Unraveling nonadiabatic ionization and Coulomb potential effect in strong-field photoelectron holography

DOE PAGES

Song, Xiaohong; Lin, Cheng; Sheng, Zhihao; ...

2016-06-22

Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back and scatters off the ion(the signal wave). The interference hologram of the two waves may be used to extract target information embedded in the collision process. Unlike conventional optical holography, however, propagation of the electron wave packet is affected by the Coulomb potential as well as by the laser field. Inmore » addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. Here, we showed that photoelectron hologram can be well described only when the effect of nonadiabatic ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help paving the way for establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules.« less

Dusty Plasma Dynamics Near Surfaces in Space

NASA Technical Reports Server (NTRS)

Colwell, Joshua E.; Robertson, S.; Horanyi, M.; Nahra, Henry (Technical Monitor)

1998-01-01

The investigation 'Dusty Plasma Dynamics Near Surfaces in Space' is an experimental and theoretical study of the dynamics of dust particles on airless bodies in the solar system in the presence of a photoelectron sheath generated by solar ultraviolet light impinging on the surface. Solar UV illumination of natural and manmade surfaces in space produces photoelectrons which form a plasma sheath near the surface. Dust particles on the surface acquire a charge and may be transported by electric fields in the photoelectron sheath generated by inhomogeneities in the surface or the illumination (such as shadows). The sheath itself has a finite vertical extent leading to (at least) an electric field normal to the illuminated surface. If dust particles are launched from the surface by some other process, such as meteoroid impact, or spacecraft activity on the surface, these grains become charged and move under the influence of gravity and the electric field. This can give rise to suspension of the particles above the surface, loss from the parent body entirely (if accelerated beyond escape velocity), and a different distribution of dust ejecta from what would be expected with purely gravitational dynamics.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bhattacharyya, Swarnendu, E-mail: swarnendu.bhattacharyya@ch.tum.de; Domcke, Wolfgang, E-mail: wolfgang.domcke@ch.tum.de; Dai, Zuyang

A diabatic three-sheeted six-dimensional potential-energy surface has been constructed for the ground state and the lowest excited state of the PH{sub 3}{sup +} cation. Coupling terms of Jahn-Teller and pseudo-Jahn-Teller origin up to eighth order had to be included to describe the pronounced anharmonicity of the surface due to multiple conical intersections. The parameters of the diabatic Hamiltonian have been optimized by fitting the eigenvalues of the potential-energy matrix to ab initio data calculated at the CASSCF/MRCI level employing the correlation-consistent triple-ζ basis. The theoretical photoelectron spectrum of phosphine and the non-adiabatic nuclear dynamics of the phosphine cation have beenmore » computed by propagating nuclear wave packets with the multiconfiguration time-dependent Hartree method. The theoretical photoelectron bands obtained by Fourier transformation of the autocorrelation function agree well with the experimental results. It is shown that the ultrafast non-radiative decay dynamics of the first excited state of PH{sub 3}{sup +} is dominated by the exceptionally strong Jahn-Teller coupling of the asymmetric bending vibrational mode together with a hyperline of conical intersections with the electronic ground state induced by the umbrella mode. Time-dependent population probabilities have been computed for the three adiabatic electronic states. The non-adiabatic Jahn-Teller dynamics within the excited state takes place within ≈5 fs. Almost 80% of the excited-state population decay to the ground state within about 10 fs. The wave packets become highly complex and delocalized after 20 fs and no further significant transfer of electronic population seems to occur up to 100 fs propagation time.« less

Time-resolved photoelectron spectroscopy of adenosine and adenosine monophosphate photodeactivation dynamics in water microjets

NASA Astrophysics Data System (ADS)

Williams, Holly L.; Erickson, Blake A.; Neumark, Daniel M.

2018-05-01

The excited state relaxation dynamics of adenosine and adenosine monophosphate were studied at multiple excitation energies using femtosecond time-resolved photoelectron spectroscopy in a liquid water microjet. At pump energies of 4.69-4.97 eV, the lowest ππ* excited state, S1, was accessed and its decay dynamics were probed via ionization at 6.20 eV. By reversing the role of the pump and probe lasers, a higher-lying ππ* state was excited at 6.20 eV and its time-evolving photoelectron spectrum was monitored at probe energies of 4.69-4.97 eV. The S1 ππ* excited state was found to decay with a lifetime ranging from ˜210 to 250 fs in adenosine and ˜220 to 250 fs in adenosine monophosphate. This lifetime drops with increasing pump photon energy. Signal from the higher-lying ππ* excited state decayed on a time scale of ˜320 fs and was measureable only in adenosine monophosphate.

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics.

PubMed

Fushitani, Mizuho; Hishikawa, Akiyoshi

2016-11-01

We present applications of extreme ultraviolet (XUV) single-order laser harmonics to gas-phase ultrafast photoelectron spectroscopy. Ultrashort XUV pulses at 80 nm are obtained as the 5th order harmonics of the fundamental laser at 400 nm by using Xe or Kr as the nonlinear medium and separated from other harmonic orders by using an indium foil. The single-order laser harmonics is applied for real-time probing of vibrational wavepacket dynamics of I 2 molecules in the bound and dissociating low-lying electronic states and electronic-vibrational wavepacket dynamics of highly excited Rydberg N 2 molecules.

Valence electronic structure of cobalt phthalocyanine from an optimally tuned range-separated hybrid functional.

PubMed

Brumboiu, Iulia Emilia; Prokopiou, Georgia; Kronik, Leeor; Brena, Barbara

2017-07-28

We analyse the valence electronic structure of cobalt phthalocyanine (CoPc) by means of optimally tuning a range-separated hybrid functional. The tuning is performed by modifying both the amount of short-range exact exchange (α) included in the hybrid functional and the range-separation parameter (γ), with two strategies employed for finding the optimal γ for each α. The influence of these two parameters on the structural, electronic, and magnetic properties of CoPc is thoroughly investigated. The electronic structure is found to be very sensitive to the amount and range in which the exact exchange is included. The electronic structure obtained using the optimal parameters is compared to gas-phase photo-electron data and GW calculations, with the unoccupied states additionally compared with inverse photo-electron spectroscopy measurements. The calculated spectrum with tuned γ, determined for the optimal value of α = 0.1, yields a very good agreement with both experimental results and with GW calculations that well-reproduce the experimental data.

Real-time visualization of the vibrational wavepacket dynamics in electronically excited pyrimidine via femtosecond time-resolved photoelectron imaging

NASA Astrophysics Data System (ADS)

Li, Shuai; Long, Jinyou; Ling, Fengzi; Wang, Yanmei; Song, Xinli; Zhang, Song; Zhang, Bing

2017-07-01

The vibrational wavepacket dynamics at the very early stages of the S1-T1 intersystem crossing in photoexcited pyrimidine is visualized in real time by femtosecond time-resolved photoelectron imaging and time-resolved mass spectroscopy. A coherent superposition of the vibrational states is prepared by the femtosecond pump pulse at 315.3 nm, resulting in a vibrational wavepacket. The composition of the prepared wavepacket is directly identified by a sustained quantum beat superimposed on the parent-ion transient, possessing a frequency in accord with the energy separation between the 6a1 and 6b2 states. The dephasing time of the vibrational wavepacket is determined to be 82 ps. More importantly, the variable Franck-Condon factors between the wavepacket components and the dispersed cation vibrational levels are experimentally illustrated to identify the dark state and follow the energy-flow dynamics on the femtosecond time scale. The time-dependent intensities of the photoelectron peaks originated from the 6a1 vibrational state exhibit a clear quantum beating pattern with similar periodicity but a phase shift of π rad with respect to those from the 6b2 state, offering an unambiguous picture of the restricted intramolecular vibrational energy redistribution dynamics in the 6a1/6b2 Fermi resonance.

Inequivalence of single-particle and population lifetimes in a cuprate superconductor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Shuolong; Sobota, J. A.; Leuenberger, D.

2015-06-15

We study optimally doped Bi-2212 (T c=96 K) using femtosecond time- and angle-resolved photoelectron spectroscopy. Energy-resolved population lifetimes are extracted and compared with single-particle lifetimes measured by equilibrium photoemission. The population lifetimes deviate from the single-particle lifetimes in the low excitation limit by 1–2 orders of magnitude. Fundamental considerations of electron scattering unveil that these two lifetimes are in general distinct, yet for systems with only electron-phonon scattering they should converge in the low-temperature, low-fluence limit. As a result, the qualitative disparity in our data, even in this limit, suggests that scattering channels beyond electron-phonon interactions play a significant rolemore » in the electron dynamics of cuprate superconductors.« less

Quantitative interpretation of molecular dynamics simulations for X-ray photoelectron spectroscopy of aqueous solutions

NASA Astrophysics Data System (ADS)

Olivieri, Giorgia; Parry, Krista M.; Powell, Cedric J.; Tobias, Douglas J.; Brown, Matthew A.

2016-04-01

Over the past decade, energy-dependent ambient pressure X-ray photoelectron spectroscopy (XPS) has emerged as a powerful analytical probe of the ion spatial distributions at the vapor (vacuum)-aqueous electrolyte interface. These experiments are often paired with complementary molecular dynamics (MD) simulations in an attempt to provide a complete description of the liquid interface. There is, however, no systematic protocol that permits a straightforward comparison of the two sets of results. XPS is an integrated technique that averages signals from multiple layers in a solution even at the lowest photoelectron kinetic energies routinely employed, whereas MD simulations provide a microscopic layer-by-layer description of the solution composition near the interface. Here, we use the National Institute of Standards and Technology database for the Simulation of Electron Spectra for Surface Analysis (SESSA) to quantitatively interpret atom-density profiles from MD simulations for XPS signal intensities using sodium and potassium iodide solutions as examples. We show that electron inelastic mean free paths calculated from a semi-empirical formula depend strongly on solution composition, varying by up to 30% between pure water and concentrated NaI. The XPS signal thus arises from different information depths in different solutions for a fixed photoelectron kinetic energy. XPS signal intensities are calculated using SESSA as a function of photoelectron kinetic energy (probe depth) and compared with a widely employed ad hoc method. SESSA simulations illustrate the importance of accounting for elastic-scattering events at low photoelectron kinetic energies (<300 eV) where the ad hoc method systematically underestimates the preferential enhancement of anions over cations. Finally, some technical aspects of applying SESSA to liquid interfaces are discussed.

Phase Structure of Strong-Field Tunneling Wave Packets from Molecules.

PubMed

Liu, Ming-Ming; Li, Min; Wu, Chengyin; Gong, Qihuang; Staudte, André; Liu, Yunquan

2016-04-22

We study the phase structure of the tunneling wave packets from strong-field ionization of molecules and present a molecular quantum-trajectory Monte Carlo model to describe the laser-driven dynamics of photoelectron momentum distributions of molecules. Using our model, we reproduce and explain the alignment-dependent molecular frame photoelectron spectra of strong-field tunneling ionization of N_{2} reported by M. Meckel et al. [Nat. Phys. 10, 594 (2014)]. In addition to modeling the low-energy photoelectron angular distributions quantitatively, we extract the phase structure of strong-field molecular tunneling wave packets, shedding light on its physical origin. The initial phase of the tunneling wave packets at the tunnel exit depends on both the initial transverse momentum distribution and the molecular internuclear distance. We further show that the ionizing molecular orbital has a critical effect on the initial phase of the tunneling wave packets. The phase structure of the photoelectron wave packet is a key ingredient for modeling strong-field molecular photoelectron holography, high-harmonic generation, and molecular orbital imaging.

The Martian Photoelectron Boundary as Seen by MAVEN

NASA Astrophysics Data System (ADS)

Garnier, P.; Steckiewicz, M.; Mazelle, C.; Xu, S.; Mitchell, D.; Holmberg, M. K. G.; Halekas, J. S.; Andersson, L.; Brain, D. A.; Connerney, J. E. P.; Espley, J. R.; Lillis, R. J.; Luhmann, J. G.; Sauvaud, J.-A.; Jakosky, B. M.

2017-10-01

Photoelectron peaks in the 20-30 eV energy range are commonly observed in the planetary atmospheres, produced by the intense photoionization from solar 30.4 nm photons. At Mars, these photoelectrons are known to escape the planet down its tail, making them tracers for the atmospheric escape. Furthermore, their presence or absence allow to define the so-called photoelectron boundary (PEB), which separates the photoelectron dominated ionosphere from the external environment. We provide here a detailed statistical analysis of the location and properties of the PEB based on the Mars Atmosphere and Volatile EvolutioN (MAVEN) electron and magnetic field data obtained from September 2014 to May 2016 (including 1696 PEB crossings). The PEB appears as mostly sensitive to the solar wind dynamic and crustal fields pressures. Its variable altitude thus leads to a variable wake cross section for escape (up to ˜+50%), which is important for deriving escape rates. The PEB is not always sharp and is characterized on average by the following: a magnetic field topology typical for the end of magnetic pileup region above it, more field-aligned fluxes above than below, and a clear change of the altitude slopes of both electron fluxes and total density (that appears different from the ionopause). The PEB thus appears as a transition region between two plasma and fields configurations determined by the draping topology of the interplanetary magnetic field around Mars and much influenced by the crustal field sources below, whose dynamics also impacts the estimated escape rate of ionospheric plasma.

Energetic (above 60 eV) atmospheric photoelectrons

NASA Technical Reports Server (NTRS)

Winningham, J. D.; Decker, D. T.; Kozyra, J. U.; Nagy, A. F.; Jasperse, J. R.

1989-01-01

Data from low altitude plasma instrument (LAPI) on Dynamics Explorer 2 document a population of high-energy (up to 800 eV) atmospheric photoelectrons that has not been reported in the published literature. The source of these photoelectrons is postulated to be the soft X-ray portion of the whole sun spectrum. This conclusion is supported by sunrise-sunset characteristics that track those of the classical (below 60 eV) EUV-produced photoelectrons, and theoretical results from two models that incorporate the soft X-ray portion of the solar spectrum. The models include K-shell ionization effects and predict peaks in the photoelectron spectrum due to Auger electrons emitted from oxygen and nitrogen. The peak for nitrogen is observed as predicted, but the peak for oxygen is barely observable. Excellent quantitative agreement is achieved between theory and experiment by using reasonable adjustments to the few published soft X-ray spectra based on solar activity. The upflowing energetic photoelectrons provide a heretofore unknown source of electrons to the magnetosphere. They occur whenever and wherever the sun is up, that is, at all invariant latitudes. Their density is low, but they are steady and ubiquitous. If scattering and trapping occur on closed field lines, then photoelectrons could contribute as a significant particle source and thus represent a new facet of magnetosphere-ionosphere coupling.

