Vibrational sum-frequency generation spectroscopy of lipid bilayers at repetition rates up to 100 kHz

Science.gov (United States)

Yesudas, Freeda; Mero, Mark; Kneipp, Janina; Heiner, Zsuzsanna

2018-03-01

Broadband vibrational sum-frequency generation (BB-VSFG) spectroscopy has become a well-established surface analytical tool capable of identifying the orientation and structure of molecular layers. A straightforward way to boost the sensitivity of the technique could be to increase the laser repetition rate beyond that of standard BB-VSFG spectrometers, which rely on Ti:sapphire lasers operating at repetition rates of 1-5 kHz. Nevertheless, possible thermally induced artifacts in the vibrational spectra due to higher laser average powers are unexplored. Here, we discuss laser power induced temperature accumulation effects that distort the BB-VSFG spectra of 1,2-diacyl-sn-glycero-3-phosphocholine at an interface between two transparent phases at repetition rates of 5, 10, 50, and 100 kHz at constant pulse energy. No heat-induced distortions were found in the spectra, suggesting that the increase in the laser repetition rate provides a feasible route to an improved signal-to-noise ratio or shorter data acquisition times in BB-VSFG spectroscopy for thin films on transparent substrates. The results have implications for future BB-VSFG spectrometers pushing the detection limit for molecular layers with low surface coverage.

Atmospheric pressure reaction cell for operando sum frequency generation spectroscopy of ultrahigh vacuum grown model catalysts

Science.gov (United States)

Roiaz, Matteo; Pramhaas, Verena; Li, Xia; Rameshan, Christoph; Rupprechter, Günther

2018-04-01

A new custom-designed ultrahigh vacuum (UHV) chamber coupled to a UHV and atmospheric-pressure-compatible spectroscopic and catalytic reaction cell is described, which allows us to perform IR-vis sum frequency generation (SFG) vibrational spectroscopy during catalytic (kinetic) measurements. SFG spectroscopy is an exceptional tool to study vibrational properties of surface adsorbates under operando conditions, close to those of technical catalysis. This versatile setup allows performing surface science, SFG spectroscopy, catalysis, and electrochemical investigations on model systems, including single crystals, thin films, and deposited metal nanoparticles, under well-controlled conditions of gas composition, pressure, temperature, and potential. The UHV chamber enables us to prepare the model catalysts and to analyze their surface structure and composition by low energy electron diffraction and Auger electron spectroscopy, respectively. Thereafter, a sample transfer mechanism moves samples under UHV to the spectroscopic cell, avoiding air exposure. In the catalytic cell, SFG spectroscopy and catalytic tests (reactant/product analysis by mass spectrometry or gas chromatography) are performed simultaneously. A dedicated sample manipulation stage allows the model catalysts to be examined from LN2 temperature to 1273 K, with gaseous reactants in a pressure range from UHV to atmospheric. For post-reaction analysis, the SFG cell is rapidly evacuated and samples are transferred back to the UHV chamber. The capabilities of this new setup are demonstrated by benchmark results of CO adsorption on Pt and Pd(111) single crystal surfaces and of CO adsorption and oxidation on a ZrO2 supported Pt nanoparticle model catalyst grown by atomic layer deposition.

Total internal reflection sum-frequency generation spectroscopy and dense gold nanoparticles monolayer: a route for probing adsorbed molecules

International Nuclear Information System (INIS)

Tourillon, Gerard; Dreesen, Laurent; Volcke, Cedric; Sartenaer, Yannick; Thiry, Paul A; Peremans, Andre

2007-01-01

We show that sum-frequency generation spectroscopy performed in the total internal reflection configuration (TIR-SFG) combined with a dense gold nanoparticles monolayer allows us to study, with an excellent signal to noise ratio and high signal to background ratio, the conformation of adsorbed molecules. Dodecanethiol (DDT) was used as probe molecules in order to assess the potentialities of the approach. An enhancement of more than one order of magnitude of the SFG signals arising from the adsorbed species is observed with the TIR geometry compared to the external reflection one while the SFG non-resonant contribution remains the same for both configurations. Although further work is required to fully understand the origin of the SFG process on nanoparticles, our work opens new possibilities for studying nanostructures

Implementation of bright six-partite entanglement by coupled intracavity sum frequency generation

Science.gov (United States)

Wang, Junfeng; Liu, Le; Liu, Yuzhu; Zhang, Yanan; Wu, Hongyan; Gong, Chengxuan; Zhang, Ruofan; Zhang, Houyuan; Fan, JingYu

2018-04-01

Bright six-partite continuous-variable (CV) entanglement generated by the coupled intracavity sum frequency generation is investigated. The entanglement characteristics of reflected pump fields and the output sum frequency fields are discussed theoretically in symmetric and asymmetric cases by applying van Loock and Furusawa criteria for multipartite CV entanglement. Such compact tunable multipartite CV entanglement, generated from an experimentally feasible coupled system, could be used in integrated quantum communication and networks.

Adding a dimension to the infrared spectra of interfaces using heterodyne detected 2D sum-frequency generation (HD 2D SFG) spectroscopy.

Science.gov (United States)

Xiong, Wei; Laaser, Jennifer E; Mehlenbacher, Randy D; Zanni, Martin T

2011-12-27

In the last ten years, two-dimensional infrared spectroscopy has become an important technique for studying molecular structures and dynamics. We report the implementation of heterodyne detected two-dimensional sum-frequency generation (HD 2D SFG) spectroscopy, which is the analog of 2D infrared (2D IR) spectroscopy, but is selective to noncentrosymmetric systems such as interfaces. We implement the technique using mid-IR pulse shaping, which enables rapid scanning, phase cycling, and automatic phasing. Absorptive spectra are obtained, that have the highest frequency resolution possible, from which we extract the rephasing and nonrephasing signals that are sometimes preferred. Using this technique, we measure the vibrational mode of CO adsorbed on a polycrystalline Pt surface. The 2D spectrum reveals a significant inhomogenous contribution to the spectral line shape, which is quantified by simulations. This observation indicates that the surface conformation and environment of CO molecules is more complicated than the simple "atop" configuration assumed in previous work. Our method can be straightforwardly incorporated into many existing SFG spectrometers. The technique enables one to quantify inhomogeneity, vibrational couplings, spectral diffusion, chemical exchange, and many other properties analogous to 2D IR spectroscopy, but specifically for interfaces.

Toward a simple molecular understanding of sum frequency generation at air-water interfaces

Energy Technology Data Exchange (ETDEWEB)

Noah-Vanhoucke, Joyce; Smith, Jared D.; Geissler, Phillip L.

2009-01-13

Second-order vibrational spectroscopies successfully isolate signals from interfaces, but they report on intermolecular structure in a complicated and indirect way. Here we adapt a perspective on vibrational response developed for bulk spectroscopies to explore the microscopic fluctuations to which sum frequency generation (SFG), a popular surface-specific measurement, is most sensitive. We focus exclusively on inhomogeneous broadening of spectral susceptibilities for OH stretching of HOD as a dilute solute in D{sub 2}O. Exploiting a simple connection between vibrational frequency shifts and an electric field variable, we identify several functions of molecular orientation whose averages govern SFG. The frequency-dependence of these quantities is well captured by a pair of averages, involving alignment of OH and OD bonds with the surface normal at corresponding values of the electric field. The approximate form we obtain for SFG susceptibility highlights a dramatic sensitivity to the way a simulated liquid slab is partitioned for calculating second-order response.

Theoretical vibrational sum-frequency generation spectroscopy of water near lipid and surfactant monolayer interfaces

Energy Technology Data Exchange (ETDEWEB)

Roy, S.; Gruenbaum, S. M.; Skinner, J. L. [Theoretical Chemistry Institute and Department of Chemistry, 1101 University Ave., University of Wisconsin-Madison, Madison, Wisconsin 53706 (United States)

2014-11-14

Understanding the structure of water near cell membranes is crucial for characterizing water-mediated events such as molecular transport. To obtain structural information of water near a membrane, it is useful to have a surface-selective technique that can probe only interfacial water molecules. One such technique is vibrational sum-frequency generation (VSFG) spectroscopy. As model systems for studying membrane headgroup/water interactions, in this paper we consider lipid and surfactant monolayers on water. We adopt a theoretical approach combining molecular dynamics simulations and phase-sensitive VSFG to investigate water structure near these interfaces. Our simulated spectra are in qualitative agreement with experiments and reveal orientational ordering of interfacial water molecules near cationic, anionic, and zwitterionic interfaces. OH bonds of water molecules point toward an anionic interface leading to a positive VSFG peak, whereas the water hydrogen atoms point away from a cationic interface leading to a negative VSFG peak. Coexistence of these two interfacial water species is observed near interfaces between water and mixtures of cationic and anionic lipids, as indicated by the presence of both negative and positive peaks in their VSFG spectra. In the case of a zwitterionic interface, OH orientation is toward the interface on the average, resulting in a positive VSFG peak.

Sum frequency generation image reconstruction: Aliphatic membrane under spherical cap geometry

Energy Technology Data Exchange (ETDEWEB)

Volkov, Victor [Bereozovaya 2A, Konstantinovo, Moscow Region 140207 (Russian Federation)

2014-10-07

The article explores an opportunity to approach structural properties of phospholipid membranes using Sum Frequency Generation microscopy. To establish the principles of sum frequency generation image reconstruction in such systems, at first approach, we may adopt an idealistic spherical cap uniform assembly of hydrocarbon molecules. Quantum mechanical studies for decanoic acid (used here as a representative molecular system) provide necessary information on transition dipole moments and Raman tensors of the normal modes specific to methyl terminal – a typical moiety in aliphatic (and phospholipid) membranes. Relative degree of localization and frequencies of the normal modes of methyl terminals make nonlinearities of this moiety to be promising in structural analysis using Sum Frequency Generation imaging. Accordingly, the article describes derivations of relevant macroscopic nonlinearities and suggests a mapping procedure to translate amplitudes of the nonlinearities onto microscopy image plane according to geometry of spherical assembly, local molecular orientation, and optical geometry. Reconstructed images indicate a possibility to extract local curvature of bilayer envelopes of spherical character. This may have practical implications for structural extractions in membrane systems of practical relevance.

Sum frequency generation spectroscopy of tetraalkylphosphonium ionic liquids at the air-liquid interface

Science.gov (United States)

Peñalber-Johnstone, Chariz; Adamová, Gabriela; Plechkova, Natalia V.; Bahrami, Maryam; Ghaed-Sharaf, Tahereh; Ghatee, Mohammad Hadi; Seddon, Kenneth R.; Baldelli, Steven

2018-05-01

Sum frequency generation (SFG) spectroscopy is a nonlinear vibrational spectroscopic technique used in the study of interfaces, due to its unique ability to distinguish surface molecules that have preferential ordering compared to the isotropic bulk. Here, a series of alkyltrioctylphosphonium chloride ionic liquids, systematically varied by cation structure, were characterized at the air-liquid interface by SFG. The effect on surface structure resulting from molecular variation (i.e., addition of cyano- and methoxy-functional groups) of the cation alkyl chain was investigated. SFG spectra in the C—H stretching region (2750-3100 cm-1) for [P8 8 8 n][Cl], where n = 4, 5, 8, 10, 12, or 14, showed characteristic changes as the alkyl chain length was increased. Spectral profiles for n = 4, 5, 8, or 10 appeared similar; however, when the fourth alkyl chain was sufficiently long (as in the case of n = 12 or n = 14), abrupt changes occurred in the spectra. Molecular dynamics (MD) simulation of a slab of each ionic liquid (with n = 8, 10, or 12) confirmed gauche defects, with enhancement for the long alkyl chain and an abrupt increase of gauche occurrence from n = 8 to n = 10. A comparison of the tilt angle distribution from the simulation and the SFG analysis show a broad distribution of angles. Using experimental SFG spectra in conjunction with MD simulations, a comprehensive molecular picture at the surface of this unique class of liquids is presented.

Sum Frequency Generation Vibrational Spectroscopy of Colloidal Platinum Nanoparticle Catalysts: Disordering versus Removal of Organic Capping

KAUST Repository

Krier, James M.

2012-08-23

Recent work with nanoparticle catalysts shows that size and shape control on the nanometer scale influences reaction rate and selectivity. Sum frequency generation (SFG) vibrational spectroscopy is a powerful tool for studying heterogeneous catalysis because it enables the observation of surface intermediates during catalytic reactions. To control the size and shape of catalytic nanoparticles, an organic ligand was used as a capping agent to stabilize nanoparticles during synthesis. However, the presence of an organic capping agent presents two major challenges in SFG and catalytic reaction studies: it blocks a significant fraction of active surface sites and produces a strong signal that prevents the detection of reaction intermediates with SFG. Two methods for cleaning Pt nanoparticles capped with poly (vinylpyrrolidone) (PVP) are examined in this study: solvent cleaning and UV cleaning. Solvent cleaning leaves more PVP intact and relies on disordering with hydrogen gas to reduce the SFG signal of PVP. In contrast, UV cleaning depends on nearly complete removal of PVP to reduce SFG signal. Both UV and solvent cleaning enable the detection of reaction intermediates by SFG. However, solvent cleaning also yields nanoparticles that are stable under reaction conditions, whereas UV cleaning results in aggregation during reaction. The results of this study indicate that solvent cleaning is more advantageous for studying the effects of nanoparticle size and shape on catalytic selectivity by SFG vibrational spectroscopy. © 2012 American Chemical Society.

Highly efficient single-pass sum frequency generation by cascaded nonlinear crystals

DEFF Research Database (Denmark)

Hansen, Anders Kragh; Andersen, Peter E.; Jensen, Ole Bjarlin

2015-01-01

, despite differences in the phase relations of the involved fields. An unprecedented 5.5 W of continuous-wave diffraction-limited green light is generated from the single-pass sum frequency mixing of two diode lasers in two periodically poled nonlinear crystals (conversion efficiency 50%). The technique......The cascading of nonlinear crystals has been established as a simple method to greatly increase the conversion efficiency of single-pass second-harmonic generation compared to a single-crystal scheme. Here, we show for the first time that the technique can be extended to sum frequency generation...... is generally applicable and can be applied to any combination of fundamental wavelengths and nonlinear crystals....

Catalyzed hydrogenation of nitrogen and ethylene on metal (Fe, Pt) single crystal surfaces and effects of coadsorption: A sum frequency generation vibrational spectroscopy study

Energy Technology Data Exchange (ETDEWEB)

Westerberg, Staffan Per Gustav [Univ. of California, Berkeley, CA (United States)

2004-01-01

High-pressure catalytic reactions and associated processes, such as adsorption have been studied on a molecular level on single crystal surfaces. Sum Frequency Generation (SFG) vibrational spectroscopy together with Auger Electron Spectroscopy (AES), Temperature Programmed Desorption (TPD) and Gas Chromatography (GC) were used to investigate the nature of species on catalytic surfaces and to measure the catalytic reaction rates. Special attention has been directed at studying high-pressure reactions and in particular, ammonia synthesis in order to identify reaction intermediates and the influence of adsorbates on the surface during reaction conditions. The adsorption of gases N₂, H₂, O₂ and NH₃ that play a role in ammonia synthesis have been studied on the Fe(111) crystal surface by sum frequency generation vibrational spectroscopy using an integrated Ultra-High Vacuum (UHV)/high-pressure system. SFG spectra are presented for the dissociation intermediates, NH₂ (~3325 cm^-1) and NH (~3235 cm^-1) under high pressure of ammonia (200 Torr) on the clean Fe(111) surface. Addition of 0.5 Torr of oxygen to 200 Torr of ammonia does not significantly change the bonding of dissociation intermediates to the surface. However, it leads to a phase change of nearly 180° between the resonant and non-resonant second order non-linear susceptibility of the surface, demonstrated by the reversal of the SFG spectral features. Heating the surface in the presence of 200 Torr ammonia and 0.5 Torr oxygen reduces the oxygen coverage, which can be seen from the SFG spectra as another relative phase change of 180°. The reduction of the oxide is also supported by Auger electron spectroscopy. The result suggests that the phase change of the spectral features could serve as a sensitive indicator of the chemical environment of the adsorbates.

Water Orientation at Ceramide/Water Interfaces Studied by Heterodyne-Detected Vibrational Sum Frequency Generation Spectroscopy and Molecular Dynamics Simulation

KAUST Repository

Adhikari, Aniruddha

2016-10-10

Lipid/water interaction is essential for many biological processes. The water structure at the nonionic lipid interface remains little known, and there is no scope of a priori prediction of water orientation at nonionic interfaces, either. Here, we report our study combining advanced nonlinear spectroscopy and molecular dynamics simulation on the water orientation at the ceramide/water interface. We measured χ spectrum in the OH stretch region of ceramide/isotopically diluted water interface using heterodyne-detected vibrational sum-frequency generation spectroscopy and found that the interfacial water prefers an overall hydrogen-up orientation. Molecular dynamics simulation indicates that this preferred hydrogen-up orientation of water is determined by a delicate balance between hydrogen-up and hydrogen-down orientation induced by lipid-water and intralipid hydrogen bonds. This mechanism also suggests that water orientation at neutral lipid interfaces depends highly on the chemical structure of the lipid headgroup, in contrast to the charged lipid interfaces where the net water orientation is determined solely by the charge of the lipid headgroup.

Sum-Frequency-Generation-Based Laser Sidebands for Tunable Femtosecond Raman Spectroscopy in the Ultraviolet

Directory of Open Access Journals (Sweden)

Liangdong Zhu

2015-04-01

Full Text Available Femtosecond stimulated Raman spectroscopy (FSRS is an emerging molecular structural dynamics technique for functional materials characterization typically in the visible to near-IR range. To expand its applications we have developed a versatile FSRS setup in the ultraviolet region. We use the combination of a narrowband, ~400 nm Raman pump from a home-built second harmonic bandwidth compressor and a tunable broadband probe pulse from sum-frequency-generation-based cascaded four-wave mixing (SFG-CFWM laser sidebands in a thin BBO crystal. The ground state Raman spectrum of a laser dye Quinolon 390 in methanol that strongly absorbs at ~355 nm is systematically studied as a standard sample to provide previously unavailable spectroscopic characterization in the vibrational domain. Both the Stokes and anti-Stokes Raman spectra can be collected by selecting different orders of SFG-CFWM sidebands as the probe pulse. The stimulated Raman gain with the 402 nm Raman pump is >21 times larger than that with the 550 nm Raman pump when measured at the 1317 cm−1 peak for the aromatic ring deformation and ring-H rocking mode of the dye molecule, demonstrating that pre-resonance enhancement is effectively achieved in the unique UV-FSRS setup. This added tunability in the versatile and compact optical setup enables FSRS to better capture transient conformational snapshots of photosensitive molecules that absorb in the UV range.

Sum frequency and second harmonic generation from the surface of a liquid microjet

International Nuclear Information System (INIS)

Smolentsev, Nikolay; Chen, Yixing; Roke, Sylvie; Jena, Kailash C.; Brown, Matthew A.

2014-01-01

The use of a liquid microjet as a possible source of interest for Second Harmonic Generation (SHG) and Sum Frequency Generation (SFG) spectroscopy is examined. We measured non-resonant SHG scattering patterns from the air/water interface of a microjet of pure water and observe a strong enhancement of the SHG signal for certain scattering angles. These enhancements can be explained by the optical properties and the shape of the liquid microjet. SFG experiments at the surface of a liquid microjet of ethanol in air show that it is also possible to measure the coherent vibrational SFG spectrum of the ethanol/air interface in this way. Our findings are useful for future far-UV or X-ray based nonlinear optical surface experiments on liquid jets. In addition, combined X-ray photoelectron spectroscopy and SHG/SFG measurements are feasible, which will be very useful in improving our understanding of the molecular foundations of electrostatic and chemical surface properties and phenomena

Sum frequency and second harmonic generation from the surface of a liquid microjet

Energy Technology Data Exchange (ETDEWEB)

Smolentsev, Nikolay; Chen, Yixing; Roke, Sylvie, E-mail: sylvie.roke@epfl.ch [Laboratory for Fundamental Biophotonics (LBP), Institute of Bioengineering (IBI), School of Engineering STI, École Polytechnique Fédérale de Lausanne EPFL, 1015 Lausanne (Switzerland); Jena, Kailash C. [Laboratory for Fundamental Biophotonics (LBP), Institute of Bioengineering (IBI), School of Engineering STI, École Polytechnique Fédérale de Lausanne EPFL, 1015 Lausanne (Switzerland); Department of Physics, Indian Institute of Technology Ropar, Rupnagar, 140001 (India); Brown, Matthew A. [Laboratory for Surface Science and Technology, Department of Materials, ETH Zürich, CH-8093 Zurich (Switzerland)

2014-11-14

The use of a liquid microjet as a possible source of interest for Second Harmonic Generation (SHG) and Sum Frequency Generation (SFG) spectroscopy is examined. We measured non-resonant SHG scattering patterns from the air/water interface of a microjet of pure water and observe a strong enhancement of the SHG signal for certain scattering angles. These enhancements can be explained by the optical properties and the shape of the liquid microjet. SFG experiments at the surface of a liquid microjet of ethanol in air show that it is also possible to measure the coherent vibrational SFG spectrum of the ethanol/air interface in this way. Our findings are useful for future far-UV or X-ray based nonlinear optical surface experiments on liquid jets. In addition, combined X-ray photoelectron spectroscopy and SHG/SFG measurements are feasible, which will be very useful in improving our understanding of the molecular foundations of electrostatic and chemical surface properties and phenomena.

Sum frequency and second harmonic generation from the surface of a liquid microjet

Science.gov (United States)

Smolentsev, Nikolay; Chen, Yixing; Jena, Kailash C.; Brown, Matthew A.; Roke, Sylvie

2014-11-01

The use of a liquid microjet as a possible source of interest for Second Harmonic Generation (SHG) and Sum Frequency Generation (SFG) spectroscopy is examined. We measured non-resonant SHG scattering patterns from the air/water interface of a microjet of pure water and observe a strong enhancement of the SHG signal for certain scattering angles. These enhancements can be explained by the optical properties and the shape of the liquid microjet. SFG experiments at the surface of a liquid microjet of ethanol in air show that it is also possible to measure the coherent vibrational SFG spectrum of the ethanol/air interface in this way. Our findings are useful for future far-UV or X-ray based nonlinear optical surface experiments on liquid jets. In addition, combined X-ray photoelectron spectroscopy and SHG/SFG measurements are feasible, which will be very useful in improving our understanding of the molecular foundations of electrostatic and chemical surface properties and phenomena.

Singly-resonant sum frequency generation of visible light in a semiconductor disk laser

DEFF Research Database (Denmark)

Andersen, Martin Thalbitzer; Schlosser, P.J.; Hastie, J.E.

2009-01-01

In this paper a generic approach for visible light generation is presented. It is based on sum frequency generation between a semiconductor disk laser and a solid-state laser, where the frequency mixing is achieved within the cavity of the semiconductor disk laser using a singlepass of the solid......-state laser light. This exploits the good beam quality and high intra-cavity power present in the semiconductor disk laser to achieve high conversion efficiency. Combining sum frequency mixing and semiconductor disk lasers in this manner allows in principle for generation of any wavelength within the visible...

Intrinsic Chirality and Prochirality at Air/R-(+)- and S-(-)-Limonene Interfaces: Spectral Signatures with Interference Chiral Sum-Frequency Generation Vibrational Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Fu, Li; Zhang, Yun; Wei, Zhehao; Wang, Hongfei

2014-06-04

We report in this work detailed measurements on the chiral and achiral sum-frequency vibrational spectra in the C-H stretching vibration region (2800-3050cm-1) of the air/liquid interfaces of R-limonene and S-limonene, using the recently developed high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS). The achiral SFG spectra of R-limonene and S-limonene, as well as the equal amount (50/50) racemic mixture show that the enantiomers are with the same interfacial orientations. The interference chiral SFG spectra of the limonene enantiomers exhibit spectral signature from chiral response of the Cα-H stretching mode, and spectral signature from prochiral response of the CH2 asymmetric stretching mode, respectively. The chiral spectral feature of the Cα-H stretching mode changes sign from R-limonene to S-limonene, and disappears for the 50/50 racemic mixture. While the prochiral spectral feature of the CH2 asymmetric stretching mode is the same for R-limonene and S-limonene, and also surprisingly remains the same for the 50/50 racemic mixture. These results provided detail information in understanding the structure and chirality of molecular interfaces, and demonstrated the sensitivity and potential of SFG-VS as unique spectroscopic tool for chirality characterization and chiral recognition at the molecular interface.

Sum Frequency Generation Vibrational Spectroscopy of Adsorbed Amino Acids, Peptides and Proteins of Hydrophilic and Hydrophobic Solid-Water Interfaces

Energy Technology Data Exchange (ETDEWEB)

Holinga IV, George Joseph [Univ. of California, Berkeley, CA (United States)

2010-09-01

Sum frequency generation (SFG) vibrational spectroscopy was used to investigate the interfacial properties of several amino acids, peptides, and proteins adsorbed at the hydrophilic polystyrene solid-liquid and the hydrophobic silica solid-liquid interfaces. The influence of experimental geometry on the sensitivity and resolution of the SFG vibrational spectroscopy technique was investigated both theoretically and experimentally. SFG was implemented to investigate the adsorption and organization of eight individual amino acids at model hydrophilic and hydrophobic surfaces under physiological conditions. Biointerface studies were conducted using a combination of SFG and quartz crystal microbalance (QCM) comparing the interfacial structure and concentration of two amino acids and their corresponding homopeptides at two model liquid-solid interfaces as a function of their concentration in aqueous solutions. The influence of temperature, concentration, equilibration time, and electrical bias on the extent of adsorption and interfacial structure of biomolecules were explored at the liquid-solid interface via QCM and SFG. QCM was utilized to quantify the biological activity of heparin functionalized surfaces. A novel optical parametric amplifier was developed and utilized in SFG experiments to investigate the secondary structure of an adsorbed model peptide at the solid-liquid interface.

Single-frequency blue light generation by single-pass sum-frequency generation in a coupled ring cavity tapered laser

DEFF Research Database (Denmark)

Jensen, Ole Bjarlin; Petersen, Paul Michael

2013-01-01

A generic approach for generation of tunable single frequency light is presented. 340 mW of near diffraction limited, single-frequency, and tunable blue light around 459 nm is generated by sum-frequency generation (SFG) between two tunable tapered diode lasers. One diode laser is operated in a ring...... cavity and another tapered diode laser is single-passed through a nonlinear crystal which is contained in the coupled ring cavity. Using this method, the single-pass conversion efficiency is more than 25%. In contrast to SFG in an external cavity, the system is entirely self-stabilized with no electronic...

Low energy electron diffraction (LEED) and sum frequency generation (SFG) vibrational spectroscopy studies of solid-vacuum, solid-air and solid-liquid interfaces

Energy Technology Data Exchange (ETDEWEB)

Hoffer, Saskia [Univ. of California, Berkeley, CA (United States)

2002-01-01

Electron based surface probing techniques can provide detailed information about surface structure or chemical composition in vacuum environments. The development of new surface techniques has made possible in situ molecular level studies of solid-gas interfaces and more recently, solid-liquid interfaces. The aim of this dissertation is two-fold. First, by using novel sample preparation, Low Energy Electron Diffraction (LEED) and other traditional ultra high vacuum (UHV) techniques are shown to provide new information on the insulator/vacuum interface. The surface structure of the classic insulator NaCl has been determined using these methods. Second, using sum frequency generation (SFG) surface specific vibrational spectroscopy studies were performed on both the biopolymer/air and electrode/electrolyte interfaces. The surface structure and composition of polyetherurethane-silicone copolymers were determined in air using SFG, atomic force microscopy (AFM), and X-ray photoelectron spectroscopy (XPS). SFG studies of the electrode (platinum, gold and copper)/electrolyte interface were performed as a function of applied potential in an electrochemical cell.

Self-assembled organic monolayers on gold nanoparticles: A study by sum-frequency generation combined with UV-vis spectroscopy

International Nuclear Information System (INIS)

Humbert, C.; Busson, B.; Abid, J.-P.; Six, C.; Girault, H.H.; Tadjeddine, A.

2005-01-01

We use sum-frequency generation spectroscopy (SFG) in the infrared 2800-3000 cm -1 spectral range and UV-vis spectroscopy (transmission) in the 450-650 nm spectral range in order to characterize vibrational and electronic properties of various interfaces composed of organic monolayers adsorbed on gold nanoparticles (AuNPs) with 19 nm average diameter. SFG signal is observed for AuNPs films deposited on glass substrates using the following silane intermediates: 3-(aminopropyl) triethoxysilane and 3-(mercaptopropyl) trimethoxysilane. The density of AuNPs and their aggregates are measured with a scanning electron microscope. For the samples showing a strong well-defined surface plasmon resonance (SPR), we also observe an enhancement of their non-linear optical properties. Furthermore, the SFG measurements show that 1-dodecanethiol films are rather well ordered on specific AuNPs substrates. In this way, the presence of the SFG signal, which comes from both the bulk electronic s-d interband transition and the vibrational states of the adsorbed molecules, depends on a SPR process. This phenomenon is evidenced on the AuNPs by the incident visible beam located at 532 nm, i.e. near the SPR energy maximum of these interfaces. These results open the door to experiments involving macromolecular and biological materials networks deposited on ultrathin metal electrodes in a controlled electrochemical environment

Self-assembled organic monolayers on gold nanoparticles: A study by sum-frequency generation combined with UV-vis spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Humbert, C. [LURE, CNRS-UMR 130, Centre Universitaire Paris-Sud, Ba-hat t. 209D, B.P. 34, 91898 Orsay Cedex (France) and Laboratoire de Spectroscopie Moleculaire de Surface, University of Namur, 61 Rue de Bruxelles, B-5000 Namur (Belgium)]. E-mail: christophe.humbert@fundp.ac.be; Busson, B. [LURE, CNRS-UMR 130, Centre Universitaire Paris-Sud, Ba-hat t. 209D, B.P. 34, 91898 Orsay Cedex (France); Abid, J.-P. [Ecole Polytechnique Federale de Lausanne, Laboratoire d' Electrochimie Physique et Analytique, CH-1015 Lausanne (Switzerland); Six, C. [LURE, CNRS-UMR 130, Centre Universitaire Paris-Sud, Ba-hat t. 209D, B.P. 34, 91898 Orsay Cedex (France); Girault, H.H. [Ecole Polytechnique Federale de Lausanne, Laboratoire d' Electrochimie Physique et Analytique, CH-1015 Lausanne (Switzerland); Tadjeddine, A. [LURE, CNRS-UMR 130, Centre Universitaire Paris-Sud, Ba-hat t. 209D, B.P. 34, 91898 Orsay Cedex (France)

2005-05-20

We use sum-frequency generation spectroscopy (SFG) in the infrared 2800-3000 cm{sup -1} spectral range and UV-vis spectroscopy (transmission) in the 450-650 nm spectral range in order to characterize vibrational and electronic properties of various interfaces composed of organic monolayers adsorbed on gold nanoparticles (AuNPs) with 19 nm average diameter. SFG signal is observed for AuNPs films deposited on glass substrates using the following silane intermediates: 3-(aminopropyl) triethoxysilane and 3-(mercaptopropyl) trimethoxysilane. The density of AuNPs and their aggregates are measured with a scanning electron microscope. For the samples showing a strong well-defined surface plasmon resonance (SPR), we also observe an enhancement of their non-linear optical properties. Furthermore, the SFG measurements show that 1-dodecanethiol films are rather well ordered on specific AuNPs substrates. In this way, the presence of the SFG signal, which comes from both the bulk electronic s-d interband transition and the vibrational states of the adsorbed molecules, depends on a SPR process. This phenomenon is evidenced on the AuNPs by the incident visible beam located at 532 nm, i.e. near the SPR energy maximum of these interfaces. These results open the door to experiments involving macromolecular and biological materials networks deposited on ultrathin metal electrodes in a controlled electrochemical environment.

Sum-frequency nonlinear Cherenkov radiation generated on the boundary of bulk medium crystal.

Science.gov (United States)

Wang, Xiaojing; Cao, Jianjun; Zhao, Xiaohui; Zheng, Yuanlin; Ren, Huaijin; Deng, Xuewei; Chen, Xianfeng

2015-12-14

We demonstrated experimentally a method to generate the sum-frequency Nonlinear Cherenkov radiation (NCR) on the boundary of bulk medium by using two synchronized laser beam with wavelength of 1300 nm and 800 nm. It is also an evidence that the polarization wave is always confined to the boundary. Critical conditions of surface sum-frequency NCR under normal and anomalous dispersion condition is discussed.

Studies of Heterogeneously Catalyzed Liquid-Phase Alcohol Oxidation on Platinum bySum-frequency Generation Vibrational Spectroscopy and Reaction Rate Measurements

Energy Technology Data Exchange (ETDEWEB)

Thompson, Christopher [Univ. of California, Berkeley, CA (United States)

2014-05-15

Compared to many branches of chemistry, the molecular level study of catalytically active surfaces is young. Only with the invention of ultrahigh vacuum technology in the past half century has it been possible to carry out experiments that yield useful molecular information about the reactive occurrences at a surface. The reason is two-fold: low pressure is necessary to keep a surface clean for an amount of time long enough to perform an experiment, and most atomic scale techniques that are surface speci c (x-ray photoelectron spectroscopy, electron energy loss spectroscopy, Auger electron spectroscopy, etc.) cannot be used at ambient pressures, because electrons, which act as chemical probes in these techniques, are easily scattered by molecules. Sum-frequency generation (SFG) vibrational spectroscopy is one technique that can provide molecular level information from the surface without the necessity for high vacuum. Since the advent of SFG as a surface spectroscopic tool it has proved its worth in the studies of surface catalyzed reactions in the gas phase, with numerous reactions in the gas phase having been investigated on a multitude of surfaces. However, in situ SFG characterization of catalysis at the solid-liquid interface has yet to be thoroughly pursued despite the broad interest in the use of heterogeneous catalysts in the liquid phase as replacements for homogeneous counterparts. This work describes an attempt to move in that direction, applying SFG to study the solid-liquid interface under conditions of catalytic alcohol oxidation on platinum.

Sum-frequency generation echo and grating from interface

International Nuclear Information System (INIS)

Volkov, Victor

2014-01-01

The work addresses spectroscopy of fourth-order Sum Frequency Generation Echo and Grating responses as an experimental tool to study structure and dynamics at interfaces. First, it addresses experimental geometry to extract background-free fourth-order Echo and Grating responses. Further, the article provides the analytical expressions of the response functions for these nonlinearities. The derived expressions are used to model the χ (4) two-dimensional spectral responses of a hydrated methyl acetate, which resembles a hydrated carbonyl moiety at the polar outer side of a phospholipid membrane. Orientation, transition dipole moments, and Raman tensors are obtained from the results of classical and quantum calculations, respectively. The numerical studies for the nonlinear responses under different polarization schemes and timings suggest the possibility of securely factoring of spectral contributions of χ YYYZX and χ YYYZY macroscopic susceptibilities. As such, the nonlinearities provide an experimental perspective on orientation of a generic (low-symmetry) molecular system at interfaces. Besides, the spectral properties of the tensors may reflect correlations of the in-plane and out-of-plane field components specific to the interface. For the case of a phospholipid membrane, the experiment would address in-plane and out-of-plane anisotropy of hydrogen bonding and related dynamics

Sum-frequency generation echo and grating from interface

Energy Technology Data Exchange (ETDEWEB)

Volkov, Victor [Bereozovaya 2A, Konstantinovo, Moscow Region 140207 (Russian Federation)

2014-10-14

The work addresses spectroscopy of fourth-order Sum Frequency Generation Echo and Grating responses as an experimental tool to study structure and dynamics at interfaces. First, it addresses experimental geometry to extract background-free fourth-order Echo and Grating responses. Further, the article provides the analytical expressions of the response functions for these nonlinearities. The derived expressions are used to model the χ{sup (4)} two-dimensional spectral responses of a hydrated methyl acetate, which resembles a hydrated carbonyl moiety at the polar outer side of a phospholipid membrane. Orientation, transition dipole moments, and Raman tensors are obtained from the results of classical and quantum calculations, respectively. The numerical studies for the nonlinear responses under different polarization schemes and timings suggest the possibility of securely factoring of spectral contributions of χ{sub YYYZX} and χ{sub YYYZY} macroscopic susceptibilities. As such, the nonlinearities provide an experimental perspective on orientation of a generic (low-symmetry) molecular system at interfaces. Besides, the spectral properties of the tensors may reflect correlations of the in-plane and out-of-plane field components specific to the interface. For the case of a phospholipid membrane, the experiment would address in-plane and out-of-plane anisotropy of hydrogen bonding and related dynamics.

Structure and orientation of interfacial proteins determined by sum frequency generation vibrational spectroscopy: method and application.

Science.gov (United States)

Ye, Shuji; Wei, Feng; Li, Hongchun; Tian, Kangzhen; Luo, Yi

2013-01-01

In situ and real-time characterization of molecular structures and orientation of proteins at interfaces is essential to understand the nature of interfacial protein interaction. Such work will undoubtedly provide important clues to control biointerface in a desired manner. Sum frequency generation vibrational spectroscopy (SFG-VS) has been demonstrated to be a powerful technique to study the interfacial structures and interactions at the molecular level. This paper first systematically introduced the methods for the calculation of the Raman polarizability tensor, infrared transition dipole moment, and SFG molecular hyperpolarizability tensor elements of proteins/peptides with the secondary structures of α-helix, 310-helix, antiparallel β-sheet, and parallel β-sheet, as well as the methodology to determine the orientation of interfacial protein secondary structures using SFG amide I spectra. After that, recent progresses on the determination of protein structure and orientation at different interfaces by SFG-VS were then reviewed, which provides a molecular-level understanding of the structures and interactions of interfacial proteins, specially understanding the nature of driving force behind such interactions. Although this review has focused on analysis of amide I spectra, it will be expected to offer a basic idea for the spectral analysis of amide III SFG signals and other complicated molecular systems such as RNA and DNA. Copyright © 2013 Elsevier Inc. All rights reserved.

Sum Frequency Generation Vibrational Spectroscopy and Kinetic Study of 2-Methylfuran and 2,5-Dimethylfuran Hydrogenation over 7 nm Platinum Cubic Nanoparticles

KAUST Repository

Aliaga, Cesar

2011-04-28

Sum frequency generation vibrational spectroscopy and kinetic measurements obtained from gas chromatography were used to study the adsorption and hydrogenation of 2-methylfuran (MF) and 2,5-dimethylfuran (DMF) over cubic Pt nanoparticles of 7 nm average size, synthesized by colloidal methods and cleaned by ultraviolet light and ozone treatment. Reactions carried out at atmospheric pressure in the temperature range of 20-120 °C produced dihydro and tetrahydro species, as well as ring-opening products (alcohols) and ring-cracking products, showing high selectivity toward ring opening throughout the entire temperature range. The aromatic rings (MF and DMF) adsorbed parallel to the nanoparticle surface. Results yield insight into various surface reaction intermediates and the reason for the significantly lower selectivity for ring cracking in DMF hydrogenation compared to MF hydrogenation. © 2011 American Chemical Society.

Quantification of crystalline cellulose in lignocellulosic biomass using sum frequency generation (SFG) vibration spectroscopy and comparison with other analytical methods.

Science.gov (United States)

Barnette, Anna L; Lee, Christopher; Bradley, Laura C; Schreiner, Edward P; Park, Yong Bum; Shin, Heenae; Cosgrove, Daniel J; Park, Sunkyu; Kim, Seong H

2012-07-01

The non-centrosymmetry requirement of sum frequency generation (SFG) vibration spectroscopy allows the detection and quantification of crystalline cellulose in lignocellulose biomass without spectral interferences from hemicelluloses and lignin. This paper shows a correlation between the amount of crystalline cellulose in biomass and the SFG signal intensity. Model biomass samples were prepared by mixing commercially available cellulose, xylan, and lignin to defined concentrations. The SFG signal intensity was found sensitive to a wide range of crystallinity, but varied non-linearly with the mass fraction of cellulose in the samples. This might be due to the matrix effects such as light scattering and absorption by xylan and lignin, as well as the non-linear density dependence of the SFG process itself. Comparison with other techniques such as XRD, FT-Raman, FT-IR and NMR demonstrate that SFG can be a complementary and sensitive tool to assess crystalline cellulose in biomass. Copyright © 2012 Elsevier Ltd. All rights reserved.

Quantitative spectral and orientational analysis in surface sum frequency generation vibrational spectroscopy (SFG-VS)

Science.gov (United States)

Wang, Hong-Fei; Gan, Wei; Lu, Rong; Rao, Yi; Wu, Bao-Hua

Sum frequency generation vibrational spectroscopy (SFG-VS) has been proven to be a uniquely effective spectroscopic technique in the investigation of molecular structure and conformations, as well as the dynamics of molecular interfaces. However, the ability to apply SFG-VS to complex molecular interfaces has been limited by the ability to abstract quantitative information from SFG-VS experiments. In this review, we try to make assessments of the limitations, issues and techniques as well as methodologies in quantitative orientational and spectral analysis with SFG-VS. Based on these assessments, we also try to summarize recent developments in methodologies on quantitative orientational and spectral analysis in SFG-VS, and their applications to detailed analysis of SFG-VS data of various vapour/neat liquid interfaces. A rigorous formulation of the polarization null angle (PNA) method is given for accurate determination of the orientational parameter D = /, and comparison between the PNA method with the commonly used polarization intensity ratio (PIR) method is discussed. The polarization and incident angle dependencies of the SFG-VS intensity are also reviewed, in the light of how experimental arrangements can be optimized to effectively abstract crucial information from the SFG-VS experiments. The values and models of the local field factors in the molecular layers are discussed. In order to examine the validity and limitations of the bond polarizability derivative model, the general expressions for molecular hyperpolarizability tensors and their expression with the bond polarizability derivative model for C3v, C2v and C∞v molecular groups are given in the two appendixes. We show that the bond polarizability derivative model can quantitatively describe many aspects of the intensities observed in the SFG-VS spectrum of the vapour/neat liquid interfaces in different polarizations. Using the polarization analysis in SFG-VS, polarization selection rules or

Theoretical study of sum-frequency vibrational spectroscopy on limonene surface

International Nuclear Information System (INIS)

Zheng, Ren-Hui; Liu, Hao; Jing, Yuan-Yuan; Wang, Bo-Yang; Shi, Qiang; Wei, Wen-Mei

2014-01-01

By combining molecule dynamics (MD) simulation and quantum chemistry computation, we calculate the surface sum-frequency vibrational spectroscopy (SFVS) of R-limonene molecules at the gas-liquid interface for SSP, PPP, and SPS polarization combinations. The distributions of the Euler angles are obtained using MD simulation, the ψ-distribution is between isotropic and Gaussian. Instead of the MD distributions, different analytical distributions such as the δ-function, Gaussian and isotropic distributions are applied to simulate surface SFVS. We find that different distributions significantly affect the absolute SFVS intensity and also influence on relative SFVS intensity, and the δ-function distribution should be used with caution when the orientation distribution is broad. Furthermore, the reason that the SPS signal is weak in reflected arrangement is discussed

Theoretical study of sum-frequency vibrational spectroscopy on limonene surface

Energy Technology Data Exchange (ETDEWEB)

Zheng, Ren-Hui, E-mail: zrh@iccas.ac.cn; Liu, Hao; Jing, Yuan-Yuan; Wang, Bo-Yang; Shi, Qiang [Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, Beijing 100190 (China); Wei, Wen-Mei [Department of Chemistry, College of Basic Medicine, Anhui Medical University, Hefei, Anhui 230032 (China)

2014-03-14

By combining molecule dynamics (MD) simulation and quantum chemistry computation, we calculate the surface sum-frequency vibrational spectroscopy (SFVS) of R-limonene molecules at the gas-liquid interface for SSP, PPP, and SPS polarization combinations. The distributions of the Euler angles are obtained using MD simulation, the ψ-distribution is between isotropic and Gaussian. Instead of the MD distributions, different analytical distributions such as the δ-function, Gaussian and isotropic distributions are applied to simulate surface SFVS. We find that different distributions significantly affect the absolute SFVS intensity and also influence on relative SFVS intensity, and the δ-function distribution should be used with caution when the orientation distribution is broad. Furthermore, the reason that the SPS signal is weak in reflected arrangement is discussed.

Phase transition behaviors of the supported DPPC bilayer investigated by sum frequency generation (SFG) vibrational spectroscopy and atomic force microscopy (AFM).

Science.gov (United States)

Wu, Heng-Liang; Tong, Yujin; Peng, Qiling; Li, Na; Ye, Shen

2016-01-21

The phase transition behaviors of a supported bilayer of dipalmitoylphosphatidyl-choline (DPPC) have been systematically evaluated by in situ sum frequency generation (SFG) vibrational spectroscopy and atomic force microscopy (AFM). By using an asymmetric bilayer composed of per-deuterated and per-protonated monolayers, i.e., DPPC-d75/DPPC and a symmetric bilayer of DPPC/DPPC, we were able to probe the molecular structural changes during the phase transition process of the lipid bilayer by SFG spectroscopy. It was found that the DPPC bilayer is sequentially melted from the top (adjacent to the solution) to bottom leaflet (adjacent to the substrate) over a wide temperature range. The conformational ordering of the supported bilayer does not decrease (even slightly increases) during the phase transition process. The conformational defects in the bilayer can be removed after the complete melting process. The phase transition enthalpy for the bottom leaflet was found to be approximately three times greater than that for the top leaflet, indicating a strong interaction of the lipids with the substrate. The present SFG and AFM observations revealed similar temperature dependent profiles. Based on these results, the temperature-induced structural changes in the supported lipid bilayer during its phase transition process are discussed in comparison with previous studies.

Nanoscale chemical and mechanical characterization of thin films:sum frequency generation (SFG) vibrational spectroscopy at buriedinterfaces

Energy Technology Data Exchange (ETDEWEB)

Kweskin, Sasha Joseph [Univ. of California, Berkeley, CA (United States)

2006-01-01

Sum frequency generation (SFG) surface vibrational spectroscopy was used to characterize interfaces pertinent to current surface engineering applications, such as thin film polymers and novel catalysts. An array of advanced surface science techniques like scanning probe microscopy (SPM), x-ray photoelectron spectroscopy (XPS), gas chromatography (GC) and electron microscopy were used to obtain experimental measurements complementary to SFG data elucidating polymer and catalyst surface composition, surface structure, and surface mechanical behavior. Experiments reported in this dissertation concentrate on three fundamental questions: (1) How does the interfacial molecular structure differ from that of the bulk in real world applications? (2) How do differences in chemical environment affect interface composition or conformation? (3) How do these changes correlate to properties such as mechanical or catalytic performance? The density, surface energy and bonding at a solid interface dramatically alter the polymer configuration, physics and mechanical properties such as surface glass transition, adhesion and hardness. The enhanced sensitivity of SFG at the buried interface is applied to three systems: a series of acrylates under compression, the compositions and segregation behavior of binary polymer polyolefin blends, and the changes in surface structure of a hydrogel as a function of hydration. In addition, a catalytically active thin film of polymer coated nanoparticles is investigated to evaluate the efficacy of SFG to provide in situ information for catalytic reactions involving small mass adsorption and/or product development. Through the use of SFG, in situ total internal reflection (TIR) was used to increase the sensitivity of SFG and provide the necessary specificity to investigate interfaces of thin polymer films and nanostructures previously considered unfeasible. The dynamic nature of thin film surfaces is examined and it is found that the non

Support Effects in Catalysis Studied by in-situ Sum Frequency Generation Vibrational Spectroscopy and in-situ X-Ray Spectroscopies

Science.gov (United States)

Kennedy, Griffin John

Kinetic measurements are paired with in-situ spectroscopic characterization tools to investigate colloidally based, supported Pt catalytic model systems in order to elucidate the mechanisms by which metal and support work in tandem to dictate activity and selectivity. The results demonstrate oxide support materials, while inactive in absence of Pt nanoparticles, possess unique active sites for the selective conversion of gas phase molecules when paired with an active metal catalyst. In order to establish a paradigm for metal-support interactions using colloidally synthesized Pt nanoparticles the ability of the organic capping agent to inhibit reactivity and interaction with the support must first be assessed. Pt nanoparticles capped by poly(vinylpyrrolidone) (PVP), and those from which the PVP is removed by UV light exposure, are investigated for two reactions, the hydrogenation of ethylene and the oxidation of methanol. It is shown that prior to PVP removal the particles are moderately active for both reactions. Following removal, the activity for the two reactions diverges, the ethylene hydrogenation rate increases 10-fold, while the methanol oxidation rate decreases 3-fold. To better understand this effect the capping agent prior to, and the residual carbon remaining after UV treatment are probed by sum frequency generation vibrational spectroscopy. Prior to removal no major differences are observed when the particles are exposed to alternating H2 and O2 environments. When the PVP is removed, carbonaceous fragments remain on the surface that dynamically restructure in H2 and O2. These fragments create a tightly bound shell in an oxygen environment and a porous coating of hydrogenated carbon in the hydrogen environment. Reaction rate measurements of thermally cleaned PVP and oleic acid capped particles show this effect to be independent of cleaning method or capping agent. In all this demonstrates the ability of the capping agent to mediate nanoparticle catalysis

Sum frequency generation vibrational spectroscopy (SFG-VS) for complex molecular surfaces and interfaces: Spectral lineshape measurement and analysis plus some controversial issues

Science.gov (United States)

Wang, Hong-Fei

2016-12-01

Sum-frequency generation vibrational spectroscopy (SFG-VS) was first developed in the 1980s and it has been proven a uniquely sensitive and surface/interface selective spectroscopic probe for characterization of the structure, conformation and dynamics of molecular surfaces and interfaces. In recent years, there have been many progresses in the development of methodology and instrumentation in the SFG-VS toolbox that have significantly broadened the application to complex molecular surfaces and interfaces. In this review, after presenting a unified view on the theory and methodology focusing on the SFG-VS spectral lineshape, as well as the new opportunities in SFG-VS applications with such developments, some of the controversial issues that have been puzzling the community are discussed. The aim of this review is to present to the researchers and students interested in molecular surfaces and interfacial sciences up-to-date perspectives complementary to the existing textbooks and reviews on SFG-VS.

Synthesis and characterization of aromatic self-assembled monolayers containing methylene and ethyleneglycol entities by means of sum-frequency generation spectroscopy

International Nuclear Information System (INIS)

Dreesen, L.; Sartenaer, Y.; Peremans, A.; Thiry, P.A.; Humbert, C.; Grugier, J.; Marchand-Brynaert, J.

2006-01-01

We use infrared-visible sum-frequency generation (SFG) spectroscopy in order to investigate the adsorption properties on Pt(111) of molecules having CH 3 -C 6 H 4 -(O-CH 2 -CH 2 ) n -O-(CH 2 ) m -SH as general chemical formula. We synthesized three molecules defined by the values m = 5 n = 4, m = 11 n = 4, m = 11 n = 8 and characterized them by Nuclear Magnetic Resonance spectroscopy. Thanks to spectroscopic measurements, we show that these molecules build self-assembled monolayers on Pt(111). First, the weak SFG signals arising from the ad-layer indicate low order and surface coverage of the substrate by these molecules. Next, the vibrational fingerprints of the aforementioned molecules are determined between 2825 and 3125 cm - 1 and the observed SFG spectral features are ascribed on the basis of the analysis of shorter and simpler molecules (1-dodecanethiol, 4-methylbenzenethiol and CH 3 -C 6 H 4 -O-(CH 2 ) 11 -SH) also adsorbed on Pt(111). The occurrence of methylene vibration modes indicates a significant amount of chain defects whatever the n and m numbers are. Finally, the identification of a particular vibration mode, characteristic of the aromatic ring, enables us to qualitatively discuss the effect of the number of methylene and ethylene glycol entities on its orientation. More precisely, higher these numbers, more tilted (with respect to the substrate normal) the aromatic ring plane is

Intrinsic chirality and prochirality at Air/R-(+)- and S-(-)-limonene interfaces: spectral signatures with interference chiral sum-frequency generation vibrational spectroscopy.

Science.gov (United States)

Fu, Li; Zhang, Yun; Wei, Zhe-Hao; Wang, Hong-Fei

2014-09-01

We report in this work detailed measurements of the chiral and achiral sum-frequency vibrational spectra in the C-H stretching vibration region (2800-3050 cm(-1)) of the air/liquid interfaces of R-(+)-limonene and S-(-)-limonene, using the recently developed high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS). The achiral SFG spectra of R-limonene and S-limonene, as well as the RS racemic mixture (50/50 equal amount mixture), show that the corresponding molecular groups of the R and S enantiomers are with the same interfacial orientations. The interference chiral SFG spectra of the limonene enantiomers exhibit a spectral signature from the chiral response of the Cα-H stretching mode, and a spectral signature from the prochiral response of the CH(2) asymmetric stretching mode, respectively. The chiral spectral feature of the Cα-H stretching mode changes sign from R-(+)-limonene to S-(-)-limonene surfaces, and disappears for the RS racemic mixture surface. While the prochiral spectral feature of the CH(2) asymmetric stretching mode is the same for R-(+)-limonene and S-(-)-limonene surfaces, and also surprisingly remains the same for the RS racemic mixture surface. Therefore, the structures of the R-(+)-limonene and the S-(-)-limonene at the liquid interfaces are nevertheless not mirror images to each other, even though the corresponding groups have the same tilt angle from the interfacial normal, i.e., the R-(+)-limonene and the S-(-)-limonene at the surface are diastereomeric instead of enantiomeric. These results provide detailed information in understanding the structure and chirality of molecular interfaces and demonstrate the sensitivity and potential of SFG-VS as a unique spectroscopic tool for chirality characterization and chiral recognition at the molecular interface. © 2014 Wiley Periodicals, Inc.

Wetting effect on optical sum frequency generation (SFG) spectra of D-glucose, D-fructose, and sucrose

Science.gov (United States)

Hieu, Hoang Chi; Li, Hongyan; Miyauchi, Yoshihiro; Mizutani, Goro; Fujita, Naoko; Nakamura, Yasunori

2015-03-01

We report a sum frequency generation (SFG) spectroscopy study of D-glucose, D-fructose and sucrose in the Csbnd H stretching vibration regime. Wetting effect on the SFG spectra was investigated. The SFG spectrum of D-glucose changed from that of α-D-glucose into those of α-D-glucose monohydrate by wetting. The SFG spectra showed evidence of a small change of β-D-fructopyranose into other anomers by wetting. SFG spectra of sucrose did not change by wetting. Assignments of the vibrational peaks in the SFG spectra of the three sugars in the dry and wet states were performed in the Csbnd H stretching vibration region near 3000 cm-1.

Observation of sum-frequency-generation-induced cascaded four-wave mixing using two crossing femtosecond laser pulses in a 0.1 mm beta-barium-borate crystal.

Science.gov (United States)

Liu, Weimin; Zhu, Liangdong; Fang, Chong

2012-09-15

We demonstrate the simultaneous generation of multicolor femtosecond laser pulses spanning the wavelength range from UV to near IR in a 0.1 mm Type I beta-barium borate crystal from 800 nm fundamental and weak IR super-continuum white light (SCWL) pulses. The multicolor broadband laser pulses observed are attributed to two concomitant cascaded four-wave mixing (CFWM) processes as corroborated by calculation: (1) directly from the two incident laser pulses; (2) by the sum-frequency generation (SFG) induced CFWM process (SFGFWM). The latter signal arises from the interaction between the frequency-doubled fundamental pulse (400 nm) and the SFG pulse generated in between the fundamental and IR-SCWL pulses. The versatility and simplicity of this spatially dispersed multicolor self-compressed laser pulse generation offer compact and attractive methods to conduct femtosecond stimulated Raman spectroscopy and time-resolved multicolor spectroscopy.

Sum frequency generation of CO on (III) and polycrystalline platinum electrode surfaces: Evidence for SFG invisible surface CO

Energy Technology Data Exchange (ETDEWEB)

Baldelli, S.; Markovic, N.; Ross, P.; Shen, Y.R.; Somorjai, G.

