusing causes a reduction in the efficiency of harmonic generation.

  13. Measuring Microtubule Polarity in Spindles with Second-Harmonic Generation

    PubMed Central

    Yu, Che-Hang; Langowitz, Noah; Wu, Hai-Yin; Farhadifar, Reza; Brugues, Jan; Yoo, Tae Yeon; Needleman, Daniel

    2014-01-01

    The spatial organization of microtubule polarity, and the interplay between microtubule polarity and protein localization, is thought to be crucial for spindle assembly, anaphase, and cytokinesis, but these phenomena remain poorly understood, in part due to the difficulty of measuring microtubule polarity in spindles. We develop and implement a method to nonperturbatively and quantitatively measure microtubule polarity throughout spindles using a combination of second-harmonic generation and two-photon fluorescence. We validate this method using computer simulations and by comparison to structural data on spindles obtained from electron tomography and laser ablation. This method should provide a powerful tool for studying spindle organization and function, and may be applicable for investigating microtubule polarity in other systems. PMID:24739157

  14. Second harmonic generation and crystal growth of new chalcone derivatives

    NASA Astrophysics Data System (ADS)

    Patil, P. S.; Dharmaprakash, S. M.; Ramakrishna, K.; Fun, Hoong-Kun; Sai Santosh Kumar, R.; Narayana Rao, D.

    2007-05-01

    We report on the synthesis, crystal structure and optical characterization of chalcone derivatives developed for second-order nonlinear optics. The investigation of a series of five chalcone derivatives with the second harmonic generation powder test according to Kurtz and Perry revealed that these chalcones show efficient second-order nonlinear activity. Among them, high-quality single crystals of 3-Br-4'-methoxychalcone (3BMC) were grown by solvent evaporation solution growth technique. Grown crystals were characterized by X-ray powder diffraction (XRD), laser damage threshold, UV-vis-NIR and refractive index measurement studies. Infrared spectroscopy, thermogravimetric analysis and differential thermal analysis measurements were performed to study the molecular vibration and thermal behavior of 3BMC crystal. Thermal analysis does not show any structural phase transition.

  15. High harmonic generation in the undulators for free electron lasers

    NASA Astrophysics Data System (ADS)

    Zhukovsky, K.

    2015-10-01

    We present the analysis of the undulator radiation (UR) with account for major sources of the spectral line broadening. For relativistic electrons we obtain the analytical expressions for the UR spectrum, the intensity and the emission line shape with account for the finite size of the beam, the emittance and the energy spread. Partial compensation of the divergency by properly imposed weak constant magnetic component is demonstrated in the analytical form. Considering the examples of radiation from single and double frequency undulators, we study high harmonic generation with account for all major sources of homogeneous and inhomogeneous broadening with account for the characteristics of the electrons beam. We apply our analysis to free electron laser (FEL) calculations and we compare the obtained results with the radiation of a FEL on the supposition of the ideal undulator.

  16. High-order harmonic generation enhanced by XUV light

    SciTech Connect

    Buth, Christian; Kohler, Markus C.; Ullrich, Joachim; Keitel, Christoph H.

    2012-03-19

    The combination of high-order harmonic generation (HHG) with resonant XUV excitation of a core electron into the transient valence vacancy that is created in the course of the HHG process is investigated theoretically. In this setup, the first electron performs a HHG three-step process, whereas the second electron Rabi flops between the core and the valence vacancy. The modified HHG spectrum due to recombination with the valence and the core is determined and analyzed for krypton on the 3d {yields} 4p resonance in the ion. We assume an 800 nm laser with an intensity of about 10{sup 14} Wcm{sup 2} and XUV radiation from the Free Electron Laser in Hamburg (FLASH) with an intensity in the range 10{sup 13}-10{sup 16} Wcm{sup 2}. Our prediction opens perspectives for nonlinear XUV physics, attosecond x rays, and HHG-based spectroscopy involving core orbitals.

  17. Polarization-modulated second harmonic generation in collagen.

    PubMed

    Stoller, Patrick; Reiser, Karen M; Celliers, Peter M; Rubenchik, Alexander M

    2002-06-01

    Collagen possesses a strong second-order nonlinear susceptibility, a nonlinear optical property characterized by second harmonic generation in the presence of intense laser beams. We present a new technique involving polarization modulation of an ultra-short pulse laser beam that can simultaneously determine collagen fiber orientation and a parameter related to the second-order nonlinear susceptibility. We demonstrate the ability to discriminate among different patterns of fibrillar orientation, as exemplified by tendon, fascia, cornea, and successive lamellar rings in an intervertebral disc. Fiber orientation can be measured as a function of depth with an axial resolution of approximately 10 microm. The parameter related to the second-order nonlinear susceptibility is sensitive to fiber disorganization, oblique incidence of the beam on the sample, and birefringence of the tissue. This parameter represents an aggregate measure of tissue optical properties that could potentially be used for optical imaging in vivo. PMID:12023255

  18. Thermal optimization of second harmonic generation at high pump powers.

    PubMed

    Sahm, Alexander; Uebernickel, Mirko; Paschke, Katrin; Erbert, Götz; Tränkle, Günther

    2011-11-01

    We measure the temperature distribution of a 3 cm long periodically poled LiNbO₃ crystal in a single-pass second harmonic generation (SHG) setup at 488 nm. By means of three resistance heaters and directly mounted Pt100 sensors the crystal is subdivided in three sections. 9.4 W infrared pump light and 1.3 W of SHG light cause a de-homogenized temperature distribution of 0.2 K between the middle and back section. A sectional offset heating is used to homogenize the temperature in those two sections and thus increasing the conversion efficiency. A 15% higher SHG output power matching the prediction of our theoretical model is achieved. PMID:22109182

  19. Interpreting Second-Harmonic Generation Images of Collagen I Fibrils

    PubMed Central

    Williams, Rebecca M.; Zipfel, Warren R.; Webb, Watt W.

    2005-01-01

    Fibrillar collagen, being highly noncentrosymmetric, possesses a tremendous nonlinear susceptibility. As a result, second-harmonic generation (SHG) microscopy of collagen produces extremely bright and robust signals, providing an invaluable tool for imaging tissue structure with submicron resolution. Here we discuss fundamental principles governing SHG phase matching with the tightly focusing optics used in microscopy. Their application to collagen imaging yields several biophysical features characteristic of native collagen structure: SHG radiates from the shell of a collagen fibril, rather than from its bulk. This SHG shell may correspond to the supporting element of the fibril. Physiologically relevant changes in solution ionic strength alter the ratio of forward-to-backward propagating SHG, implying a resulting change in the SHG shell thickness. Fibrillogenesis can be resolved in immature tissue by directly imaging backward-propagating SHG. Such findings are crucial to the design and development of forthcoming diagnostic and research tools. PMID:15533922

  20. High-order harmonic generation enhanced by XUV light

    NASA Astrophysics Data System (ADS)

    Buth, Christian; Kohler, Markus C.; Ullrich, Joachim; Keitel, Christoph H.

    2011-09-01

    The combination of high-order harmonic generation (HHG) with resonant XUV excitation of a core electron into the transient valence vacancy that is created in the course of the HHG process is investigated theoretically. In this setup, the first electron performs a HHG three-step process, whereas the second electron Rabi flops between the core and the valence vacancy. The modified HHG spectrum due to recombination with the valence and the core is determined and analyzed for krypton on the 3d→4p resonance in the ion. We assume an 800nm laser with an intensity of about 1014Wcm2 and XUV radiation from the Free Electron Laser in Hamburg (FLASH) with an intensity in the range 1013--1016Wcm2. Our prediction opens perspectives for nonlinear XUV physics, attosecond x rays, and HHG-basedspectroscopy involving core orbitals.