Retrieving plasmonic near-field information: A quantum-mechanical model for streaking photoelectron spectroscopy of gold nanospheres

NASA Astrophysics Data System (ADS)

Li, Jianxiong; Saydanzad, Erfan; Thumm, Uwe

2016-11-01

Streaked photoemission from nanostructures is characterized by size- and material-dependent nanometer-scale variations of the induced nanoplasmonic response to the electronic field of the streaking pulse and thus holds promise of allowing photoelectron imaging with both subfemtosecond temporal and nanometer spatial resolution. In order to scrutinize the driven collective electronic dynamics in 10-200-nm-diameter gold nanospheres, we calculated the plasmonic field induced by streaking pulses in the infrared and visible spectral range and developed a quantum-mechanical model for streaked photoemission by extreme ultraviolet pulses. Our simulated photoelectron spectra reveal a significant amplitude enhancement and phase shift of the photoelectron streaking trace relative to calculations that exclude the induced plasmonic field. Both are most pronounced for streaking pulses tuned to the plasmon frequency and retrace the plasmonic electromagnetic field enhancement and phase shift near the nanosphere surface.

Above-threshold ionization of noble gases in elliptically polarized fields: Effects of atomic polarization on photoelectron angular distributions

NASA Astrophysics Data System (ADS)

Wang, YanLan; Yu, ShaoGang; Lai, XuanYang; Liu, XiaoJun; Chen, Jing

2017-06-01

We theoretically investigate the atomic polarization effect on photoelectron angular distributions (PADs) in above-threshold ionization of noble gases with elliptically polarized laser fields at wavelength of 800 nm, ellipticity of 0.25, and intensity of 1.5 ×1014W/cm2 . Simulations based on a semiclassical model that includes both the ionic Coulomb potential and the atomic polarization effect show surprisingly little difference between PADs for Ar, Kr, and Xe, which is in good agreement with recent experimental observations. Our calculations reveal that the atomic polarization effect increases the distance of the tunnel exit point of the photoelectron to the parent ion and weakens the strength of the interaction between the parent ion and the photoelectron on its subsequent classical propagation. As a result, the forward-scattering electrons which contribute to the main lobes in PADs are substantially suppressed. Our results indicate that the insensitivity of PADs for Ar, Kr, and Xe may be closely related to the influence of the atomic polarization effect on the photoelectron dynamics in the strong laser field.

Evaluation of the amperex 56 TVP photomultiplier. [characteristics: photoelectron time spread, anode pulse amplitude and photocathode sensing area

NASA Technical Reports Server (NTRS)

Lo, C. C.; Leskovar, B.

1976-01-01

Characteristics were measured for the Amperex 56 TVP 42 mm-diameter photomultiplier. Some typical photomultiplier characteristics-such as gain, dark current, transit and rise times-are compared with data provided. Photomultiplier characteristics generally not available such as the single photoelectron time spread, the relative collection efficiency, the relative anode pulse amplitude as a function of the voltage between the photocathode and focusing electrode, and the position of the photocathode sensing area were measured and are discussed for two 56 TVP's. The single photoelectron time spread, the relative collection efficiency, and the transit time difference as a function of the voltage between photocathode and focusing electrode were also measured and are discussed, particularly with respect to the optimization of photomultiplier operating conditions for timing applications.

The PhotoElectron Boundary as observed by MAVEN instruments

NASA Astrophysics Data System (ADS)

Garnier, P.; Steckiewicz, M.; Mazelle, C. X.; Xu, S.; Mitchell, D. L.; Holmberg, M.; Halekas, J. S.; Andersson, L.; Brain, D.; Connerney, J. E. P.; Espley, J. R.; Lillis, R. J.; Luhmann, J. G.; Savaud, J. A.; Jakosky, B. M.

2017-12-01

Photoelectron peaks in the 20-30 eV energy range are commonly observed in planetary atmospheres (Earth, Mars, Titan...), produced by the intense photoionization from solar 30.4 nm photons. At Mars, these photoelectrons result from the ionization of CO2 and O atmospheric neutrals, and are known to escape the planet down its tail, making them tracers for the atmospheric escape (Frahm et al., 2006). Furthermore, their presence or absence allows us to define the so-called PhotoElectron Boundary (PEB), that separates the sunlit photoelectron-dominated ionosphere from the solar wind controlled environment, as initially observed by the Mars Global Surveyor (MGS) MAG/ER instrument (Mitchell et al. (2000, 2001). We provide here a detailed statistical analysis of the location and properties of the PEB based on the Mars Atmosphere and Volatile Evolution (MAVEN) mission electron and magnetic field data. Our dataset includes 1696 dayside PEB crossings obtained from September 2014 until May 2016 (the observations of escaping photoelectrons in the wake being not included). The PEB appears as mostly sensitive to the solar wind dynamic and crustal magnetic fields pressures, for which a quantitative dependance is derived and compared with two other important boundaries : the bow shock and magnetic pileup boundary. The PEB altitude is highly variable, leading to a variable wake cross section for escape (up to +- 50%), which is important for deriving global escape rates from in situ photoelectron escape rates. The PEB is not always sharp, and is, despite a strong variability, characterized on average by : a magnetic field topology typical for the edge of the Magnetic Pile Up Region above it, more field aligned fluxes above than below, and a clear change of the altitude dependence of both electron fluxes and total density (that appears different from the ionopause). The PEB thus appears as a transition region between two plasma and field configurations which is determined by the draping topology of the interplanetary magnetic field around Mars and strongly influenced by the crustal field sources below, and whose dynamics also impacts the estimation of ionospheric plasma escape rate.

Steering continuum electron dynamics by low-energy attosecond streaking

NASA Astrophysics Data System (ADS)

Geng, Ji-Wei; Xiong, Wei-Hao; Xiao, Xiang-Ru; Gong, Qihuang; Peng, Liang-You

2016-08-01

A semiclassical model is developed to understand the electronic dynamics in the low-energy attosecond streaking. Under a relatively strong infrared (IR) pulse, the low-energy part of photoelectrons initialized by a single attosecond pulse (SAP) can either rescatter with the ionic core and induce interferences structures in the momentum spectra of the ionized electrons or be recaptured into the Rydberg states. The Coulomb potential plays essential roles in both the electron rescattering and recapturing processes. We find that by changing the time delay between the SAP and the IR pulse, the photoelectrons yield or the population of the Rydberg states can be effectively controlled. The present study demonstrates a fascinating way to steer the electron motion in the continuum.

Vibrationally induced inversion of photoelectron forward-backward asymmetry in chiral molecule photoionization by circularly polarized light

PubMed Central

Garcia, Gustavo A.; Nahon, Laurent; Daly, Steven; Powis, Ivan

2013-01-01

Electron–nuclei coupling accompanying excitation and relaxation processes is a fascinating phenomenon in molecular dynamics. A striking and unexpected example of such coupling is presented here in the context of photoelectron circular dichroism measurements on randomly oriented, chiral methyloxirane molecules, unaffected by any continuum resonance. Here, we report that the forward-backward asymmetry in the electron angular distribution, with respect to the photon axis, which is associated with photoelectron circular dichroism can surprisingly reverse direction according to the ion vibrational mode excited. This vibrational dependence represents a clear breakdown of the usual Franck–Condon assumption, ascribed to the enhanced sensitivity of photoelectron circular dichroism (compared with other observables like cross-sections or the conventional anisotropy parameter-β) to the scattering phase off the chiral molecular potential, inducing a dependence on the nuclear geometry sampled in the photoionization process. Important consequences for the interpretation of such dichroism measurements within analytical contexts are discussed. PMID:23828557

Enhancement of antioxidant and antibacterial properties for tannin acid/chitosan/tripolyphosphate nanoparticles filled electrospinning films: Surface modification of sliver nanoparticles.

PubMed

Zhan, Fuchao; Sheng, Feng; Yan, Xiangxing; Zhu, Yingrui; Jin, Weiping; Li, Jing; Li, Bin

2017-11-01

The tannin acid/chitosan/tripolyphosphate nanoparticles were encapsulated in polyvinyl alcohol (PVA)/poly-acrylic acid (PAA) electrospinning films by electrostatic spinning technology. To optimize the prepared condition, properties and morphology of nanoparticles were characterized by dynamic light scattering (DLS) and transmission electron microscope (TEM). The optimized initial concentration of tannin, chitosan and tripolyphosphate solutions were 1, 1, 0.5mg/ml, respectively, with adding proportion for 5:5:1. The average diameter of tannin acid/chitosan/tripolyphosphate nanoparticles was ∼80nm. The electrospinning films showed an excellent water-resistant property with 0.5wt%N,N'-Methylenebisacrylamide (MBA). Due to the antioxidant and antibacterial of tannic acid, the films possessed these properties. The antioxidant and antibacterial of these fibers significantly improved after in situ formation of silver nanoparticles (AgNPs). Electrospun films were characterized by scanning electron microscopy (SEM), Fourier transform infrared spectra (FT-IR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrafast measurements of chlorine dioxide photochemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ludowise, P.D.

Time-resolved mass spectrometry and time-resolved photoelectron spectroscopy are used to study the ultrafast photodissociation dynamics of chlorine dioxide, an important constituent in stratospheric ozone depletion. Chapter 1 introduces these pump/probe techniques, in which a femtosecond pump pulse excites a molecule to a dissociative state. At a later time, a second femtosecond probe pulse ionizes the molecule. The resulting mass and photoelectron spectra are acquired as a function of the delay between the pump and probe pulses, which follows the evolution of the molecule on the excited state. A comparison to other techniques used to study reaction dynamics is discussed. Chaptermore » 2 includes a detailed description of the design and construction of the experimental apparatus, which consists of a femtosecond laser system, a molecular beam time-of-flight spectrometer, and a data acquisition system. The time-of-flight spectrometer is specifically designed to have a short flight distance to maximize the photoelectron collection efficiency without degrading the resolution, which is limited by the bandwidth of the femtosecond laser system. Typical performance of the apparatus is demonstrated in a study of the time-resolved photoelectron spectroscopy of nitric oxide. The results of the time-resolved mass spectrometry experiments of chlorine dioxide are presented in Chapter 3. Upon excitation to the A {sup 2}A{sub 2} state near 3.2 eV, the molecule dissociates through an indirect two-step mechanism. The direct dissociation channel has been predicted to be open, but is not observed. A quantum beat is observed in the OClO{sup +} species, which is described as a vibrational coherence of the optically prepared A {sup 2}A{sub 2} state. Chapter 4 presents the results of the time-resolved photoelectron experiments of chlorine dioxide. At short delay time, the quantum beat of the OClO{sup +} species is observed in the X {sup 1}A{sub 1} state of the ion. At infinite delay, the signal is dominated by the ClO{sup +} ion, observed in a variety of electronic states. The photoelectron data is shown to support the indirect two-step dissociation mechanism derived from the mass results. Conclusions of the mass and photoelectron results are discussed in context of the stratospheric ozone depletion problem.« less

Excited state non-adiabatic dynamics of pyrrole: A time-resolved photoelectron spectroscopy and quantum dynamics study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Guorong; State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023; Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026

The dynamics of pyrrole excited at wavelengths in the range 242-217 nm are studied using a combination of time-resolved photoelectron spectroscopy and wavepacket propagations performed using the multi-configurational time-dependent Hartree method. Excitation close to the origin of pyrrole’s electronic spectrum, at 242 and 236 nm, is found to result in an ultrafast decay of the system from the ionization window on a single timescale of less than 20 fs. This behaviour is explained fully by assuming the system to be excited to the A{sub 2}(πσ{sup ∗}) state, in accord with previous experimental and theoretical studies. Excitation at shorter wavelengths hasmore » previously been assumed to result predominantly in population of the bright A{sub 1}(ππ{sup ∗}) and B{sub 2}(ππ{sup ∗}) states. We here present time-resolved photoelectron spectra at a pump wavelength of 217 nm alongside detailed quantum dynamics calculations that, together with a recent reinterpretation of pyrrole’s electronic spectrum [S. P. Neville and G. A. Worth, J. Chem. Phys. 140, 034317 (2014)], suggest that population of the B{sub 1}(πσ{sup ∗}) state (hitherto assumed to be optically dark) may occur directly when pyrrole is excited at energies in the near UV part of its electronic spectrum. The B{sub 1}(πσ{sup ∗}) state is found to decay on a timescale of less than 20 fs by both N-H dissociation and internal conversion to the A{sub 2}(πσ{sup ∗}) state.« less

Imaging a multidimensional multichannel potential energy surface: Photodetachment of H(-)(NH3) and NH4 (.).

PubMed

Hu, Qichi; Song, Hongwei; Johnson, Christopher J; Li, Jun; Guo, Hua; Continetti, Robert E

2016-06-28

Probes of the Born-Oppenheimer potential energy surfaces governing polyatomic molecules often rely on spectroscopy for the bound regions or collision experiments in the continuum. A combined spectroscopic and half-collision approach to image nuclear dynamics in a multidimensional and multichannel system is reported here. The Rydberg radical NH4 and the double Rydberg anion NH4 (-) represent a polyatomic system for benchmarking electronic structure and nine-dimensional quantum dynamics calculations. Photodetachment of the H(-)(NH3) ion-dipole complex and the NH4 (-) DRA probes different regions on the neutral NH4 PES. Photoelectron energy and angular distributions at photon energies of 1.17, 1.60, and 2.33 eV compare well with quantum dynamics. Photoelectron-photofragment coincidence experiments indicate dissociation of the nascent NH4 Rydberg radical occurs to H + NH3 with a peak kinetic energy of 0.13 eV, showing the ground state of NH4 to be unstable, decaying by tunneling-induced dissociation on a time scale beyond the present scope of multidimensional quantum dynamics.