1999-10-21

The vibrational spectroscopy sum frequency generation (SFG) is used to investigate the adsorption of carbon monoxide on the single crystal (111) and polycrystalline platinum surfaces. By varying the frequency and polarization of the light beams, different surface species of CO species are probed. SFG signal intensities for different polarization indicate that adsorbed CO polarizability is significantly perturbed from the gas-phase molecule. The SFG signal of CO disappears well below the main oxidation potential of CO to CO{sub 2}. The disappearance of the CO signal is interpreted as a transformation in the CO layer to a state which is invisible to SFG. The invisible state is suggested to be CO with the bond axis nearly parallel to the platinum surface.

Efficient generation of 509 nm light by sum-frequency mixing between two tapered diode lasers

DEFF Research Database (Denmark)

Tawfieq, Mahmoud; Jensen, Ole Bjarlin; Hansen, Anders Kragh

2015-01-01

We demonstrate a concept for visible laser sources based on sum-frequency generation of beam com- bined tapered diode lasers. In this specific case, a 1.7 W sum-frequency generated green laser at 509 nm is obtained, by frequency adding of 6.17 W from a 978 nm tapered diode laser with 8.06 W from...... a 1063 nm tapered diode laser, inside a periodically poled MgO doped lithium niobate crystal. This corresponds to an optical to optical conversion ef fi ciency of 12.1%. As an example of potential applica- tions, the generated nearly diffraction-limited green light is used for pumping a Ti:sapphire laser......, thus demonstrating good beam quality and power stability. The maximum output powers achieved when pumping the Ti:sapphire laser are 226 mW (CW) and 185 mW (mode-locked) at 1.7 W green pump power. The optical spectrum emitted by the mode-locked Ti:sapphire laser shows a spectral width of about 54 nm...

Correlation of molecular conformation with adhesion at AlOx/poly (ethylene terephthalate) interface studied by sum-frequency generation spectroscopy

International Nuclear Information System (INIS)

Miyamae, Takayuki; Nozoye, Hisakazu

2004-01-01

The interface between AlO x and poly(ethylene terephthalate) has been investigated by sum-frequency generation (SFG). A considerable improvement in adhesion strength was achieved by short time Ar plasma modification. The increase of the adhesion strength shows good correlation with the increase of the SFG peak strength. By depositing AlO x , the increase of SFG intensities and appearance of a new peak are observed, indicating the formation of a C=O···Al bond at the interface. Surface-modification and interfacial adhesion property are discussed

Efficient concept for generation of diffraction-limited green light by sum-frequency generation of spectrally combined tapered diode lasers

DEFF Research Database (Denmark)

Müller, André; Jensen, Ole Bjarlin; Hasler, Karl-Heinz

2012-01-01

In order to increase the power of visible diode laser systems in an efficient manner, we propose spectral beam combining with subsequent sum-frequency generation. We show that this approach, in comparison with second harmonic generation of single emitters, can enhance the available power signific......In order to increase the power of visible diode laser systems in an efficient manner, we propose spectral beam combining with subsequent sum-frequency generation. We show that this approach, in comparison with second harmonic generation of single emitters, can enhance the available power...... significantly. By combining two distributed Bragg reflector tapered diode lasers we achieve a 2.5–3.2 fold increase in power and a maximum of 3.9 W of diffraction-limited green light. At this power level, green diode laser systems have a high application potential, e.g., within the biomedical field. Our concept...

Sum frequency generation for studying plasma-wall interactions

International Nuclear Information System (INIS)

Roke, Sylvie

2010-01-01

Interaction of a plasma with a surface results in chemical and physical restructuring of the surface as well as the plasma in the vicinity of the surface. Studying such a reorganization of the atoms and molecules in the surface layer requires optical tools that can penetrate the plasma environment. At the same time, surface specificity is required. Sum Frequency Generation (SFG) is an optical method that fulfills these requirements. SFG has been developed into a surface specific probe during the eighties and nineties. Nowadays SFG is routinely applied in the research of complex interfaces. In such experiments, liquid/gas, solid/gas, solid/liquid, or liquid/liquid interfaces are probed, and the chemical surface composition, orientational distribution, order and chirality can be retrieved. An application to investigate plasma-wall interactions is feasible too.

Studies of Interfacial Regions by Sum-Frequency Generation with a Free-Electron Laser

NARCIS (Netherlands)

Eliel, E. R.; van der Ham, E. W. M.; Vrehen, Q. H. F.; Thooft, G. W.; Barmentlo, M.; Auerhammer, J. M.; van der Meer, A. F. G.; van Amersfoort, P. W.

1995-01-01

The use of a Free-Electron Laser (FEL) allows the study of (non)linear optical properties of materials over unsurpassed large spectral intervals. As an example, we report on the use of a FEL as the infrared source in spectroscopic infrared-visible Sum-Frequency Generation (SFG). Employing the

Cooperative Effects of Zwitterionic-Ionic Surfactant Mixtures on the Interfacial Water Structure Revealed by Sum Frequency Generation Vibrational Spectroscopy.

Science.gov (United States)

Pan, Xuecong; Yang, Fangyuan; Chen, Shunli; Zhu, Xuefeng; Wang, Chuanyi

2018-05-08

Cooperative effects of a series of equimolar binary zwitterionic-ionic surfactant mixtures on the interfacial water structure at the air-water interfaces have been studied by sum frequency generation vibrational spectroscopy (SFG-VS). For zwitterionic surfactant palmityl sulfobetaine (SNC 16 ), anionic surfactant sodium hexadecyl sulfate (SHS), and cationic surfactant cetyltrimethylammonium bromide (CTAB) with the same length of alkyl chain, significantly enhanced ordering of interfacial water molecules was observed for the zwitterionic-anionic surfactant mixtures SNC 16 -SHS, indicating that SNC 16 interacts more strongly with SHS than with CTAB because of the strong headgroup-headgroup electrostatic attraction for SNC 16 -SHS. Meanwhile, the SFG amplitude ratio of methyl and methylene symmetric stretching modes was used to verify the stronger interaction between SNC 16 and SHS. The conformational order indicator increased from 0.64 for SNC 16 to 7.17 for SNC 16 -SHS but only 0.94 for SNC 16 -CTAB. In addition, another anionic surfactant sodium dodecyl sulfate (SDS) was introduced to study the influence of chain-chain interaction. Decreased SFG amplitude of interfacial water molecules for SNC 16 -SDS was observed. Therefore, both the headgroup-headgroup electrostatic interaction and chain-chain van der Waals attractive interaction of the surfactants play an important role in enhancing the ordering of interfacial water molecules. The results provided experimental and theoretical bases for practical applications of the surfactants.

Sum-frequency generation spectroscopy on metals, oxides, and oxide-supported metal particles; Summenfrequenzerzeugungsspektroskopie an Metallen, Oxiden und oxidgetraegerten Metallpartikeln

Energy Technology Data Exchange (ETDEWEB)

Aumer, Andreas

2010-06-21

This thesis focuses on 4 different model systems of surface science. The experimental techniques used for the measurements include sum frequency generation (SFG), thermal desorption spectroscopy (TDS), low energy electron diffraction (LEED), Auger electron spectroscopy (AES), infrared adsorption spectrosocopy (IRAS) and scanning tunneling microscopy (STM). By using SFG, measurements could be performed up to a pressure of 50 mbar. The systems under investigation were: CO on Pt(111), water on Ag(001) and on MgO/Ag(001), CO on Au/MgO/Ag(001), and CO on Au-Pd/MgO/Ag(001). The system of CO on Pt(111) exhibits a two peak-pattern under certain pressure and temperature conditions which has not been studied so far. Various experiments helped to elucidate the origin of this distinct behaviour. The measurements of water on Ag(001) and MgO/Ag(001) show that on MgO, water first adsorbs as a monolayer with a following multilayer, whereas on Ag(001) it adsorbs as a multilayer from the beginning. The monolayer can be studied below the multilayer and some resonances can be identified. For the case of Au/MgO/Ag(001), STM shows that the growth mode of Au depends on the thickness of the supporting MgO film, which can not be seen with spectroscopic methods. For mixed Au-Pd particles on MgO/Ag(001) a clear difference in the adsorption behaviour between pure metal particles and mixed particles can be seen, which is explained by an interaction between these metals. Annealing the mixed particles to 600 K leads to a segregation of the metals, where the Au atoms diffuse to the shell and the Pd atoms make up the core. The results of all these measurements are discussed in the light of recent publications. (orig.)

Efficient yellow beam generation by intracavity sum frequency ...

Indian Academy of Sciences (India)

2014-02-06

Feb 6, 2014 ... petition leading to instability in the output sum frequency power and ... Nd:YVO4 crystal has been identified as one of the promising laser materials for diode ... very important to achieve small laser mode size as well as proper ...

Small Molecules and Sum Frequency Generation Probes of Nanoparticulate TiO2

Science.gov (United States)

Shultz, Mary Jane

2006-03-01

Anatase TiO2 is known to photo catalytically mineralize a wide variety of pollutants and pathogens, both airborne and in aqueous solution. One of the major benefits of basing water treatment systems on TiO2 is that it is environmentally benign and so non toxic that it is used as a colorant in creamy salad dressing. The primary impediment to wide spread implementation of a TiO2 based system for water decontamination is that the quantum efficiency in contact with condense phase water is less than 5%. Since the quantum efficiency for destruction of airborne materials is greater than 80%, the potential for increased efficiency is very real. To convert the potential to practice, the oxidation mechanism needs to be more fully understood. We will report on the results of using a nonlinear optical spectroscopy, sum frequency generation (SFG) as an in situ probe of interactions at the TiO2 surface. Results suggest that the dominant oxidation mechanism converts from a direct to an indirect mechanism as the water content (vapor pressure) increases. This presentation will discuss the probe technique as well as the results.

Two-dimensional sum-frequency generation (2D SFG) spectroscopy: summary of principles and its application to amyloid fiber monolayers.

Science.gov (United States)

Ghosh, Ayanjeet; Ho, Jia-Jung; Serrano, Arnaldo L; Skoff, David R; Zhang, Tianqi; Zanni, Martin T

2015-01-01

By adding a mid-infrared pulse shaper to a sum-frequency generation (SFG) spectrometer, we have built a 2D SFG spectrometer capable of measuring spectra analogous to 2D IR spectra but with monolayer sensitivity and SFG selection rules. In this paper, we describe the experimental apparatus and provide an introduction to 2D SFG spectroscopy to help the reader interpret 2D SFG spectra. The main aim of this manuscript is to report 2D SFG spectra of the amyloid forming peptide FGAIL. FGAIL is a critical segment of the human islet amyloid polypeptide (hIAPP or amylin) that aggregates in people with type 2 diabetes. FGAIL is catalyzed into amyloid fibers by many types of surfaces. Here, we study the structure of FGAIL upon deposition onto a gold surface covered with a self-assembled monolayer of methyl-4-mercaptobenzoate (MMB) that produces an ester coating. FGAIL deposited on bare gold does not form ordered layers. The measured 2D SFG spectrum is consistent with amyloid fiber formation, exhibiting both the parallel (a+) and perpendicular (a-) symmetry modes associated with amyloid β-sheets. Cross peaks are observed between the ester stretches of the coating and the FGAIL peptides. Simulations are presented for two possible structures of FGAIL amyloid β-sheets that illustrate the sensitivity of the 2D SFG spectra to structure and orientation. These results provide some of the first molecular insights into surface catalyzed amyloid fiber structure.

Elucidation of Compression-Induced Surface Crystallization in Amorphous Tablets Using Sum Frequency Generation (SFG) Microscopy.

Science.gov (United States)

Mah, Pei T; Novakovic, Dunja; Saarinen, Jukka; Van Landeghem, Stijn; Peltonen, Leena; Laaksonen, Timo; Isomäki, Antti; Strachan, Clare J

2017-05-01

To investigate the effect of compression on the crystallization behavior in amorphous tablets using sum frequency generation (SFG) microscopy imaging and more established analytical methods. Tablets containing neat amorphous griseofulvin with/without excipients (silica, hydroxypropyl methylcellulose acetate succinate (HPMCAS), microcrystalline cellulose (MCC) and polyethylene glycol (PEG)) were prepared. They were analyzed upon preparation and storage using attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, scanning electron microscopy (SEM) and SFG microscopy. Compression-induced crystallization occurred predominantly on the surface of the neat amorphous griseofulvin tablets, with minimal crystallinity being detected in the core of the tablets. The presence of various types of excipients was not able to mitigate the compression-induced surface crystallization of the amorphous griseofulvin tablets. However, the excipients affected the crystallization rate of amorphous griseofulvin in the core of the tablet upon compression and storage. SFG microscopy can be used in combination with ATR-FTIR spectroscopy and SEM to understand the crystallization behaviour of amorphous tablets upon compression and storage. When selecting excipients for amorphous formulations, it is important to consider the effect of the excipients on the physical stability of the amorphous formulations.

Sum frequency generation and catalytic reaction studies of the removal of the organic capping agents from Pt nanoparticles by UV-ozone treatment

Energy Technology Data Exchange (ETDEWEB)

Aliaga, Cesar; Park, Jeong Y.; Yamada, Yusuke; Lee, Hyun Sook; Tsung, Chia-Kuang; Yang, Peidong; Somorjai, Gabor A.

2009-12-10

We report the structure of the organic capping layers of platinum colloid nanoparticles and their removal by UV-ozone exposure. Sum frequency generation vibrational spectroscopy (SFGVS) studies identify the carbon-hydrogen stretching modes on poly(vinylpyrrolidone) (PVP) and tetradecyl tributylammonium bromide (TTAB)-capped platinum nanoparticles. We found that the UV-ozone treatment technique effectively removes the capping layer on the basis of several analytical measurements including SFGVS, X-ray photoelectron spectroscopy, and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The overall shape of the nanoparticles was preserved after the removal of capping layers, as confirmed by transmission electron microscopy (TEM). SFGVS of ethylene hydrogenation on the clean platinum nanoparticles demonstrates the existence of ethylidyne and di-{sigma}-bonded species, indicating the similarity between single-crystal and nanoparticle systems.

Efficient generation of continuous-wave yellow-orange light using sum-frequency in periodically poled KTP

DEFF Research Database (Denmark)

Janousek, Jiri; Johansson, Sandra; Tidemand-Lichtenberg, Peter

We present highly efficient sum-frequency generation between two CW 1064 and 1342 nm laser lines of two Nd:YVO4 lasers using periodically poled KTP. This is an all solid-state light source in the yellow-orange spectral range....

Study of confinement and sliding friction of fluids using sum frequency generation spectroscopy

Science.gov (United States)

Nanjundiah, Kumar

2007-12-01

Friction and wear are important technologically. Tires on wet roads, windshield wipers and human joints are examples where nanometer-thick liquids are confined between flexible-rigid contact interfaces. Fundamental understanding of the structure of these liquids can assist in the design of products such as artificial joints and lubricants for Micro-electromechanical systems [MEMS]. Prior force measurements have suggested an increase in apparent viscosity of confined liquid and sometimes solid-like responses. But, these have not given the state of molecules under confinement. In the present study, we have used a surface sensitive, non-linear optical technique (infrared-visible sum frequency generation spectroscopy [SFG]) to investigate molecular structure at hidden interfaces. SFG can identify chemical groups, concentration and orientation of molecules at an interface. A friction cell was developed to study sliding of a smooth elastomeric lens against a sapphire surface. Experiments were done with dry sliding as well as lubricated sliding in the presence of linear alkane liquids. SFG spectra at the alkane/sapphire interface revealed ordering of the confined alkane molecules. These were more ordered than alkane liquid, but less ordered than alkane crystal. Cooling of the confined alkane below its melting temperature [TM] led to molecular orientation that was different from that of bulk crystal next to a sapphire surface. Molecules were oriented with their symmetry axis parallel to the surface normal. In addition, the melting temperature [Tconf] under confinement for a series of linear alkanes (n =15--27) showed a surprising trend. Intermediate molecular weights showed melting point depression. The T conf values suggested that melting started at the alkane/sapphire interface. In another investigation, confinement of water between an elastomeric PDMS lens and sapphire was studied. SFG spectra at the sapphire/water/PDMS interface revealed a heterogeneous morphology. The

Surface and buried interfacial structures of epoxy resins used as underfills studied by sum frequency generation vibrational spectroscopy.

Science.gov (United States)

Vázquez, Anne V; Holden, Brad; Kristalyn, Cornelius; Fuller, Mike; Wilkerson, Brett; Chen, Zhan

2011-05-01

Flip chip technology has greatly improved the performance of semiconductor devices, but relies heavily on the performance of epoxy underfill adhesives. Because epoxy underfills are cured in situ in flip chip semiconductor devices, understanding their surface and interfacial structures is critical for understanding their adhesion to various substrates. Here, sum frequency generation (SFG) vibrational spectroscopy was used to study surface and buried interfacial structures of two model epoxy resins used as underfills in flip chip devices, bisphenol A digylcidyl ether (BADGE) and 1,4-butanediol diglycidyl ether (BDDGE). The surface structures of these epoxies were compared before and after cure, and the orientations of their surface functional groups were deduced to understand how surface structural changes during cure may affect adhesion properties. Further, the effect of moisture exposure, a known cause of adhesion failure, on surface structures was studied. It was found that the BADGE surface significantly restructured upon moisture exposure while the BDDGE surface did not, showing that BADGE adhesives may be more prone to moisture-induced delamination. Lastly, although surface structure can give some insight into adhesion, buried interfacial structures more directly correspond to adhesion properties of polymers. SFG was used to study buried interfaces between deuterated polystyrene (d-PS) and the epoxies before and after moisture exposure. It was shown that moisture exposure acted to disorder the buried interfaces, most likely due to swelling. These results correlated with lap shear adhesion testing showing a decrease in adhesion strength after moisture exposure. The presented work showed that surface and interfacial structures can be correlated to adhesive strength and may be helpful in understanding and designing optimized epoxy underfill adhesives.

Hydrogenation of the alpha,beta-Unsaturated Aldehydes Acrolein, Crotonaldehyde, and Prenal over Pt Single Crystals: A Kinetic and Sum-Frequency Generation Vibrational Spectroscopy Study

Energy Technology Data Exchange (ETDEWEB)

Kliewer, C.J.; Somorjai, G.A.

2008-11-26

Sum-frequency generation vibrational spectroscopy (SFG-VS) and kinetic measurements using gas chromatography have been used to study the surface reaction intermediates during the hydrogenation of three {alpha},{beta}-unsaturated aldehydes, acrolein, crotonaldehyde, and prenal, over Pt(111) at Torr pressures (1 Torr aldehyde, 100 Torr hydrogen) in the temperature range of 295K to 415K. SFG-VS data showed that acrolein has mixed adsorption species of {eta}{sub 2}-di-{sigma}(CC)-trans, {eta}{sub 2}-di-{sigma}(CC)-cis as well as highly coordinated {eta}{sub 3} or {eta}{sub 4} species. Crotonaldehyde adsorbed to Pt(111) as {eta}{sub 2} surface intermediates. SFG-VS during prenal hydrogenation also suggested the presence of the {eta}{sub 2} adsorption species, and became more highly coordinated as the temperature was raised to 415K, in agreement with its enhanced C=O hydrogenation. The effect of catalyst surface structure was clarified by carrying out the hydrogenation of crotonaldehyde over both Pt(111) and Pt(100) single crystals while acquiring the SFG-VS spectra in situ. Both the kinetics and SFG-VS showed little structure sensitivity. Pt(100) generated more decarbonylation 'cracking' product while Pt(111) had a higher selectivity for the formation of the desired unsaturated alcohol, crotylalcohol.

Optical sum-frequency generation in a whispering-gallery-mode resonator

International Nuclear Information System (INIS)

Strekalov, Dmitry V; Kowligy, Abijith S; Huang, Yu-Ping; Kumar, Prem

2014-01-01

We demonstrate sum-frequency generation between a telecom wavelength and the Rb D2 line, achieved through natural phase matching in a nonlinear whispering gallery mode resonator. Due to the strong optical field confinement and ultra high Q of the cavity, the process saturates already at sub-mW pump peak power, at least two orders of magnitude lower than in existing waveguide-based devices. The experimental data are in agreement with the nonlinear dynamics and phase matching theory based on spherical geometry. Our experimental and theoretical results point toward a new platform for manipulating the color and quantum states of light waves for applications such as atomic memory based quantum networking and logic operations with optical signals. (paper)

Adsorption of 1- and 2-butylimidazoles at the copper/air and steel/air interfaces studied by sum frequency generation vibrational spectroscopy.

Science.gov (United States)

Casford, Michael T L; Davies, Paul B

2012-07-24

The structure of thin films of 1- and 2-butylimidazoles adsorbed on copper and steel surfaces under air was examined using sum frequency generation (SFG) vibrational spectroscopy in the ppp and ssp polarizations. Additionally, the SFG spectra of both isomers were recorded at 55 °C at the liquid imidazole/air interface for reference. Complementary bulk infrared, reflection-absorption infrared spectroscopy (RAIRS), and Raman spectra of both imidazoles were recorded for assignment purposes. The SFG spectra in the C-H stretching region at the liquid/air interface are dominated by resonances from the methyl end group of the butyl side chain of the imidazoles, indicating that they are aligned parallel or closely parallel to the surface normal. These are also the most prominent features in the SFG spectra on copper and steel. In addition, both the ppp and ssp spectra on copper show resonances from the C-H stretching modes of the imidazole ring for both isomers. The ring C-H resonances are completely absent from the spectra on steel and at the liquid/air interface. The relative intensities of the SFG spectra can be interpreted as showing that, on copper, under air, both butylimidazoles are adsorbed with their butyl side chains perpendicular to the interface and with the ring significantly inclined away from the surface plane and toward the surface normal. The SFG spectra of both imidazoles on steel indicate an orientation where the imidazole rings are parallel or nearly parallel to the surface. The weak C-H resonances from the ring at the liquid/air interface suggest that the tilt angle of the ring from the surface normal at this interface is significantly greater than it is on copper.

Effects of cations and cholesterol with sphingomyelin membranes investigated by high-resolution broadband sum frequency vibrational spectroscopy

Science.gov (United States)

Zhang, Zhen; Feng, Rong-juan; Li, Yi-yi; Liu, Ming-hua; Guo, Yuan

2017-08-01

Sphingomyelin(SM) is specifically enriched in the plasma membrane of mammalian cells. Its molecular structure is compose by N-acyl-Derythro-sphingosylphosphorylcholine. The function of the SM related to membrane signaling and protein trafficking are relied on the interactions of the SM, cations, cholesterol and proteins. In this report, the interaction of three different nature SMs, cations and cholesterol at air/aqueous interfaces studied by high-resolution broadband sum frequency vibrational spectroscopy, respectively. Our results shed lights on understanding the relationship between SMs monolayer, cholesterol and Cations.

High-order sum and difference-frequency generation in helium

International Nuclear Information System (INIS)

Crane, J.K.; Perry, M.D.

1993-01-01

High-order harmonic generation provides a new method for generating coherent, XUV radiation. These harmonics are characterized by a rapid, pertubative drop at low orders, followed by a broad plateau extending to photon energies of 150 eV in the lighter, rare gas atoms. An experimentally observed limit coincides with the theoretical limit for harmonic generation in neutral atoms given by the expression E c (eV)=IP(0)+3U p (I), where E c is the energy cutoff of the harmonic plateau, IP(O) is the field-free ionization potential and U p is the electron quiver energy at the maximum intensity, I seen by the atom. As part of an effort to develop this technique into a general purpose XUV source, extensive work to understand the phase-matching between the harmonic and driving fields, and the resulting effect on the conversion efficiency, angular distribution and spectral brightness has been undertaken at several. Though, certain aspects of the harmonically generated radiation such as the polarization, relative strength of a given harmonic, and the plateau extent, are defined by the single atom-field interaction. Specifically, the single-atom harmonic spectrum is determined primarily by the interaction of a driven, quasi-free electron with the atomic potential. Using two, independent fields one can affect the electron motion by controlling the relative strength, polarization, and phase of the fields and alter the harmonic spectrum. In this paper we discuss initial, two-color experiments where we drive the atom with two fields of different frequencies: 1053 nm (1ω) and 526 nm (2ω). In addition to the higher, odd harmonics, we observe sets of three additional peaks that we attribute to sum and difference-frequency generation between the two fields. By controlling the relative polarization between the two fields we can control the relative strength of the harmonic and mixing components, as well as the polarization of the output XUV photon

Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Chase, Hilary M.; Chen, Shunli; Fu, Li; Upshur, Mary Alice; Rudshteyn, Benjamin; Thomson, Regan J.; Wang, Hong-Fei; Batista, Victor S.; Geiger, Franz M.

2017-09-01

Inferring molecular orientations from vibrational sum frequency generation (SFG) spectra is challenging in polarization combinations that result in low signal intensities, or when the local point group symmetry approximation fails. While combining experiments with density functional theory (DFT) could overcome this problem, the scope of the combined method has yet to be established. Here, we assess its feasibility of determining the distributions of molecular orientations for one monobasic ester, two epoxides and three alcohols at the vapor/fused silica interface. We find that molecular orientations of nonlocal vibrational modes cannot be determined using polarization-resolved SFG measurements alone.

Combining total internal reflection sum frequency spectroscopy spectral imaging and confocal fluorescence microscopy.

Science.gov (United States)

Allgeyer, Edward S; Sterling, Sarah M; Gunewardene, Mudalige S; Hess, Samuel T; Neivandt, David J; Mason, Michael D

2015-01-27

Understanding surface and interfacial lateral organization in material and biological systems is critical in nearly every field of science. The continued development of tools and techniques viable for elucidation of interfacial and surface information is therefore necessary to address new questions and further current investigations. Sum frequency spectroscopy (SFS) is a label-free, nonlinear optical technique with inherent surface specificity that can yield critical organizational information on interfacial species. Unfortunately, SFS provides no spatial information on a surface; small scale heterogeneities that may exist are averaged over the large areas typically probed. Over the past decade, this has begun to be addressed with the advent of SFS microscopy. Here we detail the construction and function of a total internal reflection (TIR) SFS spectral and confocal fluorescence imaging microscope directly amenable to surface investigations. This instrument combines, for the first time, sample scanning TIR-SFS imaging with confocal fluorescence microscopy.

Sum Frequency Generation Vibrational Spectroscopy of 1,3-Butadiene Hydrogenation on 4 nm Pt@SiO 2 , Pd@SiO 2 , and Rh@SiO 2 Core–Shell Catalysts

KAUST Repository

Krier, James M.

2015-01-14

© 2014 American Chemical Society. 1,3-Butadiene (1,3-BD) hydrogenation was performed on 4 nm Pt, Pd, and Rh nanoparticles (NPs) encapsulated in SiO2 shells at 20, 60, and 100 °C. The core-shells were grown around polyvinylpyrrolidone (PVP) coated NPs (Stöber encapsulation) prepared by colloidal synthesis. Sum frequency generation (SFG) vibrational spectroscopy was performed to correlate surface intermediates observed in situ with reaction selectivity. It is shown that calcination is effective in removing PVP, and the SFG signal can be generated from the metal surface. Using SFG, it is possible to compare the surface vibrational spectrum of Pt@SiO2 (1,3-BD is hydrogenated through multiple paths and produces butane, 1-butene, and cis/trans-2-butene) to Pd@SiO2 (1,3-BD favors one path and produces 1-butene and cis/trans-2-butene). In contrast to Pt@SiO2 and Pd@SiO2, SFG and kinetic experiments of Rh@SiO2 show a permanent accumulation of organic material.

Sum Frequency Generation Vibrational Spectroscopy Studies on ModelPeptide Adsorption at the Hydrophobic Solid-Water and HydrophilicSolid-Water Interfaces

Energy Technology Data Exchange (ETDEWEB)

York, Roger L. [Univ. of California, Berkeley, CA (United States)

2007-01-01

Sum frequency generation (SFG) vibrational spectroscopy has been used to study the interfacial structure of several polypeptides and amino acids adsorbed to hydrophobic and hydrophilic surfaces under a variety of experimental conditions. Peptide sequence, peptide chain length, peptide hydrophobicity, peptide side-chain type, surface hydrophobicity, and solution ionic strength all affect an adsorbed peptide's interfacial structure. Herein, it is demonstrated that with the choice of simple, model peptides and amino acids, surface specific SFG vibrational spectroscopy can be a powerful tool to elucidate the interfacial structure of these adsorbates. Herein, four experiments are described. In one, a series of isosequential amphiphilic peptides are synthesized and studied when adsorbed to both hydrophobic and hydrophilic surfaces. On hydrophobic surfaces of deuterated polystyrene, it was determined that the hydrophobic part of the peptide is ordered at the solid-liquid interface, while the hydrophilic part of the peptide appears to have a random orientation at this interface. On a hydrophilic surface of silica, it was determined that an ordered peptide was only observed if a peptide had stable secondary structure in solution. In another experiment, the interfacial structure of a model amphiphilic peptide was studied as a function of the ionic strength of the solution, a parameter that could change the peptide's secondary structure in solution. It was determined that on a hydrophobic surface, the peptide's interfacial structure was independent of its structure in solution. This was in contrast to the adsorbed structure on a hydrophilic surface, where the peptide's interfacial structure showed a strong dependence on its solution secondary structure. In a third experiment, the SFG spectra of lysine and proline amino acids on both hydrophobic and hydrophilic surfaces were obtained by using a different experimental geometry that increases the SFG signal

Hydration of Sulphobetaine (SB) and Tetra(ethylene glycol) (EG4)-Terminated Self-Assembled Monolayers Studied by Sum Frequency Generation (SFG) Vibrational Spectroscopy

Science.gov (United States)

Stein, M. Jeanette; Weidner, Tobias; McCrea, Keith; Castner, David G.; Ratner, Buddy D.

2010-01-01

Sum frequency generation (SFG) vibrational spectroscopy is used to study the surface and the underlying substrate of both homogeneous and mixed self-assembled monolayers (SAMs) of 11-mercaptoundecyl-1-sulphobetainethiol (HS(CH2)11N+(CH3)2(CH2)3SO3−, SB) and 1-mercapto-11-undecyl tetra(ethylene glycol) (HS(CH2)11O(CH2CH2O)4OH, EG4) with an 11-mercapto-1-undecanol (HS(CH2)11OH, MCU) diluent. SFG results on the C–H region of the dry and hydrated SAMs gave an in situ look into the molecular orientation and suggested an approach to maximize signal-to-noise ratio on these difficult to analyze hydrophilic SAMs. Vibrational fingerprint studies in the 3000–3600 cm−1 spectral range for the SAMs exposed serially to air, water, and deuterated water revealed that a layer of tightly-bound structured water was associated with the surface of a non-fouling monolayer but was not present on a hydrophobic N-undecylmercaptan (HS(CH2)10CH3, UnD) control. The percentage of water retained upon submersion in D2O correlated well with the relative amount of protein that was previously shown to absorb onto the monolayers. These results provide evidence supporting the current theory regarding the role of a tightly-bound vicinal water layer in the protein resistance of a non-fouling group. PMID:19639981

Characterisation of the membrane affinity of an isoniazide peptide conjugate by tensiometry, atomic force microscopy and sum-frequency vibrational spectroscopy, using a phospholipid Langmuir monolayer model.

Science.gov (United States)

Hill, Katalin; Pénzes, Csanád Botond; Schnöller, Donát; Horváti, Kata; Bosze, Szilvia; Hudecz, Ferenc; Keszthelyi, Tamás; Kiss, Eva

2010-10-07

Tensiometry, sum-frequency vibrational spectroscopy, and atomic force microscopy were employed to assess the cell penetration ability of a peptide conjugate of the antituberculotic agent isoniazide. Isoniazide was conjugated to peptide (91)SEFAYGSFVRTVSLPV(106), a functional T-cell epitope of the immunodominant 16 kDa protein of Mycobacterium tuberculosis. As a simple but versatile model of the cell membrane a phospholipid Langmuir monolayer at the liquid/air interface was used. Changes induced in the structure of the phospholipid monolayer by injection of the peptide conjugate into the subphase were followed by tensiometry and sum-frequency vibrational spectroscopy. The drug penetrated lipid films were transferred to a solid support by the Langmuir-Blodgett technique, and their structures were characterized by atomic force microscopy. Peptide conjugation was found to strongly enhance the cell penetration ability of isoniazide.

Conformation, orientation and interaction in molecular monolayers: A surface second harmonic and sum frequency generation study

International Nuclear Information System (INIS)

Superfine, R.; Huang, J.Y.; Shen, Y.R.

1988-12-01

We have used sum frequency generation (SFG) to study the order in a silane monolayer before and after the deposition of a coadsorbed liquid crystal monolayer. We observe an increase in the order of the chain of the silane molecule induced by the interpenetration of the liquid crystal molecules. By using second harmonic generation (SHG) and SFG, we have studied the orientation and conformation of the liquid crystal molecule on clean and silane coated glass surfaces. On both surfaces, the biphenyl group is tilted by 70 degree with the alkyl chain end pointing away from the surface. The shift in the C-H stretch frequencies in the coadsorbed system indicates a significant interaction between molecules. 9 refs., 3 figs

Determining In Situ Protein Conformation and Orientation from the Amide-I Sum-Frequency Generation Spectrum: Theory and Experiment

NARCIS (Netherlands)

Roeters, S.J.; van Dijk, C.N.; Torres Knoop, A.; Backus, E.H.G.; Campen, R.K.; Bonn, M.; Woutersen, S.

2013-01-01

Vibrational sum-frequency generation (VSFG) spectra of the amide-I band of proteins can give detailed insight into biomolecular processes near membranes. However, interpreting these spectra in terms of the conformation and orientation of a protein can be difficult, especially in the case of complex

Capturing inhomogeneous broadening of the -CN stretch vibration in a Langmuir monolayer with high-resolution spectra and ultrafast vibrational dynamics in sum-frequency generation vibrational spectroscopy (SFG-VS)

Science.gov (United States)

Velarde, Luis; Wang, Hong-fei

2013-08-01

While in principle the frequency-domain and time-domain spectroscopic measurements should generate identical information for a given molecular system, the inhomogeneous character of surface vibrations in sum-frequency generation vibrational spectroscopy (SFG-VS) studies has only been studied with time-domain SFG-VS by mapping the decay of the vibrational polarization using ultrafast lasers, this due to the lack of SFG vibrational spectra with high enough spectral resolution and accurate enough lineshape. Here, with the recently developed high-resolution broadband SFG-VS (HR-BB-SFG-VS) technique, we show that the inhomogeneous lineshape can be obtained in the frequency-domain for the anchoring CN stretch of the 4-n-octyl-4'-cyanobiphenyl (8CB) Langmuir monolayer at the air-water interface, and that an excellent agreement with the time-domain SFG free-induction-decay can be established. We found that the 8CB CN stretch spectrum consists of a single peak centered at 2234.00 ± 0.01 cm-1 with a total linewidth of 10.9 ± 0.3 cm-1 at half maximum. The Lorentzian contribution accounts only for 4.7 ± 0.4 cm-1 to this width and the Gaussian (inhomogeneous) broadening for as much as 8.1 ± 0.2 cm-1. Polarization analysis of the -CN spectra showed that the -CN group is tilted 57° ± 2° from the surface normal. The large heterogeneity in the -CN spectrum is tentatively attributed to the -CN group interactions with the interfacial water molecules penetrated/accommodated into the 8CB monolayer, a unique phenomenon for the nCB Langmuir monolayers reported previously.

Two-dimensional sum-frequency generation (2D SFG) reveals structure and dynamics of a surface-bound peptide

Science.gov (United States)

Laaser, Jennifer E.; Skoff, David R.; Ho, Jia-Jung; Joo, Yongho; Serrano, Arnaldo L.; Steinkruger, Jay D.; Gopalan, Padma; Gellman, Samuel H.; Zanni, Martin T.

2014-01-01

Surface-bound polypeptides and proteins are increasingly used to functionalize inorganic interfaces such as electrodes, but their structural characterization is exceedingly difficult with standard technologies. In this paper, we report the first two-dimensional sum-frequency generation (2D SFG) spectra of a peptide monolayer, which is collected by adding a mid-IR pulse shaper to a standard femtosecond SFG spectrometer. On a gold surface, standard FTIR spectroscopy is inconclusive about the peptide structure because of solvation-induced frequency shifts, but the 2D lineshapes, anharmonic shifts, and lifetimes obtained from 2D SFG reveal that the peptide is largely α-helical and upright. Random coil residues are also observed, which do not themselves appear in SFG spectra due to their isotropic structural distribution, but which still absorb infrared light and so can be detected by cross-peaks in 2D SFG spectra. We discuss these results in the context of peptide design. Because of the similar way in which the spectra are collected, these 2D SFG spectra can be directly compared to 2D IR spectra, thereby enabling structural interpretations of surface-bound peptides and biomolecules based on the well-studied structure/2D IR spectra relationships established from soluble proteins. PMID:24372101

Spectrally- and Time-Resolved Sum Frequency Generation (STiR-SFG): a new tool for ultrafast hydrogen bond dynamics at interfaces.

Science.gov (United States)

Benderskii, Alexander; Bordenyuk, Andrey; Weeraman, Champika

2006-03-01

The recently developed spectrally- and time-resolved Sum Frequency Generation (STiR-SFG) is a surface-selective 3-wave mixing (IR+visible) spectroscopic technique capable of measuring ultrafast spectral evolution of vibrational coherences. A detailed description of this measurement will be presented, and a noniterative method or deconvolving the laser pulses will be introduced to obtain the molecular response function. STiR-SFG, combined with the frequency-domain SFG spectroscopy, was applied to study hydrogen bonding dynamics at aqueous interfaces (D2O/CaF2). Spectral dynamics of the OD-stretch on the 50-150 fs time scale provides real-time observation of ultrafast H-bond rearrangement. Tuning the IR wavelength to the blue or red side of the OD-stretch transition, we selectively monitor the dynamics of different sub-ensembles in the distribution of the H-bond structures. The blue-side excitation (weaker H-bonding) shows monotonic red-shift of the OD-frequency. In contrast, the red-side excitation (stronger H-bonding structures) produces a blue-shift and a recursion, which may indicate the presence of an underdamped intermolecular mode of interfacial water. Effect of electrolyte concentration on the H-bond dynamics will be discussed.

Photon wave function formalism for analysis of Mach–Zehnder interferometer and sum-frequency generation

Energy Technology Data Exchange (ETDEWEB)

Ritboon, Atirach, E-mail: atirach.3.14@gmail.com [School of Physics and Astronomy, University of Glasgow, Glasgow, G12 8QQ (United Kingdom); Department of Physics, Faculty of Science, Prince of Songkla University, Hat Yai 90112 (Thailand); Daengngam, Chalongrat, E-mail: chalongrat.d@psu.ac.th [Department of Physics, Faculty of Science, Prince of Songkla University, Hat Yai 90112 (Thailand); Pengpan, Teparksorn, E-mail: teparksorn.p@psu.ac.th [Department of Physics, Faculty of Science, Prince of Songkla University, Hat Yai 90112 (Thailand)

2016-08-15

Biakynicki-Birula introduced a photon wave function similar to the matter wave function that satisfies the Schrödinger equation. Its second quantization form can be applied to investigate nonlinear optics at nearly full quantum level. In this paper, we applied the photon wave function formalism to analyze both linear optical processes in the well-known Mach–Zehnder interferometer and nonlinear optical processes for sum-frequency generation in dispersive and lossless medium. Results by photon wave function formalism agree with the well-established Maxwell treatments and existing experimental verifications.

Photon wave function formalism for analysis of Mach–Zehnder interferometer and sum-frequency generation

International Nuclear Information System (INIS)

Ritboon, Atirach; Daengngam, Chalongrat; Pengpan, Teparksorn

2016-01-01

Biakynicki-Birula introduced a photon wave function similar to the matter wave function that satisfies the Schrödinger equation. Its second quantization form can be applied to investigate nonlinear optics at nearly full quantum level. In this paper, we applied the photon wave function formalism to analyze both linear optical processes in the well-known Mach–Zehnder interferometer and nonlinear optical processes for sum-frequency generation in dispersive and lossless medium. Results by photon wave function formalism agree with the well-established Maxwell treatments and existing experimental verifications.

Broadband short pulse measurement by autocorrelation with a sum-frequency generation set-up

International Nuclear Information System (INIS)

Glotin, F.; Jaroszynski, D.; Marcouille, O.

1995-01-01

Previous spectral and laser pulse length measurements carried out on the CLIO FEL at wavelength λ=8.5 μm suggested that very short light pulses could be generated, about 500 fs wide (FWHM). For these measurements a Michelson interferometer with a Te crystal, as a non-linear detector, was used as a second order autocorrelation device. More recent measurements in similar conditions have confirmed that the laser pulses observed are indeed single: they are not followed by other pulses distant by the slippage length Nλ. As the single micropulse length is likely to depend on the slippage, more measurements at different wavelengths would be useful. This is not directly possible with our actual interferometer set-up, based on a phase-matched non-linear crystal. However, we can use the broadband non-linear medium provided by one of our users' experiments: Sum-Frequency Generation over surfaces. With such autocorrelation set-up, interference fringes are no more visible, but this is largely compensated by the frequency range provided. First tests at 8 μm have already been performed to validate the technic, leading to results similar to those obtained with our previous Michelson set-up

Sum-frequency generation from molecular monolayers using 14 μm radiation from the FELIX free-electron laser

International Nuclear Information System (INIS)

Van der Ham, E.W.M.; Vrehen, Q.H.F.; Eliel, E.R.

1995-01-01

Sum-frequency generation (SFG) has developed into a widely applied tool for study of surfaces and interfaces where molecules are present. It combines the surface specificity of a second-order nonlinear optical technique with the power of a spectroscopic method, and it can be used under widely varying experimental conditions ranging from UHV to electrochemical cells. The important characteristic of SFG is that it allows one to study the average spatial orientation of a molecular bond in a monolayer of molecules at an interface. Until recently SFG measurements were confined to the frequency interval Y μ > 1700 cm -1 because of a lack of suitable laser sources at wave-lengths λ > 6 μm. So for most molecules only a few vibrational modes and thus intramolecular bonds can be studied. We have developed a universal sum-frequency spectrometer around the FELIX free-electron law that covers the complete molecular fingerprint since we can generate any IR wavelength between 2.75 and 110 fμ at the FELIX facility. We have used this setup for a series of exploratory SFG experiments in a frequency range that was hitherto unexplored in the study of molecular monolayers. We have studied thiol monolayers chemisorbed on a variety of noble metals (Au, Ag, Pt) where we focussed on the C-S stretch vibration at ν = 702 cm -1 (λ = 14.3 μm). We have found spectroscopic features revealing the presence of both the trane and gauche conformers of the adsorbed molecules. The present measurements open a whole new wavelength range for nonlinear optical studies of interfaces

Effect of surface structure on catalytic reactions: A sum frequency generation surface vibrational spectroscopy study

International Nuclear Information System (INIS)

McCrea, Keith R.

2001-01-01

In the results discussed above, it is clear that Sum Frequency Generation (SFG) is a unique tool that allows the detection of vibrational spectra of adsorbed molecules present on single crystal surfaces under catalytic reaction conditions. Not only is it possible to detect active surface intermediates, it is also possible to detect spectator species which are not responsible for the measured turnover rates. By correlating high-pressure SFG spectra under reaction conditions and gas chromatography (GC) kinetic data, it is possible to determine which species are important under reaction intermediates. Because of the flexibility of this technique for studying surface intermediates, it is possible to determine how the structures of single crystal surfaces affect the observed rates of catalytic reactions. As an example of a structure insensitive reaction, ethylene hydrogenation was explored on both Pt(111) and Pt(100). The rates were determined to be essentially the same. It was observed that both ethylidyne and di-(sigma) bonded ethylene were present on the surface under reaction conditions on both crystals, although in different concentrations. This result shows that these two species are not responsible for the measured turnover rate, as it would be expected that one of the two crystals would be more active than the other, since the concentration of the surface intermediate would be different on the two crystals. The most likely active intermediates are weakly adsorbed molecules such as(pi)-bonded ethylene and ethyl. These species are not easily detected because their concentration lies at the detection limit of SFG. The SFG spectra and GC data essentially show that ethylene hydrogenation is structure insensitive for Pt(111) and Pt(100). SFG has proven to be a unique and excellent technique for studying adsorbed species on single crystal surfaces under high-pressure catalytic reactions. Coupled with kinetic data obtained from gas chromatography measurements, it can

Unidirectional ring-laser operation using sum-frequency mixing

DEFF Research Database (Denmark)

Tidemand-Lichtenberg, Peter; Cheng, Haynes Pak Hay; Pedersen, Christian

2010-01-01

A technique enforcing unidirectional operation of ring lasers is proposed and demonstrated. The approach relies on sum-frequency mixing between a single-pass laser and one of the two counterpropagating intracavity fields of the ring laser. Sum-frequency mixing introduces a parametric loss for the...... where lossless second-order nonlinear materials are available. Numerical modeling and experimental demonstration of parametric-induced unidirectional operation of a diode-pumped solid-state 1342 nm cw ring laser are presented.......A technique enforcing unidirectional operation of ring lasers is proposed and demonstrated. The approach relies on sum-frequency mixing between a single-pass laser and one of the two counterpropagating intracavity fields of the ring laser. Sum-frequency mixing introduces a parametric loss...

Direct comparison of phase-sensitive vibrational sum frequency generation with maximum entropy method: case study of water.

Science.gov (United States)

de Beer, Alex G F; Samson, Jean-Sebastièn; Hua, Wei; Huang, Zishuai; Chen, Xiangke; Allen, Heather C; Roke, Sylvie

2011-12-14

We present a direct comparison of phase sensitive sum-frequency generation experiments with phase reconstruction obtained by the maximum entropy method. We show that both methods lead to the same complex spectrum. Furthermore, we discuss the strengths and weaknesses of each of these methods, analyzing possible sources of experimental and analytical errors. A simulation program for maximum entropy phase reconstruction is available at: http://lbp.epfl.ch/. © 2011 American Institute of Physics

In Situ Adsorption Studies at the Solid/Liquid Interface: Characterization of Biological Surfaces and Interfaces Using Sum Frequency Generation Vibrational Spectroscopy, Atomic Force Microscopy, and Quartz Crystal Microbalance

International Nuclear Information System (INIS)

Phillips, D.C.

2006-01-01

Sum frequency generation (SFG) vibrational spectroscopy, atomic force microscopy (AFM), and quartz crystal microbalance (QCM) have been used to study the molecular surface structure, surface topography and mechanical properties, and quantitative adsorbed amount of biological molecules at the solid-liquid interface. The molecular-level behavior of designed peptides adsorbed on hydrophobic polystyrene and hydrophilic silica substrates has been examined as a model of protein adsorption on polymeric biomaterial surfaces. Proteins are such large and complex molecules that it is difficult to identify the features in their structure that lead to adsorption and interaction with solid surfaces. Designed peptides which possess secondary structure provide simple model systems for understanding protein adsorption. Depending on the amino acid sequence of a peptide, different secondary structures (α-helix and β-sheet) can be induced at apolar (air/liquid or air/solid) interfaces. Having a well-defined secondary structure allows experiments to be carried out under controlled conditions, where it is possible to investigate the affects of peptide amino acid sequence and chain length, concentration, buffering effects, etc. on adsorbed peptide structure. The experiments presented in this dissertation demonstrate that SFG vibrational spectroscopy can be used to directly probe the interaction of adsorbing biomolecules with a surface or interface. The use of well designed model systems aided in isolation of the SFG signal of the adsorbing species, and showed that surface functional groups of the substrate are sensitive to surface adsorbates. The complementary techniques of AFM and QCM allowed for deconvolution of the effects of surface topography and coverage from the observed SFG spectra. Initial studies of biologically relevant surfaces are also presented: SFG spectroscopy was used to study the surface composition of common soil bacteria for use in bioremediation of nuclear waste

In Situ Adsorption Studies at the Solid/Liquid Interface:Characterization of Biological Surfaces and Interfaces Using SumFrequency Generation Vibrational Spectroscopy, Atomic Force Microscopy,and Quartz Crystal Microbalance

Energy Technology Data Exchange (ETDEWEB)

Phillips, Diana Christine [Univ. of California, Berkeley, CA (United States)

2006-01-01

Sum frequency generation (SFG) vibrational spectroscopy, atomic force microscopy (AFM), and quartz crystal microbalance (QCM) have been used to study the molecular surface structure, surface topography and mechanical properties, and quantitative adsorbed amount of biological molecules at the solid-liquid interface. The molecular-level behavior of designed peptides adsorbed on hydrophobic polystyrene and hydrophilic silica substrates has been examined as a model of protein adsorption on polymeric biomaterial surfaces. Proteins are such large and complex molecules that it is difficult to identify the features in their structure that lead to adsorption and interaction with solid surfaces. Designed peptides which possess secondary structure provide simple model systems for understanding protein adsorption. Depending on the amino acid sequence of a peptide, different secondary structures (α-helix and β-sheet) can be induced at apolar (air/liquid or air/solid) interfaces. Having a well-defined secondary structure allows experiments to be carried out under controlled conditions, where it is possible to investigate the affects of peptide amino acid sequence and chain length, concentration, buffering effects, etc. on adsorbed peptide structure. The experiments presented in this dissertation demonstrate that SFG vibrational spectroscopy can be used to directly probe the interaction of adsorbing biomolecules with a surface or interface. The use of well designed model systems aided in isolation of the SFG signal of the adsorbing species, and showed that surface functional groups of the substrate are sensitive to surface adsorbates. The complementary techniques of AFM and QCM allowed for deconvolution of the effects of surface topography and coverage from the observed SFG spectra. Initial studies of biologically relevant surfaces are also presented: SFG spectroscopy was used to study the surface composition of common soil bacteria for use in bioremediation of nuclear waste.

A Tunable CW Orange Laser Based on a Cascaded MgO:PPLN Single-Pass Sum-Frequency Generation Module

OpenAIRE

Dismas K. Choge; Huai-Xi Chen; Bao-Lu Tian; Yi-Bin Xu; Guang-Wei Li; Wan-Guo Liang

2018-01-01

We report an all-solid-state continuous wave (CW) tunable orange laser based on cascaded single-pass sum-frequency generation with fundamental wavelengths at 1545.7 and 975.2 nm using two quasi-phase-matched (QPM) MgO-doped periodically poled lithium niobate (MgO:PPLN) crystals. Up to 10 mW of orange laser is generated in the cascaded module corresponding to a 10.4%/W nonlinear conversion efficiency. The orange output showed a temperature tuning rate of ~0.05 nm/°C, and the beam quality (M2) ...

The structure of oleamide films at the aluminum/oil interface and aluminum/air interface studied by Sum Frequency Generation (SFG) vibrational spectroscopy and Reflection Absorption Infrared Spectroscopy (RAIRS).

Science.gov (United States)

Casford, Michael T L; Davies, Paul B

2009-08-01

The structure of oleamide (cis-9-octadecenamide) films on aluminum has been investigated by sum frequency generation vibrational spectroscopy (SFG) and reflection absorption infrared spectroscopy (RAIRS). Three different film deposition strategies were investigated: (i) films formed by equilibrium adsorption from oleamide solutions in oil, (ii) Langmuir-Blodgett films cast at 1 and 25 mN m(-1), (iii) thick spin-cast films. Both L-B and spin-cast films were examined in air and under oil. The adsorbate formed in the 1 mN m(-1) film in air showed little orientational order. For this film, the spectroscopic results and the ellipsometric thickness point to a relatively conformationally disordered monolayer that is oriented principally in the plane of the interface. Direct adsorption to the metal interface from oil results in SFG spectra of oleamide that are comparable to those observed for the 1 mN m(-1) L-B film in air. In contrast, SFG and RAIRS results for the 25 mN m(-1) film in air and SFG spectra of the spin-cast film in air both show strong conformational ordering and orientational alignment normal to the interface. The 25 mN m(-1) film has an ellipsometric thickness almost twice that of the 1 mN m(-1) L-B film. Taken in combination with the spectroscopic results, this is indicative of a well packed monolayer in air in which the hydrocarbon chain is in an essentially defect-free extended conformation with the methyl terminus oriented away from the surface. A similar structure is also deduced for the surface of the spin-cast film in air. Upon immersion of the 25 mN m(-1) L-B film in oil the SFG spectra show that this film rapidly adopts a relatively disordered structure similar to that seen for the 1 mN m(-1) L-B film in air. Immersion of the spin-cast film in oil results in the gradual disordering of the amide film over a period of several days until the observed spectra become essentially identical to those observed for direct adsorption of oleamide from oil.

All-solid-state quasi-CW yellow laser with intracavity self-Raman conversion and sum frequency generation

International Nuclear Information System (INIS)

Kananovich, A; Grabtchikov, A; Orlovich, V; Demidovich, A; Danailov, M

2010-01-01

Quasi continuous-wave (qCW) yellow emission (pulse duration 5 ms, repetition rate 20 Hz) at 559 nm is demonstrated through intracavity sum frequency generation (SFG) of Stokes and fundamental fields in Nd:YVO 4 diode pumped self-Raman laser for the first time. Average in pulse output power at 559 nm was 0.47 W for 22 W of pump power, which corresponds to 2.1% of diode-to-yellow efficiency. The pulsed mode of operation was due to diode pump modulation and was used to reduce thermal stress of the crystal

Continuous-wave sodium D2 resonance radiation generated in single-pass sum-frequency generation with periodically poled lithium niobate.

Science.gov (United States)

Yue, J; She, C-Y; Williams, B P; Vance, J D; Acott, P E; Kawahara, T D

2009-04-01

With two cw single-mode Nd:YAG lasers at 1064 and 1319 nm and a periodically poled lithium niobate crystal, 11 mW of 2 kHz/100 ms bandwidth single-mode tunable 589 nm cw radiation has been detected using single-pass sum-frequency generation. The demonstrated conversion efficiency is approximately 3.2%[W(-1) cm(-1)]. This compact solid-state light source has been used in a solid-state-dye laser hybrid sodium fluorescence lidar transmitter to measure temperatures and winds in the upper atmosphere (80-105 km); it is being implemented into the transmitter of a mobile all-solid-state sodium temperature and wind lidar under construction.

Giant enhancement of sum-frequency yield by surface-plasmon excitation

NARCIS (Netherlands)

van der Ham, E. W. M.; Vrehen, Q. H. F.; Eliel, E. R.; Yakovlev, V. A.; Valieva, E. V.; Kuzik, L. A.; Petrov, J. E.; Sychugov, V. A.; van der Meer, A. F. G.

1999-01-01

We show experimentally that the radiation generated in infrared-visible sum-frequency mixing at an air-silver interface can be greatly enhanced when the visible input beam excites a surface plasmon-polariton at the interface. With either a prism or a grating used to couple the visible radiation with

Difference frequency generation spectroscopy as a vibrational optical activity measurement tool.

Science.gov (United States)

Cheon, Sangheon; Cho, Minhaeng

2009-03-19

Vibrational optical activity (VOA) of chiral molecules in condensed phases can be studied by using vibrational circular dichroism and Raman optical activity measurement techniques. Recently, IR-vis sum frequency generation has shown to be an alternative VOA measurement method. Such a three-wave-mixing method employing a polarization modulation technique can be a potentially useful VOA measurement tool. Here, a theoretical description of difference frequency generation (DFG) employing circularly polarized visible radiations is presented. Frequency scanning to obtain a VOA-DFG spectrum is achieved by controlling the difference between the two electronically nonresonant incident radiation frequencies. If the two incident beams are linearly polarized and their polarization directions are perpendicular to each other, one can selectively measure the all-electric-dipole-allowed chiral component of the DFG susceptibility. In addition, by using circularly polarized beams and taking the DFG difference intensity signal, which is defined as the difference between left and right circularly polarized DFG signals, additional chiral susceptibility components originating from the electric quadrupole transition can be measured. The DFG as a novel VOA measurement technique for solution samples containing chiral molecules will therefore be a useful coherent spectroscopic tool for determining absolute configuration of chiral molecules in condensed phases.