  1. Second Harmonic Generation in a Graphe Armchair Nanoribbon

    NASA Astrophysics Data System (ADS)

    Gumbs, Godfrey; Abranyos, Yonatan

    2013-03-01

    The second order nonlinear optical susceptibility χ (2) for second harmonic generation is calculated for the 11H transition of a graded double quantum well (DQW) structure of undoped- GaAs / Alx Ga1 - x As . These results are compared with the single quantum well (QW). Our results show that the values of χ (2) have optimal magnitudes dependent on the width, depth and separation between the QWs in a DQW structure. When the electric field increases, the dipole moment increases due to the increasing separation between the electron and hole wave functions. On the other hand, the oscillator strength of the 11H transition is reduced as a result of the decrease in the overlap of the electron and hole envelope functions. These two competing factors give rise to optimal conditions for the enhancement of the second order nonlinear susceptibility χ (2). It is demonstrated that χ (2) for the DQW structure is more enhanced than for the biased single QW.

  2. Molecular alignment allows low-order harmonic generation by circular light in a gas

    NASA Astrophysics Data System (ADS)

    Houzet, J.; Hertz, E.; Billard, F.; Lavorel, B.; Faucher, O.

    2013-08-01

    We experimentally investigate odd-order harmonic generation in molecular gases produced by circularly polarized laser fields. While forbidden in isotropic medium, this effect is allowed by symmetry breaking resulting from nonadiabatic laser-induced molecular alignment. The demonstration is provided by generating the third harmonic in CO2 molecules. Attractive properties and challenging potential applications are discussed in the context of higher-order harmonic generation.

  3. Polarization-Modulated Second Harmonic Generation Microscopy in Collagen

    SciTech Connect

    Stoller, P C

    2002-09-30

    Collagen is a key structural protein in the body; several pathological conditions lead to changes in collagen. Among imaging modalities that can be used in vivo, second harmonic generation (SHG) microscopy has a key advantage: it provides {approx}1 {micro}m resolution information about collagen structure as a function of depth. A new technique--polarization-modulated SHG--is presented: it permits simultaneous measurement of collagen orientation, of a lower bound on the magnitude of the second order nonlinear susceptibility tensor, and of the ratio of the two independent elements in this tensor. It is applied to characterizing SHG in collagen and to determining effects of biologically relevant changes in collagen structure. The magnitude of the second harmonic signal in two dimensional images varies with position even in structurally homogeneous tissue; this phenomenon is due to interference between second harmonic light generated by neighboring fibrils, which are randomly oriented parallel or anti-parallel to each other. Studies in which focal spot size was varied indicated that regions where fibrils are co-oriented are less than {approx}1.5 {micro}m in diameter. A quartz reference was used to determine the spot size as well as a lower limit (d{sub xxx} > 0.3 pm/V) for the magnitude of the second order nonlinear susceptibility. The ratio of the two independent tensor elements ranged between d{sub XYY}/d{sub XXX} = 0.60 and 0.75. SHG magnitude alone was not useful for identifying structural anomalies in collagenous tissue. Instead, changes in the polarization dependence of SHG were used to analyze biologically relevant perturbations in collagen structure. Changes in polarization dependence were observed in dehydrated samples, but not in highly crosslinked samples, despite significant alterations in packing structure. Complete thermal denaturation and collagenase digestion produced samples with no detectable SHG signal. Collagen orientation was measured in thin

  4. Enhanced third harmonic generation from the epsilon-near-zero modes of ultrathin films

    SciTech Connect

    Luk, Ting S. Liu, Sheng; Campione, Salvatore; Ceglia, Domenico de; Vincenti, Maria A.; Keeler, Gordon A.; Sinclair, Michael B.; Prasankumar, Rohit P.; Scalora, Michael

    2015-04-13

    We experimentally demonstrate efficient third harmonic generation from an indium tin oxide nanofilm (λ/42 thick) on a glass substrate for a pump wavelength of 1.4 μm. A conversion efficiency of 3.3 × 10{sup −6} is achieved by exploiting the field enhancement properties of the epsilon-near-zero mode with an enhancement factor of 200. This nanoscale frequency conversion method is applicable to other plasmonic materials and reststrahlen materials in proximity of the longitudinal optical phonon frequencies.

  5. Enhanced third harmonic generation from the epsilon-near-zero modes of ultrathin films

    NASA Astrophysics Data System (ADS)

    Luk, Ting S.; de Ceglia, Domenico; Liu, Sheng; Keeler, Gordon A.; Prasankumar, Rohit P.; Vincenti, Maria A.; Scalora, Michael; Sinclair, Michael B.; Campione, Salvatore

    2015-04-01

    We experimentally demonstrate efficient third harmonic generation from an indium tin oxide nanofilm (λ/42 thick) on a glass substrate for a pump wavelength of 1.4 μm. A conversion efficiency of 3.3 × 10-6 is achieved by exploiting the field enhancement properties of the epsilon-near-zero mode with an enhancement factor of 200. This nanoscale frequency conversion method is applicable to other plasmonic materials and reststrahlen materials in proximity of the longitudinal optical phonon frequencies.

  6. Optical Cherenkov radiation in ultrafast cascaded second-harmonic generation

    NASA Astrophysics Data System (ADS)

    Bache, M.; Bang, O.; Zhou, B. B.; Moses, J.; Wise, F. W.

    2010-12-01

    We show through theory and numerics that when few-cycle femtosecond solitons are generated through cascaded (phase-mismatched) second-harmonic generation, these broadband solitons can emit optical Cherenkov radiation in the form of linear dispersive waves located in the red part of the spectrum. The beating between the dispersive wave and the soliton generates trailing temporal oscillations on the compressed soliton. Insertion of a simple short-wave pass filter after the crystal can restore a clean soliton. On the other hand, bandpass filtering around the dispersive wave peak results in near-transform-limited ultrashort mid-IR pulses with pulse durations much shorter than the input near-IR pulse. The Cherenkov radiation for the crystal considered (β-barium borate) is found for pump wavelengths in the range λ=0.95-1.45μm, and is located in the regime λ=1.5-3.5μm. For shorter pump wavelengths, the phase-matching point is located in the absorption region of the crystal, effectively absorbing the generated dispersive wave. By calculating the phase-matching curves for typically used frequency conversion crystals, we point out that the mid-IR absorption in the crystal in many cases automatically will filter away the dispersive wave. Finally, an investigation of recent experimental results uncovers a four-wave-mixing phenomenon related to Cherenkov radiation that is an additional generation mechanism of long-wavelength radiation that can occur during soliton compression. We discuss the conditions that lead to this alternative dynamics rather than generation of Cherenkov radiation.

  7. Spatial coherence measurements of non-resonant and resonant high harmonics generated in laser ablation plumes

    SciTech Connect

    Ganeev, R. A.; Abdelrahman, Z. Frank, F.; Witting, T.; Okell, W. A.; Fabris, D.; Hutchison, C.; Marangos, J. P.; Tisch, J. W. G.

    2014-01-13

    We present measurements of the spatial coherence of the high-order harmonics generated in laser-produced ablation plumes. Harmonics were generated using 4 fs, 775 nm pulses with peak intensity 3 × 10{sup 14} W cm{sup −2}. Double-slit fringe visibilities in the range of ≈0.6–0.75 were measured for non-resonant harmonics in carbon and resonantly enhanced harmonics in zinc and indium. These are somewhat higher than the visibility obtained for harmonics generated in argon gas under similar conditions. This is attributed to lower time-dependent ionization of the plasma ablation targets compared to argon during the high harmonics generation process.