The time-resolved photoelectron spectrum of toluene using a perturbation theory approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Richings, Gareth W.; Worth, Graham A., E-mail: g.a.worth@bham.ac.uk

A theoretical study of the intra-molecular vibrational-energy redistribution of toluene using time-resolved photo-electron spectra calculated using nuclear quantum dynamics and a simple, two-mode model is presented. Calculations have been carried out using the multi-configuration time-dependent Hartree method, using three levels of approximation for the calculation of the spectra. The first is a full quantum dynamics simulation with a discretisation of the continuum wavefunction of the ejected electron, whilst the second uses first-order perturbation theory to calculate the wavefunction of the ion. Both methods rely on the explicit inclusion of both the pump and probe laser pulses. The third method includesmore » only the pump pulse and generates the photo-electron spectrum by projection of the pumped wavepacket onto the ion potential energy surface, followed by evaluation of the Fourier transform of the autocorrelation function of the subsequently propagated wavepacket. The calculations performed have been used to study the periodic population flow between the 6a and 10b16b modes in the S{sub 1} excited state, and compared to recent experimental data. We obtain results in excellent agreement with the experiment and note the efficiency of the perturbation method.« less

Nonadiabatic Dynamics May Be Probed through Electronic Coherence in Time-Resolved Photoelectron Spectroscopy.

PubMed

Bennett, Kochise; Kowalewski, Markus; Mukamel, Shaul

2016-02-09

We present a hierarchy of Fermi golden rules (FGRs) that incorporate strongly coupled electronic/nuclear dynamics in time-resolved photoelectron spectroscopy (TRPES) signals at different levels of theory. Expansion in the joint electronic and nuclear eigenbasis yields the numerically most challenging exact FGR (eFGR). The quasistatic Fermi Golden Rule (qsFGR) neglects nuclear motion during the photoionization process but takes into account electronic coherences as well as populations initially present in the pumped matter as well as those generated internally by coupling between electronic surfaces. The standard semiclassical Fermi Golden Rule (scFGR) neglects the electronic coherences and the nuclear kinetic energy during the ionizing pulse altogether, yielding the classical Condon approximation. The coherence contributions depend on the phase-profile of the ionizing field, allowing coherent control of TRPES signals. The photoelectron spectrum from model systems is simulated using these three levels of theory. The eFGR and the qsFGR show temporal oscillations originating from the electronic or vibrational coherences generated as the nuclear wave packet traverses a conical intersection. These oscillations, which are missed by the scFGR, directly reveal the time-evolving splitting between electronic states of the neutral molecule in the curve-crossing regime.

Low-Energy Electron Effects on the Polar Wind Observed by the POLAR Spacecraft

NASA Technical Reports Server (NTRS)

Horwitz, J. L.; Su, Y.-J.; Dors, E. E.; Moore, Thomas E.; Giles, Barbara L.; Chandler, Michael O.; Craven, Paul D.; Chang, S.-W.; Scudder, J.

1998-01-01

Large ion outflow velocity variation at POLAR apogee have been observed. The observed H+ flow velocities were in the range of 23-110 km/s and 0+ flow velocities were in the range of 5-25 km/s. These velocity ranges lie between those predicted by simulations of the photoelectron-driven polar wind and "baseline" polar wind. The electric current contributions of the photoelectrons and polar rain are expected to control the size and altitude of an electric potential drop which accelerates the polar wind at relatively high altitudes. In this presentation, we compare polar wind characteristics observed near 5000 km and 8 RE altitudes by the Thermal Ion Dynamics Experiment (TIDE) with measurements of low-energy electrons sampled by HYDRA, both from the POLAR spacecraft, to examine possible effects of the polar rain and photoelectrons on the polar wind. Both correlations and anti-correlations are found between the polar wind velocities and the polar rain fluxes at POLAR apogee during different polar cap crossings. Also, the low-altitude upward/downward photoelectron spectra are used to estimates the potential drops above the spacecraft. We interpret these observations in terms of the effects that both photoelectrons and polar rain may have on the electric potential and polar wind acceleration along polar cap magnetic field lines.

Communication: Direct evidence for sequential dissociation of gas-phase Fe(CO)5 via a singlet pathway upon excitation at 266 nm

PubMed Central

Leitner, T.; Mazza, T.; Schröder, H.; Kunnus, K.; Schreck, S.; Radcliffe, P.; Düsterer, S.; Meyer, M.; Föhlisch, A.

2017-01-01

We prove the hitherto hypothesized sequential dissociation of Fe(CO)5 in the gas phase upon photoexcitation at 266 nm via a singlet pathway with time-resolved valence and core-level photoelectron spectroscopy with an x-ray free-electron laser. Valence photoelectron spectra are used to identify free CO molecules and to determine the time constants of stepwise dissociation to Fe(CO)4 within the temporal resolution of the experiment and further to Fe(CO)3 within 3 ps. Fe 3p core-level photoelectron spectra directly reflect the singlet spin state of the Fe center in Fe(CO)5, Fe(CO)4, and Fe(CO)3 showing that the dissociation exclusively occurs along a singlet pathway without triplet-state contribution. Our results are important for assessing intra- and intermolecular relaxation processes in the photodissociation dynamics of the prototypical Fe(CO)5 complex in the gas phase and in solution, and they establish time-resolved core-level photoelectron spectroscopy as a powerful tool for determining the multiplicity of transition metals in photochemical reactions of coordination complexes. PMID:28595420

Dynamic light scattering and X-ray photoelectron spectroscopy characterization of PEGylated polymer nanocarriers: internal structure and surface properties.

PubMed

Celasco, Edvige; Valente, Ilaria; Marchisio, Daniele L; Barresi, Antonello A

2014-07-22

In this work, nanospheres and nanocapsules are precipitated in confined impinging jet mixers through solvent displacement and characterized. Acetone and water are used as the solvent and antisolvent, respectively, together with polymethoxypolyethylene glycol cyanoacrylate-co-hexadecylcyanoacrylate and Miglyol as the copolymer and oil, respectively. Characterization is performed with dynamic light scattering, with electrophoretic measurements, and for the first time with X-ray photoelectron spectroscopy. Results show that the presence of polyethylene glycol chains seems to be more pronounced on the surface of nanospheres than on that of nanocapsules. The thickness of the copolymer layer in nanocapsules ranges from 1 to 10 nm, depending on the value of the oil:copolymer mass ratio. Fast dilution is confirmed to have a positive effect in suppressing aggregation but can induce further copolymer precipitation.

Strong Field Theories beyond Dipole Approximations in Nonrelativistic Regimes

NASA Astrophysics Data System (ADS)

He, Pei-Lun; Lao, Di; He, Feng

2017-04-01

The exact nondipole Volkov solutions to the Schrödinger equation and Pauli equation are found, based on which a strong field theory beyond the dipole approximation is built for describing the nondipole effects in nonrelativistic laser driven electron dynamics. This theory is applied to investigate momentum partition laws for multiphoton and tunneling ionization and explicitly shows that the complex interplay of a laser field and Coulomb action may reverse the expected photoelectron momentum along the laser propagation direction. The magnetic-spin coupling does not bring observable effects on the photoelectron momentum distribution and can be neglected. Compared to the strong field approximation within the dipole approximation, this theory works in a much wider range of laser parameters and lays a solid foundation for describing nonrelativistic electron dynamics in both short wavelength and midinfrared regimes where nondipole effects are unavoidable.

The effect of vibrational autoionization on the H2+ X 2Σg+ state rotationally resolved photoionization dynamics

NASA Astrophysics Data System (ADS)

Holland, D. M. P.; Shaw, D. A.

2014-01-01

The effect of vibrational autoionization on the H2+ X 2Σg+ v+ = 3, N+ state rotationally resolved photoelectron angular distributions and branching ratios has been investigated with a velocity map imaging spectrometer and synchrotron radiation. In photon excitation regions free from the influence of autoionizing Rydberg states, where direct ionization dominates, the photoelectron anisotropy parameter associated with the X 1Σg+ v″ = 0, N″ = 1 → X 2Σg+ v+ = 3, N+ = 1 transition has a value close to the theoretical maximum. However, in the vicinity of a Rydberg state, vibrational autoionization leads to a substantial reduction in anisotropy. The value of the anisotropy parameter associated with the S-branch of the photoelectron spectrum is found to be considerably higher than that predicted under the assumption that the outgoing electron can be represented solely as a p-wave. This suggests that the f-wave contribution must be taken into account to obtain a proper description of the photoionization dynamics. The observed variations in the rotationally resolved branching ratios, in the vicinity of an autoionizing resonance, depend upon the rotational level of the Rydberg state. The rotationally averaged photoelectron anisotropy parameters have been compared with the corresponding, previously calculated, theoretical results and reasonable agreement has been found. The influence of vibrational autoionization on the H2+ X 2Σg+ v+ = 0, 1, 2, 3 vibrational branching ratios has also been investigated, and the experimental results show that, in energy regions encompassing Rydberg states, these ratios deviate strongly from the Franck-Condon factors for direct ionization.

Tin and germanium based two-dimensional Ruddlesden-Popper hybrid perovskites for potential lead-free photovoltaic and photoelectronic applications.

PubMed

Ma, Liang; Ju, Ming-Gang; Dai, Jun; Zeng, Xiao Cheng

2018-06-21

Despite their high power conversion efficiency, the commercial applications of hybrid organic-inorganic lead (Pb) halide perovskite based solar cells are still hampered by concerns about the toxicity of Pb and the structural stability in open air. Herein, based on density-functional theory computation, we show that lead-free tin (Sn) and germanium (Ge) based two-dimensional (2D) Ruddlesden-Popper hybrid organic-inorganic perovskites with a thickness of a few unit-cells, BA2MAn-1MnI3n+1 (M = Sn or Ge, n = 2-4), possess desirable electronic, excitonic and light absorption properties, thereby showing promise for photovoltaic and/or photoelectronic applications. In particular, we show that by increasing the layer thickness of the Sn-based 2D perovskites, the bandgap can be lowered towards the optimal range (0.9-1.6 eV) for solar cells. Meanwhile, the exciton binding energy is reduced to a more optimal value. In addition, theoretical assessment indicates that the thermodynamic stability of Sn-/Ge-based 2D perovskites is notably enhanced compared to that of their 3D analogues. These features render the Sn-/Ge-based 2D hybrid perovskites with a thickness of a few tens of unit cells promising lead-free perovskites with much improved structural stabilities for photovoltaic and/or photoelectronic applications.

Probing long-range structural order in SnPc/Ag(111) by umklapp process assisted low-energy angle-resolved photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Jauernik, Stephan; Hein, Petra; Gurgel, Max; Falke, Julian; Bauer, Michael

2018-03-01

Laser-based angle-resolved photoelectron spectroscopy is performed on tin-phthalocyanine (SnPc) adsorbed on silver Ag(111). Upon adsorption of SnPc, strongly dispersing bands are observed which are identified as secondary Mahan cones formed by surface umklapp processes acting on photoelectrons from the silver substrate as they transit through the ordered adsorbate layer. We show that the photoemission data carry quantitative structural information on the adsorbate layer similar to what can be obtained from a conventional low-energy electron diffraction (LEED) study. More specifically, we compare photoemission data and LEED data probing an incommensurate-to-commensurate structural phase transition of the adsorbate layer. Based on our results we propose that Mahan-cone spectroscopy operated in a pump-probe configuration can be used in the future to probe structural dynamics at surfaces with a temporal resolution in the sub-100-fs regime.

Morphology Analysis and Optimization: Crucial Factor Determining the Performance of Perovskite Solar Cells.

PubMed

Zeng, Wenjin; Liu, Xingming; Guo, Xiangru; Niu, Qiaoli; Yi, Jianpeng; Xia, Ruidong; Min, Yong

2017-03-24

This review presents an overall discussion on the morphology analysis and optimization for perovskite (PVSK) solar cells. Surface morphology and energy alignment have been proven to play a dominant role in determining the device performance. The effect of the key parameters such as solution condition and preparation atmosphere on the crystallization of PVSK, the characterization of surface morphology and interface distribution in the perovskite layer is discussed in detail. Furthermore, the analysis of interface energy level alignment by using X-ray photoelectron spectroscopy and ultraviolet photoelectron spectroscopy is presented to reveals the correlation between morphology and charge generation and collection within the perovskite layer, and its influence on the device performance. The techniques including architecture modification, solvent annealing, etc. were reviewed as an efficient approach to improve the morphology of PVSK. It is expected that further progress will be achieved with more efforts devoted to the insight of the mechanism of surface engineering in the field of PVSK solar cells.

Imaging a multidimensional multichannel potential energy surface: Photodetachment of H{sup −}(NH{sub 3}) and NH{sub 4}{sup −}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Qichi; Johnson, Christopher J.; Continetti, Robert E., E-mail: hguo@umn.edu, E-mail: rcontinetti@ucsd.edu

2016-06-28

Probes of the Born-Oppenheimer potential energy surfaces governing polyatomic molecules often rely on spectroscopy for the bound regions or collision experiments in the continuum. A combined spectroscopic and half-collision approach to image nuclear dynamics in a multidimensional and multichannel system is reported here. The Rydberg radical NH{sub 4} and the double Rydberg anion NH{sub 4}{sup −} represent a polyatomic system for benchmarking electronic structure and nine-dimensional quantum dynamics calculations. Photodetachment of the H{sup −}(NH{sub 3}) ion-dipole complex and the NH{sub 4}{sup −} DRA probes different regions on the neutral NH{sub 4} PES. Photoelectron energy and angular distributions at photon energiesmore » of 1.17, 1.60, and 2.33 eV compare well with quantum dynamics. Photoelectron-photofragment coincidence experiments indicate dissociation of the nascent NH{sub 4} Rydberg radical occurs to H + NH{sub 3} with a peak kinetic energy of 0.13 eV, showing the ground state of NH{sub 4} to be unstable, decaying by tunneling-induced dissociation on a time scale beyond the present scope of multidimensional quantum dynamics.« less

Hair sensor using a photoelectronic principle for sensing airflow and its direction

NASA Astrophysics Data System (ADS)

Huang, Kuang-Yuh; Huang, Chien-Tai

2011-01-01

Many organisms have diverse hair cells to instantaneously perceive the change of surroundings so that they can keep away from threats. These organs can precisely detect the tiny variations of airflow, water flow, sound, or pressure, and also resolve their affecting directions. Through this brilliant inspiration by the insects' cilia, we decided to design and develop a hair sensor for detecting two-dimensional airflow and pressure waves by using photoelectronic principles. The hair sensor inherently consists of an artificial cilium supported by an elastic membrane. A light-emitting diode and a quadrant photodiode are used as the photoelectronic sensor. The airflow or pressure wave directly stimulates the cilium to sway, and this motion contributes to let the projected light beam shift over the quadrant photodiode, whose four photodiodes produce then corresponding output signals. Because of dynamic and high-sensitive properties of the photoelectronic sensor, the hair sensor we developed possesses a high measurement resolution to be able to detect very tiny stimulation and its affecting direction. According to its multifaceted characteristics and simple structure, the hair sensor can be applied in numerous potential application fields, such as intrusion alarm system, noise detection system, as well as a tactile sensor.

