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Separation of High Order Harmonics with Fluoride Windows

Description: The lower orders produced in high order harmonic generation can be effciently temporally separated into monochromatic pulses by propagation in a Fluoride window while still preserving their femtosecond pulse duration. We present calculations for MgF2, CaF2, and LiF windows for the third, fifth, and seventh harmonics of 800 nm. We demonstrate the use of this simple and inexpensive technique in a femtosecond pump/probe experiment using the fifth harmonic.
Date: August 2, 2010
Creator: Allison, Tom; van Tilborg, Jeroen; Wright, Travis; Hertlein, Marcus; Falcone, Roger & Belkacem, Ali
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A source for quantum control: generation and measurement of attosecond ultraviolet light pulses

Description: This project has pursued the possibility of producing ultra-short pulses of coherent light using harmonic conversion of a mid-infrared light source, focused into an atomic gas medium. This was a joint effort with Louis DiMauro's experimental group at Brookhaven National Laboratory and in collaboration with Ken Schafer from Louisiana State University and Mette Gaarde from Lund University on the theoretical part. High order harmonic generation (HHG) in nobel gas media using short-pulse visible and near infrared lasers has become an established method for producing coherent, short pulse radiation at wavelengths from the ultraviolet to soft x-rays. We recently proposed that this approach could lead to extremely short pulses, potentially less than one fs, provided the unavoidable frequency chirp of the highest harmonics, could be removed by compressing the pulses with a grating pair. Sources of sub-fs pulses would provide unique opportunities to study dynamical processes on time scales short compared to those associated with nuclear motion. Truly stroboscopic pictures of chemical reaction dynamics would be possible, for example. In this research project we have chosen much smaller driving frequencies than used previously in HHG studies for two reasons. First, this will allow us to measure the pulse lengths of the compressed harmonics because they will be in the vacuum ultraviolet where coincidence measurements are possible. Second, the wavelengths of these harmonics will be idea for pump-probe experiments of quantum dynamical control studies. Our theoretical effort was concentrated in two areas. We used our time-dependent quantum numerical codes to evaluate the harmonic response of alkali atoms to the mid-IR laser excitation. Results were obtained for potassium, the initial species to be used in the experiments, then sodium and rubidium to investigate the possibility of higher conversion efficiencies. In fact, rubidium was found to be significantly better than potassium, both because it ...
Date: February 19, 1999
Creator: Kulander, K C
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Modulation compression for short wavelength harmonic generation

Description: 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.
Date: January 11, 2010
Creator: Qiang, J.
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Control of visible harmonic generation using polarization in photonic crystal fibers

Description: The polarization state of the input pulses to a segment of microstructured fiber controls the harmonic generation yielding specific frequencies depending on of the input state.
Date: January 1, 2001
Creator: Omenetto, F. G. (Fiorenzo G.); Efimov, A. V. (Anatoly V.); Taylor, Antoinette J.,; Knight, J. C. (Jonathan C.); Wadsworth, W. J. (William J.) & Russell, P. S. J. (Philip St. J.)
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Nonlinear and Quantum Optics Near Nanoparticles

Description: We study the behavior of electric fields in and around dielectric and metal nanoparticles, and prepare the ground for their applications to a variety of systems viz. photovoltaics, imaging and detection techniques, and molecular spectroscopy. We exploit the property of nanoparticles being able to focus the radiation field into small regions and study some of the interesting nonlinear, and quantum coherence and interference phenomena near them. The traditional approach to study the nonlinear light-matter interactions involves the use of the slowly varying amplitude approximation (SVAA) as it simplifies the theoretical analysis. However, SVVA cannot be used for systems which are of the order of the wavelength of the light. We use the exact solutions of the Maxwell's equations to obtain the fields created due to metal and dielectric nanoparticles, and study nonlinear and quantum optical phenomena near these nanoparticles. We begin with the theoretical description of the electromagnetic fields created due to the nonlinear wavemixing process, namely, second-order nonlinearity in an nonlinear sphere. The phase-matching condition has been revisited in such particles and we found that it is not satisfied in the sphere. We have suggested a way to obtain optimal conditions for any type and size of material medium. We have also studied the modifications of the electromagnetic fields in a collection of nanoparticles due to strong near field nonlinear interactions using the generalized Mie theory for the case of many particles applicable in photovoltaics (PV). We also consider quantum coherence phenomena such as modification of dark states, stimulated Raman adiabatic passage (STIRAP), optical pumping in $4$-level atoms near nanoparticles by using rotating wave approximation to describe the Hamiltonian of the atomic system. We also considered the behavior of atomic and the averaged atomic polarization in $7$-level atoms near nanoparticles. This could be used as a prototype to study ...
Date: December 2015
Creator: Dhayal, Suman
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Tri-material multilayer coatings with high reflectivity and wide bandwidth for 25 to 50 nm extreme ultraviolet light