Generation and tunable enhancement of a sum-frequency signal in lithium niobate nanowires

Science.gov (United States)

Sergeyev, Anton; Reig Escalé, Marc; Grange, Rachel

2017-02-01

Recent developments in the fabrication of lithium niobate (LiNbO3) structures down to the nanoscale opens up novel applications of this versatile material in nonlinear optics. Current nonlinear optical studies in sub-micron waveguides are mainly restricted to the generation of second and third harmonics. In this work, we demonstrate the generation and waveguiding of the sum-frequency generation (SFG) signal in a single LiNbO3 nanowire with a cross-section of 517 nm  ×  654 nm. Furthermore, we enhance the guided SFG signal 17.9 times by means of modal phase matching. We also display tuning of the phase-matched wavelength by varying the nanowire cross-section and changing the polarization of the incident laser. The results prove that LiNbO3 nanowires can be successfully used for nonlinear wave-mixing applications and assisting the miniaturization of optical devices. , which features invited work from the best early-career researchers working within the scope of J Phys D. This project is part of the Journal of Physics series’ 50th anniversary celebrations in 2017. Rachel Grange was selected by the Editorial Board of J Phys D as an Emerging Leader.

Study of the Imidazolium-Based Ionic Liquid - ag Electrified Interface on the CO_{2} Electroreduction by Sum Frequency Spectroscopy.

Science.gov (United States)

Garcia Rey, Natalia; Dlott, Dana

2017-06-01

Imidazolium based ionic liquids (ILs) have been used as a promising system to improve the CO_{2} electroreduction at lower overpotential than other organic or aqueous electrolytes^{1}. Although the detailed mechanism of the CO_{2} electroreduction on Ag has not been elucidated yet, we have developed a methodology to study the electrified interface during the CO_{2} electroreduction using sum frequency generation (SFG) spectroscopy in combination with cyclic voltammetry^{2}. In this work, we tuned the composition of imidazolium-based ILs by exchanging the anion or the functional groups of the imidazolium. We use the nonresonant SFG (NR-SFG) to study the IL-Ag interface and resonant SFG (RES-SFG) to identify the CO adsorbed on the electrode and monitor the Stark shift as a function of cell potential. In previous studies on CO_{2} electroreduction in the IL: 1-ethyl-3-methylimidazolium tetrafluorborate (EMIM-BF_{4}) on Ag, we showed three events occurred at the same potential (-1.33 V vs. Ag/AgCl): the current associated with CO_{2} electroreduction increased, the Stark shift of the adsorbed atop CO doubled in magnitude and the EMIM-BF_{4} underwent a structural transition^{3}. In addition, we also observed how the structural transition of the EMIM-BF_{4} electrolyte shift to lower potentials when the IL is mixed with water. It is known that water enhances the CO_{2} electroreduction producing more CO^{4}. Moreover, the CO is adsorbed in multi-bonded and in atop sites when more water is present in the electrolyte. ^{1}Lau, G. P. S.; Schreier, M.; Vasilyev, D.; Scopelliti, R.; Grätzel, M.; Dyson, P. J., New Insights into the Role of Imidazolium-Based Promoters for the Electroreduction of CO_{2} on a Silver Electrode. J. Am. Chem. Soc. 2016, 138, 7820-7823. ^{2}Garcia Rey, N.; Dlott, D. D., Studies of Electrochemical Interfaces by Broadband Sum Frequency Generation. J. Electroanal. Chem. 2016. DOI:10.1016/j.jelechem.2016.12.023. ^{3}Garcia Rey, N.; Dlott, D. D

Laser Spectroscopy and Frequency Combs

International Nuclear Information System (INIS)

Hänsch, Theodor W; Picqué, Nathalie

2013-01-01

The spectrum of a frequency comb, commonly generated by a mode-locked femtosecond laser consists of several hundred thousand precisely evenly spaced spectral lines. Such laser frequency combs have revolutionized the art measuring the frequency of light, and they provide the long-missing clockwork for optical atomic clocks. The invention of the frequency comb technique has been motivated by precision laser spectroscopy of the simple hydrogen atom. The availability of commercial instruments is facilitating the evolution of new applications far beyond the original purpose. Laser combs are becoming powerful instruments for broadband molecular spectroscopy by dramatically improving the resolution and recording speed of Fourier spectrometers and by creating new opportunities for highly multiplexed nonlinear spectroscopy, such as two-photon spectroscopy or coherent Raman spectroscopy. Other emerging applications of frequency combs range from fundamental research in astronomy, chemistry, or attosecond science to telecommunications and satellite navigation

Nonlinear beam clean-up using resonantly enhanced sum-frequency mixing

DEFF Research Database (Denmark)

Karamehmedovic, Emir; Pedersen, Christian; Jensen, Ole Bjarlin

2009-01-01

We investigate the possibility of improving the beam quality and obtaining high conversion efficiency in nonlinear sum-frequency generation. A 765 nm beam from an external cavity tapered diode laser is single-passed through a nonlinear crystal situated in the high intracavity field of a 1342 nm N......:YVO4 laser, generating a SFG beam at 488 nm. The ECDL have MH^2=1.9 and MV^2=2.4 and the solid-state laser has M^2...

Dense electro-optic frequency comb generated by two-stage modulation for dual-comb spectroscopy.

Science.gov (United States)

Wang, Shuai; Fan, Xinyu; Xu, Bingxin; He, Zuyuan

2017-10-01

An electro-optic frequency comb enables frequency-agile comb-based spectroscopy without using sophisticated phase-locking electronics. Nevertheless, dense electro-optic frequency combs over broad spans have yet to be developed. In this Letter, we propose a straightforward and efficient method for electro-optic frequency comb generation with a small line spacing and a large span. This method is based on two-stage modulation: generating an 18 GHz line-spacing comb at the first stage and a 250 MHz line-spacing comb at the second stage. After generating an electro-optic frequency comb covering 1500 lines, we set up an easily established mutually coherent hybrid dual-comb interferometer, which combines the generated electro-optic frequency comb and a free-running mode-locked laser. As a proof of concept, this hybrid dual-comb interferometer is used to measure the absorption and dispersion profiles of the molecular transition of H 13 CN with a spectral resolution of 250 MHz.

Facet-specific interaction between methanol and TiO2 probed by sum-frequency vibrational spectroscopy.

Science.gov (United States)

Yang, Deheng; Li, Yadong; Liu, Xinyi; Cao, Yue; Gao, Yi; Shen, Y Ron; Liu, Wei-Tao

2018-04-24

The facet-specific interaction between molecules and crystalline catalysts, such as titanium dioxides (TiO 2 ), has attracted much attention due to possible facet-dependent reactivity. Using surface-sensitive sum-frequency vibrational spectroscopy, we have studied how methanol interacts with different common facets of crystalline TiO 2 , including rutile(110), (001), (100), and anatase(101), under ambient temperature and pressure. We found that methanol adsorbs predominantly in the molecular form on all of the four surfaces, while spontaneous dissociation into methoxy occurs preferentially when these surfaces become defective. Extraction of Fermi resonance coupling between stretch and bending modes of the methyl group in analyzing adsorbed methanol spectra allows determination of the methanol adsorption isotherm. The isotherms obtained for the four surfaces are nearly the same, yielding two adsorbed Gibbs free energies associated with two different adsorption configurations singled out by ab initio calculations. They are ( i ) ∼-20 kJ/mol for methanol with its oxygen attached to a low-coordinated surface titanium, and ( ii ) ∼-5 kJ/mol for methanol hydrogen-bonded to a surface oxygen and a neighboring methanol molecule. Despite similar adsorption energetics, the Fermi resonance coupling strength for adsorbed methanol appears to depend sensitively on the surface facet and coverage.

Discovery of deep and shallow trap states from step structures of rutile TiO2 vicinal surfaces by second harmonic and sum frequency generation spectroscopy

International Nuclear Information System (INIS)

Takahashi, Hiroaki; Watanabe, Ryosuke; Miyauchi, Yoshihiro; Mizutani, Goro

2011-01-01

In this report, local electronic structures of steps and terraces on rutile TiO 2 single crystal faces were studied by second harmonic and sum frequency generation (SHG/SFG) spectroscopy. We attained selective measurement of the local electronic states of the step bunches formed on the vicinal (17 18 1) and (15 13 0) surfaces using a recently developed step-selective probing technique. The electronic structures of the flat (110)-(1x1) (the terrace face of the vicinal surfaces) and (011)-(2x1) surfaces were also discussed. The SHG/SFG spectra showed that step structures are mainly responsible for the formation of trap states, since significant resonances from the trap states were observed only from the vicinal surfaces. We detected deep hole trap (DHT) states and shallow electron trap (SET) states selectively from the step bunches on the vicinal surfaces. Detailed analysis of the SHG/SFG spectra showed that the DHT and SET states are more likely to be induced at the top edges of the step bunches than on their hillsides. Unlike the SET states, the DHT states were observed only at the step bunches parallel to [1 1 1][equivalent to the step bunches formed on the (17 18 1) surface]. Photocatalytic activity for each TiO 2 sample was also measured through methylene blue photodegradation reactions and was found to follow the sequence: (110) < (17 18 1) < (15 13 0) < (011), indicating that steps along [0 0 1] are more reactive than steps along [1 1 1]. This result implies that the presence of the DHT states observed from the step bunches parallel to [1 1 1] did not effectively contribute to the methylene blue photodegradation reactions.

Sensibility to Changes of Vibrational Modes of Excited Electron: Sum Frequency Signals Versus Difference Frequency Signals

International Nuclear Information System (INIS)

Gu Anna; Liang Xianting

2011-01-01

In this paper, we investigate a two electronic level system with vibrational modes coupled to a Brownian oscillator bath. The difference frequency generation (DFG) signals and sum frequency generation (SFG) signals are calculated. It is shown that, for the same model, the SFG signals are more sensitive than the DFG signals to the changes of the vibrational modes of the electronic two-level system. Because the SFG conversion efficiency can be improved by using the time-delay method, the findings in this paper predict that the SFG spectrum may probe the changes of the microstructure more effectively. (electromagnetism, optics, acoustics, heat transfer, classical mechanics, and fluid dynamics)

NOLM-based all-optical 40 Gbit/s format conversion through sum-frequency generation (SFG) in a PPLN waveguide

Science.gov (United States)

Wang, Jian; Sun, Junqiang

2005-11-01

A novel all-optical format conversion scheme from NRZ to RZ based on sum-frequency generation (SFG) in a periodically poled LiNbO 3 (PPLN) waveguide is proposed, using a nonlinear optical loop mirror (NOLM). The conversion mechanism relies on the combination of attenuation and nonlinear phase shift induced on the clockwise signal field during the SFG process. The SFG between pump, and co- and counter- propagating signals in the PPLN waveguide are numerically studied, showing that counter-propagating SFG can be ignored when quasi-phase matching (QPM) for SFG during co-propagating interaction. The nonlinear phase shift induced on the clockwise signal field is analyzed in detail, showing that it is more effective to yield large values for nonlinear phase shift when appropriately phase mismatched for the SFG process. Two tuning schemes are proposed depend on whether the sum-frequency wavelength is variable or fixed. It is found that the latter has a rather wide 3dB signal conversion bandwidth approximately 154nm. Finally, the influence of reversible process of SFG is discussed and the optimum arrangement of pump and signal peak powers is theoretically demonstrated. The result shows that proper power arrangement, pump width, and waveguide length are necessary for achieving a good conversion effect.

Frequency-agile dual-comb spectroscopy

OpenAIRE

Millot, Guy; Pitois, Stéphane; Yan, Ming; Hovannysyan, Tatevik; Bendahmane, Abdelkrim; Hänsch, Theodor W.; Picqué, Nathalie

2015-01-01

We propose a new approach to near-infrared molecular spectroscopy, harnessing advanced concepts of optical telecommunications and supercontinuum photonics. We generate, without mode-locked lasers, two frequency combs of slightly different repetition frequencies and moderate, but rapidly tunable, spectral span. The output of a frequency-agile continuous wave laser is split and sent into two electro-optic intensity modulators. Flat-top low-noise frequency combs are produced by wave-breaking in ...

Mid-Infrared Frequency-Agile Dual-Comb Spectroscopy

Science.gov (United States)

Luo, Pei-Ling; Yan, Ming; Iwakuni, Kana; Millot, Guy; Hänsch, Theodor W.; Picqué, Nathalie

2016-06-01

We demonstrate a new approach to mid-infrared dual-comb spectroscopy. It opens up new opportunities for accurate real-time spectroscopic diagnostics and it significantly simplifies the technique of dual-comb spectroscopy. Two mid-infrared frequency combs of slightly different repetition frequencies and moderate, but rapidly tunable, spectral span are generated in the 2800-3200 cm-1 region. The generators rely on electro-optic modulators, nonlinear fibers for spectral broadening and difference frequency generation and do not involve mode-locked lasers. Flat-top frequency combs span up to 10 cm-1 with a comb line spacing of 100 MHz (3×10-3 cm-1). The performance of the spectrometer without any phase-lock electronics or correction scheme is illustrated with spectra showing resolved comb lines and Doppler-limited spectra of methane. High precision on the spectroscopic parameter (line positions and intensities) determination is demonstrated for spectra measured on a millisecond time scale and it is validated with comparison with literature data. G. Millot, S. Pitois, M. Yan, T. Hovannysyan, A. Bendahmane, T.W. Hänsch, N. Picqué, Frequency-agile dual-comb spectroscopy, Nature Photonics 10, 27-30 (2016).

Polarization entanglement of sum-frequency photons: A tool to probe the Markovian limit

Science.gov (United States)

Volkov, Victor; Chelli, Riccardo

2015-06-01

The article addresses the possibility of entanglement-specific infrared-visible sum-frequency generation spectroscopy. In the case of an anisotropic interface, it is possible to employ SSS and PSS polarizations to detect responses not only specific to χY Y Y and χX Y Y nonlinearities, but also to higher-order χ(Y Y Y )(X Y Y ) and χ(X Y Y )(Y Y Y ) nonlinearities. Using quantum mechanical studies of the rhenium complex [Re (OH) 3(CO) 3] as a molecular model, we demonstrate that if such complexes would form an anisotropic orientational distribution at a surface, under the considered geometry and the polarization settings, we may prepare quantum correlated C =O vibrational states to emit polarization-entangled photons. Accordingly, we explore the possibility of a polarization-measurement protocol to extract spectral signatures of the entangled states. The response would be informative on intramolecular interactions. As a result, we discuss the possible practical implications in probing dynamics at interfaces, and different opportunities in the preparation of entangled vibrational states of quantified fidelity.

Vibrational Dynamics of Interfacial Water by Free Induction Decay Sum Frequency Generation (FID-SFG) at the Al2O3(1120)/H2O Interface.

Science.gov (United States)

Boulesbaa, Abdelaziz; Borguet, Eric

2014-02-06

The dephasing dynamics of a vibrational coherence may reveal the interactions of chemical functional groups with their environment. To investigate this process at a surface, we employ free induction decay sum frequency generation (FID-SFG) to measure the time that it takes for free OH stretch oscillators at the charged (pH ≈ 13, KOH) interface of alumina/water (Al2O3/H2O) to lose their collective coherence. By employing noncollinear optical parametric amplification (NOPA) technology and nonlinear vibrational spectroscopy, we showed that the single free OH peak actually corresponds to two distinct oscillators oriented opposite to each other and measured the total dephasing time, T2, of the free OH stretch modes at the Al2O3/H2O interface with a sub-40 fs temporal resolution. Our results suggested that the free OH oscillators associated with interfacial water dephase on the time scale of 89.4 ± 6.9 fs, whereas the homogeneous dephasing of interfacial alumina hydroxyls is an order of magnitude slower.

Quantum Mechanical Calculations of Vibrational Sum-Frequency-Generation (SFG) Spectra of Cellulose: Dependence of the CH and OH Peak Intensity on the Polarity of Cellulose Chains within the SFG Coherence Domain.

Science.gov (United States)

Lee, Christopher M; Chen, Xing; Weiss, Philip A; Jensen, Lasse; Kim, Seong H

2017-01-05

Vibrational sum-frequency-generation (SFG) spectroscopy is capable of selectively detecting crystalline biopolymers interspersed in amorphous polymer matrices. However, the spectral interpretation is difficult due to the lack of knowledge on how spatial arrangements of crystalline segments influence SFG spectra features. Here we report time-dependent density functional theory (TD-DFT) calculations of cellulose crystallites in intimate contact with two different polarities: parallel versus antiparallel. TD-DFT calculations reveal that the CH/OH intensity ratio is very sensitive to the polarity of the crystallite packing. Theoretical calculations of hyperpolarizability tensors (β abc ) clearly show the dependence of SFG intensities on the polarity of crystallite packing within the SFG coherence length, which provides the basis for interpretation of the empirically observed SFG features of native cellulose in biological systems.

Experimental evidence for an optical interference model for vibrational sum frequency generation on multilayer organic thin film systems. I. Electric dipole approximation

International Nuclear Information System (INIS)

O’Brien, Daniel B.; Massari, Aaron M.

2015-01-01

In the field of vibrational sum frequency generation spectroscopy (VSFG) applied to organic thin film systems, a significant challenge to data analysis is in the accurate description of optical interference effects. Herein, we provide experimental evidence that a model recently developed in our lab provides an accurate description of this phenomenon. We studied the organic small molecule N,N′-dioctyl-3,4,9,10-perylenedicarboximide vapor deposited as a thickness gradient on silicon wafer substrates with two oxide thicknesses and two surface preps. VSFG data were obtained using the ssp and the sps polarization combinations in the imide carbonyl stretching region as a function of organic thickness. In this first of two reports, the data are modeled and interpreted within the ubiquitous electric dipole approximation for VSFG. The intrinsic sample responses are parameterized during the fitting routines while optical interference effects are simply calculated from the model using known refractive indices, thin film thicknesses, and beam angles. The results indicate that the thin film model provides a good description of optical interferences, indicating that interfacial terms are significant. Inconsistencies between the fitting results within the bounds of the electric dipole response motivate deliberation for additional effects to be considered in the second report

Experimental evidence for an optical interference model for vibrational sum frequency generation on multilayer organic thin film systems. I. Electric dipole approximation.

Science.gov (United States)

O'Brien, Daniel B; Massari, Aaron M

2015-01-14

In the field of vibrational sum frequency generation spectroscopy (VSFG) applied to organic thin film systems, a significant challenge to data analysis is in the accurate description of optical interference effects. Herein, we provide experimental evidence that a model recently developed in our lab provides an accurate description of this phenomenon. We studied the organic small molecule N,N'-dioctyl-3,4,9,10-perylenedicarboximide vapor deposited as a thickness gradient on silicon wafer substrates with two oxide thicknesses and two surface preps. VSFG data were obtained using the ssp and the sps polarization combinations in the imide carbonyl stretching region as a function of organic thickness. In this first of two reports, the data are modeled and interpreted within the ubiquitous electric dipole approximation for VSFG. The intrinsic sample responses are parameterized during the fitting routines while optical interference effects are simply calculated from the model using known refractive indices, thin film thicknesses, and beam angles. The results indicate that the thin film model provides a good description of optical interferences, indicating that interfacial terms are significant. Inconsistencies between the fitting results within the bounds of the electric dipole response motivate deliberation for additional effects to be considered in the second report.

Experimental evidence for an optical interference model for vibrational sum frequency generation on multilayer organic thin film systems. I. Electric dipole approximation

Energy Technology Data Exchange (ETDEWEB)

O’Brien, Daniel B.; Massari, Aaron M., E-mail: massari@umn.edu [Department of Chemistry, University of Minnesota—Twin Cities, 207 Pleasant Street SE, Minneapolis, Minnesota 55455 (United States)

2015-01-14

In the field of vibrational sum frequency generation spectroscopy (VSFG) applied to organic thin film systems, a significant challenge to data analysis is in the accurate description of optical interference effects. Herein, we provide experimental evidence that a model recently developed in our lab provides an accurate description of this phenomenon. We studied the organic small molecule N,N′-dioctyl-3,4,9,10-perylenedicarboximide vapor deposited as a thickness gradient on silicon wafer substrates with two oxide thicknesses and two surface preps. VSFG data were obtained using the ssp and the sps polarization combinations in the imide carbonyl stretching region as a function of organic thickness. In this first of two reports, the data are modeled and interpreted within the ubiquitous electric dipole approximation for VSFG. The intrinsic sample responses are parameterized during the fitting routines while optical interference effects are simply calculated from the model using known refractive indices, thin film thicknesses, and beam angles. The results indicate that the thin film model provides a good description of optical interferences, indicating that interfacial terms are significant. Inconsistencies between the fitting results within the bounds of the electric dipole response motivate deliberation for additional effects to be considered in the second report.

Broader energy distribution of CO adsorbed at polycrystalline Pt electrode in comparison with that at Pt(111) electrode in H_2SO_4 solution confirmed by potential dependent IR/visible double resonance sum frequency generation spectroscopy

International Nuclear Information System (INIS)

Yang, Shuo; Noguchi, Hidenori; Uosaki, Kohei

2017-01-01

Highlights: • Electrochemical SFG spectroscopy is an efficient in situ probe of electronic structure at electrochemical interface. • Electrooxidation performances of CO adsorbed on polycrystalline Pt and Pt(111) electrodes were compared. • The enhanced SFG signal of CO on Pt electrodes was observed due to a vibrational-electronic double resonance effect. • The broader energy distribution of 5sa state of CO on polycrystalline Pt than on Pt(111) is proved by SFG results. - Abstract: Electrochemical cyclic voltammetry and potential dependent double resonance sum frequency generation (DR-SFG) spectroscopy were performed on CO adsorbed on polycrystalline Pt and Pt(111) electrodes in H_2SO_4 solution to examine the effect of substrate on the electronic structure of CO. The dependence of SFG intensity on potential and visible energy for atop CO band was observed on both polycrystalline and single crystalline Pt electrodes. Enhancement of the SFG intensity was determined to be a direct result of a surface electronic resonance of the visible/SF light with the electronic transition from Fermi level of Pt to the 5σ_a anti-bonding state of adsorbed CO, in agreement with previous results. Interestingly, when compared to the Pt(111) electrode, the distribution width of the intensity enhancement region on polycrystalline Pt is broader than on Pt(111). This suggests that the energy distribution of the 5σ_a state of CO on polycrystalline Pt surface is broader than that on Pt(111) due to the complex surface structure of the polycrystalline Pt electrode.

Amine Chemistry at Aqueous Interfaces: The Study of Organic Amines in Neutralizing Acidic Gases at an Air/Water Surface Using Vibrational Sum Frequency Spectroscopy

Science.gov (United States)

McWilliams, L.; Wren, S. N.; Valley, N. A.; Richmond, G.

2014-12-01

Small organic bases have been measured in atmospheric samples, with their sources ranging from industrial processing to animal husbandry. These small organic amines are often highly soluble, being found in atmospheric condensed phases such as fogwater and rainwater. Additionally, they display acid-neutralization ability often greater than ammonia, yet little is known regarding their kinetic and thermodynamic properties. This presentation will describe the molecular level details of a model amine system at the vapor/liquid interface in the presence of acidic gas. We find that this amine system shows very unique properties in terms of its bonding, structure, and orientation at aqueous surfaces. The results of our studies using a combination of computation, vibrational sum frequency spectroscopy, and surface tension will report the properties inherent to these atmospherically relevant species at aqueous surfaces.

Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope.

Science.gov (United States)

Lee, Christopher M; Kafle, Kabindra; Huang, Shixin; Kim, Seong H

2016-01-14

A broadband sum frequency generation (BB-SFG) spectrometer with multimodal (MM) capabilities was constructed, which could be routinely reconfigured for tabletop experiments in reflection, transmission, and total internal reflection (TIR) geometries, as well as microscopic imaging. The system was constructed using a Ti:sapphire amplifier (800 nm, pulse width = 85 fs, repetition rate = 2 kHz), an optical parameter amplification (OPA) system for production of broadband IR pulses tunable between 1000 and 4000 cm(-1), and two Fabry-Pérot etalons arranged in series for production of narrowband 800 nm pulses. The key feature allowing the MM operation was the nearly collinear alignment of the visible (fixed, 800 nm) and infrared (tunable, 1000-4000 cm(-1)) pulses which were spatially separated. Physical insights discussed in this paper include the comparison of spectral bandwidth produced with 40 and 85 fs pump beams, the improvement of spectral resolution using etalons, the SFG probe volume in bulk analysis, the normalization of SFG signals, the stitching of multiple spectral segments, and the operation in different modes for air/liquid and adsorbate/solid interfaces, bulk samples, as well as spectral imaging combined with principle component analysis (PCA). The SFG spectral features obtained with the MM-BB-SFG system were compared with those obtained with picosecond-scanning-SFG system and high-resolution BB-SFG system (HR-BB-SFG) for dimethyl sulfoxide, α-pinene, and various samples containing cellulose (purified commercial products, Cladophora cell wall, cotton and flax fibers, and onion epidermis cell wall).

2D heterodyne-detected sum frequency generation study on the ultrafast vibrational dynamics of H{sub 2}O and HOD water at charged interfaces

Energy Technology Data Exchange (ETDEWEB)

Inoue, Ken-ichi; Singh, Prashant C. [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Nihonyanagi, Satoshi; Tahara, Tahei, E-mail: tahei@riken.jp [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Ultrafast Spectroscopy Research Team, RIKEN Center for Advanced Photonics, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Yamaguchi, Shoichi [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Department of Applied Chemistry, Saitama University, 255 Shimo-Okubo, Saitama 338-8570 (Japan)

2015-06-07

Two-dimensional heterodyne-detected vibrational sum-frequency generation (2D HD-VSFG) spectroscopy is applied to study the ultrafast vibrational dynamics of water at positively charged aqueous interfaces, and 2D HD-VSFG spectra of cetyltrimethylammonium bromide (CTAB)/water interfaces in the whole hydrogen-bonded OH stretch region (3000 cm{sup −1} ≤ ω{sub pump} ≤ 3600 cm{sup −1}) are measured. 2D HD-VSFG spectrum of the CTAB/isotopically diluted water (HOD-D{sub 2}O) interface exhibits a diagonally elongated bleaching lobe immediately after excitation, which becomes round with a time constant of ∼0.3 ps due to spectral diffusion. In contrast, 2D HD-VSFG spectrum of the CTAB/H{sub 2}O interface at 0.0 ps clearly shows two diagonal peaks and their cross peaks in the bleaching region, corresponding to the double peaks observed at 3230 cm{sup −1} and 3420 cm{sup −1} in the steady-state HD-VSFG spectrum. Horizontal slices of the 2D spectrum show that the relative intensity of the two peaks of the bleaching at the CTAB/H{sub 2}O interface gradually change with the change of the pump frequency. We simulate the pump-frequency dependence of the bleaching feature using a model that takes account of the Fermi resonance and inhomogeneity of the OH stretch vibration, and the simulated spectra reproduce the essential features of the 2D HD-VSFG spectra of the CTAB/H{sub 2}O interface. The present study demonstrates that heterodyne detection of the time-resolved VSFG is critically important for studying the ultrafast dynamics of water interfaces and for unveiling the underlying mechanism.

High-resolution broadband terahertz spectroscopy via electronic heterodyne detection of photonically generated terahertz frequency comb.

Science.gov (United States)

Pavelyev, D G; Skryl, A S; Bakunov, M I

2014-10-01

We report an alternative approach to the terahertz frequency-comb spectroscopy (TFCS) based on nonlinear mixing of a photonically generated terahertz pulse train with a continuous wave signal from an electronic synthesizer. A superlattice is used as a nonlinear mixer. Unlike the standard TFCS technique, this approach does not require a complex double-laser system but retains the advantages of TFCS-high spectral resolution and wide bandwidth.

All-solid-state continuous-wave doubly resonant all-intracavity sum-frequency mixer.

Science.gov (United States)

Kretschmann, H M; Heine, F; Huber, G; Halldórsson, T

1997-10-01

A new resonator design for doubly resonant continuous-wave intracavity sum-frequency mixing is presented. We generated 212 mW of coherent radiation at 618 nm by mixing the radiation of a 1080-nm Nd(3+):YAlO(3) laser and a 1444-nm Nd(3+):YAG laser. Two different mixing resonator setups and several nonlinear-optical crystals were investigated. So far output is limited by unequal performance of the two fundamental lasers and coating problems of the nonlinear crystals.

Harmonic generation with a dual frequency pulse.

Science.gov (United States)

Keravnou, Christina P; Averkiou, Michalakis A

2014-05-01

Nonlinear imaging was implemented in commercial ultrasound systems over the last 15 years offering major advantages in many clinical applications. In this work, pulsing schemes coupled with a dual frequency pulse are presented. The pulsing schemes considered were pulse inversion, power modulation, and power modulated pulse inversion. The pulse contains a fundamental frequency f and a specified amount of its second harmonic 2f. The advantages and limitations of this method were evaluated with both acoustic measurements of harmonic generation and theoretical simulations based on the KZK equation. The use of two frequencies in a pulse results in the generation of the sum and difference frequency components in addition to the other harmonic components. While with single frequency pulses, only power modulation and power modulated pulse inversion contained odd harmonic components, with the dual frequency pulse, pulse inversion now also contains odd harmonic components.

Harmonic sums and polylogarithms generated by cyclotomic polynomials

Energy Technology Data Exchange (ETDEWEB)

Ablinger, Jakob; Schneider, Carsten [Johannes Kepler Univ., Linz (Austria). Research Inst. for Symbolic Computation; Bluemlein, Johannes [Deutsches Elektronen-Synchrotron (DESY), Zeuthen (Germany)

2011-05-15

The computation of Feynman integrals in massive higher order perturbative calculations in renormalizable Quantum Field Theories requires extensions of multiply nested harmonic sums, which can be generated as real representations by Mellin transforms of Poincare-iterated integrals including denominators of higher cyclotomic polynomials. We derive the cyclotomic harmonic polylogarithms and harmonic sums and study their algebraic and structural relations. The analytic continuation of cyclotomic harmonic sums to complex values of N is performed using analytic representations. We also consider special values of the cyclotomic harmonic polylogarithms at argument x=1, resp., for the cyclotomic harmonic sums at N{yields}{infinity}, which are related to colored multiple zeta values, deriving various of their relations, based on the stuffle and shuffle algebras and three multiple argument relations. We also consider infinite generalized nested harmonic sums at roots of unity which are related to the infinite cyclotomic harmonic sums. Basis representations are derived for weight w=1,2 sums up to cyclotomy l=20. (orig.)

Tunable, continuous-wave, ultraviolet source based on intracavity sum-frequency-generation in an optical parametric oscillator using BiB₃O₆.

Science.gov (United States)

Devi, Kavita; Kumar, S Chaitanya; Ebrahim-Zadeh, M

2013-10-21

We report a continuous-wave (cw) source of tunable radiation across 333-345 nm in the ultraviolet (UV) using bismuth triborate, BiB₃O₆ (BIBO) as the nonlinear gain material. The source is based on internal sum-frequency-generation (SFG) in a cw singly-resonant optical parametric oscillator (OPO) pumped at 532 nm. The compact tunable source employs a 30-mm-long MgO:sPPLT crystal as the OPO gain medium and a 5-mm-long BIBO crystal for intracavity SFG of the signal and pump, providing up to 21.6 mW of UV power at 339.7 nm, with >15 mW over 64% of the SFG tuning range. The cw OPO is also tunable across 1158-1312 nm in the idler, delivering as much as 1.7 W at 1247 nm, with >1W over 65% of the tuning range. The UV output at maximum power exhibits passive power stability better than 3.4% rms and frequency stability of 193 GHz over more than one minute.

Efficient near diffraction limited blue light source by sum-frequency mixing of a BAL and a solid-state laser

DEFF Research Database (Denmark)

Sørensen, Knud Palmelund; Tidemand-Lichtenberg, Peter; Pedersen, Christian

2011-01-01

and slow axis of the diode, respectively. The BAL output beam is single-passed through a periodically poled KTiOPO4 (PPKTP) crystal placed in an intra-cavity beam waist of a 1064 nm Nd:YVO4 laser, resulting in 100 mW of sum-frequency generated blue output power. This corresponds to a power conversion......Sum-frequency mixing of an 808 nm broad area laser (BAL) with a build-in grating structure for spectral control and a 1064 nm solid-state laser is experimentally investigated. The spectrally improved 20 mu m wide BAL can deliver up to 700 mW of output power with an M-2 of 1.4 and 5.3 in the fast...

Ultrasensitive detection of atmospheric trace gases using frequency modulation spectroscopy

Science.gov (United States)

Cooper, David E.

1986-01-01

Frequency modulation (FM) spectroscopy is a new technique that promises to significantly extend the state-of-the-art in point detection of atmospheric trace gases. FM spectroscopy is essentially a balanced bridge optical heterodyne approach in which a small optical absorption or dispersion from an atomic or molecular species of interest generates an easily detected radio frequency (RF) signal. This signal can be monitored using standard RF signal processing techniques and is, in principle, limited only by the shot noise generated in the photodetector by the laser source employed. The use of very high modulation frequencies which exceed the spectral width of the probed absorption line distinguishes this technique from the well-known derivative spectroscopy which makes use of low (kHz) modulation frequencies. FM spectroscopy was recently extended to the 10 micron infrared (IR) spectral region where numerous polyatomic molecules exhibit characteristic vibrational-rotational bands. In conjunction with tunable semiconductor diode lasers, the quantum-noise-limited sensitivity of the technique should allow for the detection of absorptions as small as .00000001 in the IR spectral region. This sensitivity would allow for the detection of H2O2 at concentrations as low as 1 pptv with an integration time of 10 seconds.

In-Situ Measurement of Chirality of Molecules and Molecular Assemblies with Surface Nonlinear Spectroscopy

International Nuclear Information System (INIS)

Wang, Hongfei

2012-01-01

Developments in quantitative measurement and analysis in nonlinear surface spectroscopy, namely, second harmonic generation linear dichroism (SHG-LD) and sum frequency generation vibrational spectroscopy linear dichroism (SFG-VS-LD), provide new opportunities for probing the surface chirality of monolayers and thin films. In this book chapter, the up-to-date theoretical background and experimental methodology, as well as examples and future perspectives on the developments with surface nonlinear spectroscopy in surface chirality studies are to be summarized and outlined for general readers.

Self-assembled organic and fullerene monolayers characterisation by two-colour SFG spectroscopy: a pathway to meet doubly resonant SFG process

OpenAIRE

Humbert, C.; Caudano, Y.; Dreesen, Laurent; Sartenaer, Y.; Mani, A. A.; Silien, C.; Lemaire, J.-J.; Thiry, P. A.; Peremans, A.

2004-01-01

Two-colour sum-frequency generation (two-colour SFG) spectroscopy was used to probe both vibrational and electronic properties of 1-dodecanethiol/Ag(1 1 1), Au(1 1 1), and Pt(1 1 1), of 5-[p-(6-mercaptohexoxy)-phenyl]-10,15,20-triphenylporphin/Pt(1 1 1), and of C60/Ag(1 1 1). The role of the various physical parameters determining the sum-frequency generation (SFG) intensity equation is highlighted. The enhancement of the non-linear second order susceptibility in the aforementioned interfaces...

Femtosecond nonlinear spectroscopy at surfaces: Second-harmonic probing of hole burning at the Si(111)7x7 surface and Fourier-transform sum-frequency vibrational spectroscopy

International Nuclear Information System (INIS)

McGuire, John Andrew

2004-01-01

The high temporal resolution and broad bandwidth of a femtosecond laser system are exploited in a pair of nonlinear optical studies of surfaces. The dephasing dynamics of resonances associated with the adatom dangling bonds of the Si(111)7 x 7 surface are explored by transient second-harmonic hole burning, a process that can be described as a fourth-order nonlinear optical process. Spectral holes produced by a 100 fs pump pulse at about 800 nm are probed by the second harmonic signal of a 100 fs pulse tunable around 800 nm. The measured spectral holes yield homogeneous dephasing times of a few tens of femtoseconds. Fits with a Lorentzian spectral hole centered at zero probe detuning show a linear dependence of the hole width on pump fluence, which suggests that charge carrier-carrier scattering dominates the dephasing dynamics at the measured excitation densities. Extrapolation of the deduced homogeneous dephasing times to zero excitation density yields an intrinsic dephasing time of ∼ 70 fs. The presence of a secondary spectral hole indicates that scattering of the surface electrons with surface optical phonons at 570 cm -1 occurs within the first 200 fs after excitation. The broad bandwidth of femtosecond IR pulses is used to perform IR-visible sum frequency vibrational spectroscopy. By implementing a Fourier-transform technique, we demonstrate the ability to obtain sub-laser-bandwidth spectral resolution. FT-SFG yields a greater signal when implemented with a stretched visible pulse than with a femtosecond visible pulse. However, when compared with multichannel spectroscopy using a femtosecond IR pulse but a narrowband visible pulse, Fourier-transform SFG is found to have an inferior signal-to-noise ratio. A mathematical analysis of the signal-to-noise ratio illustrates the constraints on the Fourier-transform approach

Femtosecond nonlinear spectroscopy at surfaces: Second-harmonic probing of hole burning at the Si(111)7x7 surface and fourier-transform sum-frequency vibrational spectroscopy

Energy Technology Data Exchange (ETDEWEB)

McGuire, John Andrew [Univ. of California, Berkeley, CA (United States)

2004-11-24

The high temporal resolution and broad bandwidth of a femtosecond laser system are exploited in a pair of nonlinear optical studies of surfaces. The dephasing dynamics of resonances associated with the adatom dangling bonds of the Si(111)7 x 7 surface are explored by transient second-harmonic hole burning, a process that can be described as a fourth-order nonlinear optical process. Spectral holes produced by a 100 fs pump pulse at about 800 nm are probed by the second harmonic signal of a 100 fs pulse tunable around 800 nm. The measured spectral holes yield homogeneous dephasing times of a few tens of femtoseconds. Fits with a Lorentzian spectral hole centered at zero probe detuning show a linear dependence of the hole width on pump fluence, which suggests that charge carrier-carrier scattering dominates the dephasing dynamics at the measured excitation densities. Extrapolation of the deduced homogeneous dephasing times to zero excitation density yields an intrinsic dephasing time of {approx} 70 fs. The presence of a secondary spectral hole indicates that scattering of the surface electrons with surface optical phonons at 570 cm^-1 occurs within the first 200 fs after excitation. The broad bandwidth of femtosecond IR pulses is used to perform IR-visible sum frequency vibrational spectroscopy. By implementing a Fourier-transform technique, we demonstrate the ability to obtain sub-laser-bandwidth spectral resolution. FT-SFG yields a greater signal when implemented with a stretched visible pulse than with a femtosecond visible pulse. However, when compared with multichannel spectroscopy using a femtosecond IR pulse but a narrowband visible pulse, Fourier-transform SFG is found to have an inferior signal-to-noise ratio. A mathematical analysis of the signal-to-noise ratio illustrates the constraints on the Fourier-transform approach.

IR visible sum-frequency vibrational spectroscopy of Biphenyl-3 methylene thiol monolayer on gold and silver: effect of the visible wavelength on the SFG spectrum

Science.gov (United States)

Humbert, C.; Dreesen, L.; Mani, A. A.; Caudano, Y.; Lemaire, J.-J.; Thiry, P. A.; Peremans, A.

2002-04-01

We measured IR-visible sum-frequency generation spectra of CH 3-(C 6H 4) 2-(CH 2) 3-S-H (Biphenyl-3) self-assembled monolayers on a silver and a gold substrate. For the latter substrate, we observed different interference patterns between the resonant signal of the CH vibration and the non-resonant contribution of the substrate as a function of the visible beam wavelength. The non-linear response of the gold substrate is enhanced around 480 nm corresponding to the s-d interband transition. Such effect is not observed for the silver substrate the interband transition of which is located out of the investigated visible spectral range of 450-700 nm.

In-situ Studies of the Reactions of Bifunctional and Heterocyclic Molecules over Noble Metal Single Crystal and Nanoparticle Catalysts Studied with Kinetics and Sum-Frequency Generation Vibrational Spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Kliewer, Christopher J. [Univ. of California, Berkeley, CA (United States)

2009-06-30

Sum frequency generation surface vibrational spectroscopy (SFG-VS) in combination with gas chromatography (GC) was used in-situ to monitor surface bound reaction intermediates and reaction selectivities for the hydrogenation reactions of pyrrole, furan, pyridine, acrolein, crotonaldehyde, and prenal over Pt(111), Pt(100), Rh(111), and platinum nanoparticles under Torr reactant pressures and temperatures of 300K to 450K. The focus of this work is the correlation between the SFG-VS observed surface bound reaction intermediates and adsorption modes with the reaction selectivity, and how this is affected by catalyst structure and temperature. Pyrrole hydrogenation was investigated over Pt(111) and Rh(111) single crystals at Torr pressures. It was found that pyrrole adsorbs to Pt(111) perpendicularly by cleaving the N-H bond and binding through the nitrogen. However, over Rh(111) pyrrole adsorbs in a tilted geometry binding through the {pi}-aromatic orbitals. A surface-bound pyrroline reaction intermediate was detected over both surfaces with SFG-VS. It was found that the ring-cracking product butylamine is a reaction poison over both surfaces studied. Furan hydrogenation was studied over Pt(111), Pt(100), 10 nm cubic platinum nanoparticles and 1 nm platinum nanoparticles. The product distribution was observed to be highly structure sensitive and the acquired SFG-VS spectra reflected this sensitivity. Pt(100) exhibited more ring-cracking to form butanol than Pt(111), while the nanoparticles yielded higher selectivities for the partially saturated ring dihydrofuran. Pyridine hydrogenation was investigated over Pt(111) and Pt(100). The α-pyridyl surface adsorption mode was observed with SFG-VS over both surfaces. 1,4-dihydropyridine was seen as a surface intermediate over Pt(100) but not Pt(111). Upon heating the surfaces to 350K, the adsorbed pyridine changes to a flat-lying adsorption mode. No evidence was found for the pyridinium cation. The hydrogenation of the �

Dynamical local field, compressibility, and frequency sum rules for quasiparticles

International Nuclear Information System (INIS)

Morawetz, Klaus

2002-01-01

The finite temperature dynamical response function including the dynamical local field is derived within a quasiparticle picture for interacting one-, two-, and three-dimensional Fermi systems. The correlations are assumed to be given by a density-dependent effective mass, quasiparticle energy shift, and relaxation time. The latter one describes disorder or collisional effects. This parametrization of correlations includes local-density functionals as a special case and is therefore applicable for density-functional theories. With a single static local field, the third-order frequency sum rule can be fulfilled simultaneously with the compressibility sum rule by relating the effective mass and quasiparticle energy shift to the structure function or pair-correlation function. Consequently, solely local-density functionals without taking into account effective masses cannot fulfill both sum rules simultaneously with a static local field. The comparison to the Monte Carlo data seems to support such a quasiparticle picture

Experimental demonstration of wavelength conversion between ps-pulses based on cascaded sum- and difference frequency generation (SFG+DFG) in LiNbO3 waveguides

Science.gov (United States)

Wang, Jian; Sun, Junqiang; Lou, Chuanhong; Sun, Qizhen

2005-09-01

All-optical wavelength conversion between ps-pulses based on cascaded sum- and difference frequency generation (SFG+DFG) is proposed and experimentally demonstrated in periodically poled LiNbO3 (PPLN) waveguides. The signal pulse with 40-GHz repetition rate and 1.57- ps pulse width is adopted. The converted idler wavelength can be tuned from 1527.4 to 1540.5nm as the signal wavelength is varied from 1561.9 to 1548.4nm. No obvious changes of the pulse shape and width, also no chirp are observed in the converted idler pulse. The results imply that single-to-multiple channel wavelength conversions can be achieved by appropriately tuning the two pump wavelengths.

A new approach to sum frequency generation of single-frequency blue light in a coupled ring cavity

DEFF Research Database (Denmark)

Jensen, Ole Bjarlin; Petersen, Paul Michael

2014-01-01

We present a generic approach for the generation of tunable single-frequency light and demonstrate generation of more than 300 mW tunable light around 460 nm. One tapered diode laser is operated in a coupled ring cavity containing the nonlinear crystal and another tapered diode laser is sent thro...... through the nonlinear crystal in a single pass. A high conversion efficiency of more than 25 % of the single-pass laser is enabled by the high circulating power in the coupled cavity. The system is entirely self-stabilized with no need for electronic locking....

Alkyl chain interaction at the surface of room temperature ionic liquids: systematic variation of alkyl chain length (R = C(1)-C(4), C(8)) in both cation and anion of [RMIM][R-OSO(3)] by sum frequency generation and surface tension.

Science.gov (United States)

Santos, Cherry S; Baldelli, Steven

2009-01-29

The gas-liquid interface of halide-free 1,3-dialkylimidazolium alkyl sulfates [RMIM][R-OSO(3)] with R chain length from C(1)-C(4) and C(8) has been studied systematically using the surface-specific sum frequency generation (SFG) vibrational spectroscopy and surface tension measurements. From the SFG spectra, vibrational modes from the methyl group of both cation and anion are observed for all ionic liquid samples considered in the present study. These results suggest the presence of both ions at the gas-liquid interface, which is further supported by surface tension measurements. Surface tension data show a decreasing trend as the alkyl chain in the imidazolium cation is varied from methyl to butyl chain, with a specific anion. A similar trend is observed when the alkyl chain of the anion is modified and the cation is fixed.

Self-assembled organic and fullerene monolayers characterisation by two-colour SFG spectroscopy: a pathway to meet doubly resonant SFG process

International Nuclear Information System (INIS)

Humbert, C.; Caudano, Y.; Dreesen, L.; Sartenaer, Y.; Mani, A.A.; Silien, C.; Lemaire, J.-J.; Thiry, P.A.; Peremans, A.

2004-01-01

Two-colour sum-frequency generation (two-colour SFG) spectroscopy was used to probe both vibrational and electronic properties of 1-dodecanethiol/Ag(1 1 1), Au(1 1 1), and Pt(1 1 1), of 5-[p-(6-mercaptohexoxy)-phenyl]-10,15,20-triphenylporphin/Pt(1 1 1), and of C 60 /Ag(1 1 1). The role of the various physical parameters determining the sum-frequency generation (SFG) intensity equation is highlighted. The enhancement of the non-linear second order susceptibility in the aforementioned interfaces is explained in terms of metal interband transition, molecular electronic transition and of electron-phonon coupling, respectively

Self-assembled organic and fullerene monolayers characterisation by two-colour SFG spectroscopy: a pathway to meet doubly resonant SFG process

Science.gov (United States)

Humbert, C.; Caudano, Y.; Dreesen, L.; Sartenaer, Y.; Mani, A. A.; Silien, C.; Lemaire, J.-J.; Thiry, P. A.; Peremans, A.

2004-10-01

Two-colour sum-frequency generation (two-colour SFG) spectroscopy was used to probe both vibrational and electronic properties of 1-dodecanethiol/Ag(1 1 1), Au(1 1 1), and Pt(1 1 1), of 5-[ p-(6-mercaptohexoxy)-phenyl]-10,15,20-triphenylporphin/Pt(1 1 1), and of C 60/Ag(1 1 1). The role of the various physical parameters determining the sum-frequency generation (SFG) intensity equation is highlighted. The enhancement of the non-linear second order susceptibility in the aforementioned interfaces is explained in terms of metal interband transition, molecular electronic transition and of electron-phonon coupling, respectively.

In situ speciation of the functional groups at mineral/electrolyte interfaces by sum frequency vibrational spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Floersheimer, M.; Kruse, K.; Klenze, R.; Kim, J.I. [Institut fuer Nukleare Entsorgung, Forschungszentrum Karlsruhe, Postfach 3640, D-76021 Karlsruhe (Germany); Fanghaenel, Th. [Institut fuer Nukleare Entsorgung, Forschungszentrum Karlsruhe, Postfach 3640, D-76021 Karlsruhe (Germany); Physikalisch-Chemisches Institut, Ruprecht-Karls-Universitaet Heidelberg, Im Neuenheimer Feld 253, D-69120, Heidelberg (Germany)

2005-07-01

Full text of publication follows: In order to describe surface reactivity and adsorption/desorption processes on the molecular level, a large number of functional groups has been postulated. In most cases, however, a direct proof for the existence of these species in real aquatic environment is lacking because it is difficult to obtain chemical analytical information in situ under electrolyte with interface selectivity. Here we apply interface selective sum frequency (SF) vibrational spectroscopy to study the (001) and (110) surfaces of sapphire ({alpha}-Al{sub 2}O{sub 3}) under water between pH 4 and 12. This work is part of an ongoing fundamental study of the sorption mechanism of actinides on single crystals faces of sapphire by various experimental and theoretical techniques. Sapphire is used as a simple model for natural clay minerals and related iron phases. In the O-H stretch region of the infrared spectrum between 2800 and 4000 cm{sup -1}, we observe a surprisingly large number of 8 SF bands in total. Two of them are due to the polar ordered water film near the mineral surface which is well known from various aquatic interfaces. The other bands originate from up to 6 different aluminol species or from specifically [1] bound water molecules. The prominent peak of the (001) surface (SF intensity maximum at 3690 cm{sup -1}), we attribute to an OH species bridging two [1-4] aluminium atoms. At the (110) surface, the concentration of this species is considerably smaller. Another aluminol species that can be detected at the (001) and the (110) surface (signal maximum near 3450 cm{sup -1}) exhibits O-H bonds which are almost parallel to the interface plane. This species is probably the in-plane aluminol group predicted in recent molecular dynamics calculations [4]. SF spectroscopy allows us also to measure the absolute polar orientation of the water molecules adjacent to the mineral surface. The inversion of the molecules polar orientation upon alteration of the p

Frequency-agile dual-comb spectroscopy

Science.gov (United States)

Millot, Guy; Pitois, Stéphane; Yan, Ming; Hovhannisyan, Tatevik; Bendahmane, Abdelkrim; Hänsch, Theodor W.; Picqué, Nathalie

2016-01-01

Spectroscopic gas sensing and its applications to, for example, trace detection or chemical kinetics, require ever more demanding measurement times, acquisition rates, sensitivities, precisions and broad tuning ranges. Here, we propose a new approach to near-infrared molecular spectroscopy, utilizing advanced concepts of optical telecommunications and supercontinuum photonics. We generate, without mode-locked lasers, two frequency combs of slightly different repetition frequencies and moderate, but rapidly tunable, spectral span. The output of a frequency-agile continuous-wave laser is split and sent into two electro-optic intensity modulators. Flat-top low-noise frequency combs are produced by wave-breaking in a nonlinear optical fibre of normal dispersion. With a dual-comb spectrometer, we record Doppler-limited spectra spanning 60 GHz within 13 μs and an 80 kHz refresh rate, at a tuning speed of 10 nm s-1. The sensitivity for weak absorption is enhanced by a long gas-filled hollow-core fibre. New opportunities for real-time diagnostics may be opened up, even outside the laboratory.

Coupled-cluster sum-frequency generation nonlinear susceptibilities of methyl (CH3) and methylene (CH2) groups.

Science.gov (United States)

Tetsassi Feugmo, Conrard Giresse; Liégeois, Vincent; Champagne, Benoît

2017-11-15

The first vibrational sum frequency generation (SFG) spectra based on molecular properties calculated at the coupled cluster singles and doubles (CCSD) level of approximation have been simulated for interfacial model alkyl chains, providing benchmark data for comparisons with approximate methods, including density functional theory (DFT). The approach proceeds in three steps. In the first two steps, the molecular spectral properties are determined: the vibrational normal modes and frequencies and then the derivatives of the dipole moment and of the polarizability with respect to the normal coordinates. These derivatives are evaluated with a numerical differentiation approach, of which the accuracy was monitored using Romberg's procedure. Then, in the last step, a three-layer model is employed to evaluate the macroscopic second-order nonlinear optical responses and thereby the simulated SFG spectra of the alkyl interface. Results emphasize the following facts: (i) the dipole and polarizability derivatives calculated at the DFT level with the B3LYP exchange-correlation functional can differ, with respect to CCSD, by as much as ±10 to 20% and ±20 to 50% for the CH 3 and CH 2 vibrations, respectively; (ii) these differences are enhanced when considering the SFG intensities as well as their variations as a function of the experimental configuration (ppp versus ssp) and as a function of the tilt and rotation angles, defining the orientation of the alkyl chain at the interface; (iii) these differences originate from both the vibrational normal coordinates and the Cartesian derivatives of the dipole moment and polarizability; (iv) freezing the successive fragments of the alkyl chain strongly modifies the SFG spectrum and enables highlighting the delocalization effects between the terminal CH 3 group and its neighboring CH 2 units; and finally (v) going from the free chain to the free methyl model, and further to C 3v constraints on leads to large variations of two ratios

High-Pressure Catalytic Reactions of C6 Hydrocarbons on PlatinumSingle-Crystals and nanoparticles: A Sum Frequency Generation VibrationalSpectroscopic and Kinetic Study

Energy Technology Data Exchange (ETDEWEB)

Bratlie, Kaitlin [Univ. of California, Berkeley, CA (United States)

2007-01-01

Catalytic reactions of cyclohexene, benzene, n-hexane, 2-methylpentane, 3-methylpentane, and 1-hexene on platinum catalysts were monitored in situ via sum frequency generation (SFG) vibrational spectroscopy and gas chromatography (GC). SFG is a surface specific vibrational spectroscopic tool capable of monitoring submonolayer coverages under reaction conditions without gas-phase interference. SFG was used to identify the surface intermediates present during catalytic processes on Pt(111) and Pt(100) single-crystals and on cubic and cuboctahedra Pt nanoparticles in the Torr pressure regime and at high temperatures (300K-450K). At low pressures (<10^-6 Torr), cyclohexene hydrogenated and dehydrogenates to form cyclohexyl (C₆H₁₁) and π-allyl C₆H₉, respectively, on Pt(100). Increasing pressures to 1.5 Torr form cyclohexyl, π-allyl C₆H₉, and 1,4-cyclohexadiene, illustrating the necessity to investigate catalytic reactions at high-pressures. Simultaneously, GC was used to acquire turnover rates that were correlated to reactive intermediates observed spectroscopically. Benzene hydrogenation on Pt(111) and Pt(100) illustrated structure sensitivity via both vibrational spectroscopy and kinetics. Both cyclohexane and cyclohexene were produced on Pt(111), while only cyclohexane was formed on Pt(100). Additionally, π-allyl c-C₆H₉ was found only on Pt(100), indicating that cyclohexene rapidly dehydrogenates on the (100) surface. The structure insensitive production of cyclohexane was found to exhibit a compensation effect and was analyzed using the selective energy transfer (SET) model. The SET model suggests that the Pt-H system donates energy to the E_2u mode of free benzene, which leads to catalysis. Linear C₆ (n-hexane, 2-methylpentane, 3-methylpentane, and 1-hexene) hydrocarbons were also investigated in the presence and absence of excess hydrogen on Pt

Development of an acoustic steam generator leak detection system using delay-and-sum beamformer

International Nuclear Information System (INIS)

Chikazawa, Yoshitaka

2009-01-01

A new acoustic steam generator leak detection system using delay-and-sum beamformer is proposed. The major advantage of the delay-and-sum beamformer is it could provide information of acoustic source direction. An acoustic source of a sodium-water reaction is supposed to be localized while the background noise of the steam generator operation is uniformly distributed in the steam generator tube region. Therefore the delay-and-sum beamformer could distinguish the acoustic source of the sodium-water reaction from steam generator background noise. In this paper, results from numerical analyses are provided to show fundamental feasibility of the new method. (author)

Trace gas absorption spectroscopy using laser difference-frequency spectrometer for environmental application

Science.gov (United States)

Chen, W.; Cazier, F.; Boucher, D.; Tittel, F. K.; Davies, P. B.