Charging and exciton-mediated decharging of metal nanoparticles in organic semiconductor matrices

NASA Astrophysics Data System (ADS)

Ligorio, Giovanni; Vittorio Nardi, Marco; Christodoulou, Christos; Florea, Ileana; Monteiro, Nicolas-Crespo; Ersen, Ovidiu; Brinkmann, Martin; Koch, Norbert

2014-04-01

Gold nanoparticles (Au-NPs) were deposited on the surface of n- and p-type organic semiconductors to form defined model systems for charge storage based electrically addressable memory elements. We used ultraviolet photoelectron spectroscopy to study the electronic properties and found that the Au-NPs become positively charged because of photoelectron emission, evidenced by spectral shifts to higher binding energy. Upon illumination with light that can be absorbed by the organic semiconductors, dynamic charge neutrality of the Au-NPs could be re-established through electron transfer from excitons. The light-controlled charge state of the Au-NPs could add optical addressability to memory elements.

The photoelectron-driven polar wind: Coupled fluid- semikinetic simulations and measurements by the thermal ion dynamics experiment on the POLAR spacecraft

NASA Astrophysics Data System (ADS)

Su, Yi-Jiun

1998-11-01

The polar wind is an ambipolar outflow of thermal plasma from the terrestrial high latitude ionosphere to the magnetosphere along geomagnetic field lines. This dissertation comprises a simulation and data analysis investigation of the polar wind from the ionosphere to the magnetosphere. In order to study the transport of ionospheric plasma from the collisional lower ionosphere to the collisionless magnetosphere, a self-consistent steady state coupled fluid-semikinetic model has been developed, which incorporates photoelectron and magnetospheric plasma effects. In applying this treatment to the simulation of the photoelectron-driven polar wind, an electric potential layer of the order of 40 Volts which develops above 3 RE altitude is obtained, when the downward magnetospheric electron fluxes are insufficient to balance the ionospheric photoelectron flux. This potential layer accelerates the ionospheric ions to supersonic speeds at high altitudes, but not at low altitudes (as some previous theories have suggested). In order to experimentally investigate the polar wind, low-energy ion data obtained by the Thermal Ion Dynamics Experiment (TIDE) on the POLAR satellite has been analyzed. A survey of the polar wind characteristics as observed by TIDE at 5000 km and 8 RE altitudes is presented in this dissertation. At 5000 km altitude, the H+ polar wind exhibited a supersonic outflow, while O+ displayed subsonic downflow. Dramatic decreases of the 5000 km H+ and O+ ion densities and fluxes correlated with increasing solar zenith angle for the ionospheric base, which is consistent with solar illumination ionization control of the 5000 km ion densities. However, the polar cap downward O+ flow and the density declined from dayside to nightside, which is also consistent with a cleft ion fountain origin for the polar cap O+. At 8 RE altitude, both H+ and O+ outflows were supersonic, and H+ was the dominant ion species. The typical velocity ratios, VO+:VHe+:VH+~2:3:5, may suggest transport processes which result in comparable energy gains, such as electric potential layer produced by photoelectron effects.

Experimental and theoretical studies of metal vapor atoms

NASA Astrophysics Data System (ADS)

Whitfield, Scott B.; Wehlitz, Ralf; Martins, Michael

2004-05-01

Employing electron spectrometry in conjunction with tuneable synchrotron radiation, we will present a detailed examination of the photoionization dynamics of selected metal vapor atoms. In particular, this paper will focus on the relative partial cross sections of the atomic Li K-shell main and satellite (ionization with excitation) photoelectron lines in the region of the strong 1 snℓ n'ℓ' autoionizing transitions, the atomic Sc 3 d, 4 s main and satellite photoelectron lines in the region of the 3 p→3 d giant resonance, and also the atomic Fe 3 d, 4 s main and satellite photoelectron lines in the same resonance region. Our experimental data for Sc and Fe will be compared to our state-of-the-art calculations based on the superposition of configuration method developed by Cowan (The Theory of Atomic Structure and Spectra. University of California Berkeley Press, Berkeley and Los Angeles, 1981). Our partial cross section measurements for Li and Sc will be complemented with measurements of the angular distribution parameter, β. In addition, our Li data will also be compared with recent R-matrix calculations (Phys. Rev. 57 (1998) 1045). In the case of Fe, we will also address the term dependent behavior of the partial cross sections on resonance. These results will highlight what can be achieved with today's technology and point the way towards future endeavors in the study of the photoionization dynamics of open-shell metal vapor atoms.

Dynamics of photoionization from molecular electronic wavepacket states in intense pulse laser fields: A nonadiabatic electron wavepacket study.

PubMed

Matsuoka, Takahide; Takatsuka, Kazuo

2017-04-07

A theory for dynamics of molecular photoionization from nonadiabatic electron wavepackets driven by intense pulse lasers is proposed. Time evolution of photoelectron distribution is evaluated in terms of out-going electron flux (current of the probability density of electrons) that has kinetic energy high enough to recede from the molecular system. The relevant electron flux is in turn evaluated with the complex-valued electronic wavefunctions that are time evolved in nonadiabatic electron wavepacket dynamics in laser fields. To uniquely rebuild such wavefunctions with its electronic population being lost by ionization, we adopt the complex-valued natural orbitals emerging from the electron density as building blocks of the total wavefunction. The method has been implemented into a quantum chemistry code, which is based on configuration state mixing for polyatomic molecules. Some of the practical aspects needed for its application will be presented. As a first illustrative example, we show the results of hydrogen molecule and its isotope substitutes (HD and DD), which are photoionized by a two-cycle pulse laser. Photon emission spectrum associated with above threshold ionization is also shown. Another example is taken from photoionization dynamics from an excited state of a water molecule. Qualitatively significant effects of nonadiabatic interaction on the photoelectron spectrum are demonstrated.

Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

NASA Astrophysics Data System (ADS)

Boguslavskiy, Andrey E.; Schalk, Oliver; Gador, Niklas; Glover, William J.; Mori, Toshifumi; Schultz, Thomas; Schuurman, Michael S.; Martínez, Todd J.; Stolow, Albert

2018-04-01

The ultrafast excited state dynamics of the smallest polyene, trans-1,3-butadiene, were studied by femtosecond time-resolved photoelectron-photoion coincidence (TRPEPICO) spectroscopy. The evolution of the excited state wavepacket, created by pumping the bright 1Bu (ππ*) electronic state at its origin of 216 nm, is projected via one- and two-photon ionization at 267 nm onto several ionization continua. The results are interpreted in terms of Koopmans' correlations and Franck-Condon factors for the excited and cationic states involved. The known predissociative character of the cation excited states is utilized to assign photoelectron bands to specific continua using TRPEPICO spectroscopy. This permits us to report the direct observation of the famously elusive S1(21Ag) dark electronic state during the internal conversion of trans 1,3-butadiene. Our phenomenological analysis permits the spectroscopic determination of several important time constants. We report the overall decay lifetimes of the 11Bu and 21Ag states and observe the re-appearance of the hot ground state molecule. We argue that the apparent dephasing time of the S2(11Bu) state, which leads to the extreme breadth of the absorption spectrum, is principally due to large amplitude torsional motion on the 1Bu surface in conjunction with strong non-adiabatic couplings via conical intersections, whereupon nuclear wavepacket revivals to the initial Franck-Condon region become effectively impossible. In Paper II [W. J. Glover et al., J. Chem. Phys. 148, 164303 (2018)], ab initio multiple spawning is used for on-the-fly computations of the excited state non-adiabatic wavepacket dynamics and their associated TRPEPICO observables, allowing for direct comparisons of experiment with theory.

Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Boguslavskiy, Andrey E.; Schalk, Oliver; Gador, Niklas

The ultrafast excited state dynamics of the smallest polyene, trans-1,3-butadiene, were studied by femtosecond time-resolved photoelectron-photoion coincidence (TRPEPICO) spectroscopy. The evolution of the excited state wavepacket, created by pumping the bright 1B u (ππ*) electronic state at its origin of 216 nm, is projected via one- and two-photon ionization at 267 nm onto several ionization continua. The results are interpreted in terms of Koopmans’ correlations and Franck-Condon factors for the excited and cationic states involved. The known predissociative character of the cation excited states is utilized to assign photoelectron bands to specific continua using TRPEPICO spectroscopy. This permits us tomore » report the direct observation of the famously elusive S 1(2 1A g) dark electronic state during the internal conversion of trans 1,3-butadiene. Our phenomenological analysis permits the spectroscopic determination of several important time constants. We report the overall decay lifetimes of the 1 1B u and 2 1A g states and observe the re-appearance of the hot ground state molecule. We argue that the apparent dephasing time of the S 2(1 1B u) state, which leads to the extreme breadth of the absorption spectrum, is principally due to large amplitude torsional motion on the 1B u surface in conjunction with strong non-adiabatic couplings via conical intersections, whereupon nuclear wavepacket revivals to the initial Franck-Condon region become effectively impossible. Lastly, in Paper II [W. J. Glover et al., J. Chem. Phys. 148, 164303 (2018)], ab initio multiple spawning is used for on-the-fly computations of the excited state non-adiabatic wavepacket dynamics and their associated TRPEPICO observables, allowing for direct comparisons of experiment with theory.« less

Excited state non-adiabatic dynamics of the smallest polyene, trans 1,3-butadiene. I. Time-resolved photoelectron-photoion coincidence spectroscopy

DOE PAGES

Boguslavskiy, Andrey E.; Schalk, Oliver; Gador, Niklas; ...

2018-04-27

The ultrafast excited state dynamics of the smallest polyene, trans-1,3-butadiene, were studied by femtosecond time-resolved photoelectron-photoion coincidence (TRPEPICO) spectroscopy. The evolution of the excited state wavepacket, created by pumping the bright 1B u (ππ*) electronic state at its origin of 216 nm, is projected via one- and two-photon ionization at 267 nm onto several ionization continua. The results are interpreted in terms of Koopmans’ correlations and Franck-Condon factors for the excited and cationic states involved. The known predissociative character of the cation excited states is utilized to assign photoelectron bands to specific continua using TRPEPICO spectroscopy. This permits us tomore » report the direct observation of the famously elusive S 1(2 1A g) dark electronic state during the internal conversion of trans 1,3-butadiene. Our phenomenological analysis permits the spectroscopic determination of several important time constants. We report the overall decay lifetimes of the 1 1B u and 2 1A g states and observe the re-appearance of the hot ground state molecule. We argue that the apparent dephasing time of the S 2(1 1B u) state, which leads to the extreme breadth of the absorption spectrum, is principally due to large amplitude torsional motion on the 1B u surface in conjunction with strong non-adiabatic couplings via conical intersections, whereupon nuclear wavepacket revivals to the initial Franck-Condon region become effectively impossible. Lastly, in Paper II [W. J. Glover et al., J. Chem. Phys. 148, 164303 (2018)], ab initio multiple spawning is used for on-the-fly computations of the excited state non-adiabatic wavepacket dynamics and their associated TRPEPICO observables, allowing for direct comparisons of experiment with theory.« less

Development of a simulation method for dynamics of electrons ejected from DNA molecules irradiated with X-rays.

PubMed

Kai, Takeshi; Higuchi, Mariko; Fujii, Kentaro; Watanabe, Ritsuko; Yokoya, Akinari

2012-12-01

To develop a method for simulating the dynamics of the photoelectrons and Auger electrons ejected from DNA molecules irradiated with pulsed monochromatic X-rays. A 30-base-pair (bp) DNA molecule was used as the target model, and the X-rays were assumed to have a Gaussian-shaped time distribution. Photoionization and Auger decay were considered as the atomic processes. The atoms from which the photoelectrons or Auger electrons were emitted were specified in the DNA molecule (or DNA ion) using the Monte Carlo method, and the trajectory of each electron in the electric field formed around the positively charged DNA molecule was calculated with a Newtonian equation. The kinetics of the electrons produced by irradiation with X-rays at an intensity ranging from 1 × 10(12) to 1 × 10(16) photons/mm(2) and energies of 380 eV (below the carbon K-edge), 435 eV (above the nitrogen K-edge), and 560 eV (above the oxygen K-edge) were evaluated. It was found that at an X-ray intensity of 1 × 10(14) photons/mm(2) or less, all the produced electrons escaped from the target. However, above an X-ray intensity of 1 × 10(15) photons/mm(2) and an energy of 560 eV, some photoelectrons that were ejected from the oxygen atoms were trapped near the target DNA. A simulation method for studying the trajectories of electrons ejected from a 30-bp DNA molecule irradiated with pulsed monochromatic X-rays has been developed. The present results show that electron dynamics are strongly dependent on the charged density induced in DNA by pulsed X-ray irradiation.