Description: Magnesium/silicon carbide (Mg/SiC) multilayers have been fabricated with normal incidence reflectivity in the vicinity of 40% to 50% for wavelengths in the 25 to 50 nm wavelength range. However many applications, for example solar telescopes and ultrafast studies using high harmonic generation sources, desire larger bandwidths than provided by high reflectivity Mg/SiC multilayers. We investigate introducing a third material, Scandium, to create a tri-material Mg/Sc/SiC multilayer allowing an increase the bandwidth while maintaining high reflectivity.
Date: September 9, 2009
Creator: Aquila, Andrew; Salmassi, Farhad; Liu, Yanwei & Gullikson, Eric M.
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Structures and charging of alpha-alumina (0001)/water interfaces studies by sum-frequency vibrational spectroscopy

Description: Sum-frequency vibrational spectroscopy in the OH stretch region was employed to study structures of water/{alpha}-Al{sub 2}O{sub 3} (0001) interfaces at different pH values. Observed spectra indicate that protonation and deprotonation of the alumina surface dominate at low and high pH, respectively, with the interface positively and negatively charged accordingly. The point of zero charge (p.z.c.) appears at pH {approx}6.3, which is close to the values obtained from streaming potential and second harmonic generation studies. It is significantly lower than the p.z.c. of alumina powder. The result can be understood from the pK values of protonation and deprotonation at the water/{alpha}-Al{sub 2}O{sub 3} (0001) interface. The p.z.c. of amorphous alumina was found to be similar to that of powder alumina.
Date: November 10, 2008
Creator: Zhang, L.; Tian, C.; Waychunas, G.A. & Shen, Y.R.
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High order harmonic generation in rare gases

Description: 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 ...
Date: May 1, 1994
Creator: Budil, K.S.
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Harmonic cascade FEL designs for LUX

Description: LUX is a design concept for an ultrafast X-ray science facility, based on an electron beam accelerated to GeV energies in are circulating linac. Included in the design are short duration (200 fs or shorter FWHM) light sources using multiple stages of higher harmonic generation, seeded by a 200-250 nm laser of similar duration. This laser modulates the energy of a group of electrons within the electron bunch; this section of the electron bunch then produces radiation at a higher harmonic after entering a second, differently tuned undulator. Repeated stages in a cascade yield increasing photon energies up to 1 keV. Most of the undulators in the cascade operate in the low-gain FEL regime. Harmonic cascades have been designed for each pass of the recirculating linac up to a final electron beam energy of 3.1 GeV. For a given cascade, the photon energy can be selected over a wide range by varying the seed laser frequency and the field strength in the undulators. We present simulation results using the codes GENESIS and GINGER, as well as the results of analytical models which predict FEL performance. We discuss lattice considerations pertinent for harmonic cascade FELs, as well as sensitivity studies and requirements on the electron beam.
Date: July 16, 2004
Creator: Penn, G.; Reinsch, M.; Wurtele, J.; Corlett, J.N.; Fawley, W.M.; Zholents, A. et al.
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Three-dimensional analysis of free-electron laser performance using brightness scaled variables

Description: A three-dimensional analysis of radiation generation in a free-electron laser (FEL) is performed in the small signal regime. The analysis includes beam conditioning, harmonic generation, flat beams, and a new scaling of the FEL equations using the six-dimensional beam brightness. The six-dimensional beam brightness is an invariant under Liouvillian flow; therefore, any nondissipative manipulation of the phase-space, performed, for example, in order to optimize FEL performance, must conserve this brightness. This scaling is more natural than the commonly-used scaling with the one-dimensional growth rate. The brightness-scaled equations allow for the succinct characterization of the optimal FEL performance under various additional constraints. The analysis allows for the simple evaluation of gain enhancement schemes based on beam phase space manipulations such as emittance exchange and conditioning. An example comparing the gain in the first and third harmonics of round or flat and conditioned or unconditioned beams is presented.
Date: June 11, 2008
Creator: Penn, Gregory; Gullans, M.; Penn, G.; Wurtele, J.S. & Zolotorev, M.
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Fringe-free, Background-free, Collinear Third Harmonic Generation FROG Measurements for Multiphoton Microscopy