2001-01-01

A widely tunable infrared spectrometer based on difference frequency generation (DFG) has been developed for organic trace gas detection by laser absorption spectroscopy. On-line measurements of concentration of various hydrocarbons, such as acetylene, benzene, and ethylene, were investigated using high-resolution DFG trace gas spectroscopy for highly sensitive detection.

Correlation of zero-point energy with molecular structure and molecular forces. 3. Approximation for H/D isotope shifts and linear frequency sum rule

International Nuclear Information System (INIS)

Oi, T.; Ishida, T.

1984-01-01

The approximation methods for the zero-point energy (ZPE) previously developed using the Lanczo's tau method have been applied to the shifts in ZPE due to hydrogen isotope substitutions. Six types of approximation methods have been compared and analyzed on the basis of a weighing function Ω(lambda) varies as lambda/sup k/ and the actual eigenvalue shift spectra. The method generated by the most general optimzation treatment yields a predictable and generally satisfactory precision of the order of 1% or better. A linear frequency sum rule has been derived, which approximately holds for the sets of isotopic molecules which satisfy the second-order frequency sum rule. 19 references, 3 figures, 3 tables

Self-assembled organic and fullerene monolayers characterisation by two-colour SFG spectroscopy: a pathway to meet doubly resonant SFG process

Energy Technology Data Exchange (ETDEWEB)

Humbert, C.; Caudano, Y.; Dreesen, L.; Sartenaer, Y.; Mani, A.A.; Silien, C.; Lemaire, J.-J.; Thiry, P.A.; Peremans, A

2004-10-15

Two-colour sum-frequency generation (two-colour SFG) spectroscopy was used to probe both vibrational and electronic properties of 1-dodecanethiol/Ag(1 1 1), Au(1 1 1), and Pt(1 1 1), of 5-[p-(6-mercaptohexoxy)-phenyl]-10,15,20-triphenylporphin/Pt(1 1 1), and of C{sub 60}/Ag(1 1 1). The role of the various physical parameters determining the sum-frequency generation (SFG) intensity equation is highlighted. The enhancement of the non-linear second order susceptibility in the aforementioned interfaces is explained in terms of metal interband transition, molecular electronic transition and of electron-phonon coupling, respectively.

Application of cascaded frequency multiplication to molecular spectroscopy

International Nuclear Information System (INIS)

Drouin, Brian J.; Maiwald, Frank W.; Pearson, John C.

2005-01-01

Laboratory molecular spectroscopy provides the basis for interpretation of atmospheric, planetary, and astrophysical data gathered by remote sensing. Laboratory studies of atomic and molecular signatures across the electromagnetic spectrum provide high-precision, quantitative data used to interpret the observed environment from remote measurements. Historically, the region of the spectrum above 500 GHz has been relatively unexplored due to atmospheric absorption and technical difficulties generating and detecting radiation. Laboratory spectroscopy at these frequencies has traditionally involved measurement of one or two absorption features and relied on fitting of models to the limited data. We report a new spectrometer built around a computer-controlled commercial synthesizer and millimeter-wave module driving a series of amplifiers followed by a series of wide-bandwidth frequency doublers and triplers. The spectrometer provides the ability to rapidly measure large pieces of frequency space with higher resolution, accuracy, and sensitivity than with Fourier transform infrared techniques. The approach is simple, modular, and requires no custom-built electronics or high voltage and facilitates the use of infrared data analysis techniques on complex submillimeter spectra

Laser frequency stabilization and shifting by using modulation transfer spectroscopy

Science.gov (United States)

Cheng, Bing; Wang, Zhao-Ying; Wu, Bin; Xu, Ao-Peng; Wang, Qi-Yu; Xu, Yun-Fei; Lin, Qiang

2014-10-01

The stabilizing and shifting of laser frequency are very important for the interaction between the laser and atoms. The modulation transfer spectroscopy for the 87Rb atom with D2 line transition F = 2 → F' = 3 is used for stabilizing and shifting the frequency of the external cavity grating feedback diode laser. The resonant phase modulator with electro—optical effect is used to generate frequency sideband to lock the laser frequency. In the locking scheme, circularly polarized pump- and probe-beams are used. By optimizing the temperature of the vapor, the pump- and probe-beam intensity, the laser linewidth of 280 kHz is obtained. Furthermore, the magnetic field generated by a solenoid is added into the system. Therefore the system can achieve the frequency locking at any point in a range of hundreds of megahertz frequency shifting with very low power loss.

Optical fiber strain sensor using fiber resonator based on frequency comb Vernier spectroscopy

DEFF Research Database (Denmark)

Zhang, Liang; Lu, Ping; Chen, Li

2012-01-01

A novel (to our best knowledge) optical fiber strain sensor using a fiber ring resonator based on frequency comb Vernier spectroscopy is proposed and demonstrated. A passively mode-locked optical fiber laser is employed to generate a phased-locked frequency comb. Strain applied to the optical fib...

Laser frequency stabilization by combining modulation transfer and frequency modulation spectroscopy.

Science.gov (United States)

Zi, Fei; Wu, Xuejian; Zhong, Weicheng; Parker, Richard H; Yu, Chenghui; Budker, Simon; Lu, Xuanhui; Müller, Holger

2017-04-01

We present a hybrid laser frequency stabilization method combining modulation transfer spectroscopy (MTS) and frequency modulation spectroscopy (FMS) for the cesium D2 transition. In a typical pump-probe setup, the error signal is a combination of the DC-coupled MTS error signal and the AC-coupled FMS error signal. This combines the long-term stability of the former with the high signal-to-noise ratio of the latter. In addition, we enhance the long-term frequency stability with laser intensity stabilization. By measuring the frequency difference between two independent hybrid spectroscopies, we investigate the short-and long-term stability. We find a long-term stability of 7.8 kHz characterized by a standard deviation of the beating frequency drift over the course of 10 h and a short-term stability of 1.9 kHz characterized by an Allan deviation of that at 2 s of integration time.

Parametric Processes for Generation and Low Noise Detection of Infrared Light

DEFF Research Database (Denmark)

Høgstedt, Lasse

This thesis describes an experimentally based, and application oriented investigation of sum- and difference frequency generation for photon conversion,from one spectral domain to another. The applications in focus are coherent gas spectroscopy in the near- and mid-infrared regimes. The investiga......This thesis describes an experimentally based, and application oriented investigation of sum- and difference frequency generation for photon conversion,from one spectral domain to another. The applications in focus are coherent gas spectroscopy in the near- and mid-infrared regimes...... upconversion modules are tested as part of a detection system in two different applications for spectroscopic gas measurements. The first test was done at Lund University together with the Combustion Physics Group, where the detection level of acetylene gas in a four-wave mixing setup was improved a factor...... of 500 compared to previous measurements. The second test was performed at the Atmospheric Physics Department at the German Aerospace Center in Oberpfaffenhofen. Here the upconversion detector was tested as an alternative to an InGaAs detector in a differential absorption lidar setup for long range...

Interfacial structure of soft matter probed by SFG spectroscopy.

Science.gov (United States)

Ye, Shen; Tong, Yujin; Ge, Aimin; Qiao, Lin; Davies, Paul B

2014-10-01

Sum frequency generation (SFG) vibrational spectroscopy, an interface-specific technique in contrast to, for example, attenuated total reflectance spectroscopy, which is only interface sensitive, has been employed to investigate the surface and interface structure of soft matter on a molecular scale. The experimental arrangement required to carry out SFG spectroscopy, with particular reference to soft matter, and the analytical methods developed to interpret the spectra are described. The elucidation of the interfacial structure of soft matter systems is an essential prerequisite in order to understand and eventually control the surface properties of these important functional materials. Copyright © 2014 The Chemical Society of Japan and Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Frequency modulation spectroscopy with a THz quantum-cascade laser.

Science.gov (United States)

Eichholz, R; Richter, H; Wienold, M; Schrottke, L; Hey, R; Grahn, H T; Hübers, H-W

2013-12-30

We report on a terahertz spectrometer for high-resolution molecular spectroscopy based on a quantum-cascade laser. High-frequency modulation (up to 50 MHz) of the laser driving current produces a simultaneous modulation of the frequency and amplitude of the laser output. The modulation generates sidebands, which are symmetrically positioned with respect to the laser carrier frequency. The molecular transition is probed by scanning the sidebands across it. In this way, the absorption and the dispersion caused by the molecular transition are measured. The signals are modeled by taking into account the simultaneous modulation of the frequency and amplitude of the laser emission. This allows for the determination of the strength of the frequency as well as amplitude modulation of the laser and of molecular parameters such as pressure broadening.

Coherent radio-frequency detection for narrowband direct comb spectroscopy.

Science.gov (United States)

Anstie, James D; Perrella, Christopher; Light, Philip S; Luiten, Andre N

2016-02-22

We demonstrate a scheme for coherent narrowband direct optical frequency comb spectroscopy. An extended cavity diode laser is injection locked to a single mode of an optical frequency comb, frequency shifted, and used as a local oscillator to optically down-mix the interrogating comb on a fast photodetector. The high spectral coherence of the injection lock generates a microwave frequency comb at the output of the photodiode with very narrow features, enabling spectral information to be further down-mixed to RF frequencies, allowing optical transmittance and phase to be obtained using electronics commonly found in the lab. We demonstrate two methods for achieving this step: a serial mode-by-mode approach and a parallel dual-comb approach, with the Cs D1 transition at 894 nm as a test case.

Communication: atomic force detection of single-molecule nonlinear optical vibrational spectroscopy.

Science.gov (United States)

Saurabh, Prasoon; Mukamel, Shaul

2014-04-28

Atomic Force Microscopy (AFM) allows for a highly sensitive detection of spectroscopic signals. This has been first demonstrated for NMR of a single molecule and recently extended to stimulated Raman in the optical regime. We theoretically investigate the use of optical forces to detect time and frequency domain nonlinear optical signals. We show that, with proper phase matching, the AFM-detected signals closely resemble coherent heterodyne-detected signals. Applications are made to AFM-detected and heterodyne-detected vibrational resonances in Coherent Anti-Stokes Raman Spectroscopy (χ((3))) and sum or difference frequency generation (χ((2))).

Highly efficient deep ultraviolet generation by sum-frequency mixing ...

Indian Academy of Sciences (India)

Ultraviolet laser radiation; walk-off compensation; third harmonic generation; nonlinear optical material. ... Because of its large birefringence, BBO crystal permits the generation of UV radiation near 200 nm by THG ... A, B and C are three different configurations for THG, A – Single crystal, B – two crystals (B2 and B3 in.

Linear and Nonlinear Molecular Spectroscopy with Laser Frequency Combs

Science.gov (United States)

Picque, Nathalie

2013-06-01

The regular pulse train of a mode-locked femtosecond laser can give rise to a comb spectrum of millions of laser modes with a spacing precisely equal to the pulse repetition frequency. Laser frequency combs were conceived a decade ago as tools for the precision spectroscopy of atomic hydrogen. They are now becoming enabling tools for an increasing number of applications, including molecular spectroscopy. Recent experiments of multi-heterodyne frequency comb Fourier transform spectroscopy (also called dual-comb spectroscopy) have demonstrated that the precisely spaced spectral lines of a laser frequency comb can be harnessed for new techniques of linear absorption spectroscopy. The first proof-of-principle experiments have demonstrated a very exciting potential of dual-comb spectroscopy without moving parts for ultra-rapid and ultra-sensitive recording of complex broad spectral bandwidth molecular spectra. Compared to conventional Michelson-based Fourier transform spectroscopy, recording times could be shortened from seconds to microseconds, with intriguing prospects for spectroscopy of short lived transient species. The resolution improves proportionally to the measurement time. Therefore longer recordings allow high resolution spectroscopy of molecules with extreme precision, since the absolute frequency of each laser comb line can be known with the accuracy of an atomic clock. Moreover, since laser frequency combs involve intense ultrashort laser pulses, nonlinear interactions can be harnessed. Broad spectral bandwidth ultra-rapid nonlinear molecular spectroscopy and imaging with two laser frequency combs is demonstrated with coherent Raman effects and two-photon excitation. Real-time multiplex accessing of hyperspectral images may dramatically expand the range of applications of nonlinear microscopy. B. Bernhardt et al., Nature Photonics 4, 55-57 (2010); A. Schliesser et al. Nature Photonics 6, 440-449 (2012); T. Ideguchi et al. arXiv:1201.4177 (2012) T

Direct Frequency Comb Spectroscopy of Alkali Atoms

Science.gov (United States)

Pradhananga, Trinity; Palm, Christopher; Nguyen, Khoa; Guttikonda, Srikanth; Kimball, Derek Jackson

2011-11-01

We are using direct frequency comb spectroscopy to study transition frequencies and excited state hyperfine structure in potassium and rubidium using 2-photon transitions excited directly with the frequency-doubled output of a erbium fiber optical frequency comb. The frequency comb output is directed in two counterpropagating directions through a vapor cell containing the atomic vapor of interest. A pair of optical filters is used to select teeth of the comb in order to identify the transition wavelengths. A photomultiplier tube (PMT) measures fluorescence from a decay channel wavelength selected with another optical filter. Using different combinations of filters enables a wide range of transitions to be investigated. By scanning the repetition rate, a Doppler-free spectrum can be obtained enabling kHz-resolution spectral measurements. The thermal motion of the atoms in the vapor cell actually eliminates the need to fine-tune the offset frequency and repetition rate, alleviating a somewhat challenging requirement for spectroscopy of cold atoms. Our investigations are laying the groundwork for a long-term research program to use direct frequency comb spectroscopy to understand the complex spectra of rare-earth atoms.

Efficient frequency comb generation in AlGaAs-on-insulator

DEFF Research Database (Denmark)

Pu, Minhao; Ottaviano, Luisa; Semenova, Elizaveta

2016-01-01

The combination of nonlinear and integrated photonics enables Kerr frequency comb generation in stable chip-based microresonators. Such a comb system will revolutionize applications, including multi-wavelength lasers, metrology, and spectroscopy. Aluminum gallium arsenide (AlGaAs) exhibits very...... high material nonlinearity and low nonlinear loss. However, difficulties in device processing and low device effective nonlinearity made Kerr frequency comb generation elusive. Here, we demonstrate AlGaAs-on-insulator as a nonlinear platform at telecom wavelengths with an ultra-high device nonlinearity....... We show high-quality-factor (Q > 105) micro-resonators where optical parametric oscillations are achieved with milliwatt-level pump threshold powers, which paves the way for on-chip pumped comb generation....

Call for papers for special issue of Journal of Molecular Spectroscopy focusing on "Frequency-comb spectroscopy"

Science.gov (United States)

Foltynowicz, Aleksandra; Picqué, Nathalie; Ye, Jun

2018-05-01

Frequency combs are becoming enabling tools for many applications in science and technology, beyond the original purpose of frequency metrology of simple atoms. The precisely evenly spaced narrow lines of a laser frequency comb inspire intriguing approaches to molecular spectroscopy, designed and implemented by a growing community of scientists. Frequency-comb spectroscopy advances the frontiers of molecular physics across the entire electro-magnetic spectrum. Used as frequency rulers, frequency combs enable absolute frequency measurements and precise line shape studies of molecular transitions, for e.g. tests of fundamental physics and improved determination of fundamental constants. As light sources interrogating the molecular samples, they dramatically improve the resolution, precision, sensitivity and acquisition time of broad spectral-bandwidth spectroscopy and open up new opportunities and applications at the leading edge of molecular spectroscopy and sensing.

Characterization of the molecular structure and mechanical properties of polymer surfaces and protein/polymer interfaces by sum frequency generation vibrational spectroscopy and atomic force microscopy

Energy Technology Data Exchange (ETDEWEB)

Koffas, Telly Stelianos [Univ. of California, Berkeley, CA (United States)

2004-01-01

Sum frequency generation (SFG) vibrational spectroscopy, atomic force microscopy (AFM), and other complementary surface-sensitive techniques have been used to study the surface molecular structure and surface mechanical behavior of biologically-relevant polymer systems. SFG and AFM have emerged as powerful analytical tools to deduce structure/property relationships, in situ, for polymers at air, liquid and solid interfaces. The experiments described in this dissertation have been performed to understand how polymer surface properties are linked to polymer bulk composition, substrate hydrophobicity, changes in the ambient environment (e.g., humidity and temperature), or the adsorption of macromolecules. The correlation of spectroscopic and mechanical data by SFG and AFM can become a powerful methodology to study and engineer materials with tailored surface properties. The overarching theme of this research is the interrogation of systems of increasing structural complexity, which allows us to extend conclusions made on simpler model systems. We begin by systematically describing the surface molecular composition and mechanical properties of polymers, copolymers, and blends having simple linear architectures. Subsequent chapters focus on networked hydrogel materials used as soft contact lenses and the adsorption of protein and surfactant at the polymer/liquid interface. The power of SFG is immediately demonstrated in experiments which identify the chemical parameters that influence the molecular composition and ordering of a polymer chain's side groups at the polymer/air and polymer/liquid interfaces. In general, side groups with increasingly greater hydrophobic character will be more surface active in air. Larger side groups impose steric restrictions, thus they will tend to be more randomly ordered than smaller hydrophobic groups. If exposed to a hydrophilic environment, such as water, the polymer chain will attempt to orient more of its hydrophilic groups to

Sum-frequency spectroscopic studies: I. Surface melting of ice, II. Surface alignment of polymers

Energy Technology Data Exchange (ETDEWEB)

Wei, Xing [Univ. of California, Berkeley, CA (United States)

2000-01-01

Surface vibrational spectroscopy via infrared-visible sum-frequency generation (SFG) has been established as a useful tool to study the structures of different kinds of surfaces and interfaces. This technique was used to study the (0001) face of hexagonal ice (Ih). SFG spectra in the O-H stretch frequency range were obtained at various sample temperatures. For the vapor(air)/ice interface, the degree of orientational order of the dangling OH bonds at the surface was measured as a function of temperature. Disordering sets in around 200 K and increases dramatically with temperature, which is strong evidence of surface melting of ice. For the other ice interfaces (silica/OTS/ice and silica/ice), a similar temperature dependence of the hydrogen bonded OH stretch peak was observed; the free OH stretch mode, however, appears to be different from that of the vapor (air)/ice interface due to interactions at the interfaces. The technique was also used to measure the orientational distributions of the polymer chains on a rubbed polyvinyl alcohol surface. Results show that the polymer chains at the surface appear to be well aligned by rubbing, and the adsorbed liquid crystal molecules are aligned, in turn, by the surface polymer chains. A strong correlation exists between the orientational distributions of the polymer chains and the liquid crystal molecules, indicating that the surface-induced bulk alignment of a liquid crystal film by rubbed polymer surfaces is via an orientational epitaxy-like mechanism. This thesis also contains studies on some related issues that are crucial to the above applications. An experiment was designed to measure SFG spectra in both reflection and transmission. The result confirms that SFG in reflection is generally dominated by the surface contribution. Another issue is the motional effect due to fast orientational motion of molecules at a surface or interface. Calculations show that the effect is significant if the molecular orientation varies

SFG spectroscopy from 10 -8 to 1000 mbar: less-ordered CO structures and coadsorption on Pd (1 1 1)

Science.gov (United States)

Morkel, Matthias; Unterhalt, Holger; Salmeron, Miquel; Rupprechter, Günther; Freund, Hans-Joachim

2003-06-01

Vibrational sum frequency generation spectroscopy was employed to study "less-ordered" phases resulting from low-temperature CO exposure on Pd(1 1 1). Such imperfect structures may also occur under catalytic reaction conditions up to 1000 mbar and originate from the superposition of ordered structures when the CO mobility and flux were insufficient. The effect of coadsorbed hydrogen and water was also examined.

Time-domain SFG spectroscopy using mid-IR pulse shaping: practical and intrinsic advantages.

Science.gov (United States)

Laaser, Jennifer E; Xiong, Wei; Zanni, Martin T

2011-03-24

Sum-frequency generation (SFG) spectroscopy is a ubiquitous tool in the surface sciences. It provides infrared transition frequencies and line shapes that probe the structure and environment of molecules at interfaces. In this article, we apply techniques learned from the multidimensional spectroscopy community to SFG spectroscopy. We implement balanced heterodyne detection to remove scatter and the local oscillator background. Heterodyning also separates the resonant and nonresonant signals by acquiring both the real and imaginary parts of the spectrum. We utilize mid-IR pulse shaping to control the phase and delay of the mid-IR pump pulse. Pulse shaping allows phase cycling for data collection in the rotating frame and additional background subtraction. We also demonstrate time-domain data collection, which is a Fourier transform technique, and has many advantages in signal throughput, frequency resolution, and line shape accuracy over existing frequency domain methods. To demonstrate time-domain SFG spectroscopy, we study an aryl isocyanide on gold, and find that the system has an inhomogeneous structural distribution, in agreement with computational results, but which was not resolved by previous frequency-domain SFG studies. The ability to rapidly and actively manipulate the mid-IR pulse in an SFG pules sequence makes possible new experiments and more accurate spectra. © 2011 American Chemical Society

Up to 30 mW of broadly tunable CW green-to-orange light, based on sum-frequency mixing of Cr4+:forsterite and Nd:YVO4 lasers

DEFF Research Database (Denmark)

Mortensen, Jesper Liltorp; McWilliam, Allan; G. Leburn, Christopher

2006-01-01

Efficient generation of continuous-wave (CW) tunable light in the yellow region is reported. The method is based on sum-frequency mixing of a tunable Cr4+:forsterite laser with a Nd:YVO4 laser. A periodically poled lithium niobate crystal was placed intra-cavity in a Nd:YVO4 laser, and the Cr4...

Highly efficient deep ultraviolet generation by sum-frequency mixing ...

Indian Academy of Sciences (India)

Generation of deep ultraviolet radiation at 210 nm by Type-I third harmonic generation is achieved in a pair of BBO crystals with conversion efficiency as high as 36%. The fundamental source is the dye laser radiation pumped by the second harmonic of a Q-switched Nd : YAG laser. A walk-off compensated configuration ...

Trapped Ion Oscillation Frequencies as Sensors for Spectroscopy

Directory of Open Access Journals (Sweden)

Wilfried Nörtershäuser

2010-03-01

Full Text Available The oscillation frequencies of charged particles in a Penning trap can serve as sensors for spectroscopy when additional field components are introduced to the magnetic and electric fields used for confinement. The presence of so-called “magnetic bottles” and specific electric anharmonicities creates calculable energy-dependences of the oscillation frequencies in the radiofrequency domain which may be used to detect the absorption or emission of photons both in the microwave and optical frequency domains. The precise electronic measurement of these oscillation frequencies therefore represents an optical sensor for spectroscopy. We discuss possible applications for precision laser and microwave spectroscopy and their role in the determination of magnetic moments and excited state lifetimes. Also, the trap-assisted measurement of radiative nuclear de-excitations in the X-ray domain is discussed. This way, the different applications range over more than 12 orders of magnitude in the detectable photon energies, from below μeV in the microwave domain to beyond MeV in the X-ray domain.

Generation of continuous coherent radiation at Lyman-alpha and 1S-2P Spectroscopy of atomic hydrogen

NARCIS (Netherlands)

Pahl, A.; Fendel, P.; Henrich, B.R.; Walz, J.; Hansch, T.W.; Eikema, K.S.E.

2005-01-01

Continuous coherent radiation from wavelengths from 121 to 123 nm in the vacuum ultraviolet (VUV) was generated by four-wave sum-frequency mixing in mercury vapor. A yield of 20 nW at Lyman-alpha (121.57 nm) was achieved. We describe the experimental setup in detail and present a calculation of the

FigSum: automatically generating structured text summaries for figures in biomedical literature.

Science.gov (United States)

Agarwal, Shashank; Yu, Hong

2009-11-14

Figures are frequently used in biomedical articles to support research findings; however, they are often difficult to comprehend based on their legends alone and information from the full-text articles is required to fully understand them. Previously, we found that the information associated with a single figure is distributed throughout the full-text article the figure appears in. Here, we develop and evaluate a figure summarization system - FigSum, which aggregates this scattered information to improve figure comprehension. For each figure in an article, FigSum generates a structured text summary comprising one sentence from each of the four rhetorical categories - Introduction, Methods, Results and Discussion (IMRaD). The IMRaD category of sentences is predicted by an automated machine learning classifier. Our evaluation shows that FigSum captures 53% of the sentences in the gold standard summaries annotated by biomedical scientists and achieves an average ROUGE-1 score of 0.70, which is higher than a baseline system.

Adding a dimension to the infrared spectra of interfaces: 2D SFG spectroscopy via mid-IR pulse shaping

Science.gov (United States)

Zanni, Martin

2012-02-01

Sum-frequency generation spectroscopy provides an infrared spectrum of interfaces and thus has widespread use in the materials and chemical sciences. In this presentation, I will present our recent work in developing a 2D pulse sequence to generate 2D SFG spectra of interfaces, in analogy to 2D infrared spectra used to measure bulk species. To develop this spectroscopy, we have utilized many of the tricks-of-the-trade developed in the 2D IR and 2D Vis communities in the last decade, including mid-IR pulse shaping. With mid-IR pulse shaping, the 2D pulse sequence is manipulated by computer programming in the desired frequency resolution, rotating frame, and signal pathway. We believe that 2D SFG will become an important tool in the interfacial sciences in an analogous way that 2D IR is now being used in many disciplines.

Model Catalysis of Ammonia Synthesis ad Iron-Water Interfaces - ASum Frequency Generation Vibrational Spectroscopic Study of Solid-GasInterfaces and Anion Photoelectron Spectroscopic Study of Selected Anionclusters

Energy Technology Data Exchange (ETDEWEB)

Ferguson, Michael James [Univ. of California, Berkeley, CA (United States)

2005-01-01

The ammonia synthesis reaction has been studied using single crystal model catalysis combined with sum frequency generation (SFG) vibrational spectroscopy. The adsorption of gases N₂, H₂, O₂ and NH₃ that play a role in ammonia synthesis have been studied on the Fe(111) crystal surface by sum frequency generation vibrational spectroscopy using an integrated Ultra-High Vacuum (UHV)/high-pressure system. SFG spectra are presented for the dissociation intermediates, NH₂ (~3325 cm^-1) and NH (~3235 cm^-1) under high pressure of ammonia or equilibrium concentrations of reactants and products on Fe(111) surfaces. Special attention was paid to understand how potassium promotion of the iron catalyst affects the intermediates of ammonia synthesis. An Fe(111) surface promoted with 0.2 monolayers of potassium red shifts the vibrational frequencies of the reactive surface intermediates, NH and NH₂, providing evidence for weakened the nitrogen-hydrogen bonds relative to clean Fe(111). Spectral features of these surface intermediates persisted to higher temperatures for promoted iron surfaces than for clean Fe(111) surfaces implying that nitrogen-iron bonds are stronger for the promoted surface. The ratio of the NH to NH₂ signal changed for promoted surfaces in the presence of equilibrium concentrations of reactants and products. The order of adding oxygen and potassium to promoted surfaces does not alter the spectra indicating that ammonia induces surface reconstruction of the catalyst to produce the same surface morphology. When oxygen is co-adsorbed with nitrogen, hydrogen, ammonia or potassium on Fe(111), a relative phase shift of the spectra occurs as compared to the presence of adsorbates on clean iron surfaces. Water adsorption on iron was also probed using SFG vibrational spectroscopy. For both H₂O and D₂O, the only spectral feature was in the range of

Metastable Magnesium fluorescence spectroscopy using a frequency-stabilized 517 nm laser

DEFF Research Database (Denmark)

He, Ming; Jensen, Brian B; Therkildsen, Kasper T

2009-01-01

We present a laser operating at 517 nm for our Magnesium laser-cooling and atomic clock project. A two-stage Yb-doped fiber amplifier (YDFA) system generates more than 1.5 W of 1034 nm light when seeded with a 15 mW diode laser. Using a periodically poled lithium niobate (PPLN) waveguide, we obta...... obtained more than 40 mW of 517 nm output power by single pass frequency doubling. In addition, fluorescence spectroscopy of metastable magnesium atoms could be used to stabilize the 517 nm laser to an absolute frequency within 1 MHz.......We present a laser operating at 517 nm for our Magnesium laser-cooling and atomic clock project. A two-stage Yb-doped fiber amplifier (YDFA) system generates more than 1.5 W of 1034 nm light when seeded with a 15 mW diode laser. Using a periodically poled lithium niobate (PPLN) waveguide, we...

Detection of elemental mercury by multimode diode laser correlation spectroscopy.

Science.gov (United States)

Lou, Xiutao; Somesfalean, Gabriel; Svanberg, Sune; Zhang, Zhiguo; Wu, Shaohua

2012-02-27

We demonstrate a method for elemental mercury detection based on correlation spectroscopy employing UV laser radiation generated by sum-frequency mixing of two visible multimode diode lasers. Resonance matching of the multimode UV laser is achieved in a wide wavelength range and with good tolerance for various operating conditions. Large mode-hops provide an off-resonance baseline, eliminating interferences from other gas species with broadband absorption. A sensitivity of 1 μg/m3 is obtained for a 1-m path length and 30-s integration time. The performance of the system shows promise for mercury monitoring in industrial applications.

Studies on the substrate mediated vibrational excitation of CO/Si(100) by means of SFG spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Han, Xu; Lass, Kristian; Balgar, Thorsten; Hasselbrink, Eckart [Universitaet Duisburg-Essen, Fachbereich Chemie, 45117 Essen (Germany)

2009-07-01

Vibrational excitations of adsorbates play an important role in chemical reaction dynamics. In the past decade CO on solid surfaces was chosen as adequate model system for studying vibrational relaxation dynamics. Our work is focused on the energy dissipation of vibrationally excited CO adsorbed on a silicon surface by means of IR/Vis sum frequency generation (SFG) spectroscopy. Here we present studies on substrate mediated excitation of vibrational modes of CO on Si(100) induced by UV radiation. We suppose the observation of highly excited internal stretch vibrations of CO caused by hot electrons generated within the silicon substrate.

Second-harmonic and sum-frequency generation for surface studies

International Nuclear Information System (INIS)

Hunt, J.H.; Guyot-Sionnest, P.; Shen, Y.R.

1987-07-01

Second harmonic generation (SHG) has now been well established as a versatile surface-sensitive probe. It has been used to study electrochemical processes at electrode surfaces, molecular adsorption and desorption at metal and semiconductor surfaces, orientational phase transition of molecular monolayers on water, surface reconstruction and epitaxial growth, and so on. More recently, it has been employed as a tool to monitor monolayer polymerization and other surface reactions, to probe polar order of molecules at interfaces, and to measure molecular nonlinearity. While most surface techniques are restricted to the solid/vacuum environment, SHG is applicable to nearly all interfaces as long as the interfaces are accessible by light. In addition, SHG has the advantages of being capable of in-situ measurements with high temporal, spatial, and spectral resolutions

Rydberg-atom based radio-frequency electrometry using frequency modulation spectroscopy in room temperature vapor cells.

Science.gov (United States)

Kumar, Santosh; Fan, Haoquan; Kübler, Harald; Jahangiri, Akbar J; Shaffer, James P

2017-04-17

Rydberg atom-based electrometry enables traceable electric field measurements with high sensitivity over a large frequency range, from gigahertz to terahertz. Such measurements are particularly useful for the calibration of radio frequency and terahertz devices, as well as other applications like near field imaging of electric fields. We utilize frequency modulated spectroscopy with active control of residual amplitude modulation to improve the signal to noise ratio of the optical readout of Rydberg atom-based radio frequency electrometry. Matched filtering of the signal is also implemented. Although we have reached similarly, high sensitivity with other read-out methods, frequency modulated spectroscopy is advantageous because it is well-suited for building a compact, portable sensor. In the current experiment, ∼3 µV cm-1 Hz-1/2 sensitivity is achieved and is found to be photon shot noise limited.

Terahertz Frequency-Domain Spectroscopy of Low-Pressure Acetonitrile Gas by a Photomixing Terahertz Synthesizer Referenced to Dual Optical Frequency Combs

Science.gov (United States)

Hsieh, Yi-Da; Kimura, Hiroto; Hayashi, Kenta; Minamikawa, Takeo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Inaba, Hajime; Minoshima, Kaoru; Hindle, Francis; Yasui, Takeshi

2016-09-01

A terahertz (THz) frequency synthesizer based on photomixing of two near-infrared lasers with a sub-THz to THz frequency offset is a powerful tool for spectroscopy of polar gas molecules due to its broad spectral coverage; however, its frequency accuracy and resolution are relatively low. To tune the output frequency continuously and widely while maintaining its traceability to a frequency standard, we developed a photomixing THz synthesizer phase-locked to dual optical frequency combs (OFCs). While the phase-locking to dual OFCs ensured continuous tuning within a spectral range of 120 GHz, in addition to the traceability to the frequency standard, use of a broadband uni-traveling carrier photodiode for photomixing enabled the generation of CW-THz radiation within a frequency range from 0.2 to 1.5 THz. We demonstrated THz frequency-domain spectroscopy of gas-phase acetonitrile CH3CN and its isotope CH3 13CN in the frequency range of 0.600-0.720 THz using this THz synthesizer. Their rotational transitions were assigned with a frequency accuracy of 8.42 × 10-8 and a frequency resolution of 520 kHz. Furthermore, the concentration of the CH3CN gas at 20 Pa was determined to be (5.41 ± 0.05) × 1014 molecules/cm3 by curve fitting analysis of the measured absorbance spectrum, and the mixture ratio of the mixed CH3CN/CH3 13CN gas was determined to be 1:2.26 with a gas concentration of 1014-1015 molecules/cm3. The developed THz synthesizer is highly promising for high-precision THz-FDS of low-pressure molecular gases and will enable the qualitative and quantitative analyses of multiple gases.

Polymorph characterization of active pharmaceutical ingredients (APIs) using low-frequency Raman spectroscopy.

Science.gov (United States)

Larkin, Peter J; Dabros, Marta; Sarsfield, Beth; Chan, Eric; Carriere, James T; Smith, Brian C

2014-01-01

Polymorph detection, identification, and quantitation in crystalline materials are of great importance to the pharmaceutical industry. Vibrational spectroscopic techniques used for this purpose include Fourier transform mid-infrared (FT-MIR) spectroscopy, Fourier transform near-infrared (FT-NIR) spectroscopy, Raman spectroscopy, and terahertz (THz) and far-infrared (FIR) spectroscopy. Typically, the fundamental molecular vibrations accessed using high-frequency Raman and MIR spectroscopy or the overtone and combination of bands in the NIR spectra are used to monitor the solid-state forms of active pharmaceutical ingredients (APIs). The local environmental sensitivity of the fundamental molecular vibrations provides an indirect probe of the long-range order in molecular crystals. However, low-frequency vibrational spectroscopy provides access to the lattice vibrations of molecular crystals and, hence, has the potential to more directly probe intermolecular interactions in the solid state. Recent advances in filter technology enable high-quality, low-frequency Raman spectra to be acquired using a single-stage spectrograph. This innovation enables the cost-effective collection of high-quality Raman spectra in the 200-10 cm(-1) region. In this study, we demonstrate the potential of low-frequency Raman spectroscopy for the polymorphic characterization of APIs. This approach provides several benefits over existing techniques, including ease of sampling and more intense, information-rich band structures that can potentially discriminate among crystalline forms. An improved understanding of the relationship between the crystalline structure and the low-frequency vibrational spectrum is needed for the more widespread use of the technique.

Generation of green frequency comb from chirped χ{sup (2)} nonlinear photonic crystals

Energy Technology Data Exchange (ETDEWEB)

Lai, C.-M. [Department of Electronic Engineering, Ming Chuan University, Taoyuan, Taiwan (China); Chang, K.-H.; Yang, Z.-Y.; Fu, S.-H.; Tsai, S.-T.; Hsu, C.-W.; Peng, L.-H. [Department of Electrical Engineering and Graduate Institute of Photonics and Optoelectronics, National Taiwan University, Taipei, Taiwan (China); Yu, N. E. [Advanced Photonics Research Institute, Gwangju Institute of Science and Technology, Gwangju (Korea, Republic of); Boudrioua, A. [LPL, CNRS - UMR 7538, Université Paris 13, Sorbone Paris Cité (France); Kung, A. H. [Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei, Taiwan (China); Institute of Photonics Technologies, National Tsing Hua University, Hsinchu, Taiwan (China)

2014-12-01

Spectrally broad frequency comb generation over 510–555 nm range was reported on chirped quasi-phase-matching (QPM) χ{sup (2)} nonlinear photonic crystals of 12 mm length with periodicity stepwise increased from 5.9 μm to 7.1 μm. When pumped with nanosecond infrared (IR) frequency comb derived from a QPM optical parametric oscillator (OPO) and spanned over 1040 nm to 1090 nm wavelength range, the 520 nm to 545 nm up-converted green spectra were shown to consist of contributions from (a) second-harmonic generation among the signal or the idler modes, and (b) sum-frequency generation (SFG) from the neighboring pairs of the signal or the idler modes. These mechanisms led the up-converted green frequency comb to have the same mode spacing of 450 GHz as that in the IR-OPO pump comb. As the pump was further detuned from the aforementioned near-degeneracy point and moved toward the signal (1020–1040 nm) and the idler (1090–1110 nm) spectral range, the above QPM parametric processes were preserved in the chirped QPM devices to support up-converted green generation in the 510–520 nm and the 545–555 nm spectral regime. Additional 530–535 nm green spectral generation was also observed due to concurrence of multi-wavelength SFG processes between the (signal, idler) mode pairs. These mechanisms facilitate the chirped QPM device to support a single-pass up-conversion efficiency ∼10% when subject to an IR-OPO pump comb with 200 mW average power operated near- or off- the degeneracy point.

Frequency-comb-assisted broadband precision spectroscopy with cascaded diode lasers

DEFF Research Database (Denmark)

Liu, Junqiu; Brasch, Victor; Pfeiffer, Martin H. P.

2016-01-01

Frequency-comb-assisted diode laser spectroscopy, employing both the accuracy of an optical frequency comb and the broad wavelength tuning range of a tunable diode laser, has been widely used in many applications. In this Letter, we present a novel method using cascaded frequency agile diode lasers......, which allows us to extend the measurement bandwidth to 37.4 THz (1355-1630 nm) at megahertz resolution with scanning speeds above 1 THz/s. It is demonstrated as a useful tool to characterize a broadband spectrum for molecular spectroscopy, and in particular it enables us to characterize the dispersion...

Noise-Immune Cavity-Enhanced Optical Frequency Comb Spectroscopy

Science.gov (United States)

Rutkowski, Lucile; Khodabakhsh, Amir; Johanssson, Alexandra C.; Foltynowicz, Aleksandra

2015-06-01

We present noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS), a recently developed technique for sensitive, broadband, and high resolution spectroscopy. In NICE-OFCS an optical frequency comb (OFC) is locked to a high finesse cavity and phase-modulated at a frequency precisely equal to (a multiple of) the cavity free spectral range. Since each comb line and sideband is transmitted through a separate cavity mode in exactly the same way, any residual frequency noise on the OFC relative to the cavity affects each component in an identical manner. The transmitted intensity contains a beat signal at the modulation frequency that is immune to frequency-to-amplitude noise conversion by the cavity, in a way similar to continuous wave noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS). The light transmitted through the cavity is detected with a fast-scanning Fourier-transform spectrometer (FTS) and the NICE-OFCS signal is obtained by fast Fourier transform of the synchronously demodulated interferogram. Our NICE-OFCS system is based on an Er:fiber femtosecond laser locked to a cavity with a finesse of ˜9000 and a fast-scanning FTS equipped with a high-bandwidth commercial detector. We measured NICE-OFCS signals from the 3νb{1}+νb{3} overtone band of CO_2 around 1.57 μm and achieved absorption sensitivity 6.4×10-11cm-1 Hz-1/2 per spectral element, corresponding to a minimum detectable CO_2 concentration of 25 ppb after 330 s integration time. We will describe the principles of the technique and its technical implementation, and discuss the spectral lineshapes of the NICE-OFCS signals. A. Khodabakhsh, C. Abd Alrahman, and A. Foltynowicz, Opt. Lett. 39, 5034-5037 (2014). J. Ye, L. S. Ma, and J. L. Hall, J. Opt. Soc. Am. B 15, 6-15 (1998). A. Khodabakhsh, A. C. Johansson, and A. Foltynowicz, Appl. Phys. B (2015) doi:10.1007/s00340-015-6010-7.

Over 8 W high peak power UV laser with a high power Q-switched Nd:YVO4 oscillator and the compact extra-cavity sum-frequency mixing

International Nuclear Information System (INIS)

Yan, X P; Liu, Q; Gong, M; Wang, D S; Fu, X

2009-01-01

A 8.2 W UV laser was reported with the compact extra-cavity sum-frequency mixing. The IR fundamental frequency source was a high power and high beam quality Q-switched Nd:YVO 4 oscillator. 38 W fundamental frequency laser at 1064 nm was obtained at the pulse repetition rate of 450 kHz with the beam quality factors of M 2 x = 1.27, M 2 y = 1.21. The type I and type II phase-matched LBO crystals were used as the extra-cavity frequency doubling and mixing crystals respectively. At 38 kHz, 8.2 W UV laser at 355 nm was achieved with the pulse duration of 8 ns corresponding to the pulse peak power as high as 27 kW, and the optical-optical conversion efficiency from IR to UV was 25.6%. The output characteristics of the IR and the harmonic generations varying with the pulse repetition rate were also investigated detailedly

Phase distortions in sum- and difference-frequency mixing in crystals

International Nuclear Information System (INIS)

Smith, A.V.; Bowers, M.S.

1995-01-01

We show that if two waves are incident on a quadratically nonlinear crystal, with the third wave generated entirely within the crystal, a phase-velocity mismatch (Δk ≠ 0) leads to intensity-dependent phase shifts of the generated wave only if there is walk-off, linear absorption, or significant diffraction of at least one of the waves as well as significant energy exchange among the waves. The result is frequency broadening and wave-front distortion of the generated wave. Although the induced phase distortions are usually quite small, they may be significant in applications that require high spectral resolution or pointing accuracy

Interpreting intensities in vibrational sum frequency generation (SFG) spectroscopy: CO adsorption on Pd surfaces

Science.gov (United States)

Morkel, M.; Unterhalt, H.; Klüner, T.; Rupprechter, G.; Freund, H.-J.

2005-07-01

The lineshape and intensity of SFG signals of CO adsorbed on supported Pd nanoparticles and Pd(1 1 1) are analyzed. For CO/Pd(1 1 1) nearly symmetric lorentzian lineshapes were observed. Applying two different visible wavelengths for excitation, asymmetric lineshapes observed for the CO/Pd/Al 2O 3/NiAl(1 1 0) system are explained by a lower resonant and a higher non-resonant SFG signal and a change in the phase between resonant and non-resonant signals, most likely originating from an interband transition in the NiAl substrate. The relative intensity of different CO species (hollow, bridge, on-top) was modeled by DFT calculations of IR transition moments and Raman activities. While the (experimental) sensitivity of SFG towards different CO species strongly varies, the calculated IR and Raman activities are rather similar. The inability to exactly reproduce experimental SFG intensities suggests a strong coverage dependence of Raman activities or that non-linear effects occur that can currently not be properly accounted for.

Mid-infrared frequency comb via coherent dispersive wave generation in silicon nitride nanophotonic waveguides

Science.gov (United States)

Guo, Hairun; Herkommer, Clemens; Billat, Adrien; Grassani, Davide; Zhang, Chuankun; Pfeiffer, Martin H. P.; Weng, Wenle; Brès, Camille-Sophie; Kippenberg, Tobias J.

2018-06-01

Mid-infrared optical frequency combs are of significant interest for molecular spectroscopy due to the large absorption of molecular vibrational modes on the one hand, and the ability to implement superior comb-based spectroscopic modalities with increased speed, sensitivity and precision on the other hand. Here, we demonstrate a simple, yet effective, method for the direct generation of mid-infrared optical frequency combs in the region from 2.5 to 4.0 μm (that is, 2,500-4,000 cm-1), covering a large fraction of the functional group region, from a conventional and compact erbium-fibre-based femtosecond laser in the telecommunication band (that is, 1.55 μm). The wavelength conversion is based on dispersive wave generation within the supercontinuum process in an unprecedented large-cross-section silicon nitride (Si3N4) waveguide with the dispersion lithographically engineered. The long-wavelength dispersive wave can perform as a mid-infrared frequency comb, whose coherence is demonstrated via optical heterodyne measurements. Such an approach can be considered as an alternative option to mid-infrared frequency comb generation. Moreover, it has the potential to realize compact dual-comb spectrometers. The generated combs also have a fine teeth-spacing, making them suitable for gas-phase analysis.

Blue and Orange Two-Color CW Laser Based on Single-Pass Second-Harmonic and Sum-Frequency Generation in MgO:PPLN

Directory of Open Access Journals (Sweden)

Dismas K. Choge

2018-04-01

Full Text Available We demonstrate a compact blue and orange-two color continuous wave laser source emitting at 487 nm and from 597.4 to 600.3 nm, respectively. The temperature tunable coherent orange radiation is achieved by frequency mixing 974 nm laser diode (LD and a C-band amplified spontaneous emission laser source while the temperature insensitive blue radiation is generated by second-order quasi-phase-matching frequency doubling of 974 nm LD. We implement the simultaneous nonlinear processes in a single magnesium oxide doped periodically poled lithium niobate bulk crystal without the need of an aperiodic design.

An Adaptive Model Predictive Load Frequency Control Method for Multi-Area Interconnected Power Systems with Photovoltaic Generations

Directory of Open Access Journals (Sweden)

Guo-Qiang Zeng

2017-11-01

Full Text Available As the penetration level of renewable distributed generations such as wind turbine generator and photovoltaic stations increases, the load frequency control issue of a multi-area interconnected power system becomes more challenging. This paper presents an adaptive model predictive load frequency control method for a multi-area interconnected power system with photovoltaic generation by considering some nonlinear features such as a dead band for governor and generation rate constraint for steam turbine. The dynamic characteristic of this system is formulated as a discrete-time state space model firstly. Then, the predictive dynamic model is obtained by introducing an expanded state vector, and rolling optimization of control signal is implemented based on a cost function by minimizing the weighted sum of square predicted errors and square future control values. The simulation results on a typical two-area power system consisting of photovoltaic and thermal generator have demonstrated the superiority of the proposed model predictive control method to these state-of-the-art control techniques such as firefly algorithm, genetic algorithm, and population extremal optimization-based proportional-integral control methods in cases of normal conditions, load disturbance and parameters uncertainty.

High-resolution mid-IR spectrometer based on frequency upconversion

DEFF Research Database (Denmark)

Hu, Qi; Dam, Jeppe Seidelin; Pedersen, Christian

2012-01-01

We demonstrate a novel approach for high-resolution spectroscopy based on frequency upconversion and postfiltering by means of a scanning Fabryx2013;Perot interferometer. The system is based on sum-frequency mixing, shifting the spectral content from the mid-infrared to the near-visible region al......-frequency 1064xA0;nm laser. We investigate water vapor emission lines from a butane burner and compare the measured results to model data. The presented method we suggest to be used for real-time monitoring of specific gas lines and reference signals....

Moessbauer sum rules for use with synchrotron sources

International Nuclear Information System (INIS)

Lipkin, Harry J.

1999-01-01

The availability of tunable synchrotron radiation sources with millivolt resolution has opened new prospects for exploring dynamics of complex systems with Moessbauer spectroscopy. Early Moessbauer treatments and moment sum rules are extended to treat inelastic excitations measured in synchrotron experiments, with emphasis on the unique new conditions absent in neutron scattering and arising in resonance scattering: prompt absorption, delayed emission, recoil-free transitions and coherent forward scattering. The first moment sum rule normalizes the inelastic spectrum. New sum rules obtained for higher moments include the third moment proportional to the second derivative of the potential acting on the Moessbauer nucleus and independent of temperature in the the harmonic approximation

Metabolic costs of force generation for constant-frequency and catchlike-inducing electrical stimulation in human tibialis anterior muscle

DEFF Research Database (Denmark)

Ratkevicius, Aivaras; Quistorff, Bjørn

2002-01-01

-frequency trains, catchlike-inducing trains produced a faster force generation and were more effective in maintaining the force--time integral as well as peak force. However, ATP costs of force generation were similar for the catchlike-inducing and constant-frequency stimulation (6.7 plus/minus 1.1 and 6.6 plus......Metabolic costs of force generation were compared for constant-frequency and catchlike-inducing electrical stimulation. Repetitive catchlike-inducing trains consisted of 2 interpulse intervals (IPIs) at 12.5 ms, 1 IPI at 25 ms, and 5 IPIs at 50 ms. Constant-frequency trains consisted of 8 IPIs...... at 37.5 ms. One train was delivered to the peroneal nerve every 2.5 s for 36 times under ischemic conditions. Anaerobic adenosine triphosphate (ATP) turnover was determined using 31-phosphorus magnetic resonance spectroscopy (P-MRS) of the human tibialis anterior muscle. Compared with constant...

OH spectroscopy with frequency-doubled dye laser radiation

Energy Technology Data Exchange (ETDEWEB)

ter Meulen, J J

1979-01-01

Discusses the excitation of the OH radical by UV radiation for the determination of the hyperfine structure of the excited states. The 307 nm UV light is obtained by doubling the frequency (in double-refraction crystals) of a tunable dye laser. Details of the laser set-up are given. The method is suitable for application to other high-resolution molecular spectroscopy experiments in the area between 200 and 400 nm. Further extensions can be expected with ring compound dyes and external doubling of the frequency.

Frequency locking of an extended-cavity quantum cascade laser to a frequency comb for precision mid infrared spectroscopy

KAUST Repository

Alsaif, Bidoor; Lamperti, Marco; Gatti, Davide; Laporta, Paolo; Fermann, Martin E.; Farooq, Aamir; Marangoni, Marco

2017-01-01

Extended-cavity quantum cascade lasers (EC-QCLs) enable mode-hope-free frequency sweeps in the mid-infrared region over ranges in excess of 100 cm−1, at speeds up to 1 THz/s and with a 100-mW optical power level. This makes them ideally suited for broadband absorption spectroscopy and for the simultaneous detection of multiple gases. On the other hand, their use for precision spectroscopy has been hampered so far by a large amount of frequency noise, resulting in an optical linewidth of about 30 MHz over 50 ms [1]. This is one of the reasons why neither their frequency nor their phase have been so far locked to a frequency comb. Their use in combination with frequency combs has been performed in an open loop regime only [2], which has the merit of preserving the inherently fast modulation speed of these lasers, yet not to afford high spectral resolution and accuracy.

Frequency locking of an extended-cavity quantum cascade laser to a frequency comb for precision mid infrared spectroscopy

KAUST Repository

Alsaif, Bidoor

2017-11-02

Extended-cavity quantum cascade lasers (EC-QCLs) enable mode-hope-free frequency sweeps in the mid-infrared region over ranges in excess of 100 cm−1, at speeds up to 1 THz/s and with a 100-mW optical power level. This makes them ideally suited for broadband absorption spectroscopy and for the simultaneous detection of multiple gases. On the other hand, their use for precision spectroscopy has been hampered so far by a large amount of frequency noise, resulting in an optical linewidth of about 30 MHz over 50 ms [1]. This is one of the reasons why neither their frequency nor their phase have been so far locked to a frequency comb. Their use in combination with frequency combs has been performed in an open loop regime only [2], which has the merit of preserving the inherently fast modulation speed of these lasers, yet not to afford high spectral resolution and accuracy.

Far off-resonance laser frequency stabilization using multipass cells in Faraday rotation spectroscopy.

Science.gov (United States)

Quan, Wei; Li, Yang; Li, Rujie; Shang, Huining; Fang, Zishan; Qin, Jie; Wan, Shuangai

2016-04-01

We propose a far off-resonance laser frequency stabilization method by using multipass cells in Rb Faraday rotation spectroscopy. Based on the detuning equation, if multipass cells with several meters optical path length are used in the conventional Faraday spectroscopy, the detuning of the lock point can be extended much further from the alkali metal resonance. A plate beam splitter was used to generate two different Faraday signals at the same time. The transmitted optical path length was L=50  mm and the reflected optical path length was 2L=100  mm. When the optical path length doubled, the detuning of the lock points moved further away from the atomic resonance. The temperature dependence of the detuning of the lock point was also analyzed. A temperature-insensitive lock point was found near resonance when the cell temperature was between 110°C and 130°C. We achieved an rms fluctuation of 0.9 MHz/23 h at a detuning of 0.5 GHz. A frequency drift of 16 MHz/h at a detuning of -5.6  GHz and 4 MHz/h at a detuning of -5.2  GHz were also obtained for the transmitted and reflected light Faraday signal.

Recurrence Relations and Generating Functions of the Sequence of Sums of Corresponding Factorials and Triangular Numbers

Directory of Open Access Journals (Sweden)

Romer C. Castillo

2015-11-01

Full Text Available This study established some recurrence relations and exponential generating functions of the sequence of factoriangular numbers. A factoriangular number is defined as a sum of corresponding factorial and triangular number. The proofs utilize algebraic manipulations with some known results from calculus, particularly on power series and Maclaurin’s series. The recurrence relations were found by manipulating the formula defining a factoringular number while the ascertained exponential generating functions were in the closed form.

High-power non linear frequency converted laser diodes

DEFF Research Database (Denmark)

Jensen, Ole Bjarlin; Andersen, Peter E.; Hansen, Anders Kragh

2015-01-01

We present different methods of generating light in the blue-green spectral range by nonlinear frequency conversion of tapered diode lasers achieving state-of-the-art power levels. In the blue spectral range, we show results using single-pass second harmonic generation (SHG) as well as cavity enh...... enhanced sum frequency generation (SFG) with watt-level output powers. SHG and SFG are also demonstrated in the green spectral range as a viable method to generate up to 4 W output power with high efficiency using different configurations....

Randomly Generating Four Mixed Bell-Diagonal States with a Concurrences Sum to Unity

International Nuclear Information System (INIS)

Toh, S. P.; Zainuddin Hishamuddin; Foo Kim Eng

2012-01-01

A two-qubit system in quantum information theory is the simplest bipartite quantum system and its concurrence for pure and mixed states is well known. As a subset of two-qubit systems, Bell-diagonal states can be depicted by a very simple geometrical representation of a tetrahedron with sides of length 2√2. Based on this geometric representation, we propose a simple approach to randomly generate four mixed Bell decomposable states in which the sum of their concurrence is equal to one. (general)

Pulsed-High Field/High-Frequency EPR Spectroscopy

Science.gov (United States)

Fuhs, Michael; Moebius, Klaus

Pulsed high-field/high-frequency electron paramagnetic resonance (EPR) spectroscopy is used to disentangle many kinds of different effects often obscured in continuous wave (cw) EPR spectra at lower magnetic fields/microwave frequencies. While the high magnetic field increases the resolution of G tensors and of nuclear Larmor frequencies, the high frequencies allow for higher time resolution for molecular dynamics as well as for transient paramagnetic intermediates studied with time-resolved EPR. Pulsed EPR methods are used for example for relaxation-time studies, and pulsed Electron Nuclear DOuble Resonance (ENDOR) is used to resolve unresolved hyperfine structure hidden in inhomogeneous linewidths. In the present article we introduce the basic concepts and selected applications to structure and mobility studies on electron transfer systems, reaction centers of photosynthesis as well as biomimetic models. The article concludes with an introduction to stochastic EPR which makes use of an other concept for investigating resonance systems in order to increase the excitation bandwidth of pulsed EPR. The limited excitation bandwidth of pulses at high frequency is one of the main limitations which, so far, made Fourier transform methods hardly feasible.

Precision Spectroscopy, Diode Lasers, and Optical Frequency Measurement Technology

Science.gov (United States)

Hollberg, Leo (Editor); Fox, Richard (Editor); Waltman, Steve (Editor); Robinson, Hugh

1998-01-01

This compilation is a selected set of reprints from the Optical Frequency Measurement Group of the Time and Frequency Division of the National Institute of Standards and Technology, and consists of work published between 1987 and 1997. The two main programs represented here are (1) development of tunable diode-laser technology for scientific applications and precision measurements, and (2) research toward the goal of realizing optical-frequency measurements and synthesis. The papers are organized chronologically in five, somewhat arbitrarily chosen categories: Diode Laser Technology, Tunable Laser Systems, Laser Spectroscopy, Optical Synthesis and Extended Wavelength Coverage, and Multi-Photon Interactions and Optical Coherences.