  8. Numerical studies of third-harmonic generation in laser filament in air perturbed by plasma spot

    SciTech Connect

    Feng Liubin; Lu Xin; Liu Xiaolong; Li Yutong; Chen Liming; Ma Jinglong; Dong Quanli; Wang Weimin; Xi Tingting; Sheng Zhengming; Zhang Jie; He Duanwei

    2012-07-15

    Third-harmonic emission from laser filament intercepted by plasma spot is studied by numerical simulations. Significant enhancement of the third-harmonic generation is obtained due to the disturbance of the additional plasma. The contribution of the pure plasma effect and the possible plasma-enhanced third-order susceptibility on the third-harmonic generation enhancement are compared. It is shown that the plasma induced cancellation of destructive interference [Y. Liu et al., Opt. Commun. 284, 4706 (2011)] of two-colored filament is the dominant mechanism of the enhancement of third-harmonic generation.

  9. Vectorial approach to studying second harmonic generation in collagen using linearly and radially polarized beams

    NASA Astrophysics Data System (ADS)

    Yew, Elijah Y. S.; Sheppard, Colin J. R.

    2006-08-01

    The study of second harmonic generation (SHG) has been examined using a vectorial approach for both linearly and radially polarized beams. This approach is necessary for situations when the beam is tightly focused such as in a microscope. Using the vectorial approach, the result of including the y and z components of the electric field is that previously ignored 'cross-component' terms are now found to have an influence on the SHG polarization and the radiation patterns obtained. Since SHG is dependent on the susceptibility tensor, the inclusion of these 'cross-component' terms can help to identify structural changes in biological materials simply by studying the changes in the tensor via the SHG polarization. In particular, we calculate the second harmonic polarization induced in collagen for both linearly and radially polarized beams.

  10. Imaging leukocytes in vivo with third harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Tsai, Cheng-Kun; Chen, Chien-Kuo; Chen, Yu-Shing; Wu, Pei-Chun; Hsieh, Tsung-Yuan; Liu, Han-Wen; Yeh, Chiou-Yueh; Lin, Win-Li; Chia, Jean-San; Liu, Tzu-Ming

    2013-02-01

    Without a labeling, we demonstrated that lipid granules in leukocytes have distinctive third harmonic generation (THG) contrast. Excited by a 1230nm femtosecond laser, THG signals were generated at a significantly higher level in neutrophils than other mononuclear cells, whereas signals in agranular lymphocytes were one order smaller. These characteristic THG features can also be observed in vivo to trace the newly recruited leukocytes following lipopolysaccharide (LPS) challenge. Furthermore, using video-rate THG microscopy, we also captured images of blood cells in human capillaries. Quite different from red-blood-cells, every now and then, round and granule rich blood cells with strong THG contrast appeared in circulation. The corresponding volume densities in blood, evaluated from their frequencies of appearance and the velocity of circulation, fall within the physiological range of human white blood cell counts. These results suggested that labeling-free THG imaging may provide timely tracing of leukocyte movement and hematology inspection without disturbing the normal cellular or physiological status.

  11. Third harmonic generation microscopy of a mouse retina

    PubMed Central

    Lei, Tim C.; Domingue, Scott R.; Kahook, Malik Y.; Bartels, Randy A.; Ammar, David A.

    2015-01-01

    Purpose To demonstrate lipid-specific imaging of the retina through the use of third harmonic generation (THG), a multiphoton microscopic technique in which tissue contrast is generated from optical inhomogeneities. Methods A custom fiber laser and multiphoton microscope was constructed and optimized for simultaneous two-photon autofluorescence (TPAF) and THG retinal imaging. Imaging was performed using fixed-frozen sections of mouse eyes without the use of exogenous fluorescent dyes. In parallel experiments, a fluorescent nuclear stain was used to verify the location of the retinal cell nuclei. Results Simultaneous THG and TPAF images revealed all retinal layers with subcellular resolution. In BALB/c strains, the THG signal stems from the lipidic organelles of the cellular and nuclear membranes. In the C57BL/6 strain, the THG signal from the RPE cells originates from the pigmented granules. Conclusions THG microscopy can be used to image structures of the mouse retina using contrast inherent to the tissue and without the use of a fluorescent dye or exogenously expressed recombinant protein. PMID:25999681

  12. Avalanche of stimulated forward scattering in high harmonic generation.

    PubMed

    Serrat, Carles; Roca, David; Budesca, Josep M; Seres, Jozsef; Seres, Enikoe; Aurand, Bastian; Hoffmann, Andreas; Namba, Shinichi; Kuehl, Thomas; Spielmann, Christian

    2016-04-18

    Optical amplifiers in all ranges of the electromagnetic spectrum exhibit an essential characteristic, namely the input signal during the propagation in the amplifier medium is multiplied by the avalanche effect of the stimulated emission to produce exponential growth. We perform a theoretical study motivated and supported by experimental data on a He gas amplifier driven by intense 30-fs-long laser pulses and seeded with attosecond pulse trains generated in a separated Ne gas jet. We demonstrate that the strong-field theory in the frame of high harmonic generation fully supports the appearance of the avalanche effect in the amplification of extreme ultraviolet attosecond pulse trains. We theoretically separate and identify different physical processes taking part in the interaction and we demonstrate that X-ray parametric amplification dominates over others. In particular, we identify strong-field mediated intrapulse X-ray parametric processes as decisive for amplification at the single-atom level. We confirm that the amplification takes place at photon energies where the amplifier is seeded and when the seed pulses are perfectly synchronized with the driving strong field in the amplifier. Furthermore, propagation effects, phase matching and seed synchronization can be exploited to tune the amplified spectral range within the seed bandwidth. PMID:27137242

  13. Defects and strain enhancements of second-harmonic generation in Si/Ge superlattices

    NASA Astrophysics Data System (ADS)

    Bertocchi, Matteo; Luppi, Eleonora; Degoli, Elena; Véniard, Valérie; Ossicini, Stefano

    2014-06-01

    Starting from experimental findings and interface growth problems in Si/Ge superlattices, we have investigated through ab initio methods the concurrent and competitive behavior of strain and defects in the second-harmonic generation process. Interpreting the second-harmonic intensities as a function of the different nature and percentage of defects together with the strain induced at the interface between Si and Ge, we found a way to tune and enhance the second-harmonic generation response of these systems.

  14. High-order harmonic generation from C{sub 60}-rich plasma

    SciTech Connect

    Ganeev, R. A.; Elouga Bom, L. B.; Ozaki, T.; Wong, M. C. H.; Brichta, J.-P.; Bhardwaj, V. R.; Redkin, P. V.

    2009-10-15

    We performed systematic investigation of high-order harmonic generation from fullerene-rich laser-produced plasmas. We studied harmonic generation by varying several experimental parameters, such as the delay between the ablation and driving pulses, and divergence and polarization of the pump laser. Enhancement of harmonic yield is observed near 20 eV, which is attributed to the influence of a broadband plasmon resonance of C{sub 60} on the nonlinear optical response of fullerene-rich plasma. This increase in the harmonic intensity occurs despite the increased absorption by C{sub 60} at these wavelengths. Using simulations based on time-dependent density-functional theory, we confirm that this effect is due to the influence of collective excitations. We compare harmonic generation from fullerenes using lasers with 793 nm and 396 nm wavelengths, which show the influence of plasmon resonance on the conversion efficiency of high-order harmonics for different laser wavelengths.