Investigation of the spectral properties and magnetism of BiFeO3 by dynamical mean-field theory

NASA Astrophysics Data System (ADS)

Paul, Souvik; Iuşan, Diana; Thunström, Patrik; Kvashnin, Yaroslav O.; Hellsvik, Johan; Pereiro, Manuel; Delin, Anna; Knut, Ronny; Phuyal, Dibya; Lindblad, Andreas; Karis, Olof; Sanyal, Biplab; Eriksson, Olle

2018-03-01

Using the local density approximation plus dynamical mean-field theory (LDA+DMFT), we have computed the valence-band photoelectron spectra and magnetic excitation spectra of BiFeO3, one of the most studied multiferroics. Within the DMFT approach, the local impurity problem is tackled by the exact diagonalization solver. The solution of the impurity problem within the LDA+DMFT method for the paramagnetic and magnetically ordered phases produces result in agreement with the experimental data on electronic and magnetic structures. For comparison, we also present results obtained by the LDA +U approach which is commonly used to compute the physical properties of this compound. Our LDA+DMFT derived electronic spectra match adequately with the experimental hard x-ray photoelectron spectroscopy and resonant photoelectron spectroscopy for Fe 3 d states, whereas the LDA +U method fails to capture the general features of the measured spectra. This indicates the importance of accurately incorporating the dynamical aspect of electronic correlation among Fe 3 d orbitals to reproduce the experimental excitation spectra. Specifically, the LDA+DMFT derived density of states exhibits a significant amount of Fe 3 d states at the position of Bi lone pairs, implying that the latter are not alone in the spectral scenario. This fact might modify our interpretation about the origin of ferroelectric polarization in this material. Our study demonstrates that the combination of orbital cross sections for the constituent elements and broadening schemes for the spectral functions are crucial to explain the detailed structures of the experimental electronic spectra. Our magnetic excitation spectra computed from the LDA+DMFT result conform well with the inelastic neutron scattering data.

Coupling a versatile aerosol apparatus to a synchrotron: Vacuum ultraviolet light scattering, photoelectron imaging, and fragment free mass spectrometry

NASA Astrophysics Data System (ADS)

Shu, Jinian; Wilson, Kevin R.; Ahmed, Musahid; Leone, Stephen R.

2006-04-01

An aerosol apparatus has been coupled to the Chemical Dynamics Beamline of the Advanced Light Source at Lawrence Berkeley National Laboratory. This apparatus has multiple capabilities for aerosol studies, including vacuum ultraviolet (VUV) light scattering, photoelectron imaging, and mass spectroscopy of aerosols. By utilizing an inlet system consisting of a 200μm orifice nozzle and aerodynamic lenses, aerosol particles of ˜50nm-˜1μm in diameter can be sampled directly from atmospheric pressure. The machine is versatile and can probe carbonaceous aerosols generated by a laboratory flame, nebulized solutions of biological molecules, hydrocarbon aerosol reaction products, and synthesized inorganic nanoparticles. The sensitivity of this apparatus is demonstrated by the detection of nanoparticles with VUV light scattering, photoelectron imaging, and charged particle detection. In addition to the detection of nanoparticles, the thermal vaporization of aerosols on a heater tip leads to the generation of intact gas phase molecules. This phenomenon coupled to threshold single photon ionization, accessible with tunable VUV light, allows for fragment-free mass spectrometry of complex molecules. The initial experiments with light scattering, photoelectron imaging, and aerosol mass spectrometry reported here serve as a demonstration of the design philosophy and multiple capabilities of the apparatus.

Strategic design and fabrication of acrylic shape memory polymers

NASA Astrophysics Data System (ADS)

Park, Ju Hyuk; Kim, Hansu; Ryoun Youn, Jae; Song, Young Seok

2017-08-01

Modulation of thermomechanics nature is a critical issue for an optimized use of shape memory polymers (SMPs). In this study, a strategic approach was proposed to control the transition temperature of SMPs. Free radical vinyl polymerization was employed for tailoring and preparing acrylic SMPs. Transition temperatures of the shape memory tri-copolymers were tuned by changing the composition of monomers. X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy analyses were carried out to evaluate the chemical structures and compositions of the synthesized SMPs. The thermomechanical properties and shape memory performance of the SMPs were also examined by performing dynamic mechanical thermal analysis. Numerical simulation based on a finite element method provided consistent results with experimental cyclic shape memory tests of the specimens. Transient shape recovery tests were conducted and optical transparence of the samples was identified. We envision that the materials proposed in this study can help develop a new type of shape-memory devices in biomedical and aerospace engineering applications.

SmB6 electron-phonon coupling constant from time- and angle-resolved photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Sterzi, A.; Crepaldi, A.; Cilento, F.; Manzoni, G.; Frantzeskakis, E.; Zacchigna, M.; van Heumen, E.; Huang, Y. K.; Golden, M. S.; Parmigiani, F.

2016-08-01

SmB6 is a mixed valence Kondo system resulting from the hybridization between localized f electrons and delocalized d electrons. We have investigated its out-of-equilibrium electron dynamics by means of time- and angle-resolved photoelectron spectroscopy. The transient electronic population above the Fermi level can be described by a time-dependent Fermi-Dirac distribution. By solving a two-temperature model that well reproduces the relaxation dynamics of the effective electronic temperature, we estimate the electron-phonon coupling constant λ to range from 0.13 ±0.03 to 0.04 ±0.01 . These extremes are obtained assuming a coupling of the electrons with either a phonon mode at 10 or 19 meV. A realistic value of the average phonon energy will give an actual value of λ within this range. Our results provide an experimental report on the material electron-phonon coupling, contributing to both the electronic transport and the macroscopic thermodynamic properties of SmB6.

Materials Properties and Solvated Electron Dynamics of Isolated Nanoparticles and Nanodroplets Probed with Ultrafast Extreme Ultraviolet Beams.

PubMed

Ellis, Jennifer L; Hickstein, Daniel D; Xiong, Wei; Dollar, Franklin; Palm, Brett B; Keister, K Ellen; Dorney, Kevin M; Ding, Chengyuan; Fan, Tingting; Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana; Jimenez, Jose L; Kapteyn, Henry C; Murnane, Margaret M

2016-02-18

We present ultrafast photoemission measurements of isolated nanoparticles in vacuum using extreme ultraviolet (EUV) light produced through high harmonic generation. Surface-selective static EUV photoemission measurements were performed on nanoparticles with a wide array of compositions, ranging from ionic crystals to nanodroplets of organic material. We find that the total photoelectron yield varies greatly with nanoparticle composition and provides insight into material properties such as the electron mean free path and effective mass. Additionally, we conduct time-resolved photoelectron yield measurements of isolated oleylamine nanodroplets, observing that EUV photons can create solvated electrons in liquid nanodroplets. Using photoemission from a time-delayed 790 nm pulse, we observe that a solvated electron is produced in an excited state and subsequently relaxes to its ground state with a lifetime of 151 ± 31 fs. This work demonstrates that femotosecond EUV photoemission is a versatile surface-sensitive probe of the properties and ultrafast dynamics of isolated nanoparticles.

Enhanced ultrafast relaxation rate in the Weyl semimetal phase of MoTe2 measured by time- and angle-resolved photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Crepaldi, A.; Autès, G.; Gatti, G.; Roth, S.; Sterzi, A.; Manzoni, G.; Zacchigna, M.; Cacho, C.; Chapman, R. T.; Springate, E.; Seddon, E. A.; Bugnon, Ph.; Magrez, A.; Berger, H.; Vobornik, I.; Kalläne, M.; Quer, A.; Rossnagel, K.; Parmigiani, F.; Yazyev, O. V.; Grioni, M.

2017-12-01

MoTe2 has recently been shown to realize in its low-temperature phase the type-II Weyl semimetal (WSM). We investigated by time- and angle- resolved photoelectron spectroscopy (tr-ARPES) the possible influence of the Weyl points on the electron dynamics above the Fermi level EF, by comparing the ultrafast response of MoTe2 in the trivial and topological phases. In the low-temperature WSM phase, we report an enhanced relaxation rate of electrons optically excited to the conduction band, which we interpret as a fingerprint of the local gap closure when Weyl points form. By contrast, we find that the electron dynamics of the related compound WTe2 is slower and temperature independent, consistent with a topologically trivial nature of this material. Our results shows that tr-ARPES is sensitive to the small modifications of the unoccupied band structure accompanying the structural and topological phase transition of MoTe2.

Global search in photoelectron diffraction structure determination using genetic algorithms

NASA Astrophysics Data System (ADS)

Viana, M. L.; Díez Muiño, R.; Soares, E. A.; Van Hove, M. A.; de Carvalho, V. E.

2007-11-01

Photoelectron diffraction (PED) is an experimental technique widely used to perform structural determinations of solid surfaces. Similarly to low-energy electron diffraction (LEED), structural determination by PED requires a fitting procedure between the experimental intensities and theoretical results obtained through simulations. Multiple scattering has been shown to be an effective approach for making such simulations. The quality of the fit can be quantified through the so-called R-factor. Therefore, the fitting procedure is, indeed, an R-factor minimization problem. However, the topography of the R-factor as a function of the structural and non-structural surface parameters to be determined is complex, and the task of finding the global minimum becomes tough, particularly for complex structures in which many parameters have to be adjusted. In this work we investigate the applicability of the genetic algorithm (GA) global optimization method to this problem. The GA is based on the evolution of species, and makes use of concepts such as crossover, elitism and mutation to perform the search. We show results of its application in the structural determination of three different systems: the Cu(111) surface through the use of energy-scanned experimental curves; the Ag(110)-c(2 × 2)-Sb system, in which a theory-theory fit was performed; and the Ag(111) surface for which angle-scanned experimental curves were used. We conclude that the GA is a highly efficient method to search for global minima in the optimization of the parameters that best fit the experimental photoelectron diffraction intensities to the theoretical ones.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Olivieri, Giorgia; Brown, Matthew A., E-mail: matthew.brown@mat.ethz.ch; Parry, Krista M.

Over the past decade, energy-dependent ambient pressure X-ray photoelectron spectroscopy (XPS) has emerged as a powerful analytical probe of the ion spatial distributions at the vapor (vacuum)-aqueous electrolyte interface. These experiments are often paired with complementary molecular dynamics (MD) simulations in an attempt to provide a complete description of the liquid interface. There is, however, no systematic protocol that permits a straightforward comparison of the two sets of results. XPS is an integrated technique that averages signals from multiple layers in a solution even at the lowest photoelectron kinetic energies routinely employed, whereas MD simulations provide a microscopic layer-by-layer descriptionmore » of the solution composition near the interface. Here, we use the National Institute of Standards and Technology database for the Simulation of Electron Spectra for Surface Analysis (SESSA) to quantitatively interpret atom-density profiles from MD simulations for XPS signal intensities using sodium and potassium iodide solutions as examples. We show that electron inelastic mean free paths calculated from a semi-empirical formula depend strongly on solution composition, varying by up to 30% between pure water and concentrated NaI. The XPS signal thus arises from different information depths in different solutions for a fixed photoelectron kinetic energy. XPS signal intensities are calculated using SESSA as a function of photoelectron kinetic energy (probe depth) and compared with a widely employed ad hoc method. SESSA simulations illustrate the importance of accounting for elastic-scattering events at low photoelectron kinetic energies (<300 eV) where the ad hoc method systematically underestimates the preferential enhancement of anions over cations. Finally, some technical aspects of applying SESSA to liquid interfaces are discussed.« less

Dynamics of electron solvation in I(-)(CH3OH)n clusters (4 ≤ n ≤ 11).

PubMed

Young, Ryan M; Yandell, Margaret A; Neumark, Daniel M

2011-03-28

The dynamics of electron solvation following excitation of the charge-transfer-to-solvent precursor state in iodide-doped methanol clusters, I(-)(CH(3)OH)(n = 4-11), are studied with time-resolved photoelectron imaging. This excitation produces a I···(CH(3)OH)(n)(-) cluster that is unstable with respect to electron autodetachment and whose autodetachment lifetime increases monotonically from ~800 fs to 85 ps as n increases from 4 to 11. The vertical detachment energy (VDE) and width of the excited state feature in the photoelectron spectrum show complex time dependence during the lifetime of this state. The VDE decreases over the first 100-400 fs, then rises exponentially to a maximum with a ~1 ps time constant, and finally decreases by as much as 180 meV with timescales of 3-20 ps. The early dynamics are associated with electron transfer from the iodide to the methanol cluster, while the longer-time changes in VDE are attributed to solvent reordering, possibly in conjunction with ejection of neutral iodine from the cluster. Changes in the observed width of the spectrum largely follow those of the VDEs; the dynamics of both are attributed to the major rearrangement of the solvent cluster during relaxation. The relaxation dynamics are interpreted as a reorientation of at least one methanol molecule and the disruption and formation of the solvent network in order to accommodate the excess charge.

Arc-Dynamic Calculations In The Rail Gun

DTIC Science & Technology

1983-11-01

16. C,A.L. Westerdahl , 1. Pinto, G,L, Ferrentino, T. Gora, ’Larse-Railsun Residue Material Photoelectron Spectroscopy,’ IEEE Trans. on (1983). D...8217 Ballistic Research Laboratory Report No. ARBRL-TR-02530, Oct 83. 15. J.D. Powell, private communication. • 16. C.A.L. Westerdahl , J. Pinto, G.L

Hydrogen bond dynamics of superheated water and methanol by ultrafast IR-pump and EUV-photoelectron probe spectroscopy.

PubMed

Vöhringer-Martinez, E; Link, O; Lugovoy, E; Siefermann, K R; Wiederschein, F; Grubmüller, H; Abel, B

2014-09-28

Supercritical water and methanol have recently drawn much attention in the field of green chemistry. It is crucial to an understanding of supercritical solvents to know their dynamics and to what extent hydrogen (H) bonds persist in these fluids. Here, we show that with femtosecond infrared (IR) laser pulses water and methanol can be heated to temperatures near and above their critical temperature Tc and their molecular dynamics can be studied via ultrafast photoelectron spectroscopy at liquid jet interfaces with high harmonics radiation. As opposed to previous studies, the main focus here is the comparison between the hydrogen bonded systems of methanol and water and their interpretation by theory. Superheated water initially forms a dense hot phase with spectral features resembling those of monomers in gas phase water. On longer timescales, this phase was found to build hot aggregates, whose size increases as a function of time. In contrast, methanol heated to temperatures near Tc initially forms a broad distribution of aggregate sizes and some gas. These experimental features are also found and analyzed in extended molecular dynamics simulations. Additionally, the simulations enabled us to relate the origin of the different behavior of these two hydrogen-bonded liquids to the nature of the intermolecular potentials. The combined experimental and theoretical approach delivers new insights into both superheated phases and may contribute to understand their different chemical reactivities.