Premium Pricing of Liability Insurance Using Random Sum Model

Directory of Open Access Journals (Sweden)

Mujiati Dwi Kartikasari

2017-03-01

Full Text Available Premium pricing is one of important activities in insurance. Nonlife insurance premium is calculated from expected value of historical data claims. The historical data claims are collected so that it forms a sum of independent random number which is called random sum. In premium pricing using random sum, claim frequency distribution and claim severity distribution are combined. The combination of these distributions is called compound distribution. By using liability claim insurance data, we analyze premium pricing using random sum model based on compound distribution

Josephson admittance spectroscopy application for frequency analysis of broadband THz antennas

International Nuclear Information System (INIS)

Volkov, O Yu; Divin, Yu Yu; Gubankov, V N; Gundareva, I I; Pavlovskiy, V V

2010-01-01

Application of Josephson admittance spectroscopy for the spectral analysis of a broad-band log-periodic superconducting antenna was demonstrated at the frequency range from 50 to 700 GHz. The [001]-tilt YBa 2 Cu 3 O 7-x bicrystal Josephson junctions, integrated with sinuous log-periodic YBa 2 Cu 3 O 7-x antennas, were fabricated on NdGaO 3 bicrystal substrates. A real part of the antenna admittance ReY(f) as a function of the frequency f was reconstructed from the modification of the dc current-voltage characteristic of the junction, induced by the antenna. Resonance features were observed in the recovered ReY(f)-spectra with a periodicity in the logarithmic frequency scale, corresponding to log-periodic geometry of the antenna. The ReY(f)-spectra, recovered by Josephson spectroscopy, were compared with the ReY(f)-spectra, obtained by CAD simulation, and both spectra were shown to be similar in their main features. A value of 23 was obtained for an effective permittivity of the NdGaO3 bicrystal substrates by fitting simulated data to those obtained from Josephson spectroscopy.

Quantitative frequency-domain fluorescence spectroscopy in tissues and tissue-like media

Science.gov (United States)

Cerussi, Albert Edward

1999-09-01

In the never-ending quest for improved medical technology at lower cost, modern near-infrared optical spectroscopy offers the possibility of inexpensive technology for quantitative and non-invasive diagnoses. Hemoglobin is the dominant chromophore in the 700-900 nm spectral region and as such it allows for the optical assessment of hemoglobin concentration and tissue oxygenation by absorption spectroscopy. However, there are many other important physiologically relevant compounds or physiological states that cannot be effectively sensed via optical methods because of poor optical contrast. In such cases, contrast enhancements are required. Fluorescence spectroscopy is an attractive component of optical tissue spectroscopy. Exogenous fluorophores, as well as some endogenous ones, may furnish the desperately needed sensitivity and specificity that is lacking in near-infrared optical tissue spectroscopy. The main focus of this thesis was to investigate the generation and propagation of fluorescence photons inside tissues and tissue-like media (i.e., scattering dominated media). The standard concepts of fluorescence spectroscopy have been incorporated into a diffusion-based picture that is sometimes referred to as photon migration. The novelty of this work lies in the successful quantitative recovery of fluorescence lifetimes, absolute fluorescence quantum yields, fluorophore concentrations, emission spectra, and both scattering and absorption coefficients at the emission wavelength from a tissue-like medium. All of these parameters are sensitive to the fluorophore local environment and hence are indicators of the tissue's physiological state. One application demonstrating the capabilities of frequency-domain lifetime spectroscopy in tissue-like media is a study of the binding of ethidium bromide to bovine leukocytes in fresh milk. Ethidium bromide is a fluorescent dye that is commonly used to label DNA, and hence visualize chromosomes in cells. The lifetime of

Efficient 525 nm laser generation in single or double resonant cavity

Science.gov (United States)

Liu, Shilong; Han, Zhenhai; Liu, Shikai; Li, Yinhai; Zhou, Zhiyuan; Shi, Baosen

2018-03-01

This paper reports the results of a study into highly efficient sum frequency generation from 792 and 1556 nm wavelength light to 525 nm wavelength light using either a single or double resonant ring cavity based on a periodically poled potassium titanyl phosphate crystal (PPKTP). By optimizing the cavity's parameters, the maximum power achieved for the resultant 525 nm laser was 263 and 373 mW for the single and double resonant cavity, respectively. The corresponding quantum conversion efficiencies were 8 and 77% for converting 1556 nm photons to 525 nm photons with the single and double resonant cavity, respectively. The measured intra-cavity single pass conversion efficiency for both configurations was about 5%. The performances of the sum frequency generation in these two configurations was studied and compared in detail. This work will provide guidelines for optimizing the generation of sum frequency generated laser light for a variety of configurations. The high conversion efficiency achieved in this work will help pave the way for frequency up-conversion of non-classical quantum states, such as the squeezed vacuum and single photon states. The proposed green laser source will be used in our future experiments, which includes a plan to generate two-color entangled photon pairs and achieve the frequency down-conversion of single photons carrying orbital angular momentum.

Dispersion relations and sum rules for natural optical activity

International Nuclear Information System (INIS)

Thomaz, M.T.; Nussenzveig, H.M.

1981-06-01

Dispersion relations and sum rules are derived for the complex rotatory power of an arbitrary linear (nonmagnetic) isotropic medium showing natural optical activity. Both previously known dispersion relations and sum rules as well as new ones are obtained. It is shown that the Rosenfeld-Condon dispersion formula is inconsistent with the expected asymptotic behavior at high frequencies. A new dispersion formula based on quantum eletro-dynamics removes this inconsistency; however, it still requires modification in the low-frequency limit. (Author) [pt

Ultrashort Generation Regimes in the All-Fiber Kerr Mode-Locked Erbium-Doped Fiber Ring Laser for Terahertz Pulsed Spectroscopy

Directory of Open Access Journals (Sweden)

V. S. Voropaev

2015-01-01

Full Text Available Many femtosecond engineering applications require for a stable generation of ultrashort pulses. Thus, in the terahertz pulsed spectroscopy a measurement error in the refractive index is strongly dependent on the pulse duration stability with allowable variation of few femtoseconds. The aim of this work is to study the ultrashort pulses (USP regimes stability in the all – fiber erbium doped ring laser with Kerr mode-locking. The study was conducted at several different values of the total resonator intra-cavity dispersion. Three laser schemes with the intra-cavity dispersion values from -1.232 ps2 to +0.008 ps2 have been studied. In the experiment there were two regimes of generation observed: the stretched pulse generation and ordinary soliton generation. Main attention is focused on the stability of regimes under study. The most stable regime was that of the stretched pulse generation with a spectrum form of sech2 , possible pulse duration of 490 fs at least, repetition rate of 2.9 MHz, and average output power of 17 mW. It is worth noting, that obtained regimes had characteristics suitable for the successful use in the terahertz pulsed spectroscopy. The results may be useful in the following areas of science and technology: a high-precision spectroscopy, optical frequency standards, super-continuum generation, and terahertz pulsed spectroscopy. The future system development is expected to stabilize duration and repetition rate of the obtained regime of ultra-short pulse generation.

Radio frequency scanning tunneling spectroscopy for single-molecule spin resonance.

Science.gov (United States)

Müllegger, Stefan; Tebi, Stefano; Das, Amal K; Schöfberger, Wolfgang; Faschinger, Felix; Koch, Reinhold

2014-09-26

We probe nuclear and electron spins in a single molecule even beyond the electromagnetic dipole selection rules, at readily accessible magnetic fields (few mT) and temperatures (5 K) by resonant radio-frequency current from a scanning tunneling microscope. We achieve subnanometer spatial resolution combined with single-spin sensitivity, representing a 10 orders of magnitude improvement compared to existing magnetic resonance techniques. We demonstrate the successful resonant spectroscopy of the complete manifold of nuclear and electronic magnetic transitions of up to ΔI(z)=±3 and ΔJ(z)=±12 of single quantum spins in a single molecule. Our method of resonant radio-frequency scanning tunneling spectroscopy offers, atom-by-atom, unprecedented analytical power and spin control with an impact on diverse fields of nanoscience and nanotechnology.

Premium Pricing of Liability Insurance Using Random Sum Model

OpenAIRE

Kartikasari, Mujiati Dwi

2017-01-01

Premium pricing is one of important activities in insurance. Nonlife insurance premium is calculated from expected value of historical data claims. The historical data claims are collected so that it forms a sum of independent random number which is called random sum. In premium pricing using random sum, claim frequency distribution and claim severity distribution are combined. The combination of these distributions is called compound distribution. By using liability claim insurance data, we ...

Ultrafast spectroscopy of model biological membranes

NARCIS (Netherlands)

Ghosh, Avishek

2009-01-01

In this PhD thesis, I have described the novel time-resolved sum-frequency generation (TR-SFG) spectroscopic technique that I developed during the course of my PhD research and used it study the ultrafast vibrational, structural and orientational dynamics of water molecules at model biological

Laser frequency stabilization using bichromatic crossover spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Jeong, Taek; Seb Moon, Han, E-mail: hsmoon@pusan.ac.kr [Department of Physics, Pusan National University, Busan 609-735 (Korea, Republic of)

2015-03-07

We propose a Doppler-free spectroscopic method named bichromatic crossover spectroscopy (BCS), which we then use for the frequency stabilization of an off-resonant frequency that does not correspond to an atomic transition. The observed BCS in the 5S{sub 1/2} → 5P{sub 1/2} transition of {sup 87}Rb is related to the hyperfine structure of the conventional saturated absorption spectrum of this transition. Furthermore, the Doppler-free BCS is numerically calculated by considering all of the degenerate magnetic sublevels of the 5S{sub 1/2} → 5P{sub 1/2} transition in an atomic vapor cell, and is found to be in good agreement with the experimental results. Finally, we successfully achieve modulation-free off-resonant locking at the center frequency between the two 5S{sub 1/2}(F = 1 and 2) → 5P{sub 1/2}(F′ = 1) transitions using a polarization rotation of the BCS. The laser frequency stability was estimated to be the Allan variance of 2.1 × 10{sup −10} at 1 s.

Probing Pharmaceutical Mixtures during Milling: The Potency of Low-Frequency Raman Spectroscopy in Identifying Disorder.

Science.gov (United States)

Walker, Greg; Römann, Philipp; Poller, Bettina; Löbmann, Korbinian; Grohganz, Holger; Rooney, Jeremy S; Huff, Gregory S; Smith, Geoffrey P S; Rades, Thomas; Gordon, Keith C; Strachan, Clare J; Fraser-Miller, Sara J

2017-12-04

This study uses a multimodal analytical approach to evaluate the rates of (co)amorphization of milled drug and excipient and the effectiveness of different analytical methods in detecting these changes. Indomethacin and tryptophan were the model substances, and the analytical methods included low-frequency Raman spectroscopy (785 nm excitation and capable of measuring both low- (10 to 250 cm -1 ) and midfrequency (450 to 1800 cm -1 ) regimes, and a 830 nm system (5 to 250 cm -1 )), conventional (200-3000 cm -1 ) Raman spectroscopy, Fourier transform infrared spectroscopy (FTIR), and X-ray powder diffraction (XRPD). The kinetics of amorphization were found to be faster for the mixture, and indeed, for indomethacin, only partial amorphization occurred (after 360 min of milling). Each technique was capable of identifying the transformations, but some, such as low-frequency Raman spectroscopy and XRPD, provided less ambiguous signatures than the midvibrational frequency techniques (conventional Raman and FTIR). The low-frequency Raman spectra showed intense phonon mode bands for the crystalline and cocrystalline samples that could be used as a sensitive probe of order. Multivariate analysis has been used to further interpret the spectral changes. Overall, this study demonstrates the potential of low-frequency Raman spectroscopy, which has several practical advantages over XRPD, for probing (dis-)order during pharmaceutical processing, showcasing its potential for future development, and implementation as an in-line process monitoring method.

Effects of Second-Order Sum- and Difference-Frequency Wave Forces on the Motion Response of a Tension-Leg Platform Considering the Set-down Motion

Science.gov (United States)

Wang, Bin; Tang, Yougang; Li, Yan; Cai, Runbo

2018-04-01

This paper presents a study on the motion response of a tension-leg platform (TLP) under first- and second-order wave forces, including the mean-drift force, difference and sum-frequency forces. The second-order wave force is calculated using the full-field quadratic transfer function (QTF). The coupled effect of the horizontal motions, such as surge, sway and yaw motions, and the set-down motion are taken into consideration by the nonlinear restoring matrix. The time-domain analysis with 50-yr random sea state is performed. A comparison of the results of different case studies is made to assess the influence of second-order wave force on the motions of the platform. The analysis shows that the second-order wave force has a major impact on motions of the TLP. The second-order difference-frequency wave force has an obvious influence on the low-frequency motions of surge and sway, and also will induce a large set-down motion which is an important part of heave motion. Besides, the second-order sum-frequency force will induce a set of high-frequency motions of roll and pitch. However, little influence of second-order wave force is found on the yaw motion.

Capacitance-based frequency adjustment of micro piezoelectric vibration generator.

Science.gov (United States)

Mao, Xinhua; He, Qing; Li, Hong; Chu, Dongliang

2014-01-01

Micro piezoelectric vibration generator has a wide application in the field of microelectronics. Its natural frequency is unchanged after being manufactured. However, resonance cannot occur when the natural frequencies of a piezoelectric generator and the source of vibration frequency are not consistent. Output voltage of the piezoelectric generator will sharply decline. It cannot normally supply power for electronic devices. In order to make the natural frequency of the generator approach the frequency of vibration source, the capacitance FM technology is adopted in this paper. Different capacitance FM schemes are designed by different locations of the adjustment layer. The corresponding capacitance FM models have been established. Characteristic and effect of the capacitance FM have been simulated by the FM model. Experimental results show that the natural frequency of the generator could vary from 46.5 Hz to 42.4 Hz when the bypass capacitance value increases from 0 nF to 30 nF. The natural frequency of a piezoelectric vibration generator could be continuously adjusted by this method.

Capacitance-Based Frequency Adjustment of Micro Piezoelectric Vibration Generator

Directory of Open Access Journals (Sweden)

Xinhua Mao

2014-01-01

Full Text Available Micro piezoelectric vibration generator has a wide application in the field of microelectronics. Its natural frequency is unchanged after being manufactured. However, resonance cannot occur when the natural frequencies of a piezoelectric generator and the source of vibration frequency are not consistent. Output voltage of the piezoelectric generator will sharply decline. It cannot normally supply power for electronic devices. In order to make the natural frequency of the generator approach the frequency of vibration source, the capacitance FM technology is adopted in this paper. Different capacitance FM schemes are designed by different locations of the adjustment layer. The corresponding capacitance FM models have been established. Characteristic and effect of the capacitance FM have been simulated by the FM model. Experimental results show that the natural frequency of the generator could vary from 46.5 Hz to 42.4 Hz when the bypass capacitance value increases from 0 nF to 30 nF. The natural frequency of a piezoelectric vibration generator could be continuously adjusted by this method.

Fast Hopping Frequency Generation in Digital CMOS

CERN Document Server

Farazian, Mohammad; Gudem, Prasad S

2013-01-01

Overcoming the agility limitations of conventional frequency synthesizers in multi-band OFDM ultra wideband is a key research goal in digital technology. This volume outlines a frequency plan that can generate all the required frequencies from a single fixed frequency, able to implement center frequencies with no more than two levels of SSB mixing. It recognizes the need for future synthesizers to bypass on-chip inductors and operate at low voltages to enable the increased integration and efficiency of networked appliances. The author examines in depth the architecture of the dividers that generate the necessary frequencies from a single base frequency and are capable of establishing a fractional division ratio.   Presenting the first CMOS inductorless single PLL 14-band frequency synthesizer for MB-OFDMUWB makes this volume a key addition to the literature, and with the synthesizer capable of arbitrary band-hopping in less than two nanoseconds, it operates well within the desired range on a 1.2-volt power s...

Investigation of natural frequencies of laser inertial confinement fusion capsules using resonant ultrasound spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Ma, Xiaojun [Institute of Modern Physics, Fudan University, Shanghai 200433 (China); Research Center of Laser Fusion, CAEP, Mianyang 621900 (China); Tang, Xing; Wang, Zongwei [Research Center of Laser Fusion, CAEP, Mianyang 621900 (China); Chen, Qian; Qian, Menglu [Institute of Acoustic, Tongji University, Shanghai 200433 (China); Meng, Jie [Research Center of Laser Fusion, CAEP, Mianyang 621900 (China); Tang, Yongjian [Institute of Modern Physics, Fudan University, Shanghai 200433 (China); Research Center of Laser Fusion, CAEP, Mianyang 621900 (China); Zou, Yaming; Shen, Hao [Institute of Modern Physics, Fudan University, Shanghai 200433 (China); Gao, Dangzhong, E-mail: dgaocn@163.com [Research Center of Laser Fusion, CAEP, Mianyang 621900 (China)

2017-01-15

Highlights: • The frequency equation of isotropic multi-layer hollow spheres was derived using three-dimension (3D) elasticity theory and transfer matrix method. • The natural frequencies of the capsules with a millimeter-sized diameter are determined experimentally using resonant ultrasound spectrum (RUS) system. • The predicted natural frequencies of the frequency equation accord well with the observed results. • The theoretical and experimental investigation has proved the potential applicability of RUS to both metallic and non-metallic capsules. - Abstract: The natural frequency problem of laser inertial confinement fusion (ICF) capsules is one of the basic problems for determining non-destructively the elasticity modulus of each layer material using resonant ultrasound spectroscopy (RUS). In this paper, the frequency equation of isotropic one-layer hollow spheres was derived using three dimension (3D) elasticity theory and some simplified frequency equations were discussed under axisymmetric and spherical symmetry conditions. The corresponding equation of isotropic multi-layer hollow spheres was given employing transfer matrix method. To confirm the validity of the frequency equation and explore the feasibility of RUS for characterizing the ICF capsules, three representative capsules with a millimeter-sized diameter were determined by piezoelectric-based resonant ultrasound spectroscopy (PZT-RUS) and laser-based resonant ultrasound spectroscopy (LRUS) techniques. On the basis of both theoretical and experimental results, it is proved that the calculated and measured natural frequencies are accurate enough for determining the ICF capsules.

Support effects in catalysis studied by in-situ sum frequency generation vibrational spectroscopy and in-situ x-ray spectroscopies

Energy Technology Data Exchange (ETDEWEB)

Kennedy, Griffin John [Univ. of California, Berkeley, CA (United States)

2017-04-14

Here, kinetic measurements are paired with in-situ spectroscopic characterization tools to investigate colloidally based, supported Pt catalytic model systems in order to elucidate the mechanisms by which metal and support work in tandem to dictate activity and selectivity. The results demonstrate oxide support materials, while inactive in absence of Pt nanoparticles, possess unique active sites for the selective conversion of gas phase molecules when paired with an active metal catalyst.

Two-photon direct frequency comb spectroscopy of alkali atoms

Science.gov (United States)

Palm, Christopher; Pradhananga, Trinity; Nguyen, Khoa; Montcrieffe, Caitlin; Kimball, Derek

2012-11-01

We have studied transition frequencies and excited state hyperfine structure in rubidium using 2-photon transitions excited directly with the frequency-doubled output of a erbium fiber optical frequency comb. The frequency comb output is directed in two counterpropagating directions through a vapor cell containing the rubidium vapor. A pair of optical filters is used to select teeth of the comb in order to identify the transition wavelengths. A photomultiplier tube (PMT) measures fluorescence from a decay channel wavelength selected with another optical filter. Using different combinations of filters enables a wide range of transitions to be investigated. By scanning the repetition rate, a Doppler-free spectrum can be obtained enabling kHz-resolution spectral measurements. An interesting dependence of the 2-photon spectrum on the energy of the intermediate state of the 2-photon transition is discussed. Our investigations are laying the groundwork for a long-term research program to use direct frequency comb spectroscopy to understand the complex spectra of rare-earth atoms.

Moessbauer sum rules for use with synchrotron sources

International Nuclear Information System (INIS)

Lipkin, H.J.

1995-01-01

The availability of tunable synchrotron radiation sources with millivolt resolution has opened prospects for exploring dynamics of complex systems with Moessbauer spectroscopy. Early Moessbauer treatments and moment sum rules are extended to treat inelastic excitations measured in synchrotron experiments, with emphasis on the unique conditions absent in neutron scattering and arising in resonance scattering: prompt absorption, delayed emission, recoilfree transitions, and coherent forward scattering. The first moment sum rule normalizes the inelastic spectrum. Sum rules obtained for higher moments include the third moment proportional to the second derivative of the potential acting on the Moessbauer nucleus and independent of temperature in the harmonic approximation. Interesting information may be obtained on the behavior of the potential acting on this nucleus in samples not easily investigated with neutron scattering, e.g., small samples, thin films, time-dependent structures, and amorphous-metallic high pressure phases

Generation of optical frequencies out of the frequency comb of a femtosecond laser for DWDM telecommunication

International Nuclear Information System (INIS)

Kim, Y-J; Chun, B J; Kim, Y; Hyun, S; Kim, S-W

2010-01-01

We exploit the frequency comb of a fs laser as the frequency ruler to generate reference optical frequencies for multi-channel DWDM (dense wavelength-division-multiplexing) telecommunication. Our fiber-based scheme of single-mode extraction enables on-demand generation of optical frequencies within the telecommunication band with an absolute frequency uncertainty of 9.1×10 -13 . The linewidth of extracted optical modes is less than 1 Hz, and the instability is measured 2.3×10 -15 at 10 s averaging. This outstanding performance of optical frequency generation would lead to a drastic improvement of the spectral efficiency for the next-generation DWDM telecommunication

Optical frequency comb Faraday rotation spectroscopy

Science.gov (United States)

Johansson, Alexandra C.; Westberg, Jonas; Wysocki, Gerard; Foltynowicz, Aleksandra

2018-05-01

We demonstrate optical frequency comb Faraday rotation spectroscopy (OFC-FRS) for broadband interference-free detection of paramagnetic species. The system is based on a femtosecond doubly resonant optical parametric oscillator and a fast-scanning Fourier transform spectrometer (FTS). The sample is placed in a DC magnetic field parallel to the light propagation. Efficient background suppression is implemented via switching the direction of the field on consecutive FTS scans and subtracting the consecutive spectra, which enables long-term averaging. In this first demonstration, we measure the entire Q- and R-branches of the fundamental band of nitric oxide in the 5.2-5.4 µm range and achieve good agreement with a theoretical model.

Collective excitations of strongly coupled bilayer charged Bose liquids in the third-frequency-moment sum rule

International Nuclear Information System (INIS)

Tas, Murat; Tanatar, B.

2008-01-01

We calculate the collective excitation modes of strongly coupled bilayer charged Bose systems. We employ the dielectric matrix formulation to study the correlation effects within the random-phase approximation (RPA), the self consistent field approximation Singwi, Tosi, Land, and Sjoelander (STLS), and the quasilocalized charge approximation (QLCA), which satisfies the third-frequency-moment ( 3 >) sum rule. We find that the QLCA predicts a long-wavelength correlation-induced energy gap in the out-of-phase plasmon mode, similar to the situation in electronic bilayer systems. The energy gap and the plasmon density of states are studied as a function of interlayer separation and coupling parameter r s . The results should be helpful for experimental investigations

High resolution mid-infrared spectroscopy based on frequency upconversion

DEFF Research Database (Denmark)

Dam, Jeppe Seidelin; Hu, Qi; Tidemand-Lichtenberg, Peter

2013-01-01

signals can be analyzed. The obtainable frequency resolution is usually in the nm range where sub nm resolution is preferred in many applications, like gas spectroscopy. In this work we demonstrate how to obtain sub nm resolution when using upconversion. In the presented realization one object point...... high resolution spectral performance by observing emission from hot water vapor in a butane gas burner....

a Thz Photomixing Synthesizer Based on a Fiber Frequency Comb for High Resolution Rotational Spectroscopy

Science.gov (United States)

Hindle, Francis; Mouret, Gael; Cuisset, Arnaud; Yang, Chun; Eliet, Sophie; Bocquet, Robin

2010-06-01

To date the principal application for photomixing sources has been for high resolution spectroscopy of gases due to the large tuning range and spectral purity. New Developments of the Opto-Electronic THz Spectrometer have been performed in order to obtain a powerful tool for High-Resolution Spectroscopy. The combination of two extended cavity laser diodes and fast charge carrier lifetime semiconductor materials has allowed a continuous-wave THz spectrometer to be constructed based on optical heterodyning. Unlike many THz sources, this instrument gives access to all frequencies in the range 0.3 to 3.5 THz with a resolution of 1 MHz. The main spectroscopic applications of this spectrometer were dedicated to line profile analysis of rotational transitions referenced in the spectroscopic databases. One limitation of the THz spectrometer was accuracy with which the generated frequency is known. Recently, this obstacle has been circled with the construction of a photomixing spectrometer where the two pump lasers are phase locked to two modes of a repetition rate stabilized frequency doubled fiber laser frequency comb. In order to achieve a tuning range in excess to 100 MHz a third cw laser was required in the new configuration of the THz spectrometer. To assess the performances of this instrument, the frequencies of the pure rotational transitions of OCS molecules have been measured between 0,8 to 1,2 THz. A rms inferior to 100 kHz, deduced from the frequencies measured, demonstrates that the THz photomixing synthesizer is now able to be competitive with microwave and submillimeter techniques. S. Matton, F. Rohart, R. Bocquet, D. Bigourd, A. Cuisset, F. Hindle, G. Mouret, J. Mol. Spectrosc., 2006, 239: 182. C. Yang, J. Buldyreva, I. E. Gordon, F. Rohart, A. Cuisset, G. Mouret, R. Bocquet, F. Hindle, J. Quant. Spectrosc. Radiat. Transfer, 2008, 109: 2857. G. Mouret, F. Hindle, A. Cuisset, C. Yang, R. Bocquet, M. Lours, D. Rovera, Opt. Express, 2009, 17: 22031.

A Bayesian analysis of QCD sum rules

International Nuclear Information System (INIS)

Gubler, Philipp; Oka, Makoto

2011-01-01

A new technique has recently been developed, in which the Maximum Entropy Method is used to analyze QCD sum rules. This approach has the virtue of being able to directly generate the spectral function of a given operator, without the need of making an assumption about its specific functional form. To investigate whether useful results can be extracted within this method, we have first studied the vector meson channel, where QCD sum rules are traditionally known to provide a valid description of the spectral function. Our results show a significant peak in the region of the experimentally observed ρ-meson mass, which is in agreement with earlier QCD sum rules studies and suggests that the Maximum Entropy Method is a strong tool for analyzing QCD sum rules.

Identification of scalp EEG circadian variation using a novel correlation sum measure

Science.gov (United States)

Shahidi Zandi, Ali; Boudreau, Philippe; Boivin, Diane B.; Dumont, Guy A.

2015-10-01

Objective. In this paper, we propose a novel method to determine the circadian variation of scalp electroencephalogram (EEG) in both individual and group levels using a correlation sum measure, quantifying self-similarity of the EEG relative energy across waking epochs. Approach. We analysed EEG recordings from central-parietal and occipito-parietal montages in nine healthy subjects undergoing a 72 h ultradian sleep-wake cycle protocol. Each waking epoch (˜1 s) of every nap opportunity was decomposed using the wavelet packet transform, and the relative energy for that epoch was calculated in the desired frequency band using the corresponding wavelet coefficients. Then, the resulting set of energy values was resampled randomly to generate different subsets with equal number of elements. The correlation sum of each subset was then calculated over a range of distance thresholds, and the average over all subsets was computed. This average value was finally scaled for each nap opportunity and considered as a new circadian measure. Main results. According to the evaluation results, a clear circadian rhythm was identified in some EEG frequency ranges, particularly in 4-8 Hz and 10-12 Hz. The correlation sum measure not only was able to disclose the circadian rhythm on the group data but also revealed significant circadian variations in most individual cases, as opposed to previous studies only reporting the circadian rhythms on a population of subjects. Compared to a naive measure based on the EEG absolute energy in the frequency band of interest, the proposed measure showed a clear superiority using both individual and group data. Results also suggested that the acrophase (i.e., the peak) of the circadian rhythm in 10-12 Hz occurs close to the core body temperature minimum. Significance. These results confirm the potential usefulness of the proposed EEG-based measure as a non-invasive circadian marker.

Use of low-frequency Raman spectroscopy and chemometrics for the quantification of crystallinity in amorphous griseofulvin tablets

DEFF Research Database (Denmark)

Mah, Pei T.; Fraser, Sara J.; Reish, Matthew E.

2015-01-01

in stored amorphous samples earlier than the mid-frequency 785 nm Raman system. Overall, this study suggests that low-frequency Raman spectroscopy has at least equally good performance compared to mid-frequency Raman for quantitative analysis of crystallinity in the pharmaceutical setting. More generally......Low-frequency Raman spectroscopy, which directly probes phonon lattice modes of crystal structures, has much unexplored potential for sensitive qualitative and quantitative analysis of crystallinity in drugs and excipients. In this study, the level of crystallinity in tablets containing amorphous...

Conformational order of n-dodecanethiol and n-dodecaneselenol monolayers on polycrystalline copper investigated by PM-IRRAS and SFG spectroscopy

Science.gov (United States)

Fonder, G.; Cecchet, F.; Peremans, A.; Thiry, P. A.; Delhalle, J.; Mekhalif, Z.

2009-08-01

Self-assembled monolayers (SAMs) of n-dodecanethiol (C 12H 25SH) and n-dodecaneselenol (C 12H 25SeH) on polycrystalline copper have been elaborated with the purpose of achieving densely packed and crystalline-like assemblies. By combining the surface sensitivity of polarization modulation infrared reflection absorption spectroscopy (PM-IRRAS) and sum-frequency generation spectroscopy (SFG), the effect of the self-assembly time (15 min, 30 min, 1 h, 2 h and 24 h) on the formation of n-dodecanethiol and n-dodecaneselenol monolayers on untreated and electrochemically reduced polycrystalline copper has been investigated. On electrochemically reduced copper, PM-IRRAS spectroscopy shows that both molecules are able to form well organized layers. SFG spectroscopy indicates that the C 12H 25SeH SAMs are slightly better ordered than those achieved with C 12H 25SH. On untreated copper, the two molecules lead to different film organizations. Both PM-IRRAS and SFG indicate that C 12H 25SH SAMs are of the same film quality as those obtained on electrochemically reduced copper. On the contrary, C 12H 25SeH monolayers are invariably poorly organized at the molecular level.

QCD sum rules in a Bayesian approach

International Nuclear Information System (INIS)

Gubler, Philipp; Oka, Makoto

2011-01-01

A novel technique is developed, in which the Maximum Entropy Method is used to analyze QCD sum rules. The main advantage of this approach lies in its ability of directly generating the spectral function of a given operator. This is done without the need of making an assumption about the specific functional form of the spectral function, such as in the 'pole + continuum' ansatz that is frequently used in QCD sum rule studies. Therefore, with this method it should in principle be possible to distinguish narrow pole structures form continuum states. To check whether meaningful results can be extracted within this approach, we have first investigated the vector meson channel, where QCD sum rules are traditionally known to provide a valid description of the spectral function. Our results exhibit a significant peak in the region of the experimentally observed ρ-meson mass, which agrees with earlier QCD sum rules studies and shows that the Maximum Entropy Method is a useful tool for analyzing QCD sum rules.

A CMOS frequency generation module for 60-GHz applications

International Nuclear Information System (INIS)

Zhou Chunyuan; Zhang Lei; Wang Hongrui; Qian He

2012-01-01

A frequency generation module for 60-GHz transceivers and phased array systems is presented in this paper. It is composed of a divide-by-2 current mode logic divider (CML) and a doubler in push-push configuration. Benefiting from the CML structure and push-push configuration, the proposed frequency generation module has a wide operating frequency range to cover process, voltage, and temperature variation. It is implemented in a 90-nm CMOS process, and occupies a chip area of 0.64 × 0.65 mm 2 including pads. The measurement results show that the designed frequency generation module functions properly with input frequency over 15 GHz to 25 GHz. The whole chip dissipates 12.1 mW from a 1.2-V supply excluding the output buffers. (semiconductor integrated circuits)

Optical generation of radio-frequency power

International Nuclear Information System (INIS)

Hietala, V.M.; Vawter, G.A.; Brennan, T.M.; Hammons, B.E.; Meyer, W.J.

1994-11-01

An optical technique for high-power radio-frequency (RF) signal generation is described. The technique uses a unique photodetector based on a traveling-wave design driven by an appropriately modulated light source. The traveling-wave photodetector (TWPD) exhibits simultaneously a theoretical quantum efficiency approaching 100 % and a very large electrical bandwidth. Additionally, it is capable of dissipating the high-power levels required for the RF generation technique. The modulated light source is formed by either the beating together of two lasers or by the direct modulation of a light source. A system example is given which predicts RF power levels of 100's of mW's at millimeter wave frequencies with a theoretical ''wall-plug'' efficiency approaching 34%

Generation of plasmas in water: utilization of a high-frequency, low-voltage bipolar pulse power supply with impedance control

International Nuclear Information System (INIS)

Baroch, P; Potocky, S; Saito, N

2011-01-01

Presented work focuses on the investigation and characterization of plasma discharges generated in water by newly developed bipolar pulse power supply. The main aim of our work was to solve and overcome problems with intensive arc discharge transition when the discharge is ignited and maintained by a low output impedance pulse power supply. For this purpose a novel type of bipolar pulse power supply was developed and tested. It was found that two distinguished stable modes of discharges generated in the water can be realized. Effects of water conductivity, pulse frequency and initial water temperature on the discharge properties were investigated. Optical emission spectroscopy was employed to study plasma parameters of the discharge and the correlation between the data obtained from the optical emission spectroscopy and the chemical species measured in the water was carried out.

Investigation of the summation of copper-vapour laser frequencies

International Nuclear Information System (INIS)

Karpukhin, Vyacheslav T; Konev, Yu B; Malikov, Mikhail M

1998-01-01

An investigation was made of the conversion of the copper-vapour laser radiation ( λ 1 = 0.51 μm and λ 2 = 0.578 μm) into UV radiation at the sum frequency (λ 3 = 0.271 μm) in a DKDP crystal. The operation of this frequency converter was compared for two magnifications of the laser cavity: M = 5 and 200. The best results were obtained for M = 200 (average UV radiation power 0.75 W, conversion efficiency 12%). A study was made of the characteristics of the formation of radiation pulses representing the two lines in the laser beam as a whole and in its weakly diverging core. In a low-divergence beam the yellow- and green-line pulses were emitted practically simultaneously with approximately the same peak power, which facilitated the sum-frequency generation. (nonlinear optical phenomena)

Extremely frequency-widened terahertz wave generation using Cherenkov-type radiation.

Science.gov (United States)

Suizu, Koji; Koketsu, Kaoru; Shibuya, Takayuki; Tsutsui, Toshihiro; Akiba, Takuya; Kawase, Kodo

2009-04-13

Terahertz (THz) wave generation based on nonlinear frequency conversion is promising way for realizing a tunable monochromatic bright THz-wave source. Such a development of efficient and wide tunable THz-wave source depends on discovery of novel brilliant nonlinear crystal. Important factors of a nonlinear crystal for THz-wave generation are, 1. High nonlinearity and 2. Good transparency at THz frequency region. Unfortunately, many nonlinear crystals have strong absorption at THz frequency region. The fact limits efficient and wide tunable THz-wave generation. Here, we show that Cherenkov radiation with waveguide structure is an effective strategy for achieving efficient and extremely wide tunable THz-wave source. We fabricated MgO-doped lithium niobate slab waveguide with 3.8 microm of thickness and demonstrated difference frequency generation of THz-wave generation with Cherenkov phase matching. Extremely frequency-widened THz-wave generation, from 0.1 to 7.2 THz, without no structural dips successfully obtained. The tuning frequency range of waveguided Cherenkov radiation source was extremely widened compare to that of injection seeded-Terahertz Parametric Generator. The tuning range obtained in this work for THz-wave generation using lithium niobate crystal was the widest value in our knowledge. The highest THz-wave energy obtained was about 3.2 pJ, and the energy conversion efficiency was about 10(-5) %. The method can be easily applied for many conventional nonlinear crystals, results in realizing simple, reasonable, compact, high efficient and ultra broad band THz-wave sources.

Least square regularized regression in sum space.

Science.gov (United States)

Xu, Yong-Li; Chen, Di-Rong; Li, Han-Xiong; Liu, Lu

2013-04-01

This paper proposes a least square regularized regression algorithm in sum space of reproducing kernel Hilbert spaces (RKHSs) for nonflat function approximation, and obtains the solution of the algorithm by solving a system of linear equations. This algorithm can approximate the low- and high-frequency component of the target function with large and small scale kernels, respectively. The convergence and learning rate are analyzed. We measure the complexity of the sum space by its covering number and demonstrate that the covering number can be bounded by the product of the covering numbers of basic RKHSs. For sum space of RKHSs with Gaussian kernels, by choosing appropriate parameters, we tradeoff the sample error and regularization error, and obtain a polynomial learning rate, which is better than that in any single RKHS. The utility of this method is illustrated with two simulated data sets and five real-life databases.

Frequency metrology of a photomixing source for gas phase spectroscopy

Science.gov (United States)

Hindle, Francis; Mouret, Gael; Yang, Chun; Cuisset, Arnaud; Bocquet, Robin; Lours, Michel; Rovera, Daniele

2010-08-01

The availability of frequency combs has opened new possibilities for the measurement of optical frequencies. Photomixing is an attractive solution for high resolution THz spectroscopy of gases due to the narrow spectral resolution and ability to access the 100 GHz to 3.5 THz range. One limitation of present photomixing spectrometers is the accuracy with which the THz frequency is established. Measurement of the centre frequency gas phase molecular transitions requires an accuracy better than 100 kHz in order to allow spectroscopic constants to be determined. Standard optical techniques like those employed in wavelength meters can only provide accuracies in the order of 50 MHz. We have used a turnkey fibre based frequency comb and a standard photomixing configuration to realize a THz synthesizer with an accuracy of around 50kHz. Two ECDLs used to pump the photomixer are phase locked onto the frequency comb and provide a tuning range of 10 MHz. In order to extend the tuning range an additional phase locked ECLD has been added to obtain a range in excess of 100 MHz. The absorption profiles of many Doppler limited transitions of carbonyl sulphide and formaldehyde have been measured to validate this instrument.

Effects of three-mode field interactions in laser instabilities and in beat-frequency spectroscopy

International Nuclear Information System (INIS)

Herdow, S.T.

1982-01-01

Population pulsations are fluctuations in the population difference (of a two level system) due to the presence of two or more coherent waves interfering in the medium. In this work, the author shows that population pulsations generated by three waves, a central wave and two mode-locked sidebands, are responsible for both the multiwavelength and the single-wavelength instabilities of single-mode lasers containing homgeneously-broadened media. The role of the population pulsations in establishing these instabilities, however, diminish as the central mode is detuned away from the atomic resonance frequency. For homogeneously-broadened lasers, the author finds two regions of single-wavelength instability. The first is at line center, for which population pulsations are solely responsible, and the second is off line center where the unsaturated medium provides the required gain and anomalous dispersion. For the case of inhomogeneously-broadened lasers, the author shows that population pulsations significantly increase the instability range over that predicted by Casperson for single-mode bad-cavity lasers. Both the unidirectional ring and the standing-wave cavities are treated. The Fourier expansion technique, used in this work, for treating three-frequency operation in saturation spectroscopy is shown to be equivalent (in appropriate limits) to the linear stability analysis in laser theory and optical bistability. The author also shows, in single-sideband saturation spectroscopy, that for long interaction lengths propagation effects can significantly influence the absorption and dispersion coefficients of the medium. Finally, the author shows that under certain conditions the pronounced splitting effects of the population pulsations develop into regions of intense absorption

Simple method of generating and distributing frequency-entangled qudits

Science.gov (United States)

Jin, Rui-Bo; Shimizu, Ryosuke; Fujiwara, Mikio; Takeoka, Masahiro; Wakabayashi, Ryota; Yamashita, Taro; Miki, Shigehito; Terai, Hirotaka; Gerrits, Thomas; Sasaki, Masahide

2016-11-01

High-dimensional, frequency-entangled photonic quantum bits (qudits for d-dimension) are promising resources for quantum information processing in an optical fiber network and can also be used to improve channel capacity and security for quantum communication. However, up to now, it is still challenging to prepare high-dimensional frequency-entangled qudits in experiments, due to technical limitations. Here we propose and experimentally implement a novel method for a simple generation of frequency-entangled qudts with d\\gt 10 without the use of any spectral filters or cavities. The generated state is distributed over 15 km in total length. This scheme combines the technique of spectral engineering of biphotons generated by spontaneous parametric down-conversion and the technique of spectrally resolved Hong-Ou-Mandel interference. Our frequency-entangled qudits will enable quantum cryptographic experiments with enhanced performances. This distribution of distinct entangled frequency modes may also be useful for improved metrology, quantum remote synchronization, as well as for fundamental test of stronger violation of local realism.

On-electrode autonomous current generator for multi-frequency EIT

International Nuclear Information System (INIS)

Jivet, I; Dragoi, B

2008-01-01

The paper presents an autonomous programmable current generator module for multi-frequency EIT systems. The module incorporates all stages from the sine wave generation with frequency and amplitude tuning, D/A converter and filter, a high output resistance voltage-to-current converter to the associated digital communication and control. The paper presents in depth the original digital quadrature signal generator and the output current generator with a high resistance. The other main blocks of the design use current practice specifications, since recent technological solutions proposed in the literature were found appropriate. The proposed signal generator circuit, characterized by a very low complexity, is analyzed in its capacity to produce multiple accurate signals up to 1 MHz in frequency. The precision output current source uses a modified current conveyor of type CCII with a high output resistance and low distortion. The output current frequency spectrum and linearity parameters obtained in the simulations are also described. The simulation results indicate a good linearity and high output resistance with an acceptable output voltage swing. The calculated performance parameters are validated with simulations, and future work for the prototype fabrication of the IC is outlined

Experimental and theoretical evidence for bilayer-by-bilayer surface melting of crystalline ice

DEFF Research Database (Denmark)

Sánchez, M. Alejandra; Kling, Tanja; Ishiyama, Tatsuya

2017-01-01

, and its nature, we investigate the surface melting of hexagonal ice by combining noncontact, surfacespecific vibrational sum frequency generation (SFG) spectroscopy and spectra calculated from molecular dynamics simulations. Using SFG, we probe the outermost water layers of distinct single crystalline ice...

Frequency stabilization of a 1083 nm fiber laser to {sup 4}He transition lines with optical heterodyne saturation spectroscopies

Energy Technology Data Exchange (ETDEWEB)

Gong, W.; Peng, X., E-mail: xiangpeng@pku.edu.cn; Li, W.; Guo, H., E-mail: hongguo@pku.edu.cn [State Key Laboratory of Advanced Optical Communication Systems and Networks, School of Electronics Engineering and Computer Science, Center for Quantum Information Technology, and Center for Computational Science and Engineering (CCSE), Peking University, Beijing 100871 (China)

2014-07-15

Two kinds of optical heterodyne saturation spectroscopies, namely, frequency modulation spectroscopy (FMS) and modulation transfer spectroscopy (MTS), are demonstrated for locking a fiber laser to the transition lines of metastable {sup 4}He atoms around 1083 nm. The servo-loop error signals of FMS and MTS for stabilizing laser frequency are optimized by studying the dependence of the peak-to-peak amplitude and slope on the optical power of pump and probe beams. A comparison of the stabilization performances of FMS/MTS and polarization spectroscopy (PS) is presented, which shows that MTS exhibits relatively superior performance with the least laser frequency fluctuation due to its flat-background dispersive signal, originated from the four-wave mixing process. The Allan deviation of the stabilized laser frequency is 5.4 × 10{sup −12}@100 s with MTS for data acquired in 1000 s, which is sufficiently applicable for fields like laser cooling, optical pumping, and optical magnetometry.

Computational expressions for signals in frequency-modulation spectroscopy.

Science.gov (United States)

Di Rosa, Michael D; Reiten, M T

2015-06-01

General expressions for the signals in frequency-modulation spectroscopy (FMS) appear in the literature but are often reduced to simple analytical equations following the assumption of a weak modulation index. This is little help to the experimentalist who wants to predict signals for modulation depths of the order of unity or greater, where strong FMS signals reside. Here, we develop general formulas for FMS signals in the case of an absorber with a Voigt line shape and then link these expressions to an example and existing numerical code for the line shape. The resulting computational recipe is easy to implement and exercised here to show where the larger FMS signals are found over the coordinates of modulation index and modulation frequency. One can also estimate from provided curves the in-phase FMS signal over a wide range of modulation parameters at either the Lorentzian-broadening or Doppler-broadening limit, or anywhere in between by interpolation.

Probing electronic and vibrational properties at the electrochemical interface using SFG spectroscopy: Methanol electro-oxidation on Pt(1 1 0)

Science.gov (United States)

Vidal, F.; Busson, B.; Tadjeddine, A.

2005-02-01

We report the study of methanol electro-oxidation on Pt(1 1 0) using infrared-visible sum-frequency generation (SFG) vibrational spectroscopy. The use of this technique enables to probe the vibrational and electronic properties of the interface simultaneously in situ. We have investigated the vibrational properties of the interface in the CO ads internal stretch spectral region (1700-2150 cm -1) over a wide range of potentials. The analysis of the evolution of the C-O stretch line shape, which is related to the interference between the vibrational and electronic parts of the non-linear response, with the potential allows us to show that the onset of bulk methanol oxidation corresponds to the transition from a negatively to a positively charged surface.

Excitation of low-frequency residual currents at combination frequencies of an ionising two-colour laser pulse

Science.gov (United States)

Vvedenskii, N. V.; Kostin, V. A.; Laryushin, I. D.; Silaev, A. A.

2016-05-01

We have studied the processes of excitation of low-frequency residual currents in a plasma produced through ionisation of gases by two-colour laser pulses in laser-plasma schemes for THz generation. We have developed an analytical approach that allows one to find residual currents in the case when one of the components of a two-colour pulse is weak enough. The derived analytical expressions show that the effective generation of the residual current (and hence the effective THz generation) is possible if the ratio of the frequencies in the two-colour laser pulse is close to a rational fraction with a not very big odd sum of the numerator and denominator. The results of numerical calculations (including those based on the solution of the three-dimensional time-dependent Schrödinger equation) agree well with the analytical results.

Spectral purity and tunability of terahertz quantum cascade laser sources based on intracavity difference-frequency generation.

Science.gov (United States)

Consolino, Luigi; Jung, Seungyong; Campa, Annamaria; De Regis, Michele; Pal, Shovon; Kim, Jae Hyun; Fujita, Kazuue; Ito, Akio; Hitaka, Masahiro; Bartalini, Saverio; De Natale, Paolo; Belkin, Mikhail A; Vitiello, Miriam Serena

2017-09-01

Terahertz sources based on intracavity difference-frequency generation in mid-infrared quantum cascade lasers (THz DFG-QCLs) have recently emerged as the first monolithic electrically pumped semiconductor sources capable of operating at room temperature across the 1- to 6-THz range. Despite tremendous progress in power output, which now exceeds 1 mW in pulsed and 10 μW in continuous-wave regimes at room temperature, knowledge of the major figure of merits of these devices for high-precision spectroscopy, such as spectral purity and absolute frequency tunability, is still lacking. By exploiting a metrological grade system comprising a terahertz frequency comb synthesizer, we measure, for the first time, the free-running emission linewidth (LW), the tuning characteristics, and the absolute center frequency of individual emission lines of these sources with an uncertainty of 4 × 10 -10 . The unveiled emission LW (400 kHz at 1-ms integration time) indicates that DFG-QCLs are well suited to operate as local oscillators and to be used for a variety of metrological, spectroscopic, communication, and imaging applications that require narrow-LW THz sources.

Communication: Probing the absolute configuration of chiral molecules at aqueous interfaces

Energy Technology Data Exchange (ETDEWEB)

Lotze, Stephan, E-mail: lotze@amolf.nl; Versluis, Jan [FOM Institute for Atomic and Molecular Physics, Science Park 104, 1098 XG Amsterdam (Netherlands); Olijve, Luuk L. C.; Schijndel, Luuk van; Milroy, Lech G.; Voets, Ilja K. [Laboratory of Macromolecular and Organic Chemistry, Department of Chemical Engineering and Chemistry, and Institute for Complex Molecular Systems, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven (Netherlands); Bakker, Huib J., E-mail: bakker@amolf.nl [FOM Institute AMOLF, Science Park 104, 1098 XG Amsterdam (Netherlands)

2015-11-28

We demonstrate that the enantiomers of chiral macromolecules at an aqueous interface can be distinguished with monolayer sensitivity using heterodyne-detected vibrational sum-frequency generation (VSFG). We perform VSFG spectroscopy with a polarization combination that selectively probes chiral molecular structures. By using frequencies far detuned from electronic resonances, we probe the chiral macromolecular structures with high surface specificity. The phase of the sum-frequency light generated by the chiral molecules is determined using heterodyne detection. With this approach, we can distinguish right-handed and left-handed helical peptides at a water-air interface. We thus show that heterodyne-detected VSFG is sensitive to the absolute configuration of complex, interfacial macromolecules and has the potential to determine the absolute configuration of enantiomers at interfaces.

Laser-heating-induced displacement of surfactants on the water surface

NARCIS (Netherlands)

Backus, E.H.G.; Bonn, D.; Cantin, S.; Roke, S.; Bonn, M.

2012-01-01

We report a combined vibrational sum-frequency generation (SFG) spectroscopy, Brewster angle microscopy (BAM), and ellipsometry study of different surfactants on water as a function of surfactant density. Vibrational SFG spectra of surfactants on the water surface in a Langmuir trough have been

DPOAE generation dependence on primary frequencies ratio

Science.gov (United States)

Botti, Teresa; Sisto, Renata; Moleti, Arturo; D'Amato, Luisa; Sanjust, Filippo

2015-12-01

Two different mechanisms are responsible for the DPOAE generation. The nonlinear distortion wave-fixed mechanism generates the DPOAE Zero-Latency (ZL) component, as a backward traveling wave from the "overlap" region. Linear reflection of the forward DP wave (IDP) generates the DPOAE Long-Latency (LL) component through a place-fixed mechanism. ZL and LL components add up vectorially to generate the DPOAE recorded in the ear canal. The 2f1 - f2 and 2f2 - f1 DPOAE intensity depends on the stimulus level and on the primary frequency ratio r = f2/f1, where f1 and f2 are the primary stimuli frequencies. Here we study the behavior of the ZL and LL DPOAE components as a function of r by both numerical and laboratory experiments, measuring DPAOEs with an equal primary levels (L1 = L2) paradigm in the range [35, 75] dB SPL, with r ranging in [1.1, 1.45]. Numerical simulations of a nonlocal nonlinear model have been performed without cochlear roughness, to suppress the linear reflection mechanism. In this way the model solution at the base represents the DPOAE ZL component, and the solution at the corresponding DPOAE tonotopic place corresponds to the IDP. This technique has been not effectual to study the 2f2 - f1 DPOAE, as a consequence of its generation mechanism. While the 2f1 - f2 generation place is known to be the tonotopic place x(f2), the 2f2 - f1 DPOAE one has to be assumed basal to its corresponding reflection place. That is because ZL components generated in x(f2) cannot significantly pass through their resonant place. Moreover increasing the ratio r, 2f2 - f1 ZL and LL generation place approach each other, because the overlap region of primary tones decreases. Consequently, the distinction between the two places becomes complicated. DPOAEs have been measured in six young normal-hearing subjects. DPOAE ZL and LL components have been separated by a time-frequency filtering method based on the wavelet transform 1. due to their different phase gradient delay

Sum-rule analysis of long-wavelength excitations in electron liquids

International Nuclear Information System (INIS)

Ichimaru, Setsuo; Totsuji, Hiroo; Tange, Toshio; Pines, D.

1975-01-01

The properties of the plasma oscillations, the single-particle excitations and the collisional excitations in the classical one-component plasma are investigated in the long-wave-length domain with the aid of moment sum rules. The frequency moments of the dynamic form factor are calculated up to that term which involves the ternary correlation function. The dispersion in the plasma-wave frequency and the strengths of the single-particle and collisional excitations are computed over the thermodynamically stable domain of the plasma parameter, epsilon<=10. It is emphasized that inclusion of the collisional excitations plays a vital part in satisfying various moment-sum rules and in securing agreement with known boundary conditions such as the Vlasov description and molecular-dynamics computations. (auth.)

Multi-pollutants sensors based on near-IR telecom lasers and mid-IR difference frequency generation: development and applications; Instruments de mesure multi-polluants par spectroscopie infrarouge bases sur des lasers fibres et par generation de difference de frequences: developpement et applications

Energy Technology Data Exchange (ETDEWEB)

Cousin, J

2006-12-15

At present the detection of VOC and other anthropic trace pollutants is an important challenge in the measurement of air quality. Infrared spectroscopy, allowing spectral regions rich in molecular absorption to be probed, is a suitable technique for in-situ monitoring of the air pollution. Thus the aim of this work was to develop instruments capable of detecting multiple pollutants for in-situ monitoring by IR spectroscopy. A first project benefited from the availability of the telecommunications lasers emitting in near-IR. This instrument was based on an external cavity diode laser (1500 - 1640 nm) in conjunction with a multipass cell (100 m). The detection sensitivity was optimised by employing a balanced detection and a sweep integration procedure. The instrument developed is deployable for in-situ measurements with a sensitivity of < 10{sup -8} cm{sup -1} Hz{sup -1/2} and allowed the quantification of chemical species such as CO{sub 2}, CO, C{sub 2}H{sub 2}, CH{sub 4} and the determination of the isotopic ratio {sup 13}CO{sub 2}/{sup 12}CO{sub 2} in combustion environment The second project consisted in mixing two near-IR fiber lasers in a non-linear crystal (PPLN) in order to produce a laser radiation by difference frequency generation in the middle-IR (3.15 - 3.43 {mu}m), where the absorption bands of the molecules are the most intense. The first studies with this source were carried out on detection of ethylene (C{sub 2}H{sub 4}) and benzene (C{sub 6}H{sub 6}). Developments, characterizations and applications of these instruments in the near and middle IR are detailed and the advantages of the 2 spectral ranges is highlighted. (author)

Single-transducer dual-frequency ultrasound generation to enhance acoustic cavitation.

Science.gov (United States)

Liu, Hao-Li; Hsieh, Chao-Ming

2009-03-01

Dual- or multiple-frequency ultrasound stimulation is capable of effectively enhancing the acoustic cavitation effect over single-frequency ultrasound. Potential application of this sonoreactor design has been widely proposed such as on sonoluminescence, sonochemistry enhancement, and transdermal drug release enhancement. All currently available sonoreactor designs employed multiple piezoelectric transducers for generating single-frequency ultrasonic waves separately and then these waves were mixed and interfered in solutions. The purpose of this research is to propose a novel design of generating dual-frequency ultrasonic waves with single piezoelectric elements, thereby enhancing acoustic cavitation. Macroscopic bubbles were detected optically, and they were quantified at either a single-frequency or for different frequency combinations for determining their efficiency for enhancing acoustic cavitation. Visible bubbles were optically detected and hydrogen peroxide was measured to quantify acoustic cavitation. Test water samples with different gas concentrations and different power levels were used to determine the efficacy of enhancing acoustic cavitation of this design. The spectrum obtained from the backscattered signals was also recorded and examined to confirm the occurrence of stable cavitation. The results confirmed that single-element dual-frequency ultrasound stimulation can enhance acoustic cavitation. Under certain testing conditions, the generation of bubbles can be enhanced up to a level of five times higher than the generation of bubbles in single-frequency stimulation, and can increase the hydrogen peroxide production up to an increase of one fold. This design may serve as a useful alternative for future sonoreactor design owing to its simplicity to produce dual- or multiple-frequency ultrasound.