  15. Organized Aggregation of Porphyrins in Lipid Bilayers for Third Harmonic Generation Microscopy.

    PubMed

    Cui, Liyang; Tokarz, Danielle; Cisek, Richard; Ng, Kenneth K; Wang, Fan; Chen, Juan; Barzda, Virginijus; Zheng, Gang

    2015-11-16

    Nonlinear optical microscopy has become a powerful tool for high-resolution imaging of cellular and subcellular composition, morphology, and interactions because of its high spatial resolution, deep penetration, and low photo-damage to tissue. Developing specific harmonic probes is essential for exploiting nonlinear microscopic imaging for biomedical applications. We report an organized aggregate of porphyrins (OAP) that formed within lipidic nanoparticles showing fingerprint spectroscopic properties, structure-associated second harmonic generation, and superradiant third harmonic generation. The OAP facilitated harmonic microscopic imaging of living cells with significantly enhanced contrast. The structure-dependent switch between harmonic (OAP-intact) and fluorescence (OAP-disrupted) generation enabled real-time multi-modality imaging of the cellular fate of nanoparticles. Robustly produced under various conditions and easily incorporated into pre-formed lipid nanovesicles, OAP provides a biocompatible nanoplatform for harmonic imaging. PMID:26418395

  16. Enhanced Third Harmonic Generation in Single Germanium Nanodisks Excited at the Anapole Mode.

    PubMed

    Grinblat, Gustavo; Li, Yi; Nielsen, Michael P; Oulton, Rupert F; Maier, Stefan A

    2016-07-13

    We present an all-dielectric germanium nanosystem exhibiting a strong third order nonlinear response and efficient third harmonic generation in the optical regime. A thin germanium nanodisk shows a pronounced valley in its scattering cross section at the dark anapole mode, while the electric field energy inside the disk is maximized due to high confinement within the dielectric. We investigate the dependence of the third harmonic signal on disk size and pump wavelength to reveal the nature of the anapole mode. Each germanium nanodisk generates a high effective third order susceptibility of χ((3)) = 4.3 × 10(-9) esu, corresponding to an associated third harmonic conversion efficiency of 0.0001% at an excitation wavelength of 1650 nm, which is 4 orders of magnitude greater than the case of an unstructured germanium reference film. Furthermore, the nonlinear conversion via the anapole mode outperforms that via the radiative dipolar resonances by about 1 order of magnitude, which is consistent with our numerical simulations. These findings open new possibilities for the optimization of upconversion processes on the nanoscale through the appropriate engineering of suitable dielectric materials. PMID:27331867

  17. Self-Action of Second Harmonic Generation and Longitudinal Temperature Gradient in Nonlinear-Optical Crystals

    NASA Astrophysics Data System (ADS)

    Baranov, A. I.; Konyashkin, A. V.; Ryabushkin, O. A.

    2015-09-01

    Model of second harmonic generation with thermal self-action was developed. Second harmonic generation temperature phase matching curves were measured and calculated for periodically polled lithium niobate crystal. Both experimental and calculated data show asymmetrical shift of temperature tuning curves with pump power.

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

    NASA Technical Reports Server (NTRS)

    Tang, C. L.; Bey, P. P.

    1973-01-01

    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.

  19. Quasiresonant excitation of InP/InGaP quantum dots using second harmonic generated in a photonic crystal cavity

    NASA Astrophysics Data System (ADS)

    Buckley, Sonia; Rivoire, Kelley; Hatami, Fariba; Vučković, Jelena

    2012-10-01

    Indistinguishable single photons are necessary for quantum information processing applications. Resonant or quasiresonant excitation of single quantum dots provides greater single photon indistinguishability than incoherent pumping, but is also more challenging experimentally. Here, we demonstrate high signal to noise quasiresonant excitation of InP/InGaP quantum dots. The excitation is provided via second harmonic generated from a telecommunications wavelength laser resonant with the fundamental mode of a photonic crystal cavity, fabricated at twice the quantum dot transition wavelength. The second harmonic is generated using the χ(2) nonlinearity of the InGaP material matrix.

  20. Highly coherent vacuum ultraviolet radiation at the 15th harmonic with echo-enabled harmonic generation technique

    NASA Astrophysics Data System (ADS)

    Hemsing, E.; Dunning, M.; Hast, C.; Raubenheimer, T. O.; Weathersby, S.; Xiang, D.

    2014-07-01

    X-ray free-electron lasers are enabling access to new science by producing ultrafast and intense x rays that give researchers unparalleled power and precision in examining the fundamental nature of matter. In the quest for fully coherent x rays, the echo-enabled harmonic generation technique is one of the most promising methods. In this technique, coherent radiation at the high harmonic frequencies of two seed lasers is generated from the recoherence of electron beam phase space memory. Here we report on the generation of highly coherent and stable vacuum ultraviolet radiation at the 15th harmonic of an infrared seed laser with this technique. The experiment demonstrates two distinct advantages that are intrinsic to the highly nonlinear phase space gymnastics of echo-enabled harmonic generation in a new regime, i.e., high frequency up-conversion efficiency and insensitivity to electron beam phase space imperfections. Our results allow comparison and confirmation of predictive models and scaling laws, and mark a significant step towards fully coherent x-ray free-electron lasers that will open new scientific research.

  1. Non-collinear generation of angularly isolated circularly polarized high harmonics

    NASA Astrophysics Data System (ADS)

    Hickstein, Daniel D.; Dollar, Franklin J.; Grychtol, Patrik; Ellis, Jennifer L.; Knut, Ronny; Hernández-García, Carlos; Zusin, Dmitriy; Gentry, Christian; Shaw, Justin M.; Fan, Tingting; Dorney, Kevin M.; Becker, Andreas; Jaroń-Becker, Agnieszka; Kapteyn, Henry C.; Murnane, Margaret M.; Durfee, Charles G.

    2015-11-01

    We generate angularly isolated beams of circularly polarized extreme ultraviolet light through the first implementation of non-collinear high harmonic generation with circularly polarized driving lasers. This non-collinear technique offers numerous advantages over previous methods, including the generation of higher photon energies, the separation of the harmonics from the pump beam, the production of both left and right circularly polarized harmonics at the same wavelength and the capability of separating the harmonics without using a spectrometer. To confirm the circular polarization of the beams and to demonstrate the practicality of this new light source, we measure the magnetic circular dichroism of a 20 nm iron film. Furthermore, we explain the mechanisms of non-collinear high harmonic generation using analytical descriptions in both the photon and wave models. Advanced numerical simulations indicate that this non-collinear mixing enables the generation of isolated attosecond pulses with circular polarization.

  2. Second harmonic generation imaging in tissue engineering and cartilage pathologies

    NASA Astrophysics Data System (ADS)

    Lilledahl, Magnus; Olderøy, Magnus; Finnøy, Andreas; Olstad, Kristin; Brinchman, Jan E.