Description: Collinear pulse measurement tools useful at the full numerical aperture (NA) of multiphoton microscope objectives are a necessity for a quantitative characterization of the femtosecond pulses focused by these systems. In this letter, we demonstrate a simple new technique, for characterizing the pulse at the focus in a multiphoton microscope. This technique, a background-free, fringe-free, form of frequency-resolved optical gating, uses the third harmonic signal generated from a glass coverslip. Here it is used to characterize 100 fs pulses (typical values for a multiphoton microscope) at the focus of a 0.65 NA objective.
Date: July 21, 2006
Creator: Chadwick, R; Spahr, E; Squier, J A; Durfee, C G; Walker, B C & Fittinghoff, D N
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A comparison of observables for solid-solid phase transitions

Description: The study of solid-solid phase transformations is hindered by the difficulty of finding a volumetric probe to use as a progress variable. Solids are typically optically opaque and heterogeneous. Over the past several years, second harmonic generation (SHG) has been used as a kinetic probe for a solid-solid phase transition in which the initial and final phases have different symmetries. Bulk generation of SHG is allowed by symmetry only in noncentrosymmetric crystallographic space groups. For the organic energetic nitramine octahydro-1,3 ,5,7 -tetranitro-1,3 ,5,7 -tatrazocine (HMX), the beta phase is centro symmetric (space group P2{sub 1}/c) and the delta phase iS noncentrosymmetric (space group P6{sub 1}22) making SHG an extremely sensitive, essentially zero background probe of the phase change progress. We have used SHG as a tool to follow the progress of the transformation from beta to delta phase during the solid-solid transformation. However, kinetic models of the transformation derived using different observables from several other groups have differed, showing later onset for the phase change and faster progression to completion. In this work, we have intercompared several techniques to understand these differences. The three techniques discussed are second harmonic generation, Raman spectroscopy, and differential scanning calorimetry (DSC). The progress of the beta to delta phase transition in HMX observed with each of these different probes will be discussed and advantages and disadvantages of each technique described. This paper compares several different observables for use in measuring the kinetics of solid-solid phase transitions. Relative advantages and disadvantages for each technique are described and a direct comparison of results is made for the beta to delta polymorphic phase transition of the energetic nitramine, octahydro-1,3,5,7-tetranitro-1,3,5,7-tatrazocine.
Date: January 1, 2009
Creator: Smilowitz, Laura B; Henson, Bryan F & Romero, Jerry J
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Inclusion Analysis and Absorption Measurement in Nonlinear Crystals

Description: Yttrium calcium oxyborate (YCOB) is a newly developed nonlinear optical crystal used for second harmonic generation in the Mercury laser. As with any new crystal, optical characterization of the material properties needs to be fully investigated. We are developing two new techniques to detect inclusions and measure optical absorption. With the side illuminating detection examination (SIDE) method, we hope to identify and map the size, density, and the morphology of inclusions. The multi-pass absorption technique (MPAT) will be used to help determine the absorption coefficient of various finished crystalline pieces at near-infrared wavelengths.
Date: August 26, 2005
Creator: Smith, L L
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Nonlinear Light Generation from Optical Cavities and Antennae

Description: Semiconductor based micro- and nano-structures grown in a systematic and controlled way using selective area growth are emerging as a promising route toward devices for integrated optical circuitry in optoelectronics and photonics field. This dissertation focuses on the experimental investigation of the nonlinear optical effects in selectively grown gallium nitride micro-pyramids that act as optical cavities, zinc oxide submicron rods and indium gallium nitride multiple quantum well core shell submicron tubes on the apex of GaN micro pyramids that act as optical antennae. Localized spatial excitation of these low dimensional semiconductor structures was optimized for nonlinear optical light (NLO) generation due to second harmonic generation (SHG) and multi-photon luminescence (MPL). The evolution of both processes are mapped along the symmetric axis of the individual structures for multiple fundamental input frequencies of light. Effects such as cavity formation of generated light, electron-hole plasma generation and coherent emission are observed. The efficiency and tunability of the frequency conversion that can be achieved in the individual structures of various geometries are estimated. By controlling the local excitation cross-section within the structures along with modulation of optical excitation intensity, the nonlinear optical process generated in these structures can be manipulated to generate coherent light in the UV-Blue region via SHG process or green emission via MPL process. The results show that these unique structures hold the potential to convert red input pulsed light into blue output pulsed light which is highly directional.
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Date: May 2017
Creator: Butler, Sween J
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Nanograting-based compact VUV spectrometer and beam profiler for in-situ characterization of high-order harmonic generation light sources