Ionization, photoelectron dynamics and elastic scattering in relativistic, ultra-strong field

NASA Astrophysics Data System (ADS)

Luo, Sui

Ultrastrong laser-matter interaction has direct bearing to next generation technologies including plasma acceleration, laser fusion and attosecond X-ray generation. The commonly known physics in strong field becomes different as one progress to ultrastrong field. The works presented in this dissertation theoretically study the influence of relativistic effect and magnetic component of the laser field on the ionization, photoelectron dynamics and elastic scattering processes. The influence of magnetic component (B laser) of circularly polarized (CP) ultrastrong fields (up to3 x 1022 W/cm2) on atomic bound state dynamics is investigated. The Poincare plots are used to find the changes in trajectory energies are on the order of a few percent for intensities up to1 x 1022 W/cm2. It is found that at intensities where ionization approaches 50% for the bound state, the small changes from Blaser of the circular polarized light can actually result in a several-fold decrease in ionization probability. The force on the bound electron exerted by the Lorentz force from B laser is perpendicular to the rotating plane of the circular polarized light, and this nature makes those trajectories which are aligned away from the minimum in the potential barrier stabilized against tunneling ionization. Our results provide a classical understanding for ionization in ultrastrong fields and indicate that relativistic effects in ultrastrong field ionization may most easily be seen with CP fields. The photoelectron energy spectra from elastic rescattering in ultrastrong laser fields (up to 2x1019 W/cm2) is studied by using a relativistic adaption of a semi-classical three-step recollision model. The Hartree-Fock scattering potentials are used in calculating the elastic rescattering for both hydrogenlike and noble gas species. It is found that there is a reduction in elastic rescattering for intensities beyond 6 x 1016 W/cm2 when the laser Lorentz deflection of the photoelectron exceeds its wave-function spread. A relativistic rescattering enhancement occurs at 2 x 1018 W/cm2, commensurate with relativistic motion of a classical electron in a single field cycle. The good comparison between the results with available experiments suggests the theory approach is well suited to modeling scattering in the ultrastrong intensity regime. We investigate the elastic scattering process as it changes from strong to ultrastrong fields with the photoelectron angular distributions from Ne, Ar, and Xe. Noble gas species with Hartree-Fock scattering potentials show a reduction in elastic rescattering with the increasing energy of ultrastrong fields. It is found that as one increases the returning photoelectron energy, rescattering becomes the dominating mechanism behind the yield distribution as the emission angle for all the species extends from 0° to 90°. The relativistic effects and the magnetic field do not change the angular distribution until one is well into the Gamma r "1 regime where the Lorentz defection significantly reduces the yield. As we proceed to the highest energy, the angular emission range narrows as the mechanism changes over to backscattering into narrow angles along the electric field.

The timing resolution of scintillation-detector systems: Monte Carlo analysis

NASA Astrophysics Data System (ADS)

Choong, Woon-Seng

2009-11-01

Recent advancements in fast scintillating materials and fast photomultiplier tubes (PMTs) have stimulated renewed interest in time-of-flight (TOF) positron emission tomography (PET). It is well known that the improvement in the timing resolution in PET can significantly reduce the noise variance in the reconstructed image resulting in improved image quality. In order to evaluate the timing performance of scintillation detectors used in TOF PET, we use Monte Carlo analysis to model the physical processes (crystal geometry, crystal surface finish, scintillator rise time, scintillator decay time, photoelectron yield, PMT transit time spread, PMT single-electron response, amplifier response and time pick-off method) that can contribute to the timing resolution of scintillation-detector systems. In the Monte Carlo analysis, the photoelectron emissions are modeled by a rate function, which is used to generate the photoelectron time points. The rate function, which is simulated using Geant4, represents the combined intrinsic light emissions of the scintillator and the subsequent light transport through the crystal. The PMT output signal is determined by the superposition of the PMT single-electron response resulting from the photoelectron emissions. The transit time spread and the single-electron gain variation of the PMT are modeled in the analysis. Three practical time pick-off methods are considered in the analysis. Statistically, the best timing resolution is achieved with the first photoelectron timing. The calculated timing resolution suggests that a leading edge discriminator gives better timing performance than a constant fraction discriminator and produces comparable results when a two-threshold or three-threshold discriminator is used. For a typical PMT, the effect of detector noise on the timing resolution is negligible. The calculated timing resolution is found to improve with increasing mean photoelectron yield, decreasing scintillator decay time and decreasing transit time spread. However, only substantial improvement in the timing resolution is obtained with improved transit time spread if the first photoelectron timing is less than the transit time spread. While the calculated timing performance does not seem to be affected by the pixel size of the crystal, it improves for an etched crystal compared to a polished crystal. In addition, the calculated timing resolution degrades with increasing crystal length. These observations can be explained by studying the initial photoelectron rate. Experimental measurements provide reasonably good agreement with the calculated timing resolution. The Monte Carlo analysis developed in this work will allow us to optimize the scintillation detectors for timing and to understand the physical factors limiting their performance.

The timing resolution of scintillation-detector systems: Monte Carlo analysis.

PubMed

Choong, Woon-Seng

2009-11-07

Recent advancements in fast scintillating materials and fast photomultiplier tubes (PMTs) have stimulated renewed interest in time-of-flight (TOF) positron emission tomography (PET). It is well known that the improvement in the timing resolution in PET can significantly reduce the noise variance in the reconstructed image resulting in improved image quality. In order to evaluate the timing performance of scintillation detectors used in TOF PET, we use Monte Carlo analysis to model the physical processes (crystal geometry, crystal surface finish, scintillator rise time, scintillator decay time, photoelectron yield, PMT transit time spread, PMT single-electron response, amplifier response and time pick-off method) that can contribute to the timing resolution of scintillation-detector systems. In the Monte Carlo analysis, the photoelectron emissions are modeled by a rate function, which is used to generate the photoelectron time points. The rate function, which is simulated using Geant4, represents the combined intrinsic light emissions of the scintillator and the subsequent light transport through the crystal. The PMT output signal is determined by the superposition of the PMT single-electron response resulting from the photoelectron emissions. The transit time spread and the single-electron gain variation of the PMT are modeled in the analysis. Three practical time pick-off methods are considered in the analysis. Statistically, the best timing resolution is achieved with the first photoelectron timing. The calculated timing resolution suggests that a leading edge discriminator gives better timing performance than a constant fraction discriminator and produces comparable results when a two-threshold or three-threshold discriminator is used. For a typical PMT, the effect of detector noise on the timing resolution is negligible. The calculated timing resolution is found to improve with increasing mean photoelectron yield, decreasing scintillator decay time and decreasing transit time spread. However, only substantial improvement in the timing resolution is obtained with improved transit time spread if the first photoelectron timing is less than the transit time spread. While the calculated timing performance does not seem to be affected by the pixel size of the crystal, it improves for an etched crystal compared to a polished crystal. In addition, the calculated timing resolution degrades with increasing crystal length. These observations can be explained by studying the initial photoelectron rate. Experimental measurements provide reasonably good agreement with the calculated timing resolution. The Monte Carlo analysis developed in this work will allow us to optimize the scintillation detectors for timing and to understand the physical factors limiting their performance.

Isobutyl acetate: electronic state spectroscopy by high-resolution vacuum ultraviolet photoabsorption, He(I) photoelectron spectroscopy and ab initio calculations

NASA Astrophysics Data System (ADS)

Śmiałek, Malgorzata A.; Łabuda, Marta; Hubin-Franskin, Marie-Jeanne; Delwiche, Jacques; Hoffmann, Søren Vrønning; Jones, Nykola C.; Mason, Nigel J.; Limão-Vieira, Paulo

2017-05-01

The high-resolution vacuum ultraviolet photoabsorption spectrum of isobutyl acetate, C6H12O2, is presented here and was measured over the energy range 4.3-10.8 eV (290-115 nm). Valence and Rydberg transitions with their associated vibronic series have been observed in the photoabsorption spectrum and are assigned in accordance with new ab initio calculations of the vertical excitation energies and oscillator strengths. The measured photoabsorption cross sections have been used to calculate the photolysis lifetime of this ester in the Earth's upper atmosphere (20-50 km). Calculations have also been carried out to determine the ionization energies and fine structure of the lowest ionic state of isobutyl acetate and are compared with a photoelectron spectrum (from 9.5 to 16.7 eV), recorded for the first time. Vibrational structure is observed in the first photoelectron band of this molecule. Contribution to the Topical Issue: "Dynamics of Systems at the Nanoscale", edited by Andrey Solov'yov and Andrei Korol.

Femtosecond Time-Resolved Photoelectron Imaging of Excited Doped Helium Nanodroplets

NASA Astrophysics Data System (ADS)

Saladrigas, Catherine; Bacellar, Camila; Leone, Stephen R.; Neumark, Daniel M.; Gessner, Oliver

2017-04-01

Helium nanodroplets are excellent matrices for high resolution spectroscopy and the study of ultracold chemistry. They are optically transparent. In their electronic ground state, interact very weakly with any atomic or molecular dopant. Electronically excited droplets, however, can strongly interact with dopants through a variety of relaxation mechanisms. Previously, these host-dopant interactions were studied in the energy domain, revealing Penning ionization processes enabled by energy transfer between the droplet host and atomic dopants. Using femtosecond time resolved XUV photoelectron imaging, we plan to perform complementary experiments in the time domain to gain deeper insight into the timescales of energy transfer processes and how they compete with internal droplet relaxation. First experiments will be performed using noble gas dopants, such as Kr and Ne, which will be compared to previous energy-domain studies. Femtosecond XUV pulses produced by high harmonic generation will be used to excite the droplets, IR and near-UV light will be used to monitor the relaxation dynamics. Using velocity map imaging, both photoelectron kinetic energies and angular distributions will be recorded as a function of time. Preliminary results and proposed experiments will be presented.

Correlations Between Variations in Solar EUV and Soft X-Ray Irradiance and Photoelectron Energy Spectra Observed on Mars and Earth

NASA Technical Reports Server (NTRS)

Peterson, W. K.; Brain, D. A.; Mitchell, D. L.; Bailey, S. M.; Chamberlin, P. C.

2013-01-01

Solar extreme ultraviolet (EUV; 10-120 nm) and soft X-ray (XUV; 0-10 nm) radiation are major heat sources for the Mars thermosphere as well as the primary source of ionization that creates the ionosphere. In investigations of Mars thermospheric chemistry and dynamics, solar irradiance models are used to account for variations in this radiation. Because of limited proxies, irradiance models do a poor job of tracking the significant variations in irradiance intensity in the EUV and XUV ranges over solar rotation time scales when the Mars-Sun-Earth angle is large. Recent results from Earth observations show that variations in photoelectron energy spectra are useful monitors of EUV and XUV irradiance variability. Here we investigate photoelectron energy spectra observed by the Mars Global Surveyor (MGS) Electron Reflectometer (ER) and the FAST satellite during the interval in 2005 when Earth, Mars, and the Sun were aligned. The Earth photoelectron data in selected bands correlate well with calculations based on 1 nm resolution observations above 27 nm supplemented by broadband observations and a solar model in the 0-27 nm range. At Mars, we find that instrumental and orbital limitations to the identifications of photoelectron energy spectra in MGS/ER data preclude their use as a monitor of solar EUV and XUV variability. However, observations with higher temporal and energy resolution obtained at lower altitudes on Mars might allow the separation of the solar wind and ionospheric components of electron energy spectra so that they could be used as reliable monitors of variations in solar EUV and XUV irradiance than the time shifted, Earth-based, F(10.7) index currently used.

Correlations between variations in solar EUV and soft X-ray irradiance and photoelectron energy spectra observed on Mars and Earth

NASA Astrophysics Data System (ADS)

Peterson, W. K.; Brain, D. A.; Mitchell, D. L.; Bailey, S. M.; Chamberlin, P. C.

2013-11-01

extreme ultraviolet (EUV; 10-120 nm) and soft X-ray (XUV; 0-10 nm) radiation are major heat sources for the Mars thermosphere as well as the primary source of ionization that creates the ionosphere. In investigations of Mars thermospheric chemistry and dynamics, solar irradiance models are used to account for variations in this radiation. Because of limited proxies, irradiance models do a poor job of tracking the significant variations in irradiance intensity in the EUV and XUV ranges over solar rotation time scales when the Mars-Sun-Earth angle is large. Recent results from Earth observations show that variations in photoelectron energy spectra are useful monitors of EUV and XUV irradiance variability. Here we investigate photoelectron energy spectra observed by the Mars Global Surveyor (MGS) Electron Reflectometer (ER) and the FAST satellite during the interval in 2005 when Earth, Mars, and the Sun were aligned. The Earth photoelectron data in selected bands correlate well with calculations based on 1 nm resolution observations above 27 nm supplemented by broadband observations and a solar model in the 0-27 nm range. At Mars, we find that instrumental and orbital limitations to the identifications of photoelectron energy spectra in MGS/ER data preclude their use as a monitor of solar EUV and XUV variability. However, observations with higher temporal and energy resolution obtained at lower altitudes on Mars might allow the separation of the solar wind and ionospheric components of electron energy spectra so that they could be used as reliable monitors of variations in solar EUV and XUV irradiance than the time shifted, Earth-based, F10.7 index currently used.

Particle-In-Cell Simulations on Electric Field Antenna Characteristics in the Spacecraft Environment

NASA Astrophysics Data System (ADS)

Miyake, Y.; Usui, H.; Kojima, H.; Omura, Y.; Matsumoto, H.