    2015-03-01

    The second harmonic generation from collagen is highly sensitive to what extent collagen molecules are ordered into fibrils as the SHG signal is approximately proportional to the square of the fibril thickness. This can be problematic when interpreting SHG images as thick fibers are much brighter than thinner fibers such that quantification of the amount of collagen present is difficult. On the other hand SHG is therefore also a very sensitive probe to determine whether collagen have assembled into fibrils or are still dissolved as individual collagen molecules. This information is not available from standard histology or immunohistochemical techniques. The degree for fibrillation is an essential component for proper tissue function. We will present the usefulness of SHG imaging in tissue engineering of cartilage as well as cartilage related pathologies. When engineering cartilage it is essential to have the appropriate culturing conditions which cause the collagen molecules to assemble into fibrils. By employing SHG imaging we have studied how cell seeding densities affect the fibrillation of collagen molecules. Furthermore we have used SHG to study pathologies in developing cartilage in a porcine model. In both cases SHG reveals information which is not visible in conventional histology or immunohistochemistry

  3. Research of second harmonic generation images based on texture analysis

    NASA Astrophysics Data System (ADS)

    Liu, Yao; Li, Yan; Gong, Haiming; Zhu, Xiaoqin; Huang, Zufang; Chen, Guannan

    2014-09-01

    Texture analysis plays a crucial role in identifying objects or regions of interest in an image. It has been applied to a variety of medical image processing, ranging from the detection of disease and the segmentation of specific anatomical structures, to differentiation between healthy and pathological tissues. Second harmonic generation (SHG) microscopy as a potential noninvasive tool for imaging biological tissues has been widely used in medicine, with reduced phototoxicity and photobleaching. In this paper, we clarified the principles of texture analysis including statistical, transform, structural and model-based methods and gave examples of its applications, reviewing studies of the technique. Moreover, we tried to apply texture analysis to the SHG images for the differentiation of human skin scar tissues. Texture analysis method based on local binary pattern (LBP) and wavelet transform was used to extract texture features of SHG images from collagen in normal and abnormal scars, and then the scar SHG images were classified into normal or abnormal ones. Compared with other texture analysis methods with respect to the receiver operating characteristic analysis, LBP combined with wavelet transform was demonstrated to achieve higher accuracy. It can provide a new way for clinical diagnosis of scar types. At last, future development of texture analysis in SHG images were discussed.

  4. Second harmonic generation reveals matrix alterations during breast tumor progression

    NASA Astrophysics Data System (ADS)

    Burke, Kathleen; Tang, Ping; Brown, Edward

    2013-03-01

    Alteration of the extracellular matrix in tumor stroma influences efficiency of cell locomotion away from the primary tumor into surrounding tissues and vasculature, thereby affecting metastatic potential. We study matrix changes in breast cancer through the use of second harmonic generation (SHG) of collagen in order to improve the current understanding of breast tumor stromal development. Specifically, we utilize a quantitative analysis of the ratio of forward to backward propagating SHG signal (F/B ratio) to monitor collagen throughout ductal and lobular carcinoma development. After detection of a significant decrease in the F/B ratio of invasive but not in situ ductal carcinoma compared with healthy tissue, the collagen F/B ratio is investigated to determine the evolution of fibrillar collagen changes throughout tumor progression. Results are compared with the progression of lobular carcinoma, whose F/B signature also underwent significant evolution during progression, albeit in a different manner, which offers insight into varying methods of tissue penetration and collagen manipulation between the carcinomas. This research provides insights into trends of stromal reorganization throughout breast tumor development.

  5. Two-photon resonant second harmonic generation in atomic xeon

    SciTech Connect

    Shi, Y. J.; Al-Basheer, W.; Thompson, R. I.

    2009-03-07

    Vacuum ultraviolet (VUV) radiation at 124.8 nm (9.93 eV) was produced from two-photon resonant second harmonic generation (SHG) in a xeon gaseous medium and used to probe molecular samples of acetone, furan, thiophene, ammonia, and methane. The mass spectra recorded from the species with ionization energies below 9.93 eV were dominated by the parent ions. The parent ions were only observed when the incident UV radiation was tuned to resonate with the two-photon transition 5p{sup 5}({sup 2}P{sub 3/2}{sup 0})6p[1/2]{sub 0}(leftarrow)5p{sup 6} {sup 1}S{sub 0} of Xe at 80 119.474 cm{sup -1}. The pressure dependence and the resonant nature of the parent ions observed support the mechanism for SHG as the ionization-initiated electric field induced SHG via the third-order nonlinear susceptibility {chi}{sup (3)}, which is enhanced by the coupling between the 5p{sup 5}({sup 2}P{sub 3/2}{sup 0})6p[1/2]{sub 0} and the nearby 5p{sup 5}({sup 2}P{sub 3/2}{sup 0})5d[1/2]{sub 1} states of Xe atoms.

  6. Third-harmonic generation susceptibility spectroscopy in free fatty acids

    NASA Astrophysics Data System (ADS)

    Chen, Yu-Cheng; Hsu, Hsun-Chia; Lee, Chien-Ming; Sun, Chi-Kuang

    2015-09-01

    Lipid-correlated disease such as atherosclerosis has been an important medical research topic for decades. Many new microscopic imaging techniques such as coherent anti-Stokes Raman scattering and third-harmonic generation (THG) microscopy were verified to have the capability to target lipids in vivo. In the case of THG microscopy, biological cell membranes and lipid bodies in cells and tissues have been shown as good sources of contrast with a laser excitation wavelength around 1200 nm. We report the THG excitation spectroscopy study of two pure free fatty acids including oleic acid and linoleic acid from 1090 to 1330 nm. Different pure fatty acids presented slightly-different THG χ(3) spectra. The measured peak values of THG third-order susceptibility χ(3) in both fatty acids were surprisingly found not to match completely with the resonant absorption wavelengths around 1190 to 1210 nm, suggesting possible wavelengths selection for enhanced THG imaging of lipids while avoiding laser light absorption. Along with the recent advancement in THG imaging, this new window between 1240 to 1290 nm may offer tremendous new opportunities for sensitive label-free lipid imaging in biological tissues.

  7. Second harmonic generation of chiral-modified silver nanoparticles

    NASA Astrophysics Data System (ADS)

    Tao, Yue; Aldea-Nunzi, Gabriela; Rao Bobbara, Sanyasi; Nunzi, Jean-Michel

    2013-10-01

    Various approaches for the optical detection of chiral compounds have been developed due to their natural optical activity. Since the advantages of second harmonic generation (SHG) on noble-metal nanoparticles (NPs) have been observed, it would be interesting to study the nonlinear phenomena from chiral compounds attached Ag NPs. In the present work, we fabricated chiral-modified Ag NPs based on the self-assembly process of cysteine and Ag, and carried out the investigation on SHG on modified and unmodified Ag NPs. For modified Ag NPs, either L-Cysteine (L-C) or D-Cysteine (D-C), as a pair of enantiomers, was applied on top of the Ag NPs. The resulting chiral-modified monolayers of L-C/Ag NPs and D-C/Ag NPs exhibit a reversed optical rotation difference (ORD) at linearly +/-45° polarization of SH, where no such difference exists for Ag NPs alone. SHG efficiently probes and discriminates L-C from D-C monolayers on the modified Ag NPs, which constitutes a simple and sensitive optical diagnostic of chiral molecules.

  8. Second harmonic generation in GF(m, 1) ferroelectric superlattices

    NASA Astrophysics Data System (ADS)

    Chen, Ying; Yang, Xiangbo; Guo, Qi; Lan, Sheng

    2006-03-01

    In this paper we study under the small-signal approximation the properties of the output electric field of second harmonic generation (SHG) for vertical transmission in Family A of the generalized Fibonacci (GF(m, 1)) quasiperiodic ferroelectric domain system. It is found that under perfect quasi-phase-matched (PQPM) conditions there exists self-similarity for the intense peaks of SHG (IPSHG) in real space and the two integers q and p indexing IPSHG make an interesting zero-odd set when m is large enough. On the other hand, self-similarity for IPSHG is broken under imperfect quasi-phase-matched (IQPM) conditions and the SHG spectra comprise a group of intense peaks and another group of satellite weak lines when m is very large. The corresponding integers q and p make an interesting odd-odd set and a successive integer set, respectively. Two kinds of effects of vacancies on SHG have also been found. The analytical results are confirmed by numerical simulations.