Analysis Tools for Next-Generation Hadron Spectroscopy Experiments

Science.gov (United States)

Battaglieri, M.; Briscoe, B. J.; Celentano, A.; Chung, S.-U.; D'Angelo, A.; De Vita, R.; Döring, M.; Dudek, J.; Eidelman, S.; Fegan, S.; Ferretti, J.; Filippi, A.; Fox, G.; Galata, G.; García-Tecocoatzi, H.; Glazier, D. I.; Grube, B.; Hanhart, C.; Hoferichter, M.; Hughes, S. M.; Ireland, D. G.; Ketzer, B.; Klein, F. J.; Kubis, B.; Liu, B.; Masjuan, P.; Mathieu, V.; McKinnon, B.; Mitchel, R.; Nerling, F.; Paul, S.; Peláez, J. R.; Rademacker, J.; Rizzo, A.; Salgado, C.; Santopinto, E.; Sarantsev, A. V.; Sato, T.; Schlüter, T.; [Silva]da Silva, M. L. L.; Stankovic, I.; Strakovsky, I.; Szczepaniak, A.; Vassallo, A.; Walford, N. K.; Watts, D. P.; Zana, L.

The series of workshops on New Partial-Wave Analysis Tools for Next-Generation Hadron Spectroscopy Experiments was initiated with the ATHOS 2012 meeting, which took place in Camogli, Italy, June 20-22, 2012. It was followed by ATHOS 2013 in Kloster Seeon near Munich, Germany, May 21-24, 2013. The third, ATHOS3, meeting is planned for April 13-17, 2015 at The George Washington University Virginia Science and Technology Campus, USA. The workshops focus on the development of amplitude analysis tools for meson and baryon spectroscopy, and complement other programs in hadron spectroscopy organized in the recent past including the INT-JLab Workshop on Hadron Spectroscopy in Seattle in 2009, the International Workshop on Amplitude Analysis in Hadron Spectroscopy at the ECT*-Trento in 2011, the School on Amplitude Analysis in Modern Physics in Bad Honnef in 2011, the Jefferson Lab Advanced Study Institute Summer School in 2012, and the School on Concepts of Modern Amplitude Analysis Techniques in Flecken-Zechlin near Berlin in September 2013. The aim of this document is to summarize the discussions that took place at the ATHOS 2012 and ATHOS 2013 meetings. We do not attempt a comprehensive review of the field of amplitude analysis, but offer a collection of thoughts that we hope may lay the ground for such a document.

Analysis Tools for Next-Generation Hadron Spectroscopy Experiments

International Nuclear Information System (INIS)

Battaglieri, Marco; Briscoe, William; Celentano, Andrea; Chung, Suh-Urk; D'Angelo, Annalisa; De Vita, Rafaella; Döring, Michael; Dudek, Jozef; Eidelman, S.; Fegan, Stuart; Ferretti, J.; Filippi, A.; Fox, G.; Galata, G.; Garcia-Tecocoatzi, H.; Glazier, Derek; Grube, B.; Hanhart, C.; Hoferichter, M.; Hughes, S. M.; Ireland, David G.; Ketzer, B.; Klein, Franz J.; Kubis, B.; Liu, B.; Masjuan, P.; Mathieu, Vincent; McKinnon, Brian; Mitchel, R.; Nerling, F.; Paul, S.; Peláez, J. R.; Rademacker, J.; Rizzo, Alessandro; Salgado, Carlos; Santopinto, E.; Sarantsev, Andrey V.; Sato, Toru; Schlüter, T.; Da Silva, M. L.L.; Stankovic, I.; Strakovsky, Igor; Szczepaniak, Adam; Vassallo, A.; Walford, Natalie K.; Watts, Daniel P.

2015-01-01

The series of workshops on New Partial-Wave Analysis Tools for Next-Generation Hadron Spectroscopy Experiments was initiated with the ATHOS 2012 meeting, which took place in Camogli, Italy, June 20-22, 2012. It was followed by ATHOS 2013 in Kloster Seeon near Munich, Germany, May 21-24, 2013. The third, ATHOS3, meeting is planned for April 13-17, 2015 at The George Washington University Virginia Science and Technology Campus, USA. The workshops focus on the development of amplitude analysis tools for meson and baryon spectroscopy, and complement other programs in hadron spectroscopy organized in the recent past including the INT-JLab Workshop on Hadron Spectroscopy in Seattle in 2009, the International Workshop on Amplitude Analysis in Hadron Spectroscopy at the ECT*-Trento in 2011, the School on Amplitude Analysis in Modern Physics in Bad Honnef in 2011, the Jefferson Lab Advanced Study Institute Summer School in 2012, and the School on Concepts of Modern Amplitude Analysis Techniques in Flecken-Zechlin near Berlin in September 2013. The aim of this document is to summarize the discussions that took place at the ATHOS 2012 and ATHOS 2013 meetings. We do not attempt a comprehensive review of the field of amplitude analysis, but offer a collection of thoughts that we hope may lay the ground for such a document

Frequency-agile THz-wave generation and detection system using nonlinear frequency conversion at room temperature.

Science.gov (United States)

Guo, Ruixiang; Ikar'i, Tomofumi; Zhang, Jun; Minamide, Hiroaki; Ito, Hiromasa

2010-08-02

A surface-emitting THz parametric oscillator is set up to generate a narrow-linewidth, nanosecond pulsed THz-wave radiation. The THz-wave radiation is coherently detected using the frequency up-conversion in MgO: LiNbO(3) crystal. Fast frequency tuning and automatic achromatic THz-wave detection are achieved through a special optical design, including a variable-angle mirror and 1:1 telescope devices in the pump and THz-wave beams. We demonstrate a frequency-agile THz-wave parametric generation and THz-wave coherent detection system. This system can be used as a frequency-domain THz-wave spectrometer operated at room-temperature, and there are a high possible to develop into a real-time two-dimensional THz spectral imaging system.

Uniqueness: skews bit occurrence frequencies in randomly generated fingerprint libraries.

Science.gov (United States)

Chen, Nelson G

2016-08-01

Requiring that randomly generated chemical fingerprint libraries have unique fingerprints such that no two fingerprints are identical causes a systematic skew in bit occurrence frequencies, the proportion at which specified bits are set. Observed frequencies (O) at which each bit is set within the resulting libraries systematically differ from frequencies at which bits are set at fingerprint generation (E). Observed frequencies systematically skew toward 0.5, with the effect being more pronounced as library size approaches the compound space, which is the total number of unique possible fingerprints given the number of bit positions each fingerprint contains. The effect is quantified for varying library sizes as a fraction of the overall compound space, and for changes in the specified frequency E. The cause and implications for this systematic skew are subsequently discussed. When generating random libraries of chemical fingerprints, the imposition of a uniqueness requirement should either be avoided or taken into account.

Versatile silicon-waveguide supercontinuum for coherent mid-infrared spectroscopy

Science.gov (United States)

Nader, Nima; Maser, Daniel L.; Cruz, Flavio C.; Kowligy, Abijith; Timmers, Henry; Chiles, Jeff; Fredrick, Connor; Westly, Daron A.; Nam, Sae Woo; Mirin, Richard P.; Shainline, Jeffrey M.; Diddams, Scott

2018-03-01

Laser frequency combs, with their unique combination of precisely defined spectral lines and broad bandwidth, are a powerful tool for basic and applied spectroscopy. Here, we report offset-free, mid-infrared frequency combs and dual-comb spectroscopy through supercontinuum generation in silicon-on-sapphire waveguides. We leverage robust fabrication and geometrical dispersion engineering of nanophotonic waveguides for multi-band, coherent frequency combs spanning 70 THz in the mid-infrared (2.5 μm-6.2 μm). Precise waveguide fabrication provides significant spectral broadening with engineered spectra targeted at specific mid-infrared bands. We characterize the relative-intensity-noise of different bands and show that the measured levels do not pose any limitation for spectroscopy applications. Additionally, we use the fabricated photonic devices to demonstrate dual-comb spectroscopy of a carbonyl sulfide gas sample at 5 μm. This work forms the technological basis for applications such as point sensors for fundamental spectroscopy, atmospheric chemistry, trace and hazardous gas detection, and biological microscopy.

Versatile silicon-waveguide supercontinuum for coherent mid-infrared spectroscopy

Directory of Open Access Journals (Sweden)

Nima Nader

2018-03-01

Full Text Available Laser frequency combs, with their unique combination of precisely defined spectral lines and broad bandwidth, are a powerful tool for basic and applied spectroscopy. Here, we report offset-free, mid-infrared frequency combs and dual-comb spectroscopy through supercontinuum generation in silicon-on-sapphire waveguides. We leverage robust fabrication and geometrical dispersion engineering of nanophotonic waveguides for multi-band, coherent frequency combs spanning 70 THz in the mid-infrared (2.5 μm–6.2 μm. Precise waveguide fabrication provides significant spectral broadening with engineered spectra targeted at specific mid-infrared bands. We characterize the relative-intensity-noise of different bands and show that the measured levels do not pose any limitation for spectroscopy applications. Additionally, we use the fabricated photonic devices to demonstrate dual-comb spectroscopy of a carbonyl sulfide gas sample at 5 μm. This work forms the technological basis for applications such as point sensors for fundamental spectroscopy, atmospheric chemistry, trace and hazardous gas detection, and biological microscopy.

Frequency deviations and generation scheduling in the nordic system

DEFF Research Database (Denmark)

Li, Zhongwei; Samuelsson, Olaf; Garcia-Valle, Rodrigo

2011-01-01

to be considered, the disturbances caused to this control by the hourly dispatch of generation has received less attention and is the focus of this paper. Based on years of recorded PMU data, statistics of frequency events and analysis of frequency quality are made to demonstrate the relation between the frequency...

Non-invasive vibrational SFG spectroscopy reveals that bacterial adhesion can alter the conformation of grafted "brush" chains on SAM.

Science.gov (United States)

Bulard, Emilie; Guo, Ziang; Zheng, Wanquan; Dubost, Henri; Fontaine-Aupart, Marie-Pierre; Bellon-Fontaine, Marie-Noëlle; Herry, Jean-Marie; Briandet, Romain; Bourguignon, Bernard

2011-04-19

Understanding bacterial adhesion on a surface is a crucial step to design new materials with improved properties or to control biofilm formation and eradication. Sum Frequency Generation (SFG) vibrational spectroscopy has been employed to study in situ the conformational response of a self-assembled monolayer (SAM) of octadecanethiol (ODT) on a gold film to the adhesion of hydrophilic and hydrophobic ovococcoid model bacteria. The present work highlights vibrational SFG spectroscopy as a powerful and unique non-invasive biophysical technique to probe and control bacteria interaction with ordered surfaces. Indeed, the SFG vibrational spectral changes reveal different ODT SAM conformations in air and upon exposure to aqueous solution or bacterial adhesion. Furthermore, this effect depends on the bacterial cell surface properties. The SFG spectral modeling demonstrates that hydrophobic bacteria flatten the ODT SAM alkyl chain terminal part, whereas the hydrophilic ones raise this ODT SAM terminal part. Microorganism-induced alteration of grafted chains can thus affect the desired interfacial functionality, a result that should be considered for the design of new reactive materials. © 2011 American Chemical Society

Dual-etalon, cavity-ring-down, frequency comb spectroscopy.

Energy Technology Data Exchange (ETDEWEB)

Strecker, Kevin E.; Chandler, David W.

2010-10-01

The 'dual etalon frequency comb spectrometer' is a novel low cost spectometer with limited moving parts. A broad band light source (pulsed laser, LED, lamp ...) is split into two beam paths. One travels through an etalon and a sample gas, while the second arm is just an etalon cavity, and the two beams are recombined onto a single detector. If the free spectral ranges (FSR) of the two cavities are not identical, the intensity pattern at the detector with consist of a series of heterodyne frequencies. Each mode out of the sample arm etalon with have a unique frequency in RF (radio-frequency) range, where modern electronics can easily record the signals. By monitoring these RF beat frequencies we can then determine when an optical frequencies is absorbed. The resolution is set by the FSR of the cavity, typically 10 MHz, with a bandwidth up to 100s of cm{sup -1}. In this report, the new spectrometer is described in detail and demonstration experiments on Iodine absorption are carried out. Further we discuss powerful potential next generation steps to developing this into a point sensor for monitoring combustion by-products, environmental pollutants, and warfare agents.

Frequency Correction for MIRO Chirp Transformation Spectroscopy Spectrum

Science.gov (United States)

Lee, Seungwon

2012-01-01

This software processes the flyby spectra of the Chirp Transform Spectrometer (CTS) of the Microwave Instrument for Rosetta Orbiter (MIRO). The tool corrects the effect of Doppler shift and local-oscillator (LO) frequency shift during the flyby mode of MIRO operations. The frequency correction for CTS flyby spectra is performed and is integrated with multiple spectra into a high signal-to-noise averaged spectrum at the rest-frame RF frequency. This innovation also generates the 8 molecular line spectra by dividing continuous 4,096-channel CTS spectra. The 8 line spectra can then be readily used for scientific investigations. A spectral line that is at its rest frequency in the frame of the Earth or an asteroid will be observed with a time-varying Doppler shift as seen by MIRO. The frequency shift is toward the higher RF frequencies on approach, and toward lower RF frequencies on departure. The magnitude of the shift depends on the flyby velocity. The result of time-varying Doppler shift is that of an observed spectral line will be seen to move from channel to channel in the CTS spectrometer. The direction (higher or lower frequency) in the spectrometer depends on the spectral line frequency under consideration. In order to analyze the flyby spectra, two steps are required. First, individual spectra must be corrected for the Doppler shift so that individual spectra can be superimposed at the same rest frequency for integration purposes. Second, a correction needs to be applied to the CTS spectra to account for the LO frequency shifts that are applied to asteroid mode.

An amplitude modulated radio frequency plasma generator

Science.gov (United States)

Lei, Fan; Li, Xiaoping; Liu, Yanming; Liu, Donglin; Yang, Min; Xie, Kai; Yao, Bo

2017-04-01

A glow discharge plasma generator and diagnostic system has been developed to study the effects of rapidly variable plasmas on electromagnetic wave propagation, mimicking the plasma sheath conditions encountered in space vehicle reentry. The plasma chamber is 400 mm in diameter and 240 mm in length, with a 300-mm-diameter unobstructed clear aperture. Electron densities produced are in the mid 1010 electrons/cm3. An 800 W radio frequency (RF) generator is capacitively coupled through an RF matcher to an internally cooled stainless steel electrode to form the plasma. The RF power is amplitude modulated by a waveform generator that operates at different frequencies. The resulting plasma contains electron density modulations caused by the varying power levels. A 10 GHz microwave horn antenna pair situated on opposite sides of the chamber serves as the source and detector of probe radiation. The microwave power feed to the source horn is split and one portion is sent directly to a high-speed recording oscilloscope. On mixing this with the signal from the pickup horn antenna, the plasma-induced phase shift between the two signals gives the path-integrated electron density with its complete time dependent variation. Care is taken to avoid microwave reflections and extensive shielding is in place to minimize electronic pickup. Data clearly show the low frequency modulation of the electron density as well as higher harmonics and plasma fluctuations.

Sum rates of asynchronous GFDMA and SC-FDMA for 5G uplink

Directory of Open Access Journals (Sweden)

Woojin Park

2015-12-01

Full Text Available The fifth generation (5G of mobile communication envisions ultralow latency less than 1 ms for radio interface. To this end, frameless asynchronous multiple access may be needed to allow users to transmit instantly without waiting for the next frame start. In this paper, generalized frequency division multiple-access (GFDMA, one of the promising multiple-access candidates for 5G mobile, is compared with the conventional single-carrier FDMA (SC-FDMA in terms of the uplink sum rate when both techniques are adapted for the asynchronous scenario. In particular, a waveform windowing technique is applied to both schemes to mitigate the inter-user interference due to non-zero out-of-band emission.

Pairs of dual Gabor frame generators with compact support and desired frequency localization

DEFF Research Database (Denmark)

Christensen, Ole

2006-01-01

Let g ∈ L2(R) be a compactly supported function, whose integer-translates {T(k)g}(k ∈ Z) form a partition of unity. We prove that for certain translation and modulation parameters, such a function g generates a Gabor frame, with a (noncanonical) dual generated by a finite linear combination h of ...... tilde (k) DTkBN, where both sums are finite. It is known that for N > 1, such functions cannot generate dual wavelet frames {D(j)T(k)g} (j.k∈ Z). {D(j)T(k)h} (j.k ∈ Z). (C) 2005 Elsevier Inc. All rights reserved....

Electronuclear sum rules

International Nuclear Information System (INIS)

Arenhoevel, H.; Drechsel, D.; Weber, H.J.

1978-01-01

Generalized sum rules are derived by integrating the electromagnetic structure functions along lines of constant ratio of momentum and energy transfer. For non-relativistic systems these sum rules are related to the conventional photonuclear sum rules by a scaling transformation. The generalized sum rules are connected with the absorptive part of the forward scattering amplitude of virtual photons. The analytic structure of the scattering amplitudes and the possible existence of dispersion relations have been investigated in schematic relativistic and non-relativistic models. While for the non-relativistic case analyticity does not hold, the relativistic scattering amplitude is analytical for time-like (but not for space-like) photons and relations similar to the Gell-Mann-Goldberger-Thirring sum rule exist. (Auth.)

Bulk stress auto-correlation function in simple liquids-sum rules

International Nuclear Information System (INIS)

Tankeshwar, K.; Bhandari, R.; Pathak, K.N.

1990-10-01

Expressions for the zeroth, second and fourth frequency sum rules of the bulk stress auto correlation function have been derived. The exact expressions involve static correlation function up to four particles. Because of the non availability of any information about static quadruplet correlation function we use a low order decoupling approximation for this. In this work, we have obtained, separately, the sum rules for the different mechanism of momentum transfer in the fluids. The results are expected to be useful in the study of bulk viscosity of the fluids. (author). 9 refs

Sum rules for four-spinon dynamic structure factor in XXX model

International Nuclear Information System (INIS)

Si Lakhal, B.; Abada, A.

2005-01-01

In the context of the antiferromagnetic spin 12 Heisenberg quantum spin chain (XXX model), we estimate the contribution of the exact four-spinon dynamic structure factor S 4 by calculating a number of sum rules the total dynamic structure factor S is known to satisfy exactly. These sum rules are: the static susceptibility, the integrated intensity, the total integrated intensity, the first frequency moment and the nearest-neighbor correlation function. We find that the contribution of S 4 is between 1% and 2.5%, depending on the sum rule, whereas the contribution of the exact two-spinon dynamic structure factor S 2 is between 70% and 75%. The calculations are numerical and Monte Carlo based. Good statistics are obtained

Practical system for the generation of pulsed quantum frequency combs.

Science.gov (United States)

Roztocki, Piotr; Kues, Michael; Reimer, Christian; Wetzel, Benjamin; Sciara, Stefania; Zhang, Yanbing; Cino, Alfonso; Little, Brent E; Chu, Sai T; Moss, David J; Morandotti, Roberto

2017-08-07

The on-chip generation of large and complex optical quantum states will enable low-cost and accessible advances for quantum technologies, such as secure communications and quantum computation. Integrated frequency combs are on-chip light sources with a broad spectrum of evenly-spaced frequency modes, commonly generated by four-wave mixing in optically-excited nonlinear micro-cavities, whose recent use for quantum state generation has provided a solution for scalable and multi-mode quantum light sources. Pulsed quantum frequency combs are of particular interest, since they allow the generation of single-frequency-mode photons, required for scaling state complexity towards, e.g., multi-photon states, and for quantum information applications. However, generation schemes for such pulsed combs have, to date, relied on micro-cavity excitation via lasers external to the sources, being neither versatile nor power-efficient, and impractical for scalable realizations of quantum technologies. Here, we introduce an actively-modulated, nested-cavity configuration that exploits the resonance pass-band characteristic of the micro-cavity to enable a mode-locked and energy-efficient excitation. We demonstrate that the scheme allows the generation of high-purity photons at large coincidence-to-accidental ratios (CAR). Furthermore, by increasing the repetition rate of the excitation field via harmonic mode-locking (i.e. driving the cavity modulation at harmonics of the fundamental repetition rate), we managed to increase the pair production rates (i.e. source efficiency), while maintaining a high CAR and photon purity. Our approach represents a significant step towards the realization of fully on-chip, stable, and versatile sources of pulsed quantum frequency combs, crucial for the development of accessible quantum technologies.

In situ monitoring of cocrystals in formulation development using low-frequency Raman spectroscopy.

Science.gov (United States)

Otaki, Takashi; Tanabe, Yuta; Kojima, Takashi; Miura, Masaru; Ikeda, Yukihiro; Koide, Tatsuo; Fukami, Toshiro

2018-05-05

In recent years, to guarantee a quality-by-design approach to the development of pharmaceutical products, it is important to identify properties of raw materials and excipients in order to determine critical process parameters and critical quality attributes. Feedback obtained from real-time analyses using various process analytical technology (PAT) tools has been actively investigated. In this study, in situ monitoring using low-frequency (LF) Raman spectroscopy (10-200 cm -1 ), which may have higher discriminative ability among polymorphs than near-infrared spectroscopy and conventional Raman spectroscopy (200-1800 cm -1 ), was investigated as a possible application to PAT. This is because LF-Raman spectroscopy obtains information about intermolecular and/or lattice vibrations in the solid state. The monitoring results obtained from Furosemide/Nicotinamide cocrystal indicate that LF-Raman spectroscopy is applicable to in situ monitoring of suspension and fluidized bed granulation processes, and is an effective technique as a PAT tool to detect the conversion risk of cocrystals. LF-Raman spectroscopy is also used as a PAT tool to monitor reactions, crystallizations, and manufacturing processes of drug substances and products. In addition, a sequence of conversion behaviors of Furosemide/Nicotinamide cocrystals was determined by performing in situ monitoring for the first time. Copyright © 2018 Elsevier B.V. All rights reserved.

Generation of Electricity at Graphene Interface Governed by Underlying Surface Dipole Induced Ion Adsorption

Science.gov (United States)

Yang, Shanshan; Su, Yudan; Wu, Qiong; Zhang, Yuanbo; Tian, Chuanshan

Aqueous droplet moving along graphene surface can produce electricity This interesting phenomenon provided environment-friendly means to harvest energy from graphene interface in contact with sea wave or rain droplets. However, microscopically, the nature of charge adsorption at the graphene interface is still unclear. Here, utilizing sum-frequency spectroscopy in combined with measurement of electrical power generation, the origin of charge adsorption on graphene was investigated. It was found that the direct ion-graphene interaction is negligibly small, contrary to the early speculation, but the ordered surface dipole from the supporting substrate, such as PET, is responsible for ion adsorption at the interface. Graphene serves as a conductive layer with mild screening of Coulomb interaction when aqueous droplet slips over the surface. These results pave the way for optimization of energy harvesting efficiency of graphene-based device.

Sum Rules, Classical and Quantum - A Pedagogical Approach

Science.gov (United States)

Karstens, William; Smith, David Y.

2014-03-01

Sum rules in the form of integrals over the response of a system to an external probe provide general analytical tools for both experiment and theory. For example, the celebrated f-sum rule gives a system's plasma frequency as an integral over the optical-dipole absorption spectrum regardless of the specific spectral distribution. Moreover, this rule underlies Smakula's equation for the number density of absorbers in a sample in terms of the area under their absorption bands. Commonly such rules are derived from quantum-mechanical commutation relations, but many are fundamentally classical (independent of ℏ) and so can be derived from more transparent mechanical models. We have exploited this to illustrate the fundamental role of inertia in the case of optical sum rules. Similar considerations apply to sum rules in many other branches of physics. Thus, the ``attenuation integral theorems'' of ac circuit theory reflect the ``inertial'' effect of Lenz's Law in inductors or the potential energy ``storage'' in capacitors. These considerations are closely related to the fact that the real and imaginary parts of a response function cannot be specified independently, a result that is encapsulated in the Kramers-Kronig relations. Supported in part by the US Department of Energy, Office of Nuclear Physics under contract DE-AC02-06CH11357.

Composite Finite Sums

KAUST Repository

Alabdulmohsin, Ibrahim M.

2018-03-07

In this chapter, we extend the previous results of Chap. 2 to the more general case of composite finite sums. We describe what composite finite sums are and how their analysis can be reduced to the analysis of simple finite sums using the chain rule. We apply these techniques, next, on numerical integration and on some identities of Ramanujan.

Composite Finite Sums

KAUST Repository

Alabdulmohsin, Ibrahim M.

2018-01-01

In this chapter, we extend the previous results of Chap. 2 to the more general case of composite finite sums. We describe what composite finite sums are and how their analysis can be reduced to the analysis of simple finite sums using the chain rule. We apply these techniques, next, on numerical integration and on some identities of Ramanujan.

Dual-comb coherent Raman spectroscopy with lasers of 1-GHz pulse repetition frequency.

Science.gov (United States)

Mohler, Kathrin J; Bohn, Bernhard J; Yan, Ming; Mélen, Gwénaëlle; Hänsch, Theodor W; Picqué, Nathalie

2017-01-15

We extend the technique of multiplex coherent Raman spectroscopy with two femtosecond mode-locked lasers to oscillators of a pulse repetition frequency of 1 GHz. We demonstrate a spectra of liquids, which span 1100  cm-1 of Raman shifts. At a resolution of 6  cm-1, their measurement time may be as short as 5 μs for a refresh rate of 2 kHz. The waiting period between acquisitions is improved 10-fold compared to previous experiments with two lasers of 100-MHz repetition frequencies.

CW light sources at the 589 nm sodium D2 line by sum-frequency mixing of diode pumped neodymium lasers

International Nuclear Information System (INIS)

Lü, Y F; Lu, J; Xu, L J; Sun, G C; Zhao, Z M; Gao, X; Lin, J Q

2010-01-01

We present a laser architecture to obtain continuous-wave (CW) light sources at the 589 nm sodium D2 line. A 808 nm diode-pumped a Nd:YLiF 4 (Nd:YLF) crystal emitting at 1053 nm. A part of the pump power was then absorbed by the Nd:YLF crystal. The remaining was used to pump a Nd:YAG crystal emitting at 1338 nm. Intracavity sum-frequency mixing at 1053 and 1338 nm was then realized in a LiB 3 O 5 (LBO) crystal to reach the yellow-orange radiation. We obtained a CW output power of 235 mW at 589 nm with a pump laser diode emitting 17.8 W at 808 nm

Rapid and economical data acquisition in ultrafast frequency-resolved spectroscopy using choppers and a microcontroller.

Science.gov (United States)

Guo, Liang; Monahan, Daniele M; Fleming, Graham

2016-08-08

Spectrometers and cameras are used in ultrafast spectroscopy to achieve high resolution in both time and frequency domains. Frequency-resolved signals from the camera pixels cannot be processed by common lock-in amplifiers, which have only a limited number of input channels. Here we demonstrate a rapid and economical method that achieves the function of a lock-in amplifier using mechanical choppers and a programmable microcontroller. We demonstrate the method's effectiveness by performing a frequency-resolved pump-probe measurement on the dye Nile Blue in solution.

High-Power, Solid-State, Deep Ultraviolet Laser Generation

Directory of Open Access Journals (Sweden)

Hongwen Xuan

2018-02-01

Full Text Available At present, deep ultraviolet (DUV lasers at the wavelength of fourth harmonics of 1 μm (266 nm/258 nm and at the wavelength of 193 nm are widely utilized in science and industry. We review the generation of these DUV lasers by nonlinear frequency conversion processes using solid-state/fiber lasers as the fundamental frequency. A DUV laser at 258 nm by fourth harmonics generation (FHG could achieve an average power of 10 W with a beam quality of M2 < 1.5. Moreover, 1 W of average power at 193 nm was obtained by sum-frequency generation (SFG. A new concept of 193-nm DUV laser generation by use of the diamond Raman laser is also introduced. A proof-of-principle experiment of the diamond Raman laser is reported with the conversion efficiency of 23% from the pump to the second Stokes wavelength, which implies the potential to generate a higher power 193 nm DUV laser in the future.

The frequency-independent control method for distributed generation systems

DEFF Research Database (Denmark)

Naderi, Siamak; Pouresmaeil, Edris; Gao, Wenzhong David

2012-01-01

In this paper a novel frequency-independent control method suitable for distributed generation (DG) is presented. This strategy is derived based on the . abc/. αβ transformation and . abc/. dq transformation of the ac system variables. The active and reactive currents injected by the DG are contr......In this paper a novel frequency-independent control method suitable for distributed generation (DG) is presented. This strategy is derived based on the . abc/. αβ transformation and . abc/. dq transformation of the ac system variables. The active and reactive currents injected by the DG...

Stable optical frequency comb generation and applications in arbitrary waveform generation, signal processing and optical data mining

Science.gov (United States)

Ozharar, Sarper

This thesis focuses on the generation and applications of stable optical frequency combs. Optical frequency combs are defined as equally spaced optical frequencies with a fixed phase relation among themselves. The conventional source of optical frequency combs is the optical spectrum of the modelocked lasers. In this work, we investigated alternative methods for optical comb generation, such as dual sine wave phase modulation, which is more practical and cost effective compared to modelocked lasers stabilized to a reference. Incorporating these comblines, we have generated tunable RF tones using the serrodyne technique. The tuning range was +/-1 MHz, limited by the electronic waveform generator, and the RF carrier frequency is limited by the bandwidth of the photodetector. Similarly, using parabolic phase modulation together with time division multiplexing, RF chirp extension has been realized. Another application of the optical frequency combs studied in this thesis is real time data mining in a bit stream. A novel optoelectronic logic gate has been developed for this application and used to detect an 8 bit long target pattern. Also another approach based on orthogonal Hadamard codes have been proposed and explained in detail. Also novel intracavity modulation schemes have been investigated and applied for various applications such as (a) improving rational harmonic modelocking for repetition rate multiplication and pulse to pulse amplitude equalization, (b) frequency skewed pulse generation for ranging and (c) intracavity active phase modulation in amplitude modulated modelocked lasers for supermode noise spur suppression and integrated jitter reduction. The thesis concludes with comments on the future work and next steps to improve some of the results presented in this work.

A fast summation method for oscillatory lattice sums

Science.gov (United States)

Denlinger, Ryan; Gimbutas, Zydrunas; Greengard, Leslie; Rokhlin, Vladimir

2017-02-01

We present a fast summation method for lattice sums of the type which arise when solving wave scattering problems with periodic boundary conditions. While there are a variety of effective algorithms in the literature for such calculations, the approach presented here is new and leads to a rigorous analysis of Wood's anomalies. These arise when illuminating a grating at specific combinations of the angle of incidence and the frequency of the wave, for which the lattice sums diverge. They were discovered by Wood in 1902 as singularities in the spectral response. The primary tools in our approach are the Euler-Maclaurin formula and a steepest descent argument. The resulting algorithm has super-algebraic convergence and requires only milliseconds of CPU time.

Generation of Mid-Infrared Frequency Combs for Spectroscopic Applications

Science.gov (United States)

Maser, Daniel L.

Mid-infrared laser sources prove to be a valuable tool in exploring a vast array of phenomena, finding their way into applications ranging from trace gas detection to X-ray generation and carbon dating. Mid-infrared frequency combs, in particular, are well-suited for many of these applications, owing to their inherent low-noise and broadband nature. Frequency comb technology is well-developed in the near-infrared as a result of immense technological development by the telecommunication industry in silica fiber and the existence of readily-available glass dopants such as ytterbium and erbium that enable oscillators at 1 and 1.5 ?m. However, options become substantially more limited at longer wavelengths, as silica is no longer transparent and the components required in a mid-infrared frequency comb system (oscillators, fibers, and both fiber and free-space components) are far less technologically mature. This thesis explores several different approaches to generating frequency comb sources in the mid-infrared region, and the development of sources used in the nonlinear processes implemented to reach these wavelengths. An optical parametric oscillator, two approaches to difference frequency generation, and nonlinear spectral broadening in chip-scale waveguides are developed, characterized, and spectroscopic potential for these techniques is demonstrated. The source used for these nonlinear processes, the erbium-doped fiber amplifier, is also studied and discussed throughout the design and optimization process. The nonlinear optical processes critical to this work are numerically modeled and used to confirm and predict experimental behavior.

Simple Finite Sums

KAUST Repository

Alabdulmohsin, Ibrahim M.

2018-01-01

We will begin our treatment of summability calculus by analyzing what will be referred to, throughout this book, as simple finite sums. Even though the results of this chapter are particular cases of the more general results presented in later chapters, they are important to start with for a few reasons. First, this chapter serves as an excellent introduction to what summability calculus can markedly accomplish. Second, simple finite sums are encountered more often and, hence, they deserve special treatment. Third, the results presented in this chapter for simple finite sums will, themselves, be used as building blocks for deriving the most general results in subsequent chapters. Among others, we establish that fractional finite sums are well-defined mathematical objects and show how various identities related to the Euler constant as well as the Riemann zeta function can actually be derived in an elementary manner using fractional finite sums.

Simple Finite Sums

KAUST Repository

Alabdulmohsin, Ibrahim M.

2018-03-07

We will begin our treatment of summability calculus by analyzing what will be referred to, throughout this book, as simple finite sums. Even though the results of this chapter are particular cases of the more general results presented in later chapters, they are important to start with for a few reasons. First, this chapter serves as an excellent introduction to what summability calculus can markedly accomplish. Second, simple finite sums are encountered more often and, hence, they deserve special treatment. Third, the results presented in this chapter for simple finite sums will, themselves, be used as building blocks for deriving the most general results in subsequent chapters. Among others, we establish that fractional finite sums are well-defined mathematical objects and show how various identities related to the Euler constant as well as the Riemann zeta function can actually be derived in an elementary manner using fractional finite sums.

System and Method for Generating a Frequency Modulated Linear Laser Waveform

Science.gov (United States)

Pierrottet, Diego F. (Inventor); Petway, Larry B. (Inventor); Amzajerdian, Farzin (Inventor); Barnes, Bruce W. (Inventor); Lockard, George E. (Inventor); Hines, Glenn D. (Inventor)

2017-01-01

A system for generating a frequency modulated linear laser waveform includes a single frequency laser generator to produce a laser output signal. An electro-optical modulator modulates the frequency of the laser output signal to define a linear triangular waveform. An optical circulator passes the linear triangular waveform to a band-pass optical filter to filter out harmonic frequencies created in the waveform during modulation of the laser output signal, to define a pure filtered modulated waveform having a very narrow bandwidth. The optical circulator receives the pure filtered modulated laser waveform and transmits the modulated laser waveform to a target.

IL 6: 2D-IR spectroscopy: chemistry and biophysics in real time

International Nuclear Information System (INIS)

Bredenbeck, Jens

2010-01-01

Pulsed multidimensional experiments, daily business in the field of NMR spectroscopy, have been demonstrated only relatively recently in IR spectroscopy. Similar as nuclear spins in multidimensional NMR, molecular vibrations are employed in multidimensional IR experiments as probes of molecular structure and dynamics, albeit with femtosecond time resolution. Different types of multidimensional IR experiments have been implemented, resembling basic NMR experiments such as NOESY, COSY and EXSY. In contrast to one-dimensional linear spectroscopy, such multidimensional experiments reveal couplings and correlations of vibrations, which are closely linked to molecular structure and its change in time. The use of mixed IR/VIS pulse sequences further extends the potential of multidimensional IR spectroscopy, enabling studies of ultrafast non-equilibrium processes as well as surface specific, highly sensitive experiments. A UV/VIS pulse preceding the IR pulse sequence can be used to prepare the system under study in a non-equilibrium state. 2D-IR snapshots of the evolving non-equilibrium system are then taken, for example during a photochemical reaction or during the photo-cycle of a light sensitive protein. Preparing the system in a non-equilibrium state by UV/Vis excitation during the IR pulse sequence allows for correlating states of reactant and product of the light triggered process via their 2D-IR cross peaks - a technique that has been used to map the connectivity between different binding sites of a ligand as it migrates through a protein. Introduction of a non-resonant VIS pulse at the end of the IR part of the experiment allows to selectively up-convert the infrared signal of interfacial molecules to the visible spectral range by sum frequency generation. In this way, femtosecond interfacial 2D-IR spectroscopy can be implemented, achieving sub-monolayer sensitivity. (author)

Laser generated ultrasound sources using polymer nanocomposites for high frequency metrology

KAUST Repository

Rajagopal, Srinath

2017-11-22

Accurate characterization of ultrasound fields generated by diagnostic and therapeutic transducers is critical for patient safety. This requires hydrophones calibrated to a traceable standard and currently the upper calibration frequency range available to the user community is limited to a frequency of 40 MHz. However, the increasing use of high frequencies for both imaging and therapy necessitates calibrations to frequencies well beyond this range. For this to be possible, a source of high amplitude, broadband, quasi-planar and stable ultrasound fields is required. This is difficult to achieve using conventional piezoelectric sources, but laser generated ultrasound is a promising technique in this regard. In this study, various polymer-carbon nanotube nanocomposites (PNC) were fabricated and tested for their suitability for such an application by varying the polymer type, carbon nanotubes weight content in the polymer, and PNC thickness. A broadband hydrophone was used to measure the peak pressure and bandwidth of the laser generated ultrasound pulse. Peak-positive pressures of up to 8 MPa and −6dB bandwidths of up to 40 MHz were recorded. There is a nonlinear dependence of the peak pressure on the laser fluence and the bandwidth scales inversely proportionally to the peak pressure. The high-pressure plane waves generated from this preliminary investigation has demonstrated that laser generated ultrasound sources are a promising technique for high frequency calibration of hydrophones.

Computation of magnetic circular dichroism by sum-over-states summations

Czech Academy of Sciences Publication Activity Database

Štěpánek, Petr; Bouř, Petr

2013-01-01

Roč. 34, č. 18 (2013), s. 1531-1539 ISSN 0192-8651 R&D Projects: GA ČR GAP208/11/0105; GA MŠk(CZ) LH11033; GA ČR GA13-03978S Grant - others:AV ČR(CZ) M200551205 Institutional support: RVO:61388963 Keywords : time-dependent * density functional theory * sum over states * spectroscopy * magnetic circular dichroism * origin dependence Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.601, year: 2013

Wind Generation Participation in Power System Frequency Response: Preprint

Energy Technology Data Exchange (ETDEWEB)

Gevorgian, Vahan; Zhang, Yingchen

2017-01-01

The electrical frequency of an interconnected power system must be maintained close its nominal level at all times. Excessive under- and overfrequency excursions can lead to load shedding, instability, machine damage, and even blackouts. There is a rising concern in the electric power industry in recent years about the declining amount of inertia and primary frequency response (PFR) in many interconnections. This decline may continue due to increasing penetrations of inverter-coupled generation and the planned retirements of conventional thermal plants. Inverter-coupled variable wind generation is capable of contributing to PFR and inertia with a response that is different from that of conventional generation. It is not yet entirely understood how such a response will affect the system at different wind power penetration levels. The modeling work presented in this paper evaluates the impact of wind generation's provision of these active power control strategies on a large, synchronous interconnection. All simulations were conducted on the U.S. Western Interconnection with different levels of instantaneous wind power penetrations (up to 80%). The ability of wind power plants to provide PFR - and a combination of synthetic inertial response and PFR - significantly improved the frequency response performance of the system.

Novel Cavities in Vertical External Cavity Surface Emitting Lasers for Emission in Broad Spectral Region by Means of Nonlinear Frequency Conversion

Science.gov (United States)

Lukowski, Michal L.

Optically pumped semiconductor vertical external cavity surface emitting lasers (VECSEL) were first demonstrated in the mid 1990's. Due to the unique design properties of extended cavity lasers VECSELs have been able to provide tunable, high-output powers while maintaining excellent beam quality. These features offer a wide range of possible applications in areas such as medicine, spectroscopy, defense, imaging, communications and entertainment. Nowadays, newly developed VECSELs, cover the spectral regions from red (600 nm) to around 5 microm. By taking the advantage of the open cavity design, the emission can be further expanded to UV or THz regions by the means of intracavity nonlinear frequency generation. The objective of this dissertation is to investigate and extend the capabilities of high-power VECSELs by utilizing novel nonlinear conversion techniques. Optically pumped VECSELs based on GaAs semiconductor heterostructures have been demonstrated to provide exceptionally high output powers covering the 900 to 1200 nm spectral region with diffraction limited beam quality. The free space cavity design allows for access to the high intracavity circulating powers where high efficiency nonlinear frequency conversions and wavelength tuning can be obtained. As an introduction, this dissertation consists of a brief history of the development of VECSELs as well as wafer design, chip fabrication and resonator cavity design for optimal frequency conversion. Specifically, the different types of laser cavities such as: linear cavity, V-shaped cavity and patented T-shaped cavity are described, since their optimization is crucial for transverse mode quality, stability, tunability and efficient frequency conversion. All types of nonlinear conversions such as second harmonic, sum frequency and difference frequency generation are discussed in extensive detail. The theoretical simulation and the development of the high-power, tunable blue and green VECSEL by the means of type I

Expansion around half-integer values, binomial sums, and inverse binomial sums

International Nuclear Information System (INIS)

Weinzierl, Stefan

2004-01-01

I consider the expansion of transcendental functions in a small parameter around rational numbers. This includes in particular the expansion around half-integer values. I present algorithms which are suitable for an implementation within a symbolic computer algebra system. The method is an extension of the technique of nested sums. The algorithms allow in addition the evaluation of binomial sums, inverse binomial sums and generalizations thereof

Current state and development trends of inspections of steam generator tubes by eddy currents method

International Nuclear Information System (INIS)

Kubis, S.; Herman, M.

1988-01-01

The requirements are presented for steam generator tube testing and the factors are discussed affecting the accuracy of measurement by the eddy currents method. The individual types of the eddy currents method are described, such as the single-frequency method, the multi-frequency method and the pulse eddy currents method. The demands are summed up on manipulator systems whose design is adapted to the steam generator configuration conditions. (E.S.). 5 figs., 16 possu

Chemische Reaktionen auf Oberflächen - eine SFG Studie

OpenAIRE

Kirsch, Harald

2014-01-01

This thesis focused on the investigation of chemical reactions on surfaces by usage of Sum Frequency Generation (SFG) spectroscopy and Thermal Desorption Spectroscopy (TDS). Understanding of chemical reactions on surfaces is of critical importance for modification and optimization of a variety of environmental and industrial processes, but the complexity of the ongoing reactions under "realistic" conditions often hinders an understanding on a molecular level. The aim of this work was to get i...

Diode-pumped quasi-three-level Nd:GdV O4–Nd:YAG sum-frequency laser at 464 nm

International Nuclear Information System (INIS)

Lu, Jie

2014-01-01

We report a laser architecture to obtain continuous-wave (cw) blue radiation at 464 nm. A 808 nm diode pumped a Nd:GdV O 4 crystal emitting at 912 nm. A part of the pump power was then absorbed by the Nd:GdV O 4 crystal. The remainder was used to pump a Nd:YAG crystal emitting at 946 nm. Intracavity sum-frequency mixing at 912 and 946 nm was then realized in a LiB 3 O 5 (LBO) crystal to produce blue radiation. We obtained a cw output power of 1.52 W at 464 nm with a pump laser diode emitting 18.4 W at 808 nm. (letter)

Gas spectroscopy with integrated frequency monitoring through self-mixing in a terahertz quantum-cascade laser.

Science.gov (United States)

Chhantyal-Pun, Rabi; Valavanis, Alexander; Keeley, James T; Rubino, Pierluigi; Kundu, Iman; Han, Yingjun; Dean, Paul; Li, Lianhe; Davies, A Giles; Linfield, Edmund H

2018-05-15

We demonstrate a gas spectroscopy technique, using self-mixing in a 3.4 terahertz quantum-cascade laser (QCL). All previous QCL spectroscopy techniques have required additional terahertz instrumentation (detectors, mixers, or spectrometers) for system pre-calibration or spectral analysis. By contrast, our system self-calibrates the laser frequency (i.e., with no external instrumentation) to a precision of 630 MHz (0.02%) by analyzing QCL voltage perturbations in response to optical feedback within a 0-800 mm round-trip delay line. We demonstrate methanol spectroscopy by introducing a gas cell into the feedback path and show that a limiting absorption coefficient of ∼1×10 -4   cm -1 is resolvable.

WEAVE: the next generation wide-field spectroscopy facility for the William Herschel Telescope : The next generation wide-field spectroscopy facility for the William Herschel Telescope

NARCIS (Netherlands)

Dalton, Gavin; Trager, Scott C.; Abrams, Don Carlos; Carter, David; Bonifacio, Piercarlo; Aguerri, J. Alfonso L.; MacIntosh, Mike; Evans, Chris; Lewis, Ian; Navarro, Ramon; Agocs, Tibor; Dee, Kevin; Rousset, Sophie; Tosh, Ian; Middleton, Kevin; Pragt, Johannes; Terrett, David; Brock, Matthew; Benn, Chris; Verheijen, Marc; Cano Infantes, Diego; Bevil, Craige; Steele, Iain; Mottram, Chris; Bates, Stuart; Gribbin, Francis J.; Rey, Jürg; Rodriguez, Luis Fernando; Delgado, Jose Miguel; Guinouard, Isabelle; Walton, Nic; Irwin, Michael J.; Jagourel, Pascal; Stuik, Remko; Gerlofsma, Gerrit; Roelfsma, Ronald; Skillen, Ian; Ridings, Andy; Balcells, Marc; Daban, Jean-Baptiste; Gouvret, Carole; Venema, Lars; Girard, Paul

We present the preliminary design of the WEAVE next generation spectroscopy facility for the William Herschel Telescope (WHT), principally targeting optical ground-based follow up of upcoming ground-based (LOFAR) and spacebased (Gaia) surveys. WEAVE is a multi-object and multi-IFU facility utilizing

A New Sum Analogous to Gauss Sums and Its Fourth Power Mean

Directory of Open Access Journals (Sweden)

Shaofeng Ru

2014-01-01

Full Text Available The main purpose of this paper is to use the analytic methods and the properties of Gauss sums to study the computational problem of one kind of new sum analogous to Gauss sums and give an interesting fourth power mean and a sharp upper bound estimate for it.

Dead-Time Generation in Six-Phase Frequency Inverter

Directory of Open Access Journals (Sweden)

Aurelijus Pitrėnas

2016-06-01

Full Text Available In this paper control of multi-phase induction drives is discussed. Structure of six-phase frequency inverter is examined. The article deals with dead-time generation circuits in six-phase frequency inverter for transistor control signals. Computer models of dead-time circuits is created using LTspice software package. Simulation results are compared with experimental results of the tested dead-time circuits. Parameters obtained in simulation results are close to the parameters obtained in experimental results.

High-Frequency Electron Paramagnetic Resonance Spectroscopy of Nitroxide-Functionalized Nanodiamonds in Aqueous Solution.

Science.gov (United States)

Akiel, R D; Stepanov, V; Takahashi, S

2017-06-01

Nanodiamond (ND) is an attractive class of nanomaterial for fluorescent labeling, magnetic sensing of biological molecules, and targeted drug delivery. Many of those applications require tethering of target biological molecules on the ND surface. Even though many approaches have been developed to attach macromolecules to the ND surface, it remains challenging to characterize dynamics of tethered molecule. Here, we show high-frequency electron paramagnetic resonance (HF EPR) spectroscopy of nitroxide-functionalized NDs. Nitroxide radical is a commonly used spin label to investigate dynamics of biological molecules. In the investigation, we developed a sample holder to overcome water absorption of HF microwave. Then, we demonstrated HF EPR spectroscopy of nitroxide-functionalized NDs in aqueous solution and showed clear spectral distinction of ND and nitroxide EPR signals. Moreover, through EPR spectral analysis, we investigate dynamics of nitroxide radicals on the ND surface. The demonstration sheds light on the use of HF EPR spectroscopy to investigate biological molecule-functionalized nanoparticles.

Broadband Rotational Spectroscopy

Science.gov (United States)

Pate, Brooks

2014-06-01

The past decade has seen several major technology advances in electronics operating at microwave frequencies making it possible to develop a new generation of spectrometers for molecular rotational spectroscopy. High-speed digital electronics, both arbitrary waveform generators and digitizers, continue on a Moore's Law-like development cycle that started around 1993 with device bandwidth doubling about every 36 months. These enabling technologies were the key to designing chirped-pulse Fourier transform microwave (CP-FTMW) spectrometers which offer significant sensitivity enhancements for broadband spectrum acquisition in molecular rotational spectroscopy. A special feature of the chirped-pulse spectrometer design is that it is easily implemented at low frequency (below 8 GHz) where Balle-Flygare type spectrometers with Fabry-Perot cavity designs become technologically challenging due to the mirror size requirements. The capabilities of CP-FTMW spectrometers for studies of molecular structure will be illustrated by the collaborative research effort we have been a part of to determine the structures of water clusters - a project which has identified clusters up to the pentadecamer. A second technology trend that impacts molecular rotational spectroscopy is the development of high power, solid state sources in the mm-wave/THz regions. Results from the field of mm-wave chirped-pulse Fourier transform spectroscopy will be described with an emphasis on new problems in chemical dynamics and analytical chemistry that these methods can tackle. The third (and potentially most important) technological trend is the reduction of microwave components to chip level using monolithic microwave integrated circuits (MMIC) - a technology driven by an enormous mass market in communications. Some recent advances in rotational spectrometer designs that incorporate low-cost components will be highlighted. The challenge to the high-resolution spectroscopy community - as posed by Frank De

Wave functions constructed from an invariant sum over histories satisfy constraints

International Nuclear Information System (INIS)

Halliwell, J.J.; Hartle, J.B.

1991-01-01

Invariance of classical equations of motion under a group parametrized by functions of time implies constraints between canonical coordinates and momenta. In the Dirac formulation of quantum mechanics, invariance is normally imposed by demanding that physical wave functions are annihilated by the operator versions of these constraints. In the sum-over-histories quantum mechanics, however, wave functions are specified, directly, by appropriate functional integrals. It therefore becomes an interesting question whether the wave functions so specified obey the operator constraints of the Dirac theory. In this paper, we show for a wide class of theories, including gauge theories, general relativity, and first-quantized string theories, that wave functions constructed from a sum over histories are, in fact, annihilated by the constraints provided that the sum over histories is constructed in a manner which respects the invariance generated by the constraints. By this we mean a sum over histories defined with an invariant action, invariant measure, and an invariant class of paths summed over

Flattened optical frequency-locked multi-carrier generation by cascading one DML and one phase modulator driven by different RF frequency clocks

International Nuclear Information System (INIS)

Li, Xinying; Yu, Jianjun; Zhang, Junwen; Chi, Nan

2013-01-01

We propose a novel scheme for flattened optical frequency-locked multi-carrier generation based on one directly modulated laser (DML) and one phase modulator (PM) in cascade driven by different sinusoidal radio-frequency (RF) clocks. We experimentally demonstrate that when the clock frequencies for the cascaded DML and the PM are respectively 12.5 GHz and 25 GHz, over 24 optical subcarriers can be generated with 12.5-GHz frequency spacing and amplitude fluctuation less than 3 dB. Furthermore, the number of generated optical subcarriers can be further increased when we increase the driving power for the DML. (letter)

A tunable dual-wavelength pump source based on simulated polariton scattering for terahertz-wave generation

International Nuclear Information System (INIS)

Sun, Bo; Liu, Jinsong; Yao, Jianquan; Li, Enbang

2013-01-01

We propose a dual-wavelength pump source by utilizing stimulated polariton scattering in a LiNbO 3 crystal. The residual pump and the generated tunable Stokes waves can be combined to generate THz-wave generation via difference frequency generation (DFG). With a pump energy of 49 mJ, Stokes waves with a tuning range from 1067.8 to 1074 nm have been generated, and an output energy of up to 14.9 mJ at 1070 nm has been achieved with a conversion efficiency of 21.7%. A sum frequency generation experiment was carried out to demonstrate the feasibility of the proposed scheme for THz-wave DFG. (paper)

Summing threshold logs in a parton shower

International Nuclear Information System (INIS)

Nagy, Zoltan; Soper, Davison E.

2016-05-01

When parton distributions are falling steeply as the momentum fractions of the partons increases, there are effects that occur at each order in α s that combine to affect hard scattering cross sections and need to be summed. We show how to accomplish this in a leading approximation in the context of a parton shower Monte Carlo event generator.

Vacuum ultraviolet light generation applications to resonance ionization spectroscopy

International Nuclear Information System (INIS)

Payne, M.G.

1986-08-01

A theoretical discussion is given for sum mixing with unfocused Gaussian beams. The four-wave sum and difference mixing are carried out in two ''active'' gases: xenon and krypton. In the negatively dispersive regions buffer gases are added to achieve phase matching. 6 refs., 2 figs

Self-generation of optical frequency comb in single section quantum dot Fabry-Perot lasers: a theoretical study.

Science.gov (United States)

Bardella, Paolo; Columbo, Lorenzo Luigi; Gioannini, Mariangela

2017-10-16

Optical Frequency Comb (OFC) generated by semiconductor lasers are currently widely used in the extremely timely field of high capacity optical interconnects and high precision spectroscopy. In the last decade, several experimental evidences of spontaneous OFC generation have been reported in single section Quantum Dot (QD) lasers. Here we provide a physical understanding of these self-organization phenomena by simulating the multi-mode dynamics of a single section Fabry-Perot (FP) QD laser using a Time-Domain Traveling-Wave (TDTW) model that properly accounts for coherent radiation-matter interaction in the semiconductor active medium and includes the carrier grating generated by the optical standing wave pattern in the laser cavity. We show that the latter is the fundamental physical effect at the origin of the multi-mode spectrum appearing just above threshold. A self-mode-locking regime associated with the emission of OFC is achieved for higher bias currents and ascribed to nonlinear phase sensitive effects as Four Wave Mixing (FWM). Our results explain in detail the behaviour observed experimentally by different research groups and in different QD and Quantum Dash (QDash) devices.

Towards generalized mirror symmetry for twisted connected sum G 2 manifolds

Science.gov (United States)

Braun, Andreas P.; Del Zotto, Michele

2018-03-01

We revisit our construction of mirror symmetries for compactifications of Type II superstrings on twisted connected sum G 2 manifolds. For a given G 2 manifold, we discuss evidence for the existence of mirror symmetries of two kinds: one is an autoequivalence for a given Type II superstring on a mirror pair of G 2 manifolds, the other is a duality between Type II strings with different chiralities for another pair of mirror manifolds. We clarify the role of the B-field in the construction, and check that the corresponding massless spectra are respected by the generalized mirror maps. We discuss hints towards a homological version based on BPS spectroscopy. We provide several novel examples of smooth, as well as singular, mirror G 2 backgrounds via pairs of dual projecting tops. We test our conjectures against a Joyce orbifold example, where we reproduce, using our geometrical methods, the known mirror maps that arise from the SCFT worldsheet perspective. Along the way, we discuss non-Abelian gauge symmetries, and argue for the generation of the Affleck-Harvey-Witten superpotential in the pure SYM case.

The generalized Pell (p, i)-numbers and their Binet formulas, combinatorial representations, sums

International Nuclear Information System (INIS)

Kilic, Emrah

2009-01-01

The theory of generalized Pell p-numbers was introduced by Stakhov and then have been studied by several authors. In this paper, we consider the usual Pell numbers and as similar to the Fibonacci p-numbers, we give fair generalization of the Pell numbers, which we call the generalized Pell (p, i)-numbers for 0 ≤ i ≤ p. First we give relationships between the generalized Pell (p, i)-numbers and give the generating matrices for these numbers. Also we derive the generalized Binet formulas, sums, combinatorial representations and generating function of the generalized Pell p-numbers. Also using matrix methods, we derive an explicit formula for the sums of the generalized Fibonacci p-numbers. Finally, we derive relationships between generalized Pell (p, i)-numbers and their sums and permanents of certain matrices.