2006-12-01

The Solar Terrestrial Physics (STP) group in Japan has organized a new magnetospheric mission named SCOPE whose objective is to investigate the scale-coupling process of plasma dynamics in the Terrestrial magnetosphere. For the sophisticated electric field measurements planned in the SCOPE mission, we have to investigate the antenna characteristics which are essential for the precise calibration of observed data. Particularly, (1) realistic antenna geometries including spacecraft body and (2) inhomogeneous plasma environment created by plasma-spacecraft interactions should be taken into consideration in the antenna analysis for application to the scientific mission. However, the analysis of the antenna impedance is very complex because the plasma is a dispersive and anisotropic medium, and thus it is too difficult to consider the realistic plasma environment near the spacecraft by the theoretical approaches. In the present study, we apply the Particle-In-Cell simulations to the antenna analysis, which enables us to treat the antenna model including a spacecraft body and analyze the effects of photoelectron emission on antenna characteristics. The present antenna model consists of perfect conducting antennas and spacecraft body, and the photoelectron emission from the sunlit surfaces is also modeled. Using these models, we first performed the electrostatic simulations and examined the photoelectron environment around the spacecraft. Next, the antenna impedance under the obtained photoelectron environment was examined by the electromagnetic simulations. Impedance values obtained in photoelectron environment were much different from those in free space, and they were analogous to the impedance characteristics of an equivalent electric circuit consisting of a resistance and capacitance connected in parallel. The validity of the obtained values has been examined by the comparison with the measurements by the scientific spacecraft.

Specific Anion Effects on Na+ Adsorption at the Aqueous Solution-Air Interface: MD Simulations, SESSA Calculations, and Photoelectron Spectroscopy Experiments.

PubMed

Olivieri, Giorgia; Parry, Krista M; D'Auria, Raffaella; Tobias, Douglas J; Brown, Matthew A

2018-01-18

Specific ion effects of the large halide anions have been shown to moderate anion adsorption to the air-water interface (AWI), but little quantitative attention has been paid to the behavior of alkali cations. Here we investigate the concentration and local distribution of sodium (Na + ) at the AWI in dilute (<1 M) aqueous solutions of NaCl, NaBr, and NaI using a combination of molecular dynamics (MD) and SESSA simulations, and liquid jet ambient pressure photoelectron spectroscopy measurements. We use SESSA to simulate Na 2p photoelectron intensities on the basis of the atom density profiles obtained from MD simulations, and we compare the simulation results with photoelectron spectroscopy experiments to evaluate the performance of a nonpolarizable force field model versus that of an induced dipole polarizable one. Our results show that the nonpolarizable force model developed by Horinek and co-workers (Chem. Phys. Lett. 2009, 479, 173-183) accurately predicts the local concentration and distribution of Na + near the AWI for all three electrolytes, whereas the polarizable model does not. To our knowledge, this is the first interface-specific spectroscopic validation of a MD force field. The molecular origins of the unique Na + distributions for the three electrolytes are analyzed on the basis of electrostatic arguments, and shown to arise from an indirect anion effect wherein the identity of the anion affects the strength of the attractive Na + -H 2 O electrostatic interaction. Finally, we use the photoelectron spectroscopy results to constrain the range of inelastic mean free paths (IMFPs) for the three electrolyte solutions used in the SESSA simulations that are able to reproduce the experimental intensities. Our results suggest that earlier estimates of IMFPs for aqueous solutions are likely too high.

Probing electronic binding potentials with attosecond photoelectron wavepackets

NASA Astrophysics Data System (ADS)

Kiesewetter, D.; Jones, R. R.; Camper, A.; Schoun, S. B.; Agostini, P.; Dimauro, L. F.

2018-01-01

The central goal of attosecond science is to visualize, understand and ultimately control electron dynamics in matter over the fastest relevant timescales. To date, numerous schemes have demonstrated exquisite temporal resolution, on the order of ten attoseconds, in measurements of the response of photo-excited electrons to time-delayed probes. However, attributing this response to specific dynamical mechanisms is difficult, requiring guidance from advanced calculations. Here we show that energy transfer between an oscillating field and low-energy attosecond photoelectron wavepackets directly provides coarse-grained information on the effective binding potential from which the electrons are liberated. We employ a dense extreme ultraviolet (XUV) harmonic comb to photoionize He, Ne and Ar atoms and record the electron spectra as a function of the phase of a mid-infrared dressing field. The amplitude and phase of the resulting interference modulations in the electron spectra reveal the average momentum and change in momentum of the electron wavepackets during the first quarter-period of the dressing field after their creation, reflecting the corresponding coarse characteristics of the binding potential.

Electron accommodation dynamics in the DNA base thymine

NASA Astrophysics Data System (ADS)

King, Sarah B.; Stephansen, Anne B.; Yokoi, Yuki; Yandell, Margaret A.; Kunin, Alice; Takayanagi, Toshiyuki; Neumark, Daniel M.

2015-07-01

The dynamics of electron attachment to the DNA base thymine are investigated using femtosecond time-resolved photoelectron imaging of the gas phase iodide-thymine (I-T) complex. An ultraviolet pump pulse ejects an electron from the iodide and prepares an iodine-thymine temporary negative ion that is photodetached with a near-IR probe pulse. The resulting photoelectrons are analyzed with velocity-map imaging. At excitation energies ranging from -120 meV to +90 meV with respect to the vertical detachment energy (VDE) of 4.05 eV for I-T, both the dipole-bound and valence-bound negative ions of thymine are observed. A slightly longer rise time for the valence-bound state than the dipole-bound state suggests that some of the dipole-bound anions convert to valence-bound species. No evidence is seen for a dipole-bound anion of thymine at higher excitation energies, in the range of 0.6 eV above the I-T VDE, which suggests that if the dipole-bound anion acts as a "doorway" to the valence-bound anion, it only does so at excitation energies near the VDE of the complex.

Electron accommodation dynamics in the DNA base thymine.

PubMed

King, Sarah B; Stephansen, Anne B; Yokoi, Yuki; Yandell, Margaret A; Kunin, Alice; Takayanagi, Toshiyuki; Neumark, Daniel M

2015-07-14

The dynamics of electron attachment to the DNA base thymine are investigated using femtosecond time-resolved photoelectron imaging of the gas phase iodide-thymine (I(-)T) complex. An ultraviolet pump pulse ejects an electron from the iodide and prepares an iodine-thymine temporary negative ion that is photodetached with a near-IR probe pulse. The resulting photoelectrons are analyzed with velocity-map imaging. At excitation energies ranging from -120 meV to +90 meV with respect to the vertical detachment energy (VDE) of 4.05 eV for I(-)T, both the dipole-bound and valence-bound negative ions of thymine are observed. A slightly longer rise time for the valence-bound state than the dipole-bound state suggests that some of the dipole-bound anions convert to valence-bound species. No evidence is seen for a dipole-bound anion of thymine at higher excitation energies, in the range of 0.6 eV above the I(-)T VDE, which suggests that if the dipole-bound anion acts as a "doorway" to the valence-bound anion, it only does so at excitation energies near the VDE of the complex.

Towards Highly-Efficient Phototriggered Data Storage by Utilizing a Diketopyrrolopyrrole-Based Photoelectronic Small Molecule.

PubMed

Li, Yang; Li, Hua; He, Jinghui; Xu, Qingfeng; Li, Najun; Chen, Dongyun; Lu, Jianmei

2016-07-20

A cooperative photoelectrical strategy is proposed for effectively modulating the performance of a multilevel data-storage device. By taking advantage of organic photoelectronic molecules as storage media, the fabricated device exhibited enhanced working parameters under the action of both optical and electrical inputs. In cooperation with UV light, the operating voltages of the memory device were decreased, which was beneficial for low energy consumption. Moreover, the ON/OFF current ratio was more tunable and facilitated high-resolution multilevel storage. Compared with previous methods that focused on tuning the storage media, this study provides an easy approach for optimizing organic devices through multiple physical channels. More importantly, this method holds promise for integrating multiple functionalities into high-density data-storage devices. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Rovibrational photoionization dynamics of methyl and its isotopomers studied by high-resolution photoionization and photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Schulenburg, A. M.; Alcaraz, Ch.; Grassi, G.; Merkt, F.

2006-09-01

High-resolution photoionization and pulsed-field-ionization zero-kinetic-energy photoelectron spectra of CH3, CH2D, CHD2, and CD3 have been recorded in the vicinity of the first adiabatic ionization threshold following single-photon excitation from the ground neutral state using a narrow-bandwidth vacuum-ultraviolet laser. The radicals were produced from the precursor molecules methyl-bromide, methyl-iodide, dimethyl-thioether, acetone, and nitromethane by 193nm excimer photolysis in a quartz capillary and were subsequently cooled to a rotational temperature Trot≈30K in a supersonic expansion. Nitromethane was identified as a particularly suitable photolytic precursor of methyl for studies by photoionization and threshold photoelectron spectroscopy. Thanks to the cold rotational temperature reached in the supersonic expansion, the rotational structure of the threshold ionization spectra could be resolved, and the photoionization dynamics investigated. Rydberg series converging on excited rotational levels of CH3+ could be observed in the range of principal quantum number n =30-50, and both rotational autoionization and predissociation were identified as decay processes in the threshold region. The observed photoionization transitions can be understood in the realm of an orbital model for direct ionization but the intensity distributions can only be fully accounted for if the rotational channel interactions mediated by the quadrupole of the cation are considered. Improved values of the adiabatic ionization thresholds were derived for all isotopomers [CH3: 79356.2(15)cm-1, CH2D: 79338.8(15)cm-1, CHD2: 79319.1(15)cm-1, and CD3: 79296.4(15)cm-1].

Photodissociation dynamics of allyl chloride at 200 and 266 nm studied by time-resolved mass spectrometry and photoelectron imaging.

PubMed

Shen, Huan; Chen, Jianjun; Hua, Linqiang; Zhang, Bing

2014-06-26

The photodissociation dynamics of allyl chloride at 200 and 266 nm has been studied by femtosecond time-resolved mass spectrometry coupled with photoelectron imaging. The molecule was prepared to different excited states by selectively pumping with 400 or 266 nm pulse. The dissociated products were then probed by multiphoton ionization with 800 nm pulse. After absorbing two photons at 400 nm, several dissociation channels were directly observed from the mass spectrum. The two important channels, C-Cl fission and HCl elimination, were found to decay with multiexponential functions. For C-Cl fission, two time constants, 48 ± 1 fs and 85 ± 40 ps, were observed. The first one was due to the fast predissociation process on the repulsive nσ*/πσ* state. The second one could be ascribed to dissociation on the vibrationally excited ground state which is generated after internal conversion from the initially prepared ππ* state. HCl elimination, which is a typical example of a molecular elimination reaction, was found to proceed with two time constants, 600 ± 135 fs and 14 ± 2 ps. We assigned the first one to dissociation on the excited state and the second one to the internal conversion from the ππ* state to the ground state and then dissociation on the ground state. As we excited the molecule with 266 nm light, the transient signals decayed exponentially with a time constant of ∼48 fs, which is coincident with the time scale of C-halogen direct dissociation. Photoelectron images, which provided translational and angular distributions of the generated electron, were also recorded. Detailed analysis of the kinetic energy distribution strongly suggested that C3H4(+) and C3H5(+) were generated from ionization of the neutral radical. The present study reveals the dissociation dynamics of allyl chloride in a time-resolved way.

Sequential and direct ionic excitation in the strong-field ionization of 1-butene molecules.

PubMed

Schell, Felix; Boguslavskiy, Andrey E; Schulz, Claus Peter; Patchkovskii, Serguei; Vrakking, Marc J J; Stolow, Albert; Mikosch, Jochen

2018-05-18

We study the Strong-Field Ionization (SFI) of the hydrocarbon 1-butene as a function of wavelength using photoion-photoelectron covariance and coincidence spectroscopy. We observe a striking transition in the fragment-associated photoelectron spectra: from a single Above Threshold Ionization (ATI) progression for photon energies less than the cation D0-D1 gap to two ATI progressions for a photon energy greater than this gap. For the first case, electronically excited cations are created by SFI populating the ground cationic state D0, followed by sequential post-ionization excitation. For the second case, direct sub-cycle SFI to the D1 excited cation state contributes significantly. Our experiments access ionization dynamics in a regime where strong-field and resonance-enhanced processes can interplay.

Femtosecond-laser-induced nonadiabatic alignment in photoexcited pyrimidine

NASA Astrophysics Data System (ADS)

Li, Shuai; Ling, Fengzi; Wang, Yanmei; Long, Jinyou; Deng, Xulan; Jin, Bing; Zhang, Bing

2017-09-01

The rotational wave-packet dynamics in electronically excited pyrimidine induced by a femtosecond laser pulse at 321.5 nm has been studied by time-resolved mass spectroscopy and photoelectron velocity-map imaging. The rotational revival features at 81.3 ps, which are the direct manifestation of field-free nonadiabatic alignment, are clearly observed in both the time-dependent ion yields and photoelectron angular distributions. In particular, the out-of-phase recurrences in the parent-ion and fragment-ions transients indicate the different directions of the ionization transition-dipole moments for the generation of the parent ion and fragment ions. By tuning the polarization of the probe light parallel or perpendicular to that of the pump light, we demonstrate the potential application of nonadiabatic alignment to manipulate the branching ratio of photoionization products.

A front-end read out chip for the OPERA scintillator tracker

NASA Astrophysics Data System (ADS)

Lucotte, A.; Bondil, S.; Borer, K.; Campagne, J. E.; Cazes, A.; Hess, M.; de La Taille, C.; Martin-Chassard, G.; Raux, L.; Repellin, J. P.

2004-04-01

Multi-anode photomultipliers H7546 are used to readout signal from the OPERA Scintillator Tracker (CERN/SPSC 2000-028, SPSC/P318, LNGSP 25/2000; CERN/SPSC 2001-025, SPSC/M668, LNGS-EXP30/2001). A 32-channel front-end Read Out Chip prototype accommodating the H7546 has been designed at LAL. This device features a low-noise, variable gain preamplifier to correct for multi-anode non-uniformity, an auto-trigger capability 100% efficient at a 0.3 photo-electron, and a charge measurement extending over a large dynamic range [0-100] photo-electrons. In this article we describe the ASIC architecture that is being implemented for the Target Tracker in OPERA, with a special emphasis put on the designs and the measured performance.