  9. Imaging articular cartilage using second harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Mansfield, Jessica C.; Winlove, C. Peter; Knapp, Karen; Matcher, Stephen J.

    2006-02-01

    Sub cellular resolution images of equine articular cartilage have been obtained using both second harmonic generation microscopy (SHGM) and two-photon fluorescence microscopy (TPFM). The SHGM images clearly map the distribution of the collagen II fibers within the extracellular matrix while the TPFM images show the distribution of endogenous two-photon fluorophores in both the cells and the extracellular matrix, highlighting especially the pericellular matrix and bright 2-3μm diameter features within the cells. To investigate the source of TPF in the extracellular matrix experiments have been carried out to see if it may originate from the proteoglycans. Pure solutions of the following proteoglycans hyaluronan, chondroitin sulfate and aggrecan have been imaged, only the aggrecan produced any TPF and here the intensity was not great enough to account for the TPF in the extracellular matrix. Also cartilage samples were subjected to a process to remove proteoglycans and cellular components. After this process the TPF from the samples had decreased by a factor of two, with respect to the SHG intensity.

  10. Optical harmonic generation from animal tissues by the use of picosecond and femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Guo, Yici; Ho, P. P.; Tirksliunas, A.; Liu, Feng; Alfano, R. R.

    1996-12-01

    Second- and third-harmonic generations of femtosecond and picosecond laser pulses have been measured from chicken skin, muscle, and fat tissues. The magnitude of the harmonic signals showed a strong structural dependence with the signal from skin interface being the strongest. The polarization dependence of the signal was also measured and found to be consistent with the fact that the tissue samples were highly scattering random media. The second-harmonic- and third-harmonic-generation conversion efficiencies were found to be in the range of approximately 10 -7 to approximately 10-10.

  11. Studies of surfaces using optical second-harmonic generation

    SciTech Connect

    Tom, H.W.K.

    1984-04-01

    The experiments reported in this thesis demonstrate the use of second-harmonic generation (SHG) and sum-frequency generation (SFG) in reflection from surfaces to study various surface properties. The experiments firmly establish SHG as a viable new surface probe that complements existing surface probes in ultrahigh vacuum environments and is in many ways unique for studying interfaces between dense media. Surface structural symmetry can be revealed through the anisotropy in the SH signal from the surface as the sample is rotated about its normal. The form of this anisotropy is derived in theory and verified with an experiment on the Si(100) and (111) surfaces. The SHG and SFG signals from molecules adsorbed on noninteracting substrates have a direct relationship to the number, average orientation, and spectroscopic properties of the molecules. The SH intensity was used to measure the isotherm for adsorption of p-nitrobenzoic acid from ethanolic solution to fused silica. Experiments performed on a strongly-interacting well-characterized Rh(111) surface in ultrahigh vacuum establish the sensitivity of the SH probe in corroboration with other surface probes. For the first time, the SH coverage-dependence was fit by theory in a quantitative way for the case of O-atom adsorption. The sensitivity of SH to adsorption at different sites was established for CO on top- and bridge-sites. SHG was shown to be surface specific in that the SHG from alkali metal surfaces originates from the first two monolayers. SH sensitivity to the adsorption of catalytically-important hydrocarbons and to chemical processes such as benzene dehydrogenation was also demonstrated. 122 references, 27 figures, 2 tables.

  12. Reconstruction of correlation-driven electron-hole dynamics by high-harmonic-generation spectroscopy

    NASA Astrophysics Data System (ADS)

    Leeuwenburgh, Jonathan; Cooper, Bridgette; Averbukh, Vitali; Marangos, Jonathan P.; Ivanov, Misha

    2014-09-01

    We present detailed analysis of the recently proposed technique of high-order-harmonic generation spectroscopy of correlation-driven electron hole dynamics in atoms and molecules. This novel technique resolves Auger-type processes with attosecond-scale resolution by clocking the decay process with high-harmonic generation. The harmonic generation is driven by an attosecond, XUV pump pulse and a long-duration, infrared pulse. We present the strong-field-approximation-based theory of such an XUV-initiated high-order-harmonic generation process. We detail different ways of recovering the hole survival probability by altering experimental parameters to change the time-energy mapping of the harmonics. The various reconstruction methods are then simulated for M4,5NN Auger decay in krypton and molecular-orbital breakdown dynamics in trans-butadiene and propanal.

  13. Efficient second- and third-harmonic radiation generation from relativistic laser-plasma interactions

    SciTech Connect

    Singh, Mamta; Gupta, D. N.; Suk, H.

    2015-06-15

    We propose an idea to enhance the efficiency of second- and third-harmonic generation by considering the amplitude-modulation of the fundamental laser pulse. A short-pulse laser of finite spot size is modeled as amplitude modulated in time. Amplitude-modulation of fundamental laser contributes in quiver velocity of the plasma electrons and produces the strong plasma-density perturbations, thereby increase in current density at second- and third-harmonic frequency. In a result, the conversion efficiency of harmonic generation increases significantly. Power conversion efficiency of harmonic generation process is the increasing function of the amplitude-modulation parameter of the fundamental laser beam. Harmonic power generated by an amplitude modulated laser is many folds higher than the power obtained in an ordinary case.

  14. Characterization of muscle contraction with second harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Prent, Nicole

    Muscle cells have the ability to change length and generate force due to orchestrated action of myosin nanomotors that cause sliding of actin filaments along myosin filaments in the sarcomeres, the fundamental contractile units, of myocytes. The correlated action of hundreds of sarcomeres is needed to produce the myocyte contractions. This study probes the molecular structure of the myofilaments and investigates the movement correlations between sarcomeres during contraction. In this study, second harmonic generation (SHG) microscopy is employed for imaging striated myocytes. Myosin filaments in striated myocytes inherently have a nonzero second-order susceptibility, [special characters omitted] and therefore generate efficient SHG. Employing polarization-in polarization-out (PIPO) SHG microscopy allows for the accurate determination of the characteristic ratio, [special characters omitted] in birefringent myocytes, which describes the structure of the myosin filament. Analysis shows that the b value at the centre of the myosin filament, where the nonlinear dipoles are better aligned, is slightly lower than the value at the edges of the filament, where there is more disorder in orientation of the nonlinear dipoles from the myosin heads. Forced stretching of myocytes resulted in an SHG intensity increase with the elongation of the sarcomere. SHG microscopy captured individual sarcomeres during contraction, allowing for the measurement of sarcomere length (SL) and SHG intensity (SI) fluctuations. The fluctuations also revealed higher SHG intensity in elongated sarcomeres. The sarcomere synchronization model (SSM) for contracting and quiescent myocytes was developed, and experimentally verified for three cases (isolated cardiomyocyte, embryonic chicken cardiomyocyte, and larva myocyte). During contraction, the action of SLs and SIs between neighbouring sarcomeres partially correlated, whereas in quiescent myocytes the SLs show an anti-correlation and the SIs have no

  15. Studies of interfaces and vapors with Optical Second Harmonic Generation

    SciTech Connect

    Mullin, C. S.