The generalized Pell (p, i)-numbers and their Binet formulas, combinatorial representations, sums

Energy Technology Data Exchange (ETDEWEB)

Kilic, Emrah [TOBB University of Economics and Technology, Mathematics Department, 06560 Sogutozu, Ankara (Turkey)], E-mail: ekilic@etu.edu.tr

2009-05-30

The theory of generalized Pell p-numbers was introduced by Stakhov and then have been studied by several authors. In this paper, we consider the usual Pell numbers and as similar to the Fibonacci p-numbers, we give fair generalization of the Pell numbers, which we call the generalized Pell (p, i)-numbers for 0 {<=} i {<=} p. First we give relationships between the generalized Pell (p, i)-numbers and give the generating matrices for these numbers. Also we derive the generalized Binet formulas, sums, combinatorial representations and generating function of the generalized Pell p-numbers. Also using matrix methods, we derive an explicit formula for the sums of the generalized Fibonacci p-numbers. Finally, we derive relationships between generalized Pell (p, i)-numbers and their sums and permanents of certain matrices.

Generation of continuous-wave single-frequency 1.5 W 378 nm radiation by frequency doubling of a Ti:sapphire laser.

Science.gov (United States)

Cha, Yong-Ho; Ko, Kwang-Hoon; Lim, Gwon; Han, Jae-Min; Park, Hyun-Min; Kim, Taek-Soo; Jeong, Do-Young

2010-03-20

We have generated continuous-wave single-frequency 1.5 W 378 nm radiation by frequency doubling a high-power Ti:sapphire laser in an external enhancement cavity. An LBO crystal that is Brewster-cut and antireflection coated on both ends is used for a long-term stable frequency doubling. By optimizing the input coupler's reflectivity, we could generate 1.5 W 378 nm radiation from a 5 W 756 nm Ti:sapphire laser. According to our knowledge, this is the highest CW frequency-doubled power of a Ti:sapphire laser.

Incorporating X–ray summing into gamma–gamma signature quantification

International Nuclear Information System (INIS)

Britton, R.; Jackson, M.J.; Davies, A.V.

2016-01-01

A method for quantifying coincidence signatures has been extended to incorporate the effects of X–ray summing, and tested using a high–efficiency γ–γ system. An X–ray library has been created, allowing all possible γ, X–ray and conversion electron cascades to be generated. The equations for calculating efficiency and cascade summing corrected coincidence signature probabilities have also been extended from a two γ, two detector ‘special case’ to an arbitrarily large system. The coincidence library generated is fully searchable by energy, nuclide, coincidence pair, γ multiplicity, cascade probability and the half–life of the cascade, allowing the user to quickly identify coincidence signatures of interest. The method and software described is inherently flexible, as it only requires evaluated nuclear data, an X–ray library, and accurate efficiency characterisations to quickly and easily calculate coincidence signature probabilities for a variety of systems. Additional uses for the software include the fast identification of γ coincidence signals with required multiplicities and branching ratios, identification of the optimal coincidence signatures to measure for a particular system, and the calculation of cascade summing corrections for single detector systems. - Highlights: • Method for incorporating X-ray summing into coincidence measurements developed. • Calculation routines have been extended to an arbitrarily large detector system, and re-written to take advantage of multiple computing cores. • Data collected in list-mode with all events timestamped for offline coincidence analysis. • Coincidence analysis of environmental samples will dramatically improve the detection sensitivity achievable.

50 years of nonlinear optics

International Nuclear Information System (INIS)

Shen Yuanrang

2011-01-01

This article presents a brief introduction to the birth and early investigations of nonlinear optics, such as second harmonic generation,sum and difference frequency generation, stimulated Raman scattering,and self-action of light etc. Several important research achievements and applications of nonlinear optics are presented as well, including nonlinear optical spectroscopy, phase conjugation and adaptive optics, coherent nonlinear optics, and high-order harmonic generation. In the end, current and future research topics in nonlinear optics are summarized. (authors)

Non-invasive optical monitoring of the newborn piglet brain using continuous-wave and frequency-domain spectroscopy

International Nuclear Information System (INIS)

Fantini, S.; Franceschini, M.A.; Gratton, E.; Hueber, D.; Rosenfeld, W.; Maulik, D.; Stubblefield, P.G.; Stankovic, M.R.

1999-01-01

We have used continuous-wave (CW) and frequency-domain spectroscopy to investigate the optical properties of the newborn piglet brain in vivo and non-invasively. Three anaesthetized, intubated, ventilated and instrumented newborn piglets were placed into a stereotaxic instrument for optimal experimental stability, reproducible probe-to-scalp optical contact and 3D adjustment of the optical probe. By measuring the absolute values of the brain absorption and reduced scattering coefficients at two wavelengths (758 and 830 nm), frequency-domain spectroscopy provided absolute readings (in contrast to the relative readings of CW spectroscopy) of cerebral haemoglobin concentration and saturation during experimentally induced perturbations in cerebral haemodynamics and oxygenation. Such perturbations included a modulation of the inspired oxygen concentration, transient brain asphyxia, carotid artery occlusion and terminal brain asphyxia. The baseline cerebral haemoglobin saturation and concentration, measured with frequency-domain spectroscopy, were about 60% and 42 μM respectively. The cerebral saturation values ranged from a minimum of 17% (during transient brain asphyxia) to a maximum of 80% (during recovery from transient brain asphyxia). To analyse the CW optical data, we have (a) derived a mathematical relationship between the cerebral optical properties and the differential pathlength factor and (b) introduced a method based on the spatial dependence of the detected intensity (dc slope method). The analysis of the cerebral optical signals associated with the arterial pulse and with respiration demonstrates that motion artefacts can significantly affect the intensity recorded from a single optode pair. Motion artefacts can be strongly reduced by combining data from multiple optodes to provide relative readings in the dc slope method. We also report significant biphasic changes (initial decrease and successive increase) in the reduced scattering coefficient measured

Dual resonant structure for energy harvesting from random vibration sources at low frequency

Directory of Open Access Journals (Sweden)

Shanshan Li

2016-01-01

Full Text Available We introduce a design with dual resonant structure which can harvest energy from random vibration sources at low frequency range. The dual resonant structure consists of two spring-mass subsystems with different frequency responses, which exhibit strong coupling and broad bandwidth when the two masses collide with each other. Experiments with piezoelectric elements show that the energy harvesting device with dual resonant structure can generate higher power output than the sum of the two separate devices from random vibration sources.

SFG study of methanol dissociative adsorption at Pt(1 0 0), Pt(1 1 0) and Pt(1 1 1) electrodes surfaces

Science.gov (United States)

Vidal, F.; Busson, B.; Six, C.; Pluchery, O.; Tadjeddine, A.

2002-04-01

The Pt( hkl)/methanol in acidic solution interface which constitutes a model of the anodic part of a fuel cell is studied by infrared-visible sum frequency generation vibrational spectroscopy. Methanol dissociative adsorption leads to CO poisoning of the Pt electrode surfaces. The structure of the CO/Pt( hkl) interface depends strongly on the orientation of the surface electrode.

Raman spectroscopy for in-situ characterisation of steam generator deposits

International Nuclear Information System (INIS)

Rochefort, P.A.; Guzonas, D.A.; Turner, C.W.

1997-12-01

This report describes the effort to develop in-situ characterisation of steam generator deposits using remote raman spectroscopy to determine the chemical composition and semi-quantitative measurement of their concentrations. Information on the composition of the deposits is necessary in order to establish the optimal cleaning conditions and procedures. Furthermore, the composition of the deposits also provides information on the conditions that exist within the steam generator and the feedtrain. The raman spectra of the three most common iron oxide phases found in the CANDU deposits (hematite, magnetite and nickel ferrite) are shown

Summing threshold logs in a parton shower

Energy Technology Data Exchange (ETDEWEB)

Nagy, Zoltán [DESY,Notkestrasse 85, 22607 Hamburg (Germany); Soper, Davison E. [Institute of Theoretical Science, University of Oregon,Eugene, OR 97403-5203 (United States)

2016-10-05

When parton distributions are falling steeply as the momentum fractions of the partons increases, there are effects that occur at each order in α{sub s} that combine to affect hard scattering cross sections and need to be summed. We show how to accomplish this in a leading approximation in the context of a parton shower Monte Carlo event generator.

An abstract approach to some spectral problems of direct sum differential operators

Directory of Open Access Journals (Sweden)

Maksim S. Sokolov

2003-07-01

Full Text Available In this paper, we study the common spectral properties of abstract self-adjoint direct sum operators, considered in a direct sum Hilbert space. Applications of such operators arise in the modelling of processes of multi-particle quantum mechanics, quantum field theory and, specifically, in multi-interval boundary problems of differential equations. We show that a direct sum operator does not depend in a straightforward manner on the separate operators involved. That is, on having a set of self-adjoint operators giving a direct sum operator, we show how the spectral representation for this operator depends on the spectral representations for the individual operators (the coordinate operators involved in forming this sum operator. In particular it is shown that this problem is not immediately solved by taking a direct sum of the spectral properties of the coordinate operators. Primarily, these results are to be applied to operators generated by a multi-interval quasi-differential system studied, in the earlier works of Ashurov, Everitt, Gesztezy, Kirsch, Markus and Zettl. The abstract approach in this paper indicates the need for further development of spectral theory for direct sum differential operators.

Ultrabroadband THz time-domain spectroscopy of biomolecular crystals

DEFF Research Database (Denmark)

Kaltenecker, Korbinian J.; Engelbrecht, Sebastian; Iwaszczuk, Krzysztof

2016-01-01

Ultrabroadband THz time-domain spectroscopy based on two-color plasma generation and air biased coherent detection is used for the investigation of molecular dynamics of crystalline materials in the frequency range from 0.3 THz to 20 THz. We show that the spectral features in this extended...... frequency range are a result of inter- and intramolecular vibrations which are identified by means of simulations of the crystalline materials....

Wind/PV Generation for Frequency Regulation and Oscillation Damping in the Eastern Interconnection

Energy Technology Data Exchange (ETDEWEB)

Liu, Yong [Univ. of Tennessee, Knoxville, TN (United States); Gracia, Jose R. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Hadley, Stanton W. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Liu, Yilu [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

2013-12-01

This report presents the control of renewable energy sources, including the variable-speed wind generators and solar photovoltaic (PV) generators, for frequency regulation and inter-area oscillation damping in the U.S. Eastern Interconnection (EI). In this report, based on the user-defined wind/PV generator electrical control model and the 16,000-bus Eastern Interconnection dynamic model, the additional controllers for frequency regulation and inter-area oscillation damping are developed and incorporated and the potential contributions of renewable energy sources to the EI system frequency regulation and inter-area oscillation damping are evaluated.

High resolution spectroscopy in the microwave and far infrared

Science.gov (United States)

Pickett, Herbert M.

1990-01-01

High resolution rotational spectroscopy has long been central to remote sensing techniques in atmospheric sciences and astronomy. As such, laboratory measurements must supply the required data to make direct interpretation of data for instruments which sense atmospheres using rotational spectra. Spectral measurements in the microwave and far infrared regions are also very powerful tools when combined with infrared measurements for characterizing the rotational structure of vibrational spectra. In the past decade new techniques were developed which have pushed high resolution spectroscopy into the wavelength region between 25 micrometers and 2 mm. Techniques to be described include: (1) harmonic generation of microwave sources, (2) infrared laser difference frequency generation, (3) laser sideband generation, and (4) ultrahigh resolution interferometers.

Frequency conversion of structured light.

Science.gov (United States)

Steinlechner, Fabian; Hermosa, Nathaniel; Pruneri, Valerio; Torres, Juan P

2016-02-15

Coherent frequency conversion of structured light, i.e. the ability to manipulate the carrier frequency of a wave front without distorting its spatial phase and intensity profile, provides the opportunity for numerous novel applications in photonic technology and fundamental science. In particular, frequency conversion of spatial modes carrying orbital angular momentum can be exploited in sub-wavelength resolution nano-optics and coherent imaging at a wavelength different from that used to illuminate an object. Moreover, coherent frequency conversion will be crucial for interfacing information stored in the high-dimensional spatial structure of single and entangled photons with various constituents of quantum networks. In this work, we demonstrate frequency conversion of structured light from the near infrared (803 nm) to the visible (527 nm). The conversion scheme is based on sum-frequency generation in a periodically poled lithium niobate crystal pumped with a 1540-nm Gaussian beam. We observe frequency-converted fields that exhibit a high degree of similarity with the input field and verify the coherence of the frequency-conversion process via mode projection measurements with a phase mask and a single-mode fiber. Our results demonstrate the suitability of exploiting the technique for applications in quantum information processing and coherent imaging.

Generation of continuous-wave 194 nm laser for mercury ion optical frequency standard

Science.gov (United States)

Zou, Hongxin; Wu, Yue; Chen, Guozhu; Shen, Yong; Liu, Qu; Precision measurement; atomic clock Team

2015-05-01

194 nm continuous-wave (CW) laser is an essential part in mercury ion optical frequency standard. The continuous-wave tunable radiation sources in the deep ultraviolet (DUV) region of the spectrum is also serviceable in high-resolution spectroscopy with many atomic and molecular lines. We introduce a scheme to generate continuous-wave 194 nm radiation with SFM in a Beta Barium Borate (BBO) crystal here. The two source beams are at 718 nm and 266 nm, respectively. Due to the property of BBO, critical phase matching (CPM) is implemented. One bow-tie cavity is used to resonantly enhance the 718 nm beam while the 266 nm makes a single pass, which makes the configuration easy to implement. Considering the walk-off effect in CPM, the cavity mode is designed to be elliptical so that the conversion efficiency can be promoted. Since the 266 nm radiation is generated by a 532 nm laser through SHG in a BBO crystal with a large walk-off angle, the output mode is quite non-Gaussian. To improve mode matching, we shaped the 266 nm beam into Gaussian modes with a cylindrical lens and iris diaphragm. As a result, 2.05 mW 194 nm radiation can be generated. As we know, this is the highest power for 194 nm CW laser using SFM in BBO with just single resonance. The work is supported by the National Natural Science Foundation of China (Grant No. 91436103 and No. 11204374).

Mobile Charge Generation Dynamics in P3HT:PCBM Observed by Time-Resolved Terahertz Spectroscopy

DEFF Research Database (Denmark)

Cooke, D. G.; Krebs, Frederik C; Jepsen, Peter Uhd

2012-01-01

Ultra-broadband time-resolved terahertz spectroscopy is used to examine the sub-ps conductivity dynamics of a conjugated polymer bulk heterojunction film P3HT:PCBM. We directly observe mobile charge generation dynamics on a sub-100 fs time scale.......Ultra-broadband time-resolved terahertz spectroscopy is used to examine the sub-ps conductivity dynamics of a conjugated polymer bulk heterojunction film P3HT:PCBM. We directly observe mobile charge generation dynamics on a sub-100 fs time scale....

Mobile charge generation dynamics in P3HT: PCBM observed by time-resolved terahertz spectroscopy

DEFF Research Database (Denmark)

Cooke, D. G.; Krebs, Frederik C; Jepsen, Peter Uhd

2012-01-01

Ultra-broadband time-resolved terahertz spectroscopy is used to examine the sub-ps conductivity dynamics of a conjugated polymer bulk heterojunction film P3HT:PCBM. We directly observe mobile charge generation dynamics on a sub-100 fs time scale.......Ultra-broadband time-resolved terahertz spectroscopy is used to examine the sub-ps conductivity dynamics of a conjugated polymer bulk heterojunction film P3HT:PCBM. We directly observe mobile charge generation dynamics on a sub-100 fs time scale....

Selecting Sums in Arrays

DEFF Research Database (Denmark)

Brodal, Gerth Stølting; Jørgensen, Allan Grønlund

2008-01-01

In an array of n numbers each of the \\binomn2+nUnknown control sequence '\\binom' contiguous subarrays define a sum. In this paper we focus on algorithms for selecting and reporting maximal sums from an array of numbers. First, we consider the problem of reporting k subarrays inducing the k largest...... sums among all subarrays of length at least l and at most u. For this problem we design an optimal O(n + k) time algorithm. Secondly, we consider the problem of selecting a subarray storing the k’th largest sum. For this problem we prove a time bound of Θ(n · max {1,log(k/n)}) by describing...... an algorithm with this running time and by proving a matching lower bound. Finally, we combine the ideas and obtain an O(n· max {1,log(k/n)}) time algorithm that selects a subarray storing the k’th largest sum among all subarrays of length at least l and at most u....

Soliton generation from a multi-frequency optical signal

International Nuclear Information System (INIS)

Panoiu, N-C; Mel'nikov, I V; Mihalache, D; Etrich, C; Lederer, F

2002-01-01

We present a comprehensive analysis of the generation of optical solitons in a monomode optical fibre from a superposition of soliton-like optical pulses at different frequencies. It is demonstrated that the structure of the emerging optical field is highly dependent on the number of input channels, the inter-channel frequency separation, the time shift between the pulses belonging to adjacent channels, and the polarization of the pulses. Also, it is found that there exists a critical frequency separation above which wavelength-division multiplexing with solitons is feasible and that this critical frequency increases with the number of transmission channels. Moreover, for the case in which only two channels are considered, we analyse the propagation of the emerging two-soliton solutions in the presence of several perturbations important for optical networks: bandwidth-limited amplification, nonlinear amplification, and amplitude and phase modulation. Finally, the influence of the birefringence of the fibre on the structure of the emerging optical field is discussed. (review article)

Water Orientation at Ceramide/Water Interfaces Studied by Heterodyne-Detected Vibrational Sum Frequency Generation Spectroscopy and Molecular Dynamics Simulation

KAUST Repository

Adhikari, Aniruddha; Re, Suyong; Nishima, Wataru; Ahmed, Mohammed; Nihonyanagi, Satoshi; Klauda, Jeffery B.; Sugita, Yuji; Tahara, Tahei

2016-01-01

Lipid/water interaction is essential for many biological processes. The water structure at the nonionic lipid interface remains little known, and there is no scope of a priori prediction of water orientation at nonionic interfaces, either. Here, we

Multiharmonic Frequency-Chirped Transducers for Surface-Acoustic-Wave Optomechanics

Science.gov (United States)

Weiß, Matthias; Hörner, Andreas L.; Zallo, Eugenio; Atkinson, Paola; Rastelli, Armando; Schmidt, Oliver G.; Wixforth, Achim; Krenner, Hubert J.

2018-01-01

Wide-passband interdigital transducers are employed to establish a stable phase lock between a train of laser pulses emitted by a mode-locked laser and a surface acoustic wave generated electrically by the transducer. The transducer design is based on a multiharmonic split-finger architecture for the excitation of a fundamental surface acoustic wave and a discrete number of its overtones. Simply by introducing a variation of the transducer's periodicity p , a frequency chirp is added. This combination results in wide frequency bands for each harmonic. The transducer's conversion efficiency from the electrical to the acoustic domain is characterized optomechanically using single quantum dots acting as nanoscale pressure sensors. The ability to generate surface acoustic waves over a wide band of frequencies enables advanced acousto-optic spectroscopy using mode-locked lasers with fixed repetition rate. Stable phase locking between the electrically generated acoustic wave and the train of laser pulses is confirmed by performing stroboscopic spectroscopy on a single quantum dot at a frequency of 320 MHz. Finally, the dynamic spectral modulation of the quantum dot is directly monitored in the time domain combining stable phase-locked optical excitation and time-correlated single-photon counting. The demonstrated scheme will be particularly useful for the experimental implementation of surface-acoustic-wave-driven quantum gates of optically addressable qubits or collective quantum states or for multicomponent Fourier synthesis of tailored nanomechanical waveforms.

Frequency-tunable terahertz wave generation via excitation of phonon-polaritons in GaP

CERN Document Server

Tanabé, T; Nishizawa, J I; Saitô, K; Kimura, T

2003-01-01

High-power, wide-frequency-tunable terahertz waves were generated based on difference-frequency generation in GaP crystals with small-angle noncollinear phase matching. The tunable frequency range was as wide as 0.5-7 THz, and the peak power remained high, near 100 mW, over most of the frequency region. The tuning properties were well described by the dispersion relationship for the phonon-polariton mode of GaP up to 6 THz. We measured the spectra of crystal polyethylene and crystal quartz with high resolution using this THz-wave source.

Frequency-tunable terahertz wave generation via excitation of phonon-polaritons in GaP

International Nuclear Information System (INIS)

Tanabe, Tadao; Suto, Ken; Nishizawa, Jun-ichi; Saito, Kyosuke; Kimura, Tomoyuki

2003-01-01

High-power, wide-frequency-tunable terahertz waves were generated based on difference-frequency generation in GaP crystals with small-angle noncollinear phase matching. The tunable frequency range was as wide as 0.5-7 THz, and the peak power remained high, near 100 mW, over most of the frequency region. The tuning properties were well described by the dispersion relationship for the phonon-polariton mode of GaP up to 6 THz. We measured the spectra of crystal polyethylene and crystal quartz with high resolution using this THz-wave source

Frequency comb generation in a continuously pumped optical parametric oscillator

Science.gov (United States)

Mosca, S.; Parisi, M.; Ricciardi, I.; Leo, F.; Hansson, T.; Erkintalo, M.; Maddaloni, P.; De Natale, P.; Wabnitz, S.; De Rosa, M.

2018-02-01

We demonstrate optical frequency comb generation in a continuously pumped optical parametric oscillator, in the parametric region around half of the pump frequency. We also model the dynamics of such quadratic combs using a single time-domain mean-field equation, and obtain simulation results that are in good agreement with experimentally observed spectra. Moreover, we numerically investigate the coherence properties of simulated combs, showing the existence of correlated and phase-locked combs. Our work could pave the way for a new class of frequency comb sources, which may enable straightforward access to new spectral regions and stimulate novel applications of frequency combs.

Zero-Sum Flows in Designs

International Nuclear Information System (INIS)

Akbari, S.; Khosrovshahi, G.B.; Mofidi, A.

2010-07-01

Let D be a t-(v, k, λ) design and let N i (D), for 1 ≤ i ≤ t, be the higher incidence matrix of D, a (0, 1)-matrix of size (v/i) x b, where b is the number of blocks of D. A zero-sum flow of D is a nowhere-zero real vector in the null space of N 1 (D). A zero-sum k-flow of D is a zero-sum flow with values in {±,...,±(k-1)}. In this paper we show that every non-symmetric design admits an integral zero-sum flow, and consequently we conjecture that every non-symmetric design admits a zero-sum 5-flow. Similarly, the definition of zero-sum flow can be extended to N i (D), 1 ≤ i ≤ t. Let D = t-(v,k, (v-t/k-t)) be the complete design. We conjecture that N t (D) admits a zero-sum 3-flow and prove this conjecture for t = 2. (author)

A trough for improved SFG spectroscopy of lipid monolayers

Science.gov (United States)

Franz, Johannes; van Zadel, Marc-Jan; Weidner, Tobias

2017-05-01

Lipid monolayers are indispensable model systems for biological membranes. The main advantage over bilayer model systems is that the surface pressure within the layer can be directly and reliably controlled. The sensitive interplay between surface pressure and temperature determines the molecular order within a model membrane and consequently determines the membrane phase behavior. The lipid phase is of crucial importance for a range of membrane functions such as protein interactions and membrane permeability. A very reliable method to probe the structure of lipid monolayers is sum frequency generation (SFG) vibrational spectroscopy. Not only is SFG extremely surface sensitive but it can also directly access critical parameters such as lipid order and orientation, and it can provide valuable information about protein interactions along with interfacial hydration. However, recent studies have shown that temperature gradients caused by high power laser beams perturb the lipid layers and potentially obscure the spectroscopic results. Here we demonstrate how the local heating problem can be effectively reduced by spatially distributing the laser pulses on the sample surface using a translating Langmuir trough for SFG experiments at lipid monolayers. The efficiency of the trough is illustrated by the detection of enhanced molecular order due to reduced heat load.

Small sum privacy and large sum utility in data publishing.

Science.gov (United States)

Fu, Ada Wai-Chee; Wang, Ke; Wong, Raymond Chi-Wing; Wang, Jia; Jiang, Minhao

2014-08-01

While the study of privacy preserving data publishing has drawn a lot of interest, some recent work has shown that existing mechanisms do not limit all inferences about individuals. This paper is a positive note in response to this finding. We point out that not all inference attacks should be countered, in contrast to all existing works known to us, and based on this we propose a model called SPLU. This model protects sensitive information, by which we refer to answers for aggregate queries with small sums, while queries with large sums are answered with higher accuracy. Using SPLU, we introduce a sanitization algorithm to protect data while maintaining high data utility for queries with large sums. Empirical results show that our method behaves as desired. Copyright © 2014 Elsevier Inc. All rights reserved.

Super fast physical-random number generation using laser diode frequency noises

Science.gov (United States)

Ushiki, Tetsuro; Doi, Kohei; Maehara, Shinya; Sato, Takashi; Ohkawa, Masashi; Ohdaira, Yasuo

2011-02-01

Random numbers can be classified as either pseudo- or physical-random in character. Pseudo-random numbers' periodicity renders them inappropriate for use in cryptographic applications, but naturally-generated physical-random numbers have no calculable periodicity, thereby making them ideally-suited to the task. The laser diode naturally produces a wideband "noise" signal that is believed to have tremendous capacity and great promise, for the rapid generation of physical-random numbers for use in cryptographic applications. We measured a laser diode's output, at a fast photo detector and generated physical-random numbers from frequency noises. We then identified and evaluated the binary-number-line's statistical properties. The result shows that physical-random number generation, at speeds as high as 40Gbps, is obtainable, using the laser diode's frequency noise characteristic.

Generation of narrow peaks in spectroscopy of charged particles

Energy Technology Data Exchange (ETDEWEB)

Dubbers, Dirk, E-mail: dubbers@physi.uni-heidelberg.de; Schmidt, Ulrich, E-mail: ulrich.schmidt@physi.uni-heidelberg.de

2016-11-21

In spectroscopy of charged particles, narrow peaks may appear in continuous spectra if magnetic transport of the particles is involved. These artefacts, which so far have escaped the attention of investigators, can develop whenever geometric detection efficiency is less than 100%. As such peaks may be misinterpreted as new physics, their generation is investigated, both analytically and experimentally, for various detector configurations, including those used in searches for the spontaneous decay of the vacuum in heavy-ion collisions.

Characterization of Crystal Chirality in Amino Acids Using Low-Frequency Raman Spectroscopy.

Science.gov (United States)

Aviv, Hagit; Nemtsov, Irena; Mastai, Yitzhak; Tischler, Yaakov R

2017-10-19

We present a new method for differentiating racemic crystals from enantiopure crystals. Recently, developments in optical filters have enabled the facile use of Raman spectroscopy to detect low-frequency vibrational (LFV) modes. Here, for the first time, we use Raman spectroscopy to characterize the LFV modes for crystalline organic materials composed of chiral molecules. The LF-Raman spectra of racemic and enantiopure crystals exhibit a significant variation, which we attribute to different hydrogen-bond networks in the chiral crystal structures. Across a representative set of amino acids, we observed that when comparing racemic versus enantiopure crystals, the available LFV modes and their relative scattering intensity are strong functions of side chain polarity. Thus, LF-Raman can be used as a method that is complementary to the currently used methods for characterizing crystal chirality due to simpler, faster, and more sensitive measurements, along with the small sample size required, which is limited by the laser-beam diameter in the focus.

Autonomous generator based on Ni-Mn-Ga microactuator as a frequency selective element

Directory of Open Access Journals (Sweden)

Barandiaran J.M.

2013-01-01

Full Text Available In this work, we suggest the temperature-induced resistivity change at the martensitic transformation in the Ni-Mn-Ga ferromagnetic shape memory alloy as a driving mechanism enabling periodic signal generation. We demonstrated its practical importance by a design of the prototype of a low-frequency autonomous generator. A prominent feature of this new generator is a control of its frequency by the external magnetic field.

Understanding fifth-harmonic generation in CLBO

Science.gov (United States)

Patankar, S.; Yang, S. T.; Moody, J. D.; Bayramian, A. J.; Swadling, G. F.; Barker, D.; Datte, P.; Mennerat, G.; Norton, M.; Carr, C. W.; Begishev, I. A.; Bromage, J.; Ross, J. S.

2018-02-01

We report on results of fifth harmonic generation in Cesium Lithium Borate (CLBO) using a three-crystal cascaded frequency conversion scheme designed to study the energy balance of the final sum frequency generation stage. The experimental setup independently combines the first and fourth harmonic of a Nd:Glass laser in a 5mm thick CLBO crystal. Energy balance between the incoming and output energy is close to unity when the CLBO is out of phase matching and approximately 80% when the crystal is in phase matching. A detailed analysis of the residual fundamental and fourth harmonic energy indicates 5th harmonic light is being generated but only 26% is unaccounted for. We attribute the missing light to linear transmission loss in the CLBO oven. The ratio of the output to input energy is unity when the missing 5th harmonic is incorporated into the calculations. Two-dimensional plane wave mixing simulations show agreement with the results at lower intensities.

Dual THz comb spectroscopy

Science.gov (United States)

Yasui, Takeshi

2017-08-01

Optical frequency combs are innovative tools for broadband spectroscopy because a series of comb modes can serve as frequency markers that are traceable to a microwave frequency standard. However, a mode distribution that is too discrete limits the spectral sampling interval to the mode frequency spacing even though individual mode linewidth is sufficiently narrow. Here, using a combination of a spectral interleaving and dual-comb spectroscopy in the terahertz (THz) region, we achieved a spectral sampling interval equal to the mode linewidth rather than the mode spacing. The spectrally interleaved THz comb was realized by sweeping the laser repetition frequency and interleaving additional frequency marks. In low-pressure gas spectroscopy, we achieved an improved spectral sampling density of 2.5 MHz and enhanced spectral accuracy of 8.39 × 10-7 in the THz region. The proposed method is a powerful tool for simultaneously achieving high resolution, high accuracy, and broad spectral coverage in THz spectroscopy.

Disjoint sum forms in reliability theory

Directory of Open Access Journals (Sweden)

B. Anrig

2014-01-01

Full Text Available The structure function f of a binary monotone system is assumed to be known and given in a disjunctive normal form, i.e. as the logical union of products of the indicator variables of the states of its subsystems. Based on this representation of f, an improved Abraham algorithm is proposed for generating the disjoint sum form of f. This form is the base for subsequent numerical reliability calculations. The approach is generalized to multivalued systems. Examples are discussed.

Injection-seeded tunable mid-infrared pulses generated by difference frequency mixing

Science.gov (United States)

Miyamoto, Yuki; Hara, Hideaki; Masuda, Takahiko; Hiraki, Takahiro; Sasao, Noboru; Uetake, Satoshi

2017-03-01

We report on the generation of nanosecond mid-infrared pulses having frequency tunability, a narrow linewidth, and a high pulse energy. These pulses are obtained by frequency mixing between injection-seeded near-infrared pulses in potassium titanyl arsenate crystals. A continuous-wave external cavity laser diode or a Ti:sapphire ring laser is used as a tunable seeding source for the near-infrared pulses. The typical energy of the generated mid-infrared pulses is in the range of 0.4-1 mJ/pulse. The tuning wavelength ranges from 3142 to 4806 nm. A narrow linewidth of 1.4 GHz and good frequency reproducibility of the mid-infrared pulses are confirmed by observing a rovibrational absorption line of gaseous carbon monoxide at 4587 nm.

Dynamics of microresonator frequency comb generation: models and stability

Directory of Open Access Journals (Sweden)

Hansson Tobias

2016-06-01

Full Text Available Microresonator frequency combs hold promise for enabling a new class of light sources that are simultaneously both broadband and coherent, and that could allow for a profusion of potential applications. In this article, we review various theoretical models for describing the temporal dynamics and formation of optical frequency combs. These models form the basis for performing numerical simulations that can be used in order to better understand the comb generation process, for example helping to identify the universal combcharacteristics and their different associated physical phenomena. Moreover, models allow for the study, design and optimization of comb properties prior to the fabrication of actual devices. We consider and derive theoretical formalisms based on the Ikeda map, the modal expansion approach, and the Lugiato-Lefever equation. We further discuss the generation of frequency combs in silicon resonators featuring multiphoton absorption and free-carrier effects. Additionally, we review comb stability properties and consider the role of modulational instability as well as of parametric instabilities due to the boundary conditions of the cavity. These instability mechanisms are the basis for comprehending the process of frequency comb formation, for identifying the different dynamical regimes and the associated dependence on the comb parameters. Finally, we also discuss the phenomena of continuous wave bi- and multistability and its relation to the observation of mode-locked cavity solitons.

Fast fundamental frequency estimation

DEFF Research Database (Denmark)

Nielsen, Jesper Kjær; Jensen, Tobias Lindstrøm; Jensen, Jesper Rindom

2017-01-01

Modelling signals as being periodic is common in many applications. Such periodic signals can be represented by a weighted sum of sinusoids with frequencies being an integer multiple of the fundamental frequency. Due to its widespread use, numerous methods have been proposed to estimate the funda...

Measurement sum theory and application - Application to low level measurements

International Nuclear Information System (INIS)

Puydarrieux, S.; Bruel, V.; Rivier, C.; Crozet, M.; Vivier, A.; Manificat, G.; Thaurel, B.; Mokili, M.; Philippot, B.; Bohaud, E.

2015-09-01

In laboratories, most of the Total Sum methods implemented today use substitution or censure methods for nonsignificant or negative values, and thus create biases which can sometimes be quite large. They are usually positive, and generate, for example, becquerel (Bq) counting or 'administrative' quantities of materials (= 'virtual'), thus artificially falsifying the records kept by the laboratories under regulatory requirements (environment release records, waste records, etc.). This document suggests a methodology which will enable the user to avoid such biases. It is based on the following two fundamental rules: - The Total Sum of measurement values must be established based on all the individual measurement values, even those considered non-significant including the negative values. Any modification of these values, under the pretext that they are not significant, will inevitably lead to biases in the accumulated result and falsify the evaluation of its uncertainty. - In Total Sum operations, the decision thresholds are arrived at in a similar way to the approach used for uncertainties. The document deals with four essential aspects of the notion of 'measurement Total Sums': - The expression of results and associated uncertainties close to Decision Thresholds, and Detection or Quantification Limits, - The Total Sum of these measurements: sum or mean, - The calculation of the uncertainties associated with the Total Sums, - Result presentation (particularly when preparing balance sheets or reports, etc.) Several case studies arising from different situations are used to illustrate the methodology: environmental monitoring reports, release reports, and chemical impurity Total Sums for the qualification of a finished product. The special case of material balances, in which the measurements are usually all significant and correlated (the covariance term cannot then be ignored) will be the subject of a future second document. This

Time-Frequency Analysis of Signals Generated by Rotating Machines

Directory of Open Access Journals (Sweden)

R. Zetik

1999-06-01

Full Text Available This contribution is devoted to the higher order time-frequency analyses of signals. Firstly, time-frequency representations of higher order (TFRHO are defined. Then L-Wigner distribution (LWD is given as a special case of TFRHO. Basic properties of LWD are illustrated based on the analysis of mono-component and multi-component synthetic signals and acoustical signals generated by rotating machine. The obtained results confirm usefulness of LWD application for the purpose of rotating machine condition monitoring.

MODELING AND STUDY OF HYDROELECTRIC GENERATING SETS OF SMALL HYDRO POWER PLANTS WITH FREQUENCY-CONTROLLED PERMANENT MAGNET SYNCHRONOUS GENERATORS

Directory of Open Access Journals (Sweden)

R. I. Mustafayev

2016-01-01

Full Text Available Currently, the hydroelectric generating sets of small HPPs with Pelton turbines employ as their generating units conventional synchronous generators with electromagnetic excitation. To deal with the torque pulsatile behaviour, they generally install a supplementary flywheel on the system shaft that levels the pulsations. The Pelton turbine power output is adjusted by the needle changing water flow in the nozzle, whose advancement modifies the nozzle area and eventually – the flow. They limit the needle full stroke time to 20–40 sec. since quick shutting the nozzle for swift water flow reduction may result in pressure surges. For quick power adjustment so-called deflectors are employed, whose task is retraction of water jets from the Pelton turbine buckets. Thus, the mechanical method of power output regulation requires agreement between the needle stroke inside the turbine nozzles and the deflector. The paper offers employing frequency-controlled synchronous machines with permanent magnets qua generating units for the hydroelectric generating sets of small HPPs with Pelton turbines. The developed computer model reveals that this provides a higher level of adjustability towards rapid-changing loads in the grid. Furthermore, this will replace the power output mechanical control involving the valuable deflector drive and the turbine nozzle needles with electrical revolution rate and power output regulation by a frequency converter located in the generator stator circuit. Via frequency start, the controllable synchronous machine ensures stable operation of the hydroelectric generating set with negligibly small amount of water (energy carrier. Finally, in complete absence of water, the frequency-relay start facilitates shifting the generator operation to the synchronous capacitor mode, which the system operating parameter fluctograms obtained through computer modeling prove. 

Filterless low-phase-noise frequency-quadrupled microwave generation based on a multimode optoelectronic oscillator

Science.gov (United States)

Teng, Yichao; Zhang, Pin; Zhang, Baofu; Chen, Yiwang

2018-02-01

A scheme to realize low-phase-noise frequency-quadrupled microwave generation without any filter is demonstrated. In this scheme, a multimode optoelectronic oscillator is mainly contributed by dual-parallel Mach-Zehnder modulators, fiber, photodetector, and microwave amplifier. The local source signal is modulated by a child MZM (MZMa), which is worked at maximum transmission point. Through properly adjusting the bias voltages of the other child MZM (MZMb) and the parent MZM (MZMc), optical carrier is effectively suppressed and second sidebands are retained, then the survived optical signal is fed back to the photodetector and MZMb to form an optoelectronic hybrid resonator and realize frequency-quadrupled signal generation. Due to the high Q-factor and mode selection effect of the optoelectronic hybrid resonator, compared with the source signal, the generated frequency-quadrupled signal has a lower phase noise. The approach has verified by experiments, and 18, 22, and 26 GHz frequency-quadrupled signal are generated by 4.5, 5.5, and 6.5 GHz local source signals. Compared with 4.5 GHz source signal, the phase noise of generated 18 GHz signal at 10 kHz frequency offset has 26.5 dB reduction.

Mid-IR femtosecond frequency conversion by soliton-probe collision in phase-mismatched quadratic nonlinear crystals

DEFF Research Database (Denmark)

Liu, Xing; Zhou, Binbin; Guo, Hairun

2015-01-01

in a quadratic nonlinear crystal (beta-barium borate) in the normal dispersion regime due to cascaded (phase-mismatched) second-harmonic generation, and the mid-IR converted wave is formed in the anomalous dispersion regime between. lambda = 2.2-2.4 mu m as a resonant dispersive wave. This process relies...... on nondegenerate four-wave mixing mediated by an effective negative cross-phase modulation term caused by cascaded soliton-probe sum-frequency generation. (C) 2015 Optical Society of America...

Logarithmic residues and sums of idempotents in the Banach algebra generated by the compact operators and the identity.

NARCIS (Netherlands)

H. Bart (Harm); T. Ehrhardt; B. Silbermann

2001-01-01

textabstractA logarithmic residue is a contour integral of the (left or right) logarithmic derivative of an analytic Banach algebra valued function. Logarithmic residues are intimately related to sums of idempotents. The present paper is concerned with logarithmic residues and sums of idempotents in

Laser generated ultrasound sources using polymer nanocomposites for high frequency metrology

KAUST Repository

Rajagopal, Srinath

2017-11-22

Accurate characterisation of ultrasound fields generated by diagnostic and therapeutic transducers is critical for patient safety. This requires hydrophones calibrated to a traceable standard. The existing implementation of the primary standard at the National Measurement Institutes, e.g., NPL and PTB, can provide accurate calibration to a maximum frequency of 40MHz. However, the increasing use of high frequencies for both imaging and therapy necessitates calibrations to frequencies well beyond this range. For this to be possible, a source of high amplitude, broadband, quasi-planar and stable ultrasound fields is required. This is difficult to achieve using conventional piezoelectric sources, but laser generated ultrasound is a promising technique in this regard. In this study various polymer-carbon nanotube nanocomposites (PNC) were fabricated and tested for their suitability for such an application.

Terahertz transmission properties of silicon wafers using continuous-wave terahertz spectroscopy

Science.gov (United States)

Kim, Chihoon; Ahn, Jae Sung; Ji, Taeksoo; Eom, Joo Beom

2017-04-01

We present the spectral properties of Si wafers using continuous-wave terahertz (CW-THz) spectroscopy. By using a tunable laser source and a fixed distributed-feedback laser diode (DFB-LD), a stably tunable beat source for CW-THz spectroscopy system can be implemented. THz radiation is generated in the frequency range of 100 GHz-800 GHz by photomixing in a photoconductive antenna. We also measured CW-THz waveforms by changing the beat frequency and confirmed repeatability through repeated measurement. We calculated the peaks of the THz frequency by taking fast Fourier transforms (FFTs) of measured THz waveforms. The feasibility of CW-THz spectroscopy is demonstrated by the THz spectra of Si wafers with different resistivities, mobilities, and carrier concentrations. The results show that Si wafers with a lower resistivity absorb more THz waves. Thus, we expect our CW-THz system to have the advantage of being able to perform fast non-destructive analysis.

Terahertz transmission properties of silicon wafers using continuous-wave terahertz spectroscopy

International Nuclear Information System (INIS)

Kim, Chihoon; Ahn, Jae Sung; Eom, Joo Beom; Ji, Taeksoo

2017-01-01

We present the spectral properties of Si wafers using continuous-wave terahertz (CW-THz) spectroscopy. By using a tunable laser source and a fixed distributed-feedback laser diode (DFB-LD), a stably tunable beat source for CW-THz spectroscopy system can be implemented. THz radiation is generated in the frequency range of 100 GHz–800 GHz by photomixing in a photoconductive antenna. We also measured CW-THz waveforms by changing the beat frequency and confirmed repeatability through repeated measurement. We calculated the peaks of the THz frequency by taking fast Fourier transforms (FFTs) of measured THz waveforms. The feasibility of CW-THz spectroscopy is demonstrated by the THz spectra of Si wafers with different resistivities, mobilities, and carrier concentrations. The results show that Si wafers with a lower resistivity absorb more THz waves. Thus, we expect our CW-THz system to have the advantage of being able to perform fast non-destructive analysis. (paper)

Sums and Gaussian vectors

CERN Document Server

Yurinsky, Vadim Vladimirovich

1995-01-01

Surveys the methods currently applied to study sums of infinite-dimensional independent random vectors in situations where their distributions resemble Gaussian laws. Covers probabilities of large deviations, Chebyshev-type inequalities for seminorms of sums, a method of constructing Edgeworth-type expansions, estimates of characteristic functions for random vectors obtained by smooth mappings of infinite-dimensional sums to Euclidean spaces. A self-contained exposition of the modern research apparatus around CLT, the book is accessible to new graduate students, and can be a useful reference for researchers and teachers of the subject.

Dispersion theory and sum rules for the non-minimum phase problem in optical spectroscopy

International Nuclear Information System (INIS)

Peiponen, Kai-Erik

2009-01-01

Dispersion relations and sum rules for integer powers of an optical response function are given in the case of the non-minimum phase problem. These relations were obtained using the concept of the Hilbert transform and Blaschke product. The theory presented in this paper is useful both in basic and applied studies of non-minimum phase functions in optics, and also other fields of physics such as high energy physics.

Separation of radiation from two sources from their known radiated sum field

DEFF Research Database (Denmark)

Laitinen, Tommi; Pivnenko, Sergey

2011-01-01

This paper presents a technique for complete and exact separation of the radiated fields of two sources (at the same frequency) from the knowledge of their radiated sum field. The two sources can be arbitrary but it must be possible to enclose the sources inside their own non-intersecting minimum...

Radio Frequency Underwater Discharge Operation and Its Application to Congo Red Degradation

International Nuclear Information System (INIS)

Ji Liangliang; Zou Shuai; Shen Mingrong; Xin Yu

2012-01-01

Radio frequency (RF) underwater discharge operation was performed for different liquid conductivities driven by different frequencies ranging from 13.56 MHz to 60 MHz, and its application to organic degradation was investigated. The RF underwater discharge was observed to be generated within the bubble at electrode surface formed by RF and plasma heating. It was shown that the sizes of the bubbles and plasmas increased as the driving frequency and the input power went up. The breakdown voltage decreased rapidly with the increase of the water conductivity and driving frequency. Comparative experiments of the UV-VIS absorbance spectra of Congo Red solution before and after discharge suggested effective degradation of the organic dye due to the active species generated during the discharge, such as ·OH, ·O, ·H, etc. revealed by optical emission spectroscopy. The results show that higher exciting frequency and lower conductivity of the solution are more effective for organic degradation. With the combination of Fourier Transform Infrared Spectroscopy (FT-IR) and Liquid Chromatography-Mass Spectrometry (LC-MS) data, one possible degradation process was proposed and the main conceivable components and structures of the products were also presented.

High-field EPR spectroscopy of thermal donors in silicon

DEFF Research Database (Denmark)

Dirksen, R.; Rasmussen, F.B.; Gregorkiewicz, T.

1997-01-01

Thermal donors generated in p-type boron-doped Czochralski-grown silicon by a 450 degrees C heat treatment have been studied by high-field magnetic resonance spectroscopy. In the experiments conducted at a microwave frequency of 140 GHz and in a magnetic field of approximately 5 T four individual...

Sums over geometries and improvements on the mean field approximation

International Nuclear Information System (INIS)

Sacksteder, Vincent E. IV

2007-01-01

The saddle points of a Lagrangian due to Efetov are analyzed. This Lagrangian was originally proposed as a tool for calculating systematic corrections to the Bethe approximation, a mean-field approximation which is important in statistical mechanics, glasses, coding theory, and combinatorial optimization. Detailed analysis shows that the trivial saddle point generates a sum over geometries reminiscent of dynamically triangulated quantum gravity, which suggests new possibilities to design sums over geometries for the specific purpose of obtaining improved mean-field approximations to D-dimensional theories. In the case of the Efetov theory, the dominant geometries are locally treelike, and the sum over geometries diverges in a way that is similar to quantum gravity's divergence when all topologies are included. Expertise from the field of dynamically triangulated quantum gravity about sums over geometries may be able to remedy these defects and fulfill the Efetov theory's original promise. The other saddle points of the Efetov Lagrangian are also analyzed; the Hessian at these points is nonnormal and pseudo-Hermitian, which is unusual for bosonic theories. The standard formula for Gaussian integrals is generalized to nonnormal kernels

Using Squares to Sum Squares

Science.gov (United States)

DeTemple, Duane

2010-01-01

Purely combinatorial proofs are given for the sum of squares formula, 1[superscript 2] + 2[superscript 2] + ... + n[superscript 2] = n(n + 1) (2n + 1) / 6, and the sum of sums of squares formula, 1[superscript 2] + (1[superscript 2] + 2[superscript 2]) + ... + (1[superscript 2] + 2[superscript 2] + ... + n[superscript 2]) = n(n + 1)[superscript 2]…

Thermally controlled comb generation and soliton modelocking in microresonators.

Science.gov (United States)

Joshi, Chaitanya; Jang, Jae K; Luke, Kevin; Ji, Xingchen; Miller, Steven A; Klenner, Alexander; Okawachi, Yoshitomo; Lipson, Michal; Gaeta, Alexander L

2016-06-01

We report, to the best of our knowledge, the first demonstration of thermally controlled soliton mode-locked frequency comb generation in microresonators. By controlling the electric current through heaters integrated with silicon nitride microresonators, we demonstrate a systematic and repeatable pathway to single- and multi-soliton mode-locked states without adjusting the pump laser wavelength. Such an approach could greatly simplify the generation of mode-locked frequency combs and facilitate applications such as chip-based dual-comb spectroscopy.

Investigation of Capacitively Coupled Argon Plasma Driven by Dual-Frequency with Different Frequency Configurations

International Nuclear Information System (INIS)

Yu Yiqing; Xin Yu; Ning Zhaoyuan; Lu Wenqi

2011-01-01

Low pressure argon dual-frequency (DF) capacitively coupled plasma (CCP) is generated by using different frequency configurations, such as 13.56/2, 27/2, 41/2, and 60/2 MHz. Characteristics of the plasma are investigated by using a floating double electrical probe and optical emission spectroscopy (OES). It is shown that in the DF-CCPs, the electron temperature T e decreases with the increase in exciting frequency, while the onset of 2 MHz induces a sudden increase in T e and the electron density increases basically with the increase in low frequency (LF) power. The intensity of 750.4 nm emission line increases with the LF power in the case of 13.56/2 MHz, while different tendencies of line intensity with the LF power appear for other configurations. The reason for this is also discussed.

Direct comparison of low- and mid-frequency Raman spectroscopy for quantitative solid-state pharmaceutical analysis.

Science.gov (United States)

Lipiäinen, Tiina; Fraser-Miller, Sara J; Gordon, Keith C; Strachan, Clare J

2018-02-05

This study considers the potential of low-frequency (terahertz) Raman spectroscopy in the quantitative analysis of ternary mixtures of solid-state forms. Direct comparison between low-frequency and mid-frequency spectral regions for quantitative analysis of crystal form mixtures, without confounding sampling and instrumental variations, is reported for the first time. Piroxicam was used as a model drug, and the low-frequency spectra of piroxicam forms β, α2 and monohydrate are presented for the first time. These forms show clear spectral differences in both the low- and mid-frequency regions. Both spectral regions provided quantitative models suitable for predicting the mixture compositions using partial least squares regression (PLSR), but the low-frequency data gave better models, based on lower errors of prediction (2.7, 3.1 and 3.2% root-mean-square errors of prediction [RMSEP] values for the β, α2 and monohydrate forms, respectively) than the mid-frequency data (6.3, 5.4 and 4.8%, for the β, α2 and monohydrate forms, respectively). The better performance of low-frequency Raman analysis was attributed to larger spectral differences between the solid-state forms, combined with a higher signal-to-noise ratio. Copyright © 2017 Elsevier B.V. All rights reserved.

Credal Sum-Product Networks

NARCIS (Netherlands)

Maua, Denis Deratani; Cozman, Fabio Gagli; Conaty, Diarmaid; de Campos, Cassio P.

2017-01-01

Sum-product networks are a relatively new and increasingly popular class of (precise) probabilistic graphical models that allow for marginal inference with polynomial effort. As with other probabilistic models, sum-product networks are often learned from data and used to perform classification.

FIA BioSum: a tool to evaluate financial costs, opportunities and effectiveness of fuel treatments.

Science.gov (United States)

Jeremy Fried; Glenn. Christensen

2004-01-01

FIA BioSum, a tool developed by the USDA Forest Services Forest Inventory and Analysis (FIA) Program, generates reliable cost estimates, identifies opportunities and evaluates the effectiveness of fuel treatments in forested landscapes. BioSum is an analytic framework that integrates a suite of widely used computer models with a foundation of attribute-rich,...

State-space modeling of the radio frequency inductively-coupled plasma generator

International Nuclear Information System (INIS)

Dewangan, Rakesh Kumar; Punjabi, Sangeeta B; Mangalvedekar, H A; Lande, B K; Joshi, N K; Barve, D N

2010-01-01

Computational fluid dynamics models of RF-ICP are useful in understanding the basic transport phenomenon in an ICP torch under a wide variety of operating conditions. However, these models lack the ability to evaluate the effects of the plasma condition on the RF generator. In this paper, simulation of an induction plasma generator has been done using state space modelling by considering inductively coupled plasma as a part of RF network .The time dependent response of the RF-ICP generator circuit to given input excitation has been computed by extracting the circuit's state-space variables and their constraint matrices. MATLAB 7.1 software has been used to solve the state equations. The values of RF coil current, frequency and plasma power has been measured experimentally also at different plate bias voltage. The simulated model is able to predict RF coil current, frequency, plasma power, overall efficiency of the generator. The simulated and measured values are in agreement with each other. This model can prove useful as a design tool for the Induction plasma generator.

Estimation of allele frequency and association mapping using next-generation sequencing data

DEFF Research Database (Denmark)

Kim, Su Yeon; Lohmueller, Kirk E; Albrechtsen, Anders

2011-01-01

Estimation of allele frequency is of fundamental importance in population genetic analyses and in association mapping. In most studies using next-generation sequencing, a cost effective approach is to use medium or low-coverage data (e.g., frequency estimation...

Applications of photon-in, photon-out spectroscopy with third-generation, synchrotron-radiation sources

International Nuclear Information System (INIS)

Lindle, D.W.; Perera, R.C.C.

1991-01-01

This report discusses the following topics: Mother nature's finest test probe; soft x-ray emission spectroscopy with high-brightness synchrotron radiation sources; anisotropy and polarization of x-ray emission from atoms and molecules; valence-hole fluorescence from molecular photoions as a probe of shape-resonance ionization: progress and prospects; structural biophysics on third-generation synchrotron sources; ultra-soft x-ray fluorescence-yield XAFS: an in situ photon-in, photon-out spectroscopy; and x-ray microprobe: an analytical tool for imaging elemental composition and microstructure

Development of microwave-enhanced spark-induced breakdown spectroscopy

International Nuclear Information System (INIS)

Ikeda, Yuji; Moon, Ahsa; Kaneko, Masashi

2010-01-01

We propose microwave-enhanced spark-induced breakdown spectroscopy with the same measurement and analysis processes as in laser-induced breakdown spectroscopy, but with a different plasma generation mechanism. The size and lifetime of the plasma generated can contribute to increased measurement accuracy and expand its applicability to industrial measurement, such as an exhaust gas analyzer for automobile engine development and its regulation, which has been hard to operate by laser at an engineering evaluation site. The use of microwaves in this application helps lower the cost, reduce the system size, and increase the ease of operation to make it commercially viable. A microwave frequency of 2.45 GHz was used to enhance the volume and lifetime of the plasma at atmospheric condition even at elevated pressure.

CAMAC programmable-control frequency synthesizer

International Nuclear Information System (INIS)

Yumaguzin, T.Kh.; Vyazovkin, D.E.; Nazirov, Eh.P.; Tuktarov, R.F.

1989-01-01

Synthesizer allows to set frequency with 0.015% accuracy and to scan it with variable step. Frequency controlled divider with further summing-up of divided frequency with fundamental one is used in synthesizer, and it has allowed to use digit of the input code and to obtain 3-4 MHz frequency range. Variation of operation flowsheet in the other frequency range is possible. K-155 and K-531 series microcircuits were used during development

Dual-Comb Coherent Raman Spectroscopy with Lasers of 1-GHz Pulse Repetition Frequency

OpenAIRE

Mohler, Kathrin J.; Bohn, Bernhard J.; Yan, Ming; Hänsch, Theodor W.; Picqué, Nathalie

2016-01-01

We extend the technique of multiplex coherent Raman spectroscopy with two femtosecond mode-locked lasers to oscillators of a pulse repetition frequency of 1 GHz. We demonstrate spectra of liquids, which span 1100 cm$^{-1}$ of Raman shifts. At a resolution of 6 cm$^{-1}$, their measurement time may be as short as 5 microseconds for a refresh rate of 2 kHz. The waiting period between acquisitions is improved ten-fold compared to previous experiments with two lasers of 100-MHz repetition frequen...