Description: A compact, versatile device for VUV beam characterization is presented. It combines the functionalities of a VUV spectrometer and a VUV beam profiler in one unit and is entirely supported by a standard DN200 CF flange. The spectrometer employs a silicon nitride transmission nanograting in combination with a micro-channel plate based imaging detector. This enables the simultaneous recording of wavelengths ranging from 10 nm to 80 nm with a resolution of 0.25 nm to 0.13 nm. Spatial beam profiles with diameters up to 10 mm are imaged with 0.1 mm resolution. The setup is equipped with an in-vacuum translation stage that allows for in situ switching between the spectrometer and beam profiler modes and for moving the setup out of the beam. The simple, robust design of the device is well suited for non-intrusive routine characterization of emerging laboratory- and accelerator-based VUV light sources. Operation of the device is demonstrated by characterizing the output of a femtosecond high-order harmonic generation light source.
Date: July 9, 2010
Creator: Kornilov, Oleg; Wilcox, Russell & Gessner, Oliver
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Long-time solution of the time-dependent Schroedinger equation for an atom in an electromagnetic field using complex coordinate contours

Description: We demonstrate that exterior complex scaling (ECS) can be used to impose outgoing wave boundary conditions exactly on solutions of the time-dependent Schrodinger equation for atoms in intense electromagnetic pulses using finite grid methods. The procedure is formally exact when applied in the appropriate gauge and is demonstrated in a calculation of high harmonic generation in which multiphoton resonances are seen for long pulse durations. However, we also demonstrate that while the application of ECS in this way is formally exact, numerical error can appear for long time propagations that can only be controlled by extending the finite grid. A mathematical analysis of the origins of that numerical error, illustrated with an analytically solvable model, is also given.
Date: September 8, 2009
Creator: Tao, Liang; Vanroose, Wim; Reps, Brian; Rescigno, Thomas N. & McCurdy, C. William
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An Analysis of Shot Noise Propagation and Amplificationin Harmonic Cascade FELs

Description: The harmonic generation process in a harmonic cascade (HC) FEL is subject to noise degradation which is proportional to the square of the total harmonic order. In this paper, we study the shot noise evolution in the first-stage modulator and radiator of a HC FEL that produces the dominant noise contributions. We derive the effective input noise for a modulator operating in the low-gain regime, and analyze the radiator noise for a density-modulated beam. The significance of these noise sources in different harmonic cascade designs is also discussed.
Date: December 11, 2006
Creator: Huang, Z.
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Insertion devices at the advanced photon source

Description: The insertion devices being installed at the Advanced Photon Source cause the stored particle beam to wiggle, emitting x-rays with each wiggle. These x-rays combine to make an intense beam of radiation. Both wiggler and undulator types of insertion devices are being installed; the characteristics of the radiation produced by these two types of insertion devices are discussed, along with the reasons for those characteristics.
Date: July 1, 1996
Creator: Moog, E.R.
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Nonlinear response of superconductors to alternating fields and currents

Description: This report discusses the following topics on superconductivity: nonlinearities in hard superconductors such as surface impedance of a type II superconductimg half space and harmonic generation and intermodulation due to alternating transport currents; and nonlinearities in superconducting weak links such as harmonic generation by a long Josephson Junction in a superconducting slab.
Date: October 8, 1997
Creator: McDonald, J.
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Frequency converter development for the National Ignition Facility

Description: The design of the National Ignition Facility (NIF) incorporates a type I/type II third harmonic generator to convert the 1.053-{micro}m fundamental wavelength of the laser amplifier to a wavelength of 0.351 {micro}m for target irradiation. To understand and control the tolerances in the converter design, we have developed a comprehensive error budget that accounts for effects that are known to influence conversion efficiency, including variations in amplitude and phase of the incident laser pulse, temporal bandwidth of the incident laser pulse, crystal surface figure and bulk non-uniformities, angular alignment errors, Fresnel losses, polarization errors and crystal temperature variations. The error budget provides specifications for the detailed design of the NIF final optics assembly (FOA) and the fabrication of optical components. Validation is accomplished through both modeling and measurement, including full-scale Beamlet tests of a 37-cm aperture frequency converter in a NIF prototype final optics cell. The prototype cell incorporates full-perimeter clamping to support the crystals, and resides in a vacuum environment as per the NIF design.
Date: October 30, 1998
Creator: Auerbach, J M; Barker, C E; Burkhart, S C; Couture, S A; DeYoreo, J J; Hackel, L A et al.
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