    1993-12-01

    Optical Second Harmonic Generation (SHG) has been applied to the study of soap-like molecules adsorbed to the water-air interface. By calibrating the signal from a soluble monolayer with that of an insoluble homolog, absolute measurements of the surface density could be obtained and related to the bulk concentration and surface tension. We could then demonstrate that the soluble surfactant forms a single monolayer at the interface. Furthermore, it deviates significantly from the ideal case in that its activity coefficients are far from 1, yet those coefficients remain constant over a broad range of surface pressures. We present evidence of a first-order phase transition taking place during the adsorption of this soluble monolayer. We consider the effects of the non-ideal behavior and the phase transition on the microscopic model of adsorption, and formulate an alternative to the Langmuir picture of adsorption which is just as simple, yet it can more easily allow for non-ideal behavior. The second half of this thesis considers the problem of SHG in bulk metal vapors. The symmetry of the vapor forbids SHG, yet it has been observed. We consider several models whereby the symmetry of the vapor is broken by the presence of the laser and compare their predictions to new observations we have made using a few-picosecond laser pulse. The two-lobed output beam profile shows that it is the vapor-plus-beam combination whose symmetry is important. The dependence on vapor pressure demonstrates the coherent nature of the radiation, while the dependence on buffer gas pressure hints at a change of the symmetry in time. The time-dependence is measured directly with a preliminary pump-probe measurement. The magnitude and intensity dependence of the signal are also measured. All but one of the models are eliminated by this comparison.

  16. Second harmonic generation imaging microscopy of cellular structure and function

    NASA Astrophysics Data System (ADS)

    Millard, Andrew C.; Jin, Lei; Loew, Leslie M.

    2005-03-01

    Second harmonic generation (SHG) imaging microscopy is an important emerging technique for biological research, with many advantages over existing one- or two-photon fluorescence techniques. A non-linear phenomenon employing mode-locked Ti:sapphire or fiber-based lasers, SHG results in intrinsic optical sectioning without the need for a confocal aperture. Furthermore, as a second-order process SHG is confined to loci lacking a center of symmetry. Many important structural proteins such as collagen and cellulose show intrinsic SHG, thus providing access to sub-resolution information on symmetry. However, we are particularly interested here in "resonance-enhanced" SHG from styryl dyes. In general SHG is a combination of a true second-order process and a third-order process dependent on a static electric field, such that SHG from membrane-bound dyes depends on a cell's trans-membrane potential. With simultaneous patch-clamping and non-linear imaging of cells, we have found that SHG is a sensitive probe of trans-membrane potential with sensitivities that are up to four times better than those obtained under optimal conditions using one-photon fluorescence imaging. With the sensitivity of SHG to local electric fields from other sources such as the membrane dipole potential as well as the quadratic dependence of SHG on concentration, we have found that SHG imaging of styryl dyes is also a powerful technique for the investigation of lipid phases and rafts and for the visualization of the dynamics of membrane-vesicle fusion following fertilization of an ovum.

  17. Second harmonic generation study of liquid surface and amphilphile monolayer

    SciTech Connect

    Zhao, X.

    1992-12-31

    This thesis contains the following topics. In Chapter 2, we use temperature dependent SHC to study the surface structure of some neat liquids. It was found all the hydrogen bonding liquids have a stronger SHG dependence of temperature while for the non-hydrogen bonding liquids SH response is insensitive to temperature change. In Chapter 3, we discussed the general feature of the electric field induced second harmonic generation (EFISHG). We experimentally established the importance of the {chi}{sup (3)} mechanism at the air/water charged interface. In Chapter 4, we used SHG to study the p-nitrophenol (PNP) penetration into the insoluble monolayer of hexadecyl and pentadecyl acid. It was found that PNP preferentially adsorbs at the fatty acid monolayer. The population and orientation of PNP is strongly dependent on the fatty acid monolayer packing. In Chapter 5, SH signal fluctuation spectroscopy was used to study the surface self-diffusion within the monolayer gas-liquid co-existence region. Assuming the uniform distribution of the liquid phase cluster size, a diffusion model was developed to fit the experimental measured autocorrelation function. In Chapter 6, SH fluctuation spectroscopy was used to study the monolayer orientation spontaneous fluctuation. It was found that only the electron rich aromatic head groups exhibit the orientational fluctuation while the electron poor aromatic molecules do not have a fluctuation anomalies. Fluctuation time scale is strongly influenced by the hydrophobic chain length. A quantitative theory was presented based on Landau-Ginzburg theory to fit the time dependent orientation fluctuation. In Chapter 7, we focused on the acid-base equilibrium constant measurement at the air/water interface using both {chi}{sup (2)} and {chi}{sup (2)} method. We have measured pKa of aniline, phenol, amine, and acid at the interface. It turned out that for all these species, the neutral form is more stable at the interface.

  18. Second harmonic generation in nanoscale films of transition metal chalcogenides: Taking into account multibeam interference

    NASA Astrophysics Data System (ADS)

    Lavrov, S. D.; Kudryavtsev, A. V.; Shestakova, A. P.; Kulyuk, L.; Mishina, E. D.

    2016-05-01

    Second harmonic generation is studied in structures containing nanoscale layers of transition metal chalcogenides that are two-dimensional semiconductors and deposited on a SiO2/Si substrate. The second harmonic generation intensity is calculated with allowance for multibeam interference in layers of dichalcogenide and silicon oxide. The coefficient of reflection from the SiO2-layer-based Fabry-Perot cavity is subsequently calculated for pump wave fields initiating nonlinear polarization at every point of dichalcogenide, which is followed by integration of all second harmonic waves generated by this polarization. Calculated second harmonic intensities are presented as functions of dichalcogenide and silicon oxide layer thicknesses. The dependence of the second harmonic intensity on the MoS2 layer thickness is studied experimentally in the layer of 2-140 nm. A good coincidence of the experimental data and numerical simulation results has been obtained.

  19. Virtual biopsy of rat tympanic membrane using higher harmonic generation microscopy

    NASA Astrophysics Data System (ADS)

    Lee, Wen-Jeng; Lee, Chia-Fone; Chen, Szu-Yu; Chen, Yuh-Shyang; Sun, Chi-Kuang

    2010-07-01

    Multiharmonic optical microscopy has been widely applied in biomedical research due to its unique capability to perform noninvasive studies of biomaterials. In this study, virtual biopsy based on back-propagating multiple optical harmonics, combining second and third harmonics, is applied in unfixed rat tympanic membrane. We show that third harmonic generation can provide morphologic information on the epithelial layers of rat tympanic membrane as well as radial collagen fibers in middle fibrous layers, and that second harmonic generation can provide information on both radial and circular collagen fibers in middle fibrous layers. Through third harmonic generation, the capillary and red blood cells in the middle fibrous layer are also noted. Additionally, the 3-D relationship to adjacent bony structures and spatial variations in thickness and curvature are obtained. Our study demonstrates the feasibility of using a noninvasive optical imaging system for comprehensive evaluation of the tympanic membrane.

  20. Effect of nuclear motion on spectral broadening of high-order harmonic generation.

    PubMed

    Yuan, Xiaolong; Wei, Pengfei; Liu, Candong; Ge, Xiaochun; Zheng, Yinghui; Zeng, Zhinan; Li, Ruxin

    2016-04-18

    High-order harmonic generation (HHG) in molecular targets is experimentally investigated in order to reveal the role of the nuclear motion played in the harmonic generation process. An obvious broadening in the harmonic spectrum from the H2 molecule is observed in comparison with the harmonic spectrum generated from other molecules with relatively heavy nuclei. We also find that the harmonic yield from the H2 molecule is much weaker than the yield from those gas targets with the similar ionization potentials, such as Ar atom and N2 molecule. The yield suppression and the spectrum broadening of HHG can be attributed to the vibrational motion of nuclear induced by the driving laser pulse. Moreover, the one-dimensional (1D) time-dependent Schrödinger equation (TDSE) with the non-Born-Oppenheimer (NBO) treatment is numerically solved to provide a theoretical support to our explanation. PMID:27137258

  1. Third harmonic generation in air ambient and laser ablated carbon plasma

    SciTech Connect

    Singh, Ravi Pratap Gupta, Shyam L.; Thareja, Raj K.