Generation of THz frequency using PANDA ring resonator for THz imaging

Directory of Open Access Journals (Sweden)

Ong CT

2012-02-01

Full Text Available MA Jalil1, Afroozeh Abdolkarim2, T Saktioto2, CT Ong3, Preecha P Yupapin41Ibnu Sina Institute of Fundamental Science Studies, Nanotechnology Research Alliance, Universiti Teknologi Malaysia (UTM,81310, Johor Bahru, Malaysia; 2Institute of Advanced Photonics Science, Nanotechnology Research Alliance, Universiti Teknologi Malaysia (UTM, 81310, Johor Bahru, Malaysia; 3Department of Mathematics, Universiti Teknologi Malaysia 81310 Skudai, Johor Bahru, Malaysia; 4Nanoscale Science and Engineering Research Alliance (N'SERA, Advanced Research Center for Photonics, Faculty of Science, King Mongkut's Institute of Technology Ladkrabang, Bangkok 10520, ThailandAbstract: In this study, we have generated terahertz (THz frequency by a novel design of microring resonators for medical applications. The dense wavelength-division multiplexing can be generated and obtained by using a Gaussian pulse propagating within a modified PANDA ring resonator and an add/drop filter system. Our results show that the THz frequency region can be obtained between 40–50 THz. This area of frequency provides a reliable frequency band for THz pulsed imaging.Keywords: THz imaging, THz technology, MRRs, PANDA, add/drop filter

Compact Tunable Narrowband Terahertz-Wave Source Based on Difference Frequency Generation Pumped by Dual Fiber Lasers in MgO:LiNbO3

Science.gov (United States)

Wada, Yoshio; Satoh, Takumi; Higashi, Yasuhiro; Urata, Yoshiharu

2017-12-01

We demonstrate a high-average-power, single longitudinal-mode, and tunable terahertz (THz)-wave source based on difference frequency generation (DFG) in a MgO:LiNbO3 (MgO:LN) crystal. The waves for DFG are generated using a pair of Yb-doped pulsed fiber lasers with a master oscillator power fiber amplifier configuration. The average power of the THz-wave output reaches 450 μW at 1.07 THz (280 μm) at a linewidth of 7.2 GHz, and the tunability ranges from 0.35 to 1.07 THz under the pulse repetition frequency of 500 kHz. A short burn-in test of the THz wave is also carried out, and the output power stability is within ± 5% of the averaged power without any active stabilizing technique. The combination of MgO:LN-DFG and stable and robust fiber laser sources is highly promising for the development of high-average-power THz-wave sources, particularly in the high transmission sub-THz region. This approach may enable new applications of THz-wave spectroscopy in imaging and remote sensing.

Highly stable microwave carrier generation using a dual-frequency distributed feedback laser

NARCIS (Netherlands)

Khan, M.R.H.; Bernhardi, Edward; Marpaung, D.A.I.; Burla, M.; de Ridder, R.M.; Worhoff, Kerstin; Pollnau, Markus; Roeloffzen, C.G.H.

2012-01-01

Photonic generation of microwave carriers by using a dual-frequency distributed feedback waveguide laser in ytterbium-doped aluminum oxide is demonstrated. A highperformance optical frequency locked loop is implemented to stabilize the microwave carrier. This approach results in a microwave

Resource allocation via sum-rate maximization in the uplink of multi-cell OFDMA networks

KAUST Repository

Tabassum, Hina; Alouini, Mohamed-Slim; Dawy, Zaher

2012-01-01

In this paper, we consider maximizing the sum rate in the uplink of a multi-cell orthogonal frequency-division multiple access network. The problem has a non-convex combinatorial structure and is known to be NP-hard. Because of the inherent

Cavity-enhanced spectroscopies

CERN Document Server

van Zee, Roger

2003-01-01

""Cavity-Enhanced Spectroscopy"" discusses the use of optical resonators and lasers to make sensitive spectroscopic measurements. This volume is written by the researcchers who pioneered these methods. The book reviews both the theory and practice behind these spectroscopic tools and discusses the scientific discoveries uncovered by these techniques. It begins with a chapter on the use of optical resonators for frequency stabilization of lasers, which is followed by in-depth chapters discussing cavity ring-down spectroscopy, frequency-modulated, cavity-enhanced spectroscopy, intracavity spectr

Non-linear optical studies of adsorbates: Spectroscopy and dynamics

Energy Technology Data Exchange (ETDEWEB)

Zhu, Xiangdong.

1989-08-01

In the first part of this thesis, we have established a systematic procedure to apply the surface optical second-harmonic generation (SHG) technique to study surface dynamics of adsorbates. In particular, we have developed a novel technique for studies of molecular surface diffusions. In this technique, the laser-induced desorption with two interfering laser beams is used to produce a monolayer grating of adsorbates. The monolayer grating is detected with diffractions of optical SHG. By monitoring the first-order second-harmonic diffraction, we can follow the time evolution of the grating modulation from which we are able to deduce the diffusion constant of the adsorbates on the surface. We have successfully applied this technique to investigate the surface diffusion of CO on Ni(111). The unique advantages of this novel technique will enable us to readily study anisotropy of a surface diffusion with variable grating orientation, and to investigate diffusion processes of a large dynamic range with variable grating spacings. In the second part of this work, we demonstrate that optical infrared-visible sum-frequency generation (SFG) from surfaces can be used as a viable surface vibrational spectroscopic technique. We have successfully recorded the first vibrational spectrum of a monolayer of adsorbates using optical infrared-visible SFG. The qualitative and quantitative correlation of optical SFG with infrared absorption and Raman scattering spectroscopies are examined and experimentally demonstrated. We have further investigated the possibility to use transient infrared-visible SFG to probe vibrational transients and ultrafast relaxations on surfaces. 146 refs.

Non-linear optical studies of adsorbates: Spectroscopy and dynamics

International Nuclear Information System (INIS)

Zhu, Xiangdong.

1989-08-01

In the first part of this thesis, we have established a systematic procedure to apply the surface optical second-harmonic generation (SHG) technique to study surface dynamics of adsorbates. In particular, we have developed a novel technique for studies of molecular surface diffusions. In this technique, the laser-induced desorption with two interfering laser beams is used to produce a monolayer grating of adsorbates. The monolayer grating is detected with diffractions of optical SHG. By monitoring the first-order second-harmonic diffraction, we can follow the time evolution of the grating modulation from which we are able to deduce the diffusion constant of the adsorbates on the surface. We have successfully applied this technique to investigate the surface diffusion of CO on Ni(111). The unique advantages of this novel technique will enable us to readily study anisotropy of a surface diffusion with variable grating orientation, and to investigate diffusion processes of a large dynamic range with variable grating spacings. In the second part of this work, we demonstrate that optical infrared-visible sum-frequency generation (SFG) from surfaces can be used as a viable surface vibrational spectroscopic technique. We have successfully recorded the first vibrational spectrum of a monolayer of adsorbates using optical infrared-visible SFG. The qualitative and quantitative correlation of optical SFG with infrared absorption and Raman scattering spectroscopies are examined and experimentally demonstrated. We have further investigated the possibility to use transient infrared-visible SFG to probe vibrational transients and ultrafast relaxations on surfaces. 146 refs

Neutrino mass sum-rule

Science.gov (United States)

Damanik, Asan

2018-03-01

Neutrino mass sum-rele is a very important research subject from theoretical side because neutrino oscillation experiment only gave us two squared-mass differences and three mixing angles. We review neutrino mass sum-rule in literature that have been reported by many authors and discuss its phenomenological implications.

Probing organic field effect transistors in situ during operation using SFG.

Science.gov (United States)

Ye, Hongke; Abu-Akeel, Ashraf; Huang, Jia; Katz, Howard E; Gracias, David H

2006-05-24

In this communication, we report results obtained using surface-sensitive IR+Visible Sum Frequency Generation (SFG) nonlinear optical spectroscopy on interfaces of organic field effect transistors during operation. We observe remarkable correlations between trends in the surface vibrational spectra and electrical properties of the transistor, with changes in gate voltage (VG). These results suggest that field effects on electronic conduction in thin film organic semiconductor devices are correlated to interfacial nonlinear optical characteristics and point to the possibility of using SFG spectroscopy to monitor electronic properties of OFETs.

New Canonic Active RC Sinusoidal Oscillator Circuits Using Second-Generation Current Conveyors with Application as a Wide-Frequency Digitally Controlled Sinusoid Generator

Directory of Open Access Journals (Sweden)

Abhirup Lahiri

2011-01-01

Full Text Available This paper reports two new circuit topologies using second-generation current conveyors (CCIIs for realizing variable frequency sinusoidal oscillators with minimum passive components. The proposed topologies in this paper provide new realizations of resistance-controlled and capacitor-controlled variable frequency oscillators (VFOs using only four passive components. The first topology employs three CCIIs, while the second topology employs two CCIIs. The second topology provides an advantageous feature of frequency tuning through two grounded elements. Application of the proposed circuits as a wide-frequency range digitally controlled sinusoid generator is exhibited wherein the digital frequency control has been enabled by replacing both the capacitors by two identical variable binary capacitor banks tunable by means of the same binary code. SPICE simulations of the CMOS implementation of the oscillators using 0.35 μm TSMC CMOS technology parameters and bipolar implementation of the oscillators using process parameters for NR200N-2X (NPN and PR200N-2X (PNP of bipolar arrays ALA400-CBIC-R have validated their workability. One of the oscillators (with CMOS implementation is exemplified as a digitally controlled sinusoid generator with frequency generation from 25 kHz to 6.36 MHz, achieved by switching capacitors and with power consumption of 7 mW in the entire operating frequency range.

Sums of squares of integers

CERN Document Server

Moreno, Carlos J

2005-01-01

Introduction Prerequisites Outline of Chapters 2 - 8 Elementary Methods Introduction Some Lemmas Two Fundamental Identities Euler's Recurrence for Sigma(n)More Identities Sums of Two Squares Sums of Four Squares Still More Identities Sums of Three Squares An Alternate Method Sums of Polygonal Numbers Exercises Bernoulli Numbers Overview Definition of the Bernoulli Numbers The Euler-MacLaurin Sum Formula The Riemann Zeta Function Signs of Bernoulli Numbers Alternate The von Staudt-Clausen Theorem Congruences of Voronoi and Kummer Irregular Primes Fractional Parts of Bernoulli Numbers Exercises Examples of Modular Forms Introduction An Example of Jacobi and Smith An Example of Ramanujan and Mordell An Example of Wilton: t (n) Modulo 23 An Example of Hamburger Exercises Hecke's Theory of Modular FormsIntroduction Modular Group ? and its Subgroup ? 0 (N) Fundamental Domains For ? and ? 0 (N) Integral Modular Forms Modular Forms of Type Mk(? 0(N);chi) and Euler-Poincare series Hecke Operators Dirichlet Series and ...

Exploring Fluorescent Dyes at Biomimetic Interfaces with Second Harmonic Generation and Molecular Dynamics

Czech Academy of Sciences Publication Activity Database

Licari, G.; Cwiklik, Lukasz; Jungwirth, Pavel; Vauthey, E.

2017-01-01

Roč. 33, č. 14 (2017), s. 3373-3383 ISSN 0743-7463 R&D Projects: GA ČR(CZ) GBP208/12/G016 Institutional support: RVO:61388955 ; RVO:61388963 Keywords : sum-frequency generation * excited-state dynamics * air-water-interface * density-functional theory Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 3.833, year: 2016

Exploring Fluorescent Dyes at Biomimetic Interfaces with Second Harmonic Generation and Molecular Dynamics

Czech Academy of Sciences Publication Activity Database

Licari, G.; Cwiklik, Lukasz; Jungwirth, Pavel; Vauthey, E.

2017-01-01

Roč. 33, č. 14 (2017), s. 3373-3383 ISSN 0743-7463 R&D Projects: GA ČR(CZ) GBP208/12/G016 Institutional support: RVO:61388955 ; RVO:61388963 Keywords : sum -frequency generation * excited-state dynamics * air-water-interface * density-functional theory Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 3.833, year: 2016

RF-field generation in wide frequency range by electron beam

International Nuclear Information System (INIS)

Bogdanovich, B.; Nesterovich, A.; Minaev, S.

1996-01-01

A simple device for generating powerful RF oscillations in the frequency range of 100-250 MHz is considered. The two-gaps cavity is based on the quarter-wavelength coaxial line loaded by drift tubes. Frequency tuning is accomplished by using the movable shorting plunger. A permanent electron beam being modulated at the first gap return the energy at the second one. The additional tube with the permanent decelerating potential, introduced into the main drift tube, allows to decrease the drift tube length and keep the excitation conditions in frequency tuning. Both autogeneration and amplification modes are under consideration. RF-parameters of the cavity and experimental results are described. (author)

Direct Spectroscopy in Hollow Optical with Fiber-Based Optical Frequency Combs

Science.gov (United States)

2015-07-09

scheme is that the generation of carrier-envelope offset frequency f0 can be avoided, which reduces the system complexity . However, a high performance RF...Peterson, "Saturated absorption in acetylene and hydrogen cyanide in hollow-core photonic bandgap fibers," Opt. Express 13, 10475-10482 (2005). 56. C

Sum rules in classical scattering

International Nuclear Information System (INIS)

Bolle, D.; Osborn, T.A.

1981-01-01

This paper derives sum rules associated with the classical scattering of two particles. These sum rules are the analogs of Levinson's theorem in quantum mechanics which provides a relationship between the number of bound-state wavefunctions and the energy integral of the time delay of the scattering process. The associated classical relation is an identity involving classical time delay and an integral over the classical bound-state density. We show that equalities between the Nth-order energy moment of the classical time delay and the Nth-order energy moment of the classical bound-state density hold in both a local and a global form. Local sum rules involve the time delay defined on a finite but otherwise arbitrary coordinate space volume S and the bound-state density associated with this same region. Global sum rules are those that obtain when S is the whole coordinate space. Both the local and global sum rules are derived for potentials of arbitrary shape and for scattering in any space dimension. Finally the set of classical sum rules, together with the known quantum mechanical analogs, are shown to provide a unified method of obtaining the high-temperature expansion of the classical, respectively the quantum-mechanical, virial coefficients

Coherent spectroscopy of a {Lambda} atomic system and its prospective application to tunable frequency offset locking

Energy Technology Data Exchange (ETDEWEB)

Kale, Y B [Laser and Plasma Technology Division, Bhabha Atomic Research Centre, Mumbai 400 085 (India); Ray, Ayan [Radioactive Ion Beam Group, Variable Energy Cyclotron Centre, Kolkata 700064 (India); Lawande, Q V [Theoretical Physics Division, Bhabha Atomic Research Centre, Mumbai 400 085 (India); Jagatap, B N, E-mail: yogeshwar84@rediffmail.com, E-mail: ayan_ray_in@rediffmail.com, E-mail: bnj@barc.gov.in [Atomic and Molecular Physics Division and Homi Bhabha National Institute, Bhabha Atomic Research Centre, Mumbai 400 085 (India)

2011-09-15

We investigate the coherent pump-probe spectroscopy of a three-level {Lambda} system, 6s{sub 1/2}F = 3,4{yields}6p{sub 3/2}F{sup '}= 4, in the hyperfine manifold of D{sub 2} transition (852 nm) of cesium with particular reference to the sub-Doppler linewidth resonance arising from Aulter-Townes (AT) splitting and the possibility of using it for realizing a scheme for tunable atomic frequency offset locking (AFOL). We discuss here the theoretical framework for a {Lambda} system interacting with a coherent pump and probe and use it to describe the process of modulation transfer in the AT and electromagnetically induced transparency regimes. We further employ an experimental scheme consisting of a strong pump and a pair of weak probes to resolve the sub-Doppler linewidth ({approx}8 MHz) AT resonance and study its dependence on pump intensity and detuning. In order to explore the possibility of using such a sub-Doppler linewidth resonance for AFOL, we use its first derivative signal as a frequency discriminator to stabilize the probe laser. The frequency stability of the probe is characterized by means of error signal analysis. This study reveals that while the frequency stability of the AT locked laser is limited by the pump laser, the tuning range of the offset frequency lock can cover the entire Doppler profile and its immediate neighbourhood, thereby providing a simple and cost effective alternative to the external modulator. The study described in this paper contributes to the discussion on the subtle link between dressed state spectroscopy and AFOL, which is relevant for developing a master-slave-type laser system in the domain of coherent photon-atom interaction.

Consensus structures of the Mo(v) sites of sulfite-oxidizing enzymes derived from variable frequency pulsed EPR spectroscopy, isotopic labelling and DFT calculations.

Science.gov (United States)

Enemark, John H

2017-10-10

Sulfite-oxidizing enzymes from eukaryotes and prokaryotes have five-coordinate distorted square-pyramidal coordination about the molybdenum atom. The paramagnetic Mo(v) state is easily generated, and over the years four distinct CW EPR spectra have been identified, depending upon enzyme source and the reaction conditions, namely high and low pH (hpH and lpH), phosphate inhibited (P i ) and sulfite (or blocked). Extensive studies of these paramagnetic forms of sulfite-oxidizing enzymes using variable frequency pulsed electron spin echo (ESE) spectroscopy, isotopic labeling and density functional theory (DFT) calculations have led to the consensus structures that are described here. Errors in some of the previously proposed structures are corrected.

Laser Materials and Laser Spectroscopy - A Satellite Meeting of IQEC '88

Science.gov (United States)

Wang, Zhijiang; Zhang, Zhiming

1989-03-01

Ionization-fragmentation Patterns of Ethylamine and Dimethylamine Isomers * Cars Measurements of SF6 Pumped by a CO2 Laser Pulse * Angular Dependence of Phase Conjugation of CO2 Laser on SF6 Gas * Resolution of Stretching-vibrational and Translational Raman Bands of Liquid Water by Means of Polarization Four-photon Spectroscopy * Laser-produced Plasma as an Effective Source for X-Ray Spectroscopy * Rotational Structure of the Low Lying Electronic States of Samarium Monoxide * Effects of Poling and Stretching on Second-harmonic Generation in Amorphous Vinylidene Cyanide/Vinyl Acetate Copolymer * Laser-induced Spectroscopy of Cardiovascular Tissues * Laser-excited Malignancy Autofluorescence for Tumour Malignancy Investigation and its Origin * A Study on Several Hematoporphyrin Derivatives by Time-resolved Spectroscopy * Research on Strong Field Processes with a Subpicosecond 400 GW Ultraviolet Source * Growth, Decay and Quenching of Stimulated Raman Scattering in Transparent Liquid Droplets * Layer Condensed Ammonia Studied by Photoacoustic Spectroscopy * High Efficiency Raman Conversion of XeCl Laser Radiation in Lead Vapor * Combined Effect of Stimulated Scattering and Phase Modulation on Generation of Supercontinum * Resonant Multiwave Mixing in Sodium Vapor * High Pressure Brillouin Scattering in Liquid Toluene * Optical Nonlinearities and Bistability in Gold Colloid * Sum-frequency Generation for Surface Vibrational Spectroscopy * Optical Studies of Molecule/Surface Interactions * Optical Second Harmonic Generation with Coupled Surface Plasmons from a Multi-layer Silver/Quartz Grating * Evidence of Silver Cluster and its Role in Surface Enhanced Raman Scattering (SERS) * Study on Cold-evaporated Silver Surfaces with Second-harmonic-generation * Study of Optical Second-harmonic-generation at Metal Surface with Polarization States * Spectroscopic Studies of J-Aggregates of Pseudoisocyanine in Molecular Monolayers in the Range 300 to 20 K * Study of Polymerization of

Counting Triangles to Sum Squares

Science.gov (United States)

DeMaio, Joe

2012-01-01

Counting complete subgraphs of three vertices in complete graphs, yields combinatorial arguments for identities for sums of squares of integers, odd integers, even integers and sums of the triangular numbers.

Cosmic Sum Rules

DEFF Research Database (Denmark)

T. Frandsen, Mads; Masina, Isabella; Sannino, Francesco

2011-01-01

We introduce new sum rules allowing to determine universal properties of the unknown component of the cosmic rays and show how it can be used to predict the positron fraction at energies not yet explored by current experiments and to constrain specific models.......We introduce new sum rules allowing to determine universal properties of the unknown component of the cosmic rays and show how it can be used to predict the positron fraction at energies not yet explored by current experiments and to constrain specific models....

Self-consistent modeling of radio-frequency plasma generation in stellarators

Energy Technology Data Exchange (ETDEWEB)

Moiseenko, V. E., E-mail: moiseenk@ipp.kharkov.ua; Stadnik, Yu. S., E-mail: stadnikys@kipt.kharkov.ua [National Academy of Sciences of Ukraine, National Science Center Kharkov Institute of Physics and Technology (Ukraine); Lysoivan, A. I., E-mail: a.lyssoivan@fz-juelich.de [Royal Military Academy, EURATOM-Belgian State Association, Laboratory for Plasma Physics (Belgium); Korovin, V. B. [National Academy of Sciences of Ukraine, National Science Center Kharkov Institute of Physics and Technology (Ukraine)

2013-11-15

A self-consistent model of radio-frequency (RF) plasma generation in stellarators in the ion cyclotron frequency range is described. The model includes equations for the particle and energy balance and boundary conditions for Maxwell’s equations. The equation of charged particle balance takes into account the influx of particles due to ionization and their loss via diffusion and convection. The equation of electron energy balance takes into account the RF heating power source, as well as energy losses due to the excitation and electron-impact ionization of gas atoms, energy exchange via Coulomb collisions, and plasma heat conduction. The deposited RF power is calculated by solving the boundary problem for Maxwell’s equations. When describing the dissipation of the energy of the RF field, collisional absorption and Landau damping are taken into account. At each time step, Maxwell’s equations are solved for the current profiles of the plasma density and plasma temperature. The calculations are performed for a cylindrical plasma. The plasma is assumed to be axisymmetric and homogeneous along the plasma column. The system of balance equations is solved using the Crank-Nicholson scheme. Maxwell’s equations are solved in a one-dimensional approximation by using the Fourier transformation along the azimuthal and longitudinal coordinates. Results of simulations of RF plasma generation in the Uragan-2M stellarator by using a frame antenna operating at frequencies lower than the ion cyclotron frequency are presented. The calculations show that the slow wave generated by the antenna is efficiently absorbed at the periphery of the plasma column, due to which only a small fraction of the input power reaches the confinement region. As a result, the temperature on the axis of the plasma column remains low, whereas at the periphery it is substantially higher. This leads to strong absorption of the RF field at the periphery via the Landau mechanism.

Laser excitation of SF6: spectroscopy and coherent pulse propagation effects

International Nuclear Information System (INIS)

Cantrell, C.D.; Makarov, A.A.; Louisell, W.H.

1978-01-01

Recent theoretical studies of coherent propagation effects in SF 6 and other polyatomic molecules are summarized beginning with an account of relevant aspects of the high-resolution spectroscopy of the ν 3 band of SF 6 . A laser pulse propagating in a molecular gas can acquire new frequencies which were not initially present in the pulse, and, in fact, a wave is coherently generated at the frequency of every molecular transition accessible from the initial molecular energy levels. The possible consequences of coherent generation of sidebands for the multiple-photon excitation of SF 6 and other polyatomic molecules are discussed

Second harmonic generation spectroscopy on Si surfaces and interfaces

DEFF Research Database (Denmark)

Pedersen, Kjeld

2010-01-01

Optical second harmonic generation (SHG) spectroscopy studies of Si(111) surfaces and interfaces are reviewed for two types of systems: (1) clean 7 x 7 and root 3 x root 3-Ag reconstructed surfaces prepared under ultra-high vacuum conditions where surface states are excited and (2) interfaces...... in silicon-on-insulator (SOI) structures and thin metal films on Si surfaces where several interfaces contribute to the SHG. In all the systems resonances are seen at interband transitions near the bulk critical points E-1 and E-2. On the clean surfaces a number of resonances appear below the onset of bulk...

IR and SFG vibrational spectroscopy of the water bend in the bulk liquid and at the liquid-vapor interface, respectively

Energy Technology Data Exchange (ETDEWEB)

Ni, Yicun; Skinner, J. L. [Theoretical Chemistry Institute and Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706 (United States)

2015-07-07

Vibrational spectroscopy of the water bending mode has been investigated experimentally to study the structure of water in condensed phases. In the present work, we calculate the theoretical infrared (IR) and sum-frequency generation (SFG) spectra of the HOH bend in liquid water and at the water liquid/vapor interface using a mixed quantum/classical approach. Classical molecular dynamics simulation is performed by using a recently developed water model that explicitly includes three-body interactions and yields a better description of the water surface. Ab-initio-based transition frequency, dipole, polarizability, and intermolecular coupling maps are developed for the spectral calculations. The calculated IR and SFG spectra show good agreement with the experimental measurements. In the theoretical imaginary part of the SFG susceptibility for the water liquid/vapor interface, we find two features: a negative band centered at 1615 cm{sup −1} and a positive band centered at 1670 cm{sup −1}. We analyze this spectrum in terms of the contributions from molecules in different hydrogen-bond classes to the SFG spectral density and also compare to SFG results for the OH stretch. SFG of the water bending mode provides a complementary picture of the heterogeneous hydrogen-bond configurations at the water surface.

IR and SFG vibrational spectroscopy of the water bend in the bulk liquid and at the liquid-vapor interface, respectively

Science.gov (United States)

Ni, Yicun; Skinner, J. L.

2015-07-01

Vibrational spectroscopy of the water bending mode has been investigated experimentally to study the structure of water in condensed phases. In the present work, we calculate the theoretical infrared (IR) and sum-frequency generation (SFG) spectra of the HOH bend in liquid water and at the water liquid/vapor interface using a mixed quantum/classical approach. Classical molecular dynamics simulation is performed by using a recently developed water model that explicitly includes three-body interactions and yields a better description of the water surface. Ab-initio-based transition frequency, dipole, polarizability, and intermolecular coupling maps are developed for the spectral calculations. The calculated IR and SFG spectra show good agreement with the experimental measurements. In the theoretical imaginary part of the SFG susceptibility for the water liquid/vapor interface, we find two features: a negative band centered at 1615 cm-1 and a positive band centered at 1670 cm-1. We analyze this spectrum in terms of the contributions from molecules in different hydrogen-bond classes to the SFG spectral density and also compare to SFG results for the OH stretch. SFG of the water bending mode provides a complementary picture of the heterogeneous hydrogen-bond configurations at the water surface.

Frequency Control Strategy for Black Starts via PMSG-Based Wind Power Generation

Directory of Open Access Journals (Sweden)

Yi Tang

2017-03-01

Full Text Available The use of wind power generation (WPG as a source for black starts will significantly enhance the resiliency of power systems and shorten their recovery time from blackouts. Given that frequency stability is the most serious issue during the initial recovery period, virtual inertia control can enable wind turbines to provide frequency support to an external system. In this study, a general procedure of WPG participating in black starts is presented, and the key issues are discussed. The adaptability of existing virtual inertia control strategies is analyzed, and improvement work is performed. A new coordinated frequency control strategy is proposed based on the presented improvement work. A local power network with a permanent-magnet synchronous generator (PMSG-based wind farm is modeled and used to verify the effectiveness of the strategy.

Observational study of generation conditions of substorm-associated low-frequency AKR emissions

Directory of Open Access Journals (Sweden)

A. Olsson

2004-11-01

Full Text Available It has lately been shown that low-frequency bursts of auroral kilometric radiation (AKR are nearly exclusively associated with substorm expansion phases. Here we study low-frequency AKR using Polar PWI and Interball POLRAD instruments to constrain its possible generation mechanisms. We find that there are more low-frequency AKR emission events during wintertime and equinoxes than during summertime. The dot-AKR emission radial distance range coincides well with the region where the deepest density cavities are seen statistically during Kp>2. We suggest that the dot-AKR emissions originate in the deepest density cavities during substorm onsets. The mechanism for generating dot-AKR is possibly strong Alfvén waves entering the cavity from the magnetosphere and changing their character to more inertial, which causes the Alfvén wave associated parallel electric field to increase. This field may locally accelerate electrons inside the cavity enough to produce low-frequency AKR emission. We use Interball IESP low-frequency wave data to verify that in about half of the cases the dot-AKR is accompanied by low-frequency wave activity containing a magnetic component, i.e. probably inertial Alfvén waves. Because of the observational geometry, this result is consistent with the idea that inertial Alfvén waves might always be present in the source region when dot-AKR is generated. The paper illustrates once more the importance of radio emissions as a powerful remote diagnostic tool of auroral processes, which is not only relevant for the Earth's magnetosphere but may be relevant in the future in studying extrasolar planets.

High-precision and low-cost vibration generator for low-frequency calibration system

Science.gov (United States)

Li, Rui-Jun; Lei, Ying-Jun; Zhang, Lian-Sheng; Chang, Zhen-Xin; Fan, Kuang-Chao; Cheng, Zhen-Ying; Hu, Peng-Hao

2018-03-01

Low-frequency vibration is one of the harmful factors that affect the accuracy of micro-/nano-measuring machines because its amplitude is significantly small and it is very difficult to avoid. In this paper, a low-cost and high-precision vibration generator was developed to calibrate an optical accelerometer, which is self-designed to detect low-frequency vibration. A piezoelectric actuator is used as vibration exciter, a leaf spring made of beryllium copper is used as an elastic component, and a high-resolution, low-thermal-drift eddy current sensor is applied to investigate the vibrator’s performance. Experimental results demonstrate that the vibration generator can achieve steady output displacement with frequency range from 0.6 Hz to 50 Hz, an analytical displacement resolution of 3.1 nm and an acceleration range from 3.72 mm s-2 to 1935.41 mm s-2 with a relative standard deviation less than 1.79%. The effectiveness of the high-precision and low-cost vibration generator was verified by calibrating our optical accelerometer.

Electrochemical impedance spectroscopy of supercapacitors: A novel analysis approach using evolutionary programming

Science.gov (United States)

Oz, Alon; Hershkovitz, Shany; Tsur, Yoed

2014-11-01

In this contribution we present a novel approach to analyze impedance spectroscopy measurements of supercapacitors. Transforming the impedance data into frequency-dependent capacitance allows us to use Impedance Spectroscopy Genetic Programming (ISGP) in order to find the distribution function of relaxation times (DFRT) of the processes taking place in the tested device. Synthetic data was generated in order to demonstrate this technique and a model for supercapacitor ageing process has been obtained.

Online frequency estimation with applications to engine and generator sets

Science.gov (United States)

Manngård, Mikael; Böling, Jari M.

2017-07-01

Frequency and spectral analysis based on the discrete Fourier transform is a fundamental task in signal processing and machine diagnostics. This paper aims at presenting computationally efficient methods for real-time estimation of stationary and time-varying frequency components in signals. A brief survey of the sliding time window discrete Fourier transform and Goertzel filter is presented, and two filter banks consisting of: (i) sliding time window Goertzel filters (ii) infinite impulse response narrow bandpass filters are proposed for estimating instantaneous frequencies. The proposed methods show excellent results on both simulation studies and on a case study using angular speed data measurements of the crankshaft of a marine diesel engine-generator set.

Generation of artificial time-histories, rich in all frequencies, from given response spectra

International Nuclear Information System (INIS)

Levy, S.; Wilkinson, J.P.D.

1975-01-01

In order to apply the time-history method of seismic analysis, it is often desirable to generate a suitable artificial time-history from a given response spectrum. The method described allows the generation of such a time-history that is also rich in all frequencies in the spectrum. This richness is achieved by choosing a large number of closely-spaced frequency points such that the adjacent frequencies have their half-power points overlap. The adjacent frequencies satisfy the condition that the frequency interval Δf near a given frequency f is such that (Δf)/f<2c/csub(c) where c is the damping of the system and csub(c) is the critical damping. In developing an artificial time-history, it is desirable to specify the envelope and duration of the record, very often in such a manner as to reproduce the envelope property of a specific earthquake record, and such an option is available in the method described. Examples are given of the development of typical artificial time-histories from earthquake design response spectra and from floor response spectra

A Novel Noncircular MUSIC Algorithm Based on the Concept of the Difference and Sum Coarray.

Science.gov (United States)

Chen, Zhenhong; Ding, Yingtao; Ren, Shiwei; Chen, Zhiming

2018-01-25

In this paper, we propose a vectorized noncircular MUSIC (VNCM) algorithm based on the concept of the coarray, which can construct the difference and sum (diff-sum) coarray, for direction finding of the noncircular (NC) quasi-stationary sources. Utilizing both the NC property and the concept of the Khatri-Rao product, the proposed method can be applied to not only the ULA but also sparse arrays. In addition, we utilize the quasi-stationary characteristic instead of the spatial smoothing method to solve the coherent issue generated by the Khatri-Rao product operation so that the available degree of freedom (DOF) of the constructed virtual array will not be reduced by half. Compared with the traditional NC virtual array obtained in the NC MUSIC method, the diff-sum coarray achieves a higher number of DOFs as it comprises both the difference set and the sum set. Due to the complementarity between the difference set and the sum set for the coprime array, we choose the coprime array with multiperiod subarrays (CAMpS) as the array model and summarize the properties of the corresponding diff-sum coarray. Furthermore, we develop a diff-sum coprime array with multiperiod subarrays (DsCAMpS) whose diff-sum coarray has a higher DOF. Simulation results validate the effectiveness of the proposed method and the high DOF of the diff-sum coarray.

A Novel Noncircular MUSIC Algorithm Based on the Concept of the Difference and Sum Coarray

Science.gov (United States)

Chen, Zhenhong; Ding, Yingtao; Chen, Zhiming

2018-01-01

In this paper, we propose a vectorized noncircular MUSIC (VNCM) algorithm based on the concept of the coarray, which can construct the difference and sum (diff–sum) coarray, for direction finding of the noncircular (NC) quasi-stationary sources. Utilizing both the NC property and the concept of the Khatri–Rao product, the proposed method can be applied to not only the ULA but also sparse arrays. In addition, we utilize the quasi-stationary characteristic instead of the spatial smoothing method to solve the coherent issue generated by the Khatri–Rao product operation so that the available degree of freedom (DOF) of the constructed virtual array will not be reduced by half. Compared with the traditional NC virtual array obtained in the NC MUSIC method, the diff–sum coarray achieves a higher number of DOFs as it comprises both the difference set and the sum set. Due to the complementarity between the difference set and the sum set for the coprime array, we choose the coprime array with multiperiod subarrays (CAMpS) as the array model and summarize the properties of the corresponding diff–sum coarray. Furthermore, we develop a diff–sum coprime array with multiperiod subarrays (DsCAMpS) whose diff–sum coarray has a higher DOF. Simulation results validate the effectiveness of the proposed method and the high DOF of the diff–sum coarray. PMID:29370138

A Novel Noncircular MUSIC Algorithm Based on the Concept of the Difference and Sum Coarray

Directory of Open Access Journals (Sweden)

Zhenhong Chen

2018-01-01

Full Text Available In this paper, we propose a vectorized noncircular MUSIC (VNCM algorithm based on the concept of the coarray, which can construct the difference and sum (diff–sum coarray, for direction finding of the noncircular (NC quasi-stationary sources. Utilizing both the NC property and the concept of the Khatri–Rao product, the proposed method can be applied to not only the ULA but also sparse arrays. In addition, we utilize the quasi-stationary characteristic instead of the spatial smoothing method to solve the coherent issue generated by the Khatri–Rao product operation so that the available degree of freedom (DOF of the constructed virtual array will not be reduced by half. Compared with the traditional NC virtual array obtained in the NC MUSIC method, the diff–sum coarray achieves a higher number of DOFs as it comprises both the difference set and the sum set. Due to the complementarity between the difference set and the sum set for the coprime array, we choose the coprime array with multiperiod subarrays (CAMpS as the array model and summarize the properties of the corresponding diff–sum coarray. Furthermore, we develop a diff–sum coprime array with multiperiod subarrays (DsCAMpS whose diff–sum coarray has a higher DOF. Simulation results validate the effectiveness of the proposed method and the high DOF of the diff–sum coarray.

DEVELOPMENT OF NEXT-GENERATION DETECTORS AND INSTRUMENTATION FOR PHOTOELECTRON SPECTROSCOPY, DIFFRACTION AND HOLOGRAPHY

International Nuclear Information System (INIS)

Charles S. Fadley, Principal Investigator

2005-01-01

We have developed a new multichannel detector for use in photoelectron spectroscopy (as well as other types of high-count-rate spectroscopy) that will operate at rates of up to 1 GHz. Such detectors are crucial to the full utilization of the high-brightness radiation generated by third-generation synchrotron radiation sources. In addition, new software and hardware has been developed to permit rapidly and accurately scanning photoelectron spectra that will be accumulated in as little as a 200 micros. A versatile next-generation sample goniometer permitting equally rapid scanning of specimen angles or photon energies for angle-resolved photoemission studies, photoelectron diffraction, and photoelectron holography measurements, and cooling to below 10K has also been designed and constructed. These capabilities have been incorporated into a unique photoelectron spectrometer/diffractometer at the Advanced Light Source of the Lawrence Berkeley National Laboratory; this experimental system includes ultrahigh energy resolution, in situ rotation, variable polarization, and optional spin detection. This overall system is now being used in studies of a variety of problems including magnetic metals and oxides; metal/metal, metal/metal oxide, and metal-oxide/metal-oxide multilayers; and systems exhibiting giant and colossal magnetoresistance

Orientational analysis of dodecanethiol and p-nitrothiophenol SAMs on metals with polarisation-dependent SFG spectroscopy.

Science.gov (United States)

Cecchet, Francesca; Lis, Dan; Guthmuller, Julien; Champagne, Benoît; Caudano, Yves; Silien, Christophe; Mani, Alaa Addin; Thiry, Paul A; Peremans, André

2010-02-22

Polarisation-dependent sum frequency generation (SFG) spectroscopy is used to investigate the orientation of molecules on metallic surfaces. In particular, self-assembled monolayers (SAMs) of dodecanethiol (DDT) and of p-nitrothiophenol (p-NTP), grown on Pt and on Au, have been chosen as models to highlight the ability of combining ppp and ssp polarisations sets (representing the polarisation of the involved beams in the conventional order of SFG, Vis and IR beam) to infer orientational information at metallic interfaces. Indeed, using only the ppp set of data, as it is usually done for metallic surfaces, is not sufficient to determine the full molecular orientation. We show here that simply combining ppp and ssp polarisations enables both the tilt and rotation angles of methyl groups in DDT SAMs to be determined. Moreover, for p-NTP, while the SFG active vibrations detected with the ppp polarisation alone provide no orientational information, however, the combination with ssp spectra enables to retrieve the tilt angle of the p-NTP 1,4 axis. Though orientational information obtained by polarisation-dependent measurements has been extensively used at insulating interfaces, we report here their first application to metallic surfaces.

Orientational Analysis of Dodecanethiol and P-Nitrothiophenol SAMs on Metals with Polarisation - dependent SFG spectroscopy

International Nuclear Information System (INIS)

Manea, A.

2011-01-01

Polarisation-dependent sum frequency generation (SFG) spectroscopy is used to investigate the orientation of molecules on metallic surfaces. In particular, self-assembled monolayers (SAMs) of dodecanethiol (DDT) and of p-nitro thiophenol (p-NTP), grown on Pt and on Au, have been chosen as models to highlight the ability of combining ppp and ssp polarizations sets (representing the polarisation of the involved beams in the conventional order of SFG, Vis and IR beam) to infer orientational information at metallic interfaces. Indeed, using only the ppp set of data, as it is usually done for metallic surfaces, is not sufficient to determine the full molecular orientation. We show here that simply combining ppp and ssp polarizations enables both the tilt and rotation angles of methyl groups in DDT SAMs to be determined. Moreover, for p-NTP, while the SFG active vibrations detected with the ppp polarisation alone provide no orientational information, however, the combination with ssp spectra enables to retrieve the tilt angle of the p-NTP 1,4 axis. Though orientational information obtained by polarisation-dependent measurements has been extensively used at insulating interfaces, we report here their first application to metallic surfaces. (author)

Method of detecting system function by measuring frequency response

Science.gov (United States)

Morrison, John L.; Morrison, William H.; Christophersen, Jon P.; Motloch, Chester G.

2013-01-08

Methods of rapidly measuring an impedance spectrum of an energy storage device in-situ over a limited number of logarithmically distributed frequencies are described. An energy storage device is excited with a known input signal, and a response is measured to ascertain the impedance spectrum. An excitation signal is a limited time duration sum-of-sines consisting of a select number of frequencies. In one embodiment, magnitude and phase of each frequency of interest within the sum-of-sines is identified when the selected frequencies and sample rate are logarithmic integer steps greater than two. This technique requires a measurement with a duration of one period of the lowest frequency. In another embodiment, where selected frequencies are distributed in octave steps, the impedance spectrum can be determined using a captured time record that is reduced to a half-period of the lowest frequency.

K2 photometry and HERMES spectroscopy of the blue supergiant ρ Leo: rotational wind modulation and low-frequency waves

Science.gov (United States)

Aerts, C.; Bowman, D. M.; Símon-Díaz, S.; Buysschaert, B.; Johnston, C.; Moravveji, E.; Beck, P. G.; De Cat, P.; Triana, S.; Aigrain, S.; Castro, N.; Huber, D.; White, T.

2018-05-01

We present an 80-d long uninterrupted high-cadence K2 light curve of the B1Iab supergiant ρ Leo (HD 91316), deduced with the method of halo photometry. This light curve reveals a dominant frequency of frot = 0.0373 d-1 and its harmonics. This dominant frequency corresponds with a rotation period of 26.8 d and is subject to amplitude and phase modulation. The K2 photometry additionally reveals multiperiodic low-frequency variability (<1.5 d-1) and is in full agreement with low-cadence high-resolution spectroscopy assembled during 1800 d. The spectroscopy reveals rotational modulation by a dynamic aspherical wind with an amplitude of about 20 km s-1 in the H α line, as well as photospheric velocity variations of a few km s-1 at frequencies in the range 0.2-0.6 d-1 in the Si III 4567 Å line. Given the large macroturbulence needed to explain the spectral line broadening of the star, we interpret the detected photospheric velocity as due to travelling superinertial low-degree large-scale gravity waves with dominant tangential amplitudes and discuss why ρ Leo is an excellent target to study how the observed photospheric variability propagates into the wind.

Role of Confined Water in Underwater Adhesion

Science.gov (United States)

Dhinojwala, Ali

Surface bound water is a strong deterrent for forming strong bonds between two surfaces underwater and expelling that bound water is important for strong adhesion. I will discuss examples of different strategies used by geckos, spiders, and mussels to handle this last layer of bound water. Recent results using infrared-visible sum frequency generation spectroscopy to probe the structure of this bound water will be discussed. National Science Foundation.

Generation of ultra-wide and flat optical frequency comb based on electro absorption modulator

Science.gov (United States)

Ujjwal; Thangaraj, Jaisingh

2018-05-01

A novel technique is proposed for the generation of ultra-wide and flat optical frequency comb (OFC) based on serially cascading three stages of electro absorption modulators (EAMs) through sinusoidal radio frequency (RF) signals by setting frequencies at f GHz, f/2 GHz and f/4 GHz. Here, the first stage acts as subcarrier generator, the second stage acts as subcarrier doubler, and the third stage acts as subcarrier quadrupler. In addition, a higher number of subcarriers can easily be generated by adjusting the driving sinusoidal RF signal. In this paper, cascading three stages of EAMs driven by 50 GHz, 25 GHz and 12.5 GHz clock sources, we obtain 272 subcarriers with spacing of 2.5 GHz and power deviation within 1 dB. Theoretical analysis of serially cascaded EAMs for subcarrier generation is also investigated. Principal analysis and simulation of this technique are demonstrated.

An efficient continuous-wave 591 nm light source based on sum-frequency mixing of a diode pumped Nd:GdVO4–Nd:CNGG laser

International Nuclear Information System (INIS)

Zhao, Y D; Liu, J H

2013-01-01

We report a laser architecture to obtain continuous-wave (CW) yellow-orange light sources at the 591 nm wavelength. An 808 nm diode pumped a Nd:GdVO 4 crystal emitting at 1063 nm. A part of the pump power was then absorbed by the Nd:CNGG crystal. The remaining pump power was used to pump a Nd:CNGG crystal emitting at 1329 nm. Intracavity sum-frequency mixing at 1063 and 1329 nm was then realized in a LiB 3 O 5 (LBO) crystal to reach the yellow-orange radiation. We obtained a CW output power of 494 mW at 591 nm with a pump laser diode emitting 17.8 W at 808 nm. (paper)

Decompounding random sums: A nonparametric approach

DEFF Research Database (Denmark)

Hansen, Martin Bøgsted; Pitts, Susan M.

Observations from sums of random variables with a random number of summands, known as random, compound or stopped sums arise within many areas of engineering and science. Quite often it is desirable to infer properties of the distribution of the terms in the random sum. In the present paper we...... review a number of applications and consider the nonlinear inverse problem of inferring the cumulative distribution function of the components in the random sum. We review the existing literature on non-parametric approaches to the problem. The models amenable to the analysis are generalized considerably...

Absolute frequency atlas from 915 nm to 985 nm based on laser absorption spectroscopy of iodine

Science.gov (United States)

Nölleke, Christian; Raab, Christoph; Neuhaus, Rudolf; Falke, Stephan

2018-04-01

This article reports on laser absorption spectroscopy of iodine gas between 915 nm and 985 nm. This wavelength range is scanned utilizing a narrow linewidth and mode-hop-free tunable diode-laser whose frequency is actively controlled using a calibrated wavelength meter. This allows us to provide an iodine atlas that contains almost 10,000 experimentally observed reference lines with an uncertainty of 50 MHz. For common lines, good agreement is found with a publication by Gerstenkorn and Luc (1978). The new rich dataset allows existing models of the iodine molecule to be refined and can serve as a reference for laser frequency calibration and stabilization.

Generation and control of optical frequency combs using cavity electromagnetically induced transparency

Science.gov (United States)

Li, Jiahua; Qu, Ye; Yu, Rong; Wu, Ying

2018-02-01

We explore theoretically the generation and all-optical control of optical frequency combs (OFCs) in photon transmission based on a combination of single-atom-cavity quantum electrodynamics (CQED) and electromagnetically induced transparency (EIT). Here an external control field is used to form the cavity dark mode of the CQED system. When the strengths of the applied EIT control field are appropriately tuned, enhanced comb generation can be achieved. We discuss the properties of the dark mode and clearly show that the formation of the dark mode enables the efficient generation of OFCs. In our approach, the comb spacing is determined by the beating frequency between the driving pump and seed lasers. Our demonstrated theory may pave the way towards all-optical coherent control of OFCs using a CQED architecture.

Prediction of power system frequency response after generator outages using neural nets

Energy Technology Data Exchange (ETDEWEB)

Djukanovic, M B; Popovic, D P [Electrotechnicki Inst. ' Nikola Tesla' , Belgrade (Yugoslavia); Sobajic, D J; Pao, Y -H [Case Western Reserve Univ., Cleveland, OH (United States)

1993-09-01

A new methodology is presented for estimating the frequency behaviour of power systems necessary for an indication of under-frequency load shedding in steady-state security assessment. It is well known that large structural disturbances such as generator tripping or load outages can initiate cascading outages, system separation into islands, and even the complete breakup. The approach provides a fairly accurate method of estimating the system average frequency response without making simplifications or neglecting non-linearities and small time constants in the equations of generating units, voltage regulators and turbines. The efficiency of the new procedure is demonstrated using the New England power system model for a series of characteristic perturbations. The validity of the proposed approach is verified by comparison with the simulation of short-term dynamics including effects of control and automatic devices. (author)

Momentum sum rules for fragmentation functions

International Nuclear Information System (INIS)

Meissner, S.; Metz, A.; Pitonyak, D.

2010-01-01

Momentum sum rules for fragmentation functions are considered. In particular, we give a general proof of the Schaefer-Teryaev sum rule for the transverse momentum dependent Collins function. We also argue that corresponding sum rules for related fragmentation functions do not exist. Our model-independent analysis is supplemented by calculations in a simple field-theoretical model.

Multiparty symmetric sum types

DEFF Research Database (Denmark)

Nielsen, Lasse; Yoshida, Nobuko; Honda, Kohei

2010-01-01

This paper introduces a new theory of multiparty session types based on symmetric sum types, by which we can type non-deterministic orchestration choice behaviours. While the original branching type in session types can represent a choice made by a single participant and accepted by others...... determining how the session proceeds, the symmetric sum type represents a choice made by agreement among all the participants of a session. Such behaviour can be found in many practical systems, including collaborative workflow in healthcare systems for clinical practice guidelines (CPGs). Processes...... with the symmetric sums can be embedded into the original branching types using conductor processes. We show that this type-driven embedding preserves typability, satisfies semantic soundness and completeness, and meets the encodability criteria adapted to the typed setting. The theory leads to an efficient...

Current algebra sum rules for Reggeons

CERN Document Server

Carlitz, R

1972-01-01

The interplay between the constraints of chiral SU/sub 2/*SU/sub 2/ symmetry and Regge asymptotic behaviour is investigated. The author reviews the derivation of various current algebra sum rules in a study of the reaction pi + alpha to pi + beta . These sum rules imply that all particles may be classified in multiplets of SU/sub 2/*SU/sub 2/ and that each of these multiplets may contain linear combinations of an infinite number of physical states. Extending his study to the reaction pi + alpha to pi + pi + beta , he derives new sum rules involving commutators of the axial charge with the reggeon coupling matrices of the rho and f Regge trajectories. Some applications of these new sum rules are noted, and the general utility of these and related sum rules is discussed. (17 refs).

A Frequency Matching Method for Generation of a Priori Sample Models from Training Images

DEFF Research Database (Denmark)

Lange, Katrine; Cordua, Knud Skou; Frydendall, Jan

2011-01-01

This paper presents a Frequency Matching Method (FMM) for generation of a priori sample models based on training images and illustrates its use by an example. In geostatistics, training images are used to represent a priori knowledge or expectations of models, and the FMM can be used to generate...... new images that share the same multi-point statistics as a given training image. The FMM proceeds by iteratively updating voxel values of an image until the frequency of patterns in the image matches the frequency of patterns in the training image; making the resulting image statistically...... indistinguishable from the training image....

Bi-resonant structure with piezoelectric PVDF films for energy harvesting from random vibration sources at low frequency

DEFF Research Database (Denmark)

Liang, Shanshan; Crovetto, Andrea; Peng, Zhuoteng

2016-01-01

and experiments with piezoelectric elements show that the energy harvesting device with the bi-resonant structure can generate higher power output than that of the sum of the two separate devices from random vibration sources at low frequency, and hence significantly improves the vibration-to- electricity......This paper reports on a bi-resonant structure of piezoelectric PVDF films energy harvester (PPEH), which consists of two cantilevers with resonant frequencies of 15 Hz and 22 Hz. With increased acceleration, the vibration amplitudes of the two cantilever-mass structures are increased and collision...

Generation of artificial time-histories, rich in all frequencies from given response spectra

International Nuclear Information System (INIS)

Levy, S.; Wilkinson, J.P.D.

1975-01-01

In order to apply the time-history method of seismic analysis, it is often desirable to generate a suitable artificial time-history from a given response spectrum. The method described in this paper allows the generation of such a time-history that is also rich in all frequencies in the spectrum. This richness is achieved by choosing a large number of closely-spaced frequency points such that the adjacent frequencies have their half-power points overlap. The adjacent frequencies satisfy the condition that the frequency interval Δf near a given frequency f is such that (Δf)/f<2c/csub(c) where c is the damping of the system and csub(c) is the critical damping. In developing an artificial time-history, it is desirable to specify the envelope and duration of the record, very often in such a manner as to reproduce the envelope property of a specific earthquake record, and such an option is available in the method described. Examples are given of the development of typical articifial time-histories from earthquake design response spectra and from floor response spectra. (Auth.)

Distributed Generation Integration in the Electric Grid: Energy Storage System for Frequency Control

Directory of Open Access Journals (Sweden)

Maurizio Delfanti

2014-01-01

Full Text Available During the last few years generation from renewable energy sources (RESs has grown considerably in European electrical networks. Transmission system operators are greatly concerned about the impact of RESs on the operational security and efficiency of their networks and more in general of the ENTSO-E interconnected system. Grid codes are to be revised in order to harmonise the rules regarding the connection of RES power plants. A main issue concerns frequency control: frequency is greatly affected by RESs intermittency and its deviations must be limited as much as possible in order to guarantee a suitable level of power quality. To improve frequency stability, in the future, Grid codes could extend frequency control requirements also to RES units, whereas today they are applied only to conventional power plants. Energy storage systems can be a possible solution to increase the flexibility and performance of RES power plants: they allow generators to modulate their power injections without wasting renewable energy. In this paper, the authors studied the suitability of extending frequency control to RES units integrating them with energy storage systems. In particular, the paper focuses on the impact of frequency control on the storage lifetime by analysing the power charge/discharge in response to real frequency oscillations.

Vibrational correlation between conjugated carbonyl and diazo modes studied by single- and dual-frequency two-dimensional infrared spectroscopy

Science.gov (United States)

Maekawa, Hiroaki; Sul, Soohwan; Ge, Nien-Hui

2013-08-01

We have applied infrared three-pulse photon echo and single- and dual-frequency 2D IR spectroscopy to the ester Cdbnd O and diazo Ndbnd N stretching modes in ethyl diazoacetate (EDA), and investigated their vibrational frequency fluctuations and correlation. The two modes exhibit different vibrational dynamics and 2D lineshape, which are well simulated by frequency-frequency correlation functions (FFCFs) with two decaying components. Although the FT IR spectrum shows a single Cdbnd O band, absolute magnitude 2D IR nonrephasing spectrum displays spectral signatures supporting the presence of cis and trans conformations. The cross-peak inclined toward the anti-diagonal in the dual-frequency 2D IR spectrum, indicating that the frequency fluctuations of the two modes are anticorrelated. This behavior is attributed to anticorrelated change in the bond orders when solvent and structural fluctuations causes EDA to adopt a different mixture of the two dominant resonance structures. The effects of cross FFCF on the cross-peak line shape are discussed.

Amino Acid Insertion Frequencies Arising from Photoproducts Generated Using Aliphatic Diazirines

Science.gov (United States)

Ziemianowicz, Daniel S.; Bomgarden, Ryan; Etienne, Chris; Schriemer, David C.

2017-10-01

Mapping proteins with chemical reagents and mass spectrometry can generate a measure of accessible surface area, which in turn can be used to support the modeling and refinement of protein structures. Photolytically generated carbenes are a promising class of reagent for this purpose. Substituent effects appear to influence surface mapping properties, allowing for a useful measure of design control. However, to use carbene labeling data in a quantitative manner for modeling activities, we require a better understanding of their inherent amino acid reactivity, so that incorporation data can be normalized. The current study presents an analysis of the amino acid insertion frequency of aliphatic carbenes generated by the photolysis of three different diazirines: 3,3'-azibutyl-1-ammonium, 3,3'-azibutan-1-ol, and 4,4'-azipentan-1-oate. Leveraging an improved photolysis system for single-shot labeling of sub-microliter frozen samples, we used EThCD to localize insertion products in a large population of labeled peptides. Counting statistics were drawn from data-dependent LC-MS2 experiments and used to estimate the frequencies of insertion as a function of amino acid. We observed labeling of all 20 amino acids over a remarkably narrow range of insertion frequencies. However, the nature of the substituent could influence relative insertion frequencies, within a general preference for larger polar amino acids. We confirm a large (6-fold) increase in labeling yield when carbenes were photogenerated in the solid phase (77 K) relative to the liquid phase (293 K), and we suggest that carbene labeling should always be conducted in the frozen state to avoid information loss in surface mapping experiments. [Figure not available: see fulltext.

Sum rules for quasifree scattering of hadrons

Science.gov (United States)

Peterson, R. J.

2018-02-01

The areas d σ /d Ω of fitted quasifree scattering peaks from bound nucleons for continuum hadron-nucleus spectra measuring d2σ /d Ω d ω are converted to sum rules akin to the Coulomb sums familiar from continuum electron scattering spectra from nuclear charge. Hadronic spectra with or without charge exchange of the beam are considered. These sums are compared to the simple expectations of a nonrelativistic Fermi gas, including a Pauli blocking factor. For scattering without charge exchange, the hadronic sums are below this expectation, as also observed with Coulomb sums. For charge exchange spectra, the sums are near or above the simple expectation, with larger uncertainties. The strong role of hadron-nucleon in-medium total cross sections is noted from use of the Glauber model.