    2015-12-15

    We report the third harmonic generation of a nanosecond laser pulse (1.06 μm) in air ambient and in the presence of nanoparticles from laser ablated carbon plasma. Significant decrease in the threshold of third harmonic generation and multi-fold increment in the intensity of generated third harmonic is observed in presence of carbon plasma. The third harmonic in air is due to the quasi-resonant four photon process involving vibrationally excited states of molecular ion of nitrogen due to electron impact ionization and laser pulse. Following optical emission spectroscopic observations we conclude that the presence of C{sub 2} and CN in the ablated plume play a vital role in the observed third harmonic signals.

  2. Generation of a broadband xuv continuum in high-order-harmonic generation by spatially inhomogeneous fields

    NASA Astrophysics Data System (ADS)

    Yavuz, I.

    2012-01-01

    We address an efficient scheme to generate a broadband extreme-ultraviolet (xuv) continuum from high-order harmonic generation emerging from the concept of plasmonic field enhancement in the vicinity of metallic nanostructures [S. Kim Nature (London)NATUAS0028-083610.1038/nature07012 453, 757 (2008)]. Based on the numerical solution of a time-dependent Schrödinger equation, for moderate field intensities and depending on the inhomogeneity of the field, we are able to increase the plateau region roughly by a factor of two and generate a broadband xuv continuum. The underlying physics of the plasmon enhancement in harmonic generation is investigated in terms of the semiclassical trajectories of strong field-electron dynamics, and perfect consistency is found between quantum mechanical simulations. It is found that the field inhomogeneity plays a critical role in quantum path selection. After a critical value, we observe a systematic suppression in the long trajectories, suggesting the generation of a single isolated attosecond pulse. Finally, we investigate the dependence of cutoff position on the order of field inhomogeneity and find a β2.3∓0.2 scaling.

  3. Enhancing High-Order Harmonic Generation in Light Molecules by Using Chirped Pulses.

    PubMed

    Lara-Astiaso, M; Silva, R E F; Gubaydullin, A; Rivière, P; Meier, C; Martín, F

    2016-08-26

    One of the current challenges in high-harmonic generation is to extend the harmonic cutoff to increasingly high energies while maintaining or even increasing the efficiency of the high-harmonic emission. Here we show that the combined effect of down-chirped pulses and nuclear dynamics in light molecules allows one to achieve this goal, provided that long enough IR pulses are used to allow the nuclei to move well outside the Franck-Condon region. We also show that, by varying the duration of the chirped pulse or by performing isotopic substitution while keeping the pulse duration constant, one can control the extension of the harmonic plateau. PMID:27610851

  4. Enhancement of third-harmonic generation in a polymer-dispersed liquid-crystal grating

    NASA Astrophysics Data System (ADS)

    Markowicz, Przemyslaw P.; Hsiao, Vincent K. S.; Tiryaki, Hanifi; Cartwright, Alexander N.; Prasad, Paras N.; Dolgaleva, Ksenia; Lepeshkin, Nick N.; Boyd, Robert W.

    2005-08-01

    We report the observation of significant enhancement of one-step third-harmonic generation in a one-dimensional photonic crystal pumped by a near-infrared laser beam tuned to the low-frequency edge of the first photonic band gap. The third-harmonic phase matching can be controlled by changing the angle of incidence of the fundamental radiation, allowing tunability of the third-harmonic wavelength. The observed phenomenon was modeled theoretically using the transfer-matrix method. The enhancement is attributed to the combined action of phase-matching between the pump and harmonic waves and pump-field localization within the photonic crystal.

  5. Calculation of second-harmonic wave pattern generated by focused cylindrical vector beams

    NASA Astrophysics Data System (ADS)

    Ohtsu, A.; Kozawa, Y.; Sato, S.

    2010-03-01

    We calculated the second-harmonic wave pattern induced by focused cylindrically symmetric, polarized vector beams. The second-order nonlinear polarization was expressed for fundamental electric field components passed through a dielectric interface based on vector diffraction theory. Furthermore, the second-harmonic wave pattern was represented on the basis of the far-field approximate expression derived from the formulation of higher-order harmonic generation including a Green's function. For a (110) zinc selenide crystal, the calculated forward emission patterns of the second-harmonic wave were eight-figure shaped as observed in experiment.

  6. Harmonic generation in the free-electron laser. II. cw calculation for the linearly polarized wiggler

    SciTech Connect

    Al-Abawi, H.; Moore, G.T.; Scully, M.O.

    1982-01-01

    Harmonic generation in the free-electron laser offers a possible means to extend the wavelength range of the device towards high frequency. Numerical solutions to the basic equations describing this process are shown for cw operation using a linearly polarized wiggler. Higher harmonic emission becomes enhanced as the magnetic field is increased and as the energy spread in the electron beam is reduced.

  7. Vector treatment of second-harmonic generation produced by tightly focused vignetted Gaussian beams

    NASA Astrophysics Data System (ADS)

    Asatryan, Ara A.; Sheppard, Colin J. R.; de Sterke, C. Martijn

    2004-12-01

    We present a fast and accurate method to calculate the vector-field distribution of a focused Gaussian beam. This method is applied to calculate the second harmonic that is generated by such a beam from a sample in the undepleted pump approximation. These calculations can be used to model second-harmonic imaging in an optical microscope with a wide aperture.

  8. Observation of the second-harmonic generation from relativistically quivering electrons in exciting laser wakefield.

    PubMed

    Takahashi, Eiji; Mori, Michiaki; Yugami, Noboru; Nishida, Yasushi; Kondo, Kiminori

    2002-01-01

    The second-harmonic emission generated by the spatially asymmetric quivering electrons caused by the ponderomotive force was studied. The intensity of the second harmonic was proportional to the focused intensity of the pump pulse with the power of 1.8. This intensity dependence can be explained by the relativistic effect of the quivering electrons. PMID:11800785

  9. Second harmonic generation and two-photon luminescence from colloidal gold nanoparticles

    NASA Astrophysics Data System (ADS)

    Yashunin, D. A.; Korytin, A. I.; Smirnov, A. I.; Stepanov, A. N.

    2016-03-01

    Second harmonic generation and two-photon luminescence from colloidal gold nanoparticles in the 980-1300 nm wavelength range of exciting femtosecond radiation were investigated experimentally. The measured polarization and spectral characteristics of the second harmonic and two-photon luminescence demonstrate that the observed nonlinear optical signal is determined by the dimers constituting several percent of the total nanoparticle number.

  10. High-order-harmonic generation in gas with a flat-top laser beam

    SciTech Connect

    Boutu, W.; Auguste, T.; Binazon, L.; Gobert, O.; Carre, B.; Boyko, O.; Valentin, C.; Balcou, Ph.; Merdji, H.

    2011-12-15

    We present experimental and numerical results on high-order-harmonic generation with a flat-top laser beam. We show that a simple binary tunable phase plate, made of two concentric glass plates, can produce a flat-top profile at the focus of a Gaussian infrared beam. Both experiments and numerical calculations show that there is a scaling law between the harmonic generation efficiency and the increase of the generation volume.