Photoionization of rare gas clusters

NASA Astrophysics Data System (ADS)

Zhang, Huaizhen

This thesis concentrates on the study of photoionization of van der Waals clusters with different cluster sizes. The goal of the experimental investigation is to understand the electronic structure of van der Waals clusters and the electronic dynamics. These studies are fundamental to understand the interaction between UV-X rays and clusters. The experiments were performed at the Advanced Light Source at Lawrence Berkeley National Laboratory. The experimental method employs angle-resolved time-of-flight photoelectron spectrometry, one of the most powerful methods for probing the electronic structure of atoms, molecules, clusters and solids. The van der Waals cluster photoionization studies are focused on probing the evolution of the photoelectron angular distribution parameter as a function of photon energy and cluster size. The angular distribution has been known to be a sensitive probe of the electronic structure in atoms and molecules. However, it has not been used in the case of van der Waals clusters. We carried out outer-valence levels, inner-valence levels and core-levels cluster photoionization experiments. Specifically, this work reports on the first quantitative measurements of the angular distribution parameters of rare gas clusters as a function of average cluster sizes. Our findings for xenon clusters is that the overall photon-energy-dependent behavior of the photoelectrons from the clusters is very similar to that of the corresponding free atoms. However, distinct differences in the angular distribution point at cluster-size-dependent effects were found. For krypton clusters, in the photon energy range where atomic photoelectrons have a high angular anisotropy, our measurements show considerably more isotropic angular distributions for the cluster photoelectrons, especially right above the 3d and 4p thresholds. For the valence electrons, a surprising difference between the two spin-orbit components was found. For argon clusters, we found that the angular distribution parameter values of the two-spin-orbit components from Ar 2p clusters are slightly different. When comparing the beta values for Ar between atoms and clusters, we found different results between Ar 3s atoms and clusters, and between Ar 3p atoms and clusters. Argon cluster resonance from surface and bulk were also measured. Furthermore, the angular distribution parameters of Ar cluster photoelectrons and Ar atom photoelectrons in the 3s → np ionization region were obtained.

Recent approaches for bridging the pressure gap in photoelectron microspectroscopy

PubMed Central

Kolmakov, Andrei; Gregoratti, Luca; Kiskinova, Maya; Günther, Sebastian

2016-01-01

Ambient-pressure photoelectron spectroscopy (APPES) and microscopy are at the frontier of modern chemical analysis at liquid-gas, solid-liquid and solid-gas interfaces, bridging science and engineering of functional materials. Complementing the current state-of-the art of the instruments, we survey in this short review several alternative APPES approaches, developed recently in the scanning photoelectron microscope (SPEM) at the Elettra laboratory. In particular, we report on experimental setups for dynamic near-ambient pressure environment, using pulsed-gas injection in the vicinity of samples or reaction cells with very small apertures, allowing for experiments without introducing additional differential pumping stages. The major part of the review is dedicated to the construction and performance of novel environmental cells using ultrathin electron-transparent but molecularly impermeable membranes to isolate the gas or liquid ambient from the electron detector operating in ultra-high vacuum (UHV). We demonstrate that two dimensional materials, such as graphene and derivatives, are mechanically robust to withstand atmospheric - UHV pressure differences and are sufficiently transparent for the photoelectrons emitted from samples immersed in the liquid or gaseous media. There are many unique opportunities for APPES using X-rays over a wide energy range. We show representative results that illustrate the potential of these ‘ambient-pressure’ approaches. Combined with the ca 100 nm lateral resolution of SPEM, they can overcome the pressure gap challenges and address the evolution of chemical composition and electronic structure at surface and interfaces under realistic operation conditions with unprecedented lateral and spectral resolution. PMID:28008215

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oloff, L.-P., E-mail: oloff@physik.uni-kiel.de; Hanff, K.; Stange, A.

With the advent of ultrashort-pulsed extreme ultraviolet sources, such as free-electron lasers or high-harmonic-generation (HHG) sources, a new research field for photoelectron spectroscopy has opened up in terms of femtosecond time-resolved pump-probe experiments. The impact of the high peak brilliance of these novel sources on photoemission spectra, so-called vacuum space-charge effects caused by the Coulomb interaction among the photoemitted probe electrons, has been studied extensively. However, possible distortions of the energy and momentum distributions of the probe photoelectrons caused by the low photon energy pump pulse due to the nonlinear emission of electrons have not been studied in detail yet.more » Here, we systematically investigate these pump laser-induced space-charge effects in a HHG-based experiment for the test case of highly oriented pyrolytic graphite. Specifically, we determine how the key parameters of the pump pulse—the excitation density, wavelength, spot size, and emitted electron energy distribution—affect the measured time-dependent energy and momentum distributions of the probe photoelectrons. The results are well reproduced by a simple mean-field model, which could open a path for the correction of pump laser-induced space-charge effects and thus toward probing ultrafast electron dynamics in strongly excited materials.« less

Effects of anodizing conditions and annealing temperature on the morphology and crystalline structure of anodic oxide layers grown on iron

NASA Astrophysics Data System (ADS)

Pawlik, Anna; Hnida, Katarzyna; Socha, Robert P.; Wiercigroch, Ewelina; Małek, Kamilla; Sulka, Grzegorz D.

2017-12-01

Anodic iron oxide layers were formed by anodization of the iron foil in an ethylene glycol-based electrolyte containing 0.2 M NH4F and 0.5 M H2O at 40 V for 1 h. The anodizing conditions such as electrolyte composition and applied potential were optimized. In order to examine the influence of electrolyte stirring and applied magnetic field, the anodic samples were prepared under the dynamic and static conditions in the presence or absence of magnetic field. It was shown that ordered iron oxide nanopore arrays could be obtained at lower anodizing temperatures (10 and 20 °C) at the static conditions without the magnetic field or at the dynamic conditions with the applied magnetic field. Since the as-prepared anodic layers are amorphous in nature, the samples were annealed in air at different temperatures (200-500 °C) for a fixed duration of time (1 h). The morphology and crystal phases developed after anodization and subsequent annealing were characterized using field-emission scanning electron microscopy (FE-SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The results proved that the annealing process transforms the amorphous layer into magnetite and hematite phases. In addition, the heat treatment results in a substantial decrease in the fluorine content and increase in the oxygen content.

Mechanism of resonant electron emission from the deprotonated GFP chromophore and its biomimetics.

PubMed

Bochenkova, Anastasia V; Mooney, Ciarán R S; Parkes, Michael A; Woodhouse, Joanne L; Zhang, Lijuan; Lewin, Ross; Ward, John M; Hailes, Helen C; Andersen, Lars H; Fielding, Helen H

2017-04-01

The Green Fluorescent Protein (GFP), which is widely used in bioimaging, is known to undergo light-induced redox transformations. Electron transfer is thought to occur resonantly through excited states of its chromophore; however, a detailed understanding of the electron gateway states of the chromophore is still missing. Here, we use photoelectron spectroscopy and high-level quantum chemistry calculations to show that following UV excitation, the ultrafast electron dynamics in the chromophore anion proceeds via an excited shape resonance strongly coupled to the open continuum. The impact of this state is found across the entire 355-315 nm excitation range, from above the first bound-bound transition to below the opening of higher-lying continua. By disentangling the electron dynamics in the photodetachment channels, we provide an important reference for the adiabatic position of the electron gateway state, which is located at 348 nm, and discover the source of the curiously large widths of the photoelectron spectra that have been reported in the literature. By introducing chemical modifications to the GFP chromophore, we show that the detachment threshold and the position of the gateway state, and hence the underlying excited-state dynamics, can be changed systematically. This enables a fine tuning of the intrinsic electron emission properties of the GFP chromophore and has significant implications for its function, suggesting that the biomimetic GFP chromophores are more stable to photooxidation.

Multiphoton Rydberg and valence dynamics of CH3Br probed by mass spectrometry and slice imaging.

PubMed

Hafliðason, Arnar; Glodic, Pavle; Koumarianou, Greta; Samartzis, Peter C; Kvaran, Ágúst

2018-06-18

The multiphoton dynamics of CH3Br were probed by Mass Resolved MultiPhoton Ionization (MR-MPI), Slice Imaging and Photoelectron Imaging in the two-photon excitation region of 66 000 to 80 000 cm-1. Slice images of the CH3+ and Br+ photoproducts of ten two-photon resonant transitions to np and nd Rydberg states of the parent molecule were recorded. CH3+ ions dominate the mass spectra. Kinetic energy release spectra (KERs) were derived from slice and photoelectron images and anisotropy parameters were extracted from the angular distributions of the ions to identify the processes and the dynamics involved. At all wavelengths we observe three-photon excitations, via the two-photon resonant transitions to molecular Rydberg states, forming metastable, superexcited (CH3Br#) states which dissociate to form CH3 Rydberg states (CH3**) along with Br/Br*. A correlation between the parent Rydberg states excited and CH3** formed is evident. For the three highest excitation energies used, the CH3Br# metastable states also generate high kinetic energy fragments of CH3(X) and Br/Br*. In addition for two out of these three wavelengths we also measure one-photon photolysis of CH3Br in the A band forming CH3(X) in various vibrational modes and bromine atoms in the ground (Br) and spin-orbit excited (Br*) states.

Toward Femtosecond Time-Resolved Studies of Solvent-Solute Energy Transfer in Doped Helium Nanodroplets

NASA Astrophysics Data System (ADS)

Bacellar, C.; Ziemkiewicz, M. P.; Leone, S. R.; Neumark, D. M.; Gessner, O.

2015-05-01

Superfluid helium nanodroplets provide a unique cryogenic matrix for high resolution spectroscopy and ultracold chemistry applications. With increasing photon energy and, in particular, in the increasingly important Extreme Ultraviolet (EUV) regime, the droplets become optically dense and, therefore, participate in the EUV-induced dynamics. Energy- and charge-transfer mechanisms between the host droplets and dopant atoms, however, are poorly understood. Static energy domain measurements of helium droplets doped with noble gas atoms (Xe, Kr) indicate that Penning ionization due to energy transfer from the excited droplet to dopant atoms may be a significant relaxation channel. We have set up a femtosecond time-resolved photoelectron imaging experiment to probe these dynamics directly in the time-domain. Droplets containing 104 to 106 helium atoms and a small percentage (<10-4) of dopant atoms (Xe, Kr, Ne) are excited to the 1s2p Rydberg band by 21.6 eV photons produced by high harmonic generation (HHG). Transiently populated states are probed by 1.6 eV photons, generating time-dependent photoelectron kinetic energy distributions, which are monitored by velocity map imaging (VMI). The results will provide new information about the dynamic timescales and the different relaxation channels, giving access to a more complete physical picture of solvent-solute interactions in the superfluid environment. Prospects and challenges of the novel experiment as well as preliminary experimental results will be discussed.

Sensitive Infrared Photodetectors: Optimized Electron Kinetics for Room-Temperature Operation

DTIC Science & Technology

2010-12-20

QD levels; (iii) High photoconductive gain and responsivity; (iv) Low generation-recombination noise due to the long photoelectron lifetime. The...etc. [1-6]. For example, quantum-well infrared photodetectors ( QWIPs ) is currently a well-established technology, which is widely employed in...various imaging devices working at liquid nitrogen temperatures and below [7,8]. At 77K, modern QWIPs operating around λ = 10 μm demonstrate the

Dynamical photoionization observables of the CS molecule: The role of electron correlation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ponzi, Aurora; Coriani, Sonia; Decleva, Piero

2014-05-28

Highly correlated calculations are performed on the primary ionic states and the prominent satellite present in the outer valence photoelectron spectrum of carbon monosulfide (CS). Dyson orbitals are coupled to accurate one particle continuum orbitals to provide a correlated description of energy dependent cross sections, asymmetry parameters, branching ratios, and molecular frame photoelectron angular distributions. The comparison with results obtained at the Hartree-Fock and Density Functional Theory level shows the strong sensitivity of these observables to details of the correlation in the bound states. The behaviour of the well characterized satellite state is analyzed in detail, and shows differences frommore » the relevant primary states, revealing the limitations of a simple intensity borrowing mechanism. The results resolve the intensity disagreement with experiment obtained at the level of the sudden approximation.« less

Extracting attosecond delays from spectrally overlapping interferograms

NASA Astrophysics Data System (ADS)

Jordan, Inga; Wörner, Hans Jakob

2018-02-01

Attosecond interferometry is becoming an increasingly popular technique for measuring the dynamics of photoionization in real time. Whereas early measurements focused on atomic systems with very simple photoelectron spectra, the technique is now being applied to more complex systems including isolated molecules and solids. The increase in complexity translates into an augmented spectral congestion, unavoidably resulting in spectral overlap in attosecond interferograms. Here, we discuss currently used methods for phase retrieval and introduce two new approaches for determining attosecond photoemission delays from spectrally overlapping photoelectron spectra. We show that the previously used technique, consisting in the spectral integration of the areas of interest, does in general not provide reliable results. Our methods resolve this problem, thereby opening the technique of attosecond interferometry to complex systems and fully exploiting its specific advantages in terms of spectral resolution compared to attosecond streaking.

Unraveling the electronic relaxation dynamics in photoexcited 2,4-difluoroaniline via femtosecond time-resolved photoelectron imaging

NASA Astrophysics Data System (ADS)

Ling, Fengzi; Li, Shuai; Wei, Jie; Liu, Kai; Wang, Yanmei; Zhang, Bing

2018-04-01

Time-resolved photoelectron imaging is employed to investigate the relaxation dynamics of the lowest two excited electronic states S1(ππ*) and S2(π3s/πσ*) in 2,4-difluoroaniline (24DFA). As the S1(ππ*) state is populated directly following 289 nm excitation, the population undergoes ultrafast intramolecular vibrational redistribution on a 540 fs time scale, followed by efficient intersystem crossing from S1(ππ*) to the triplet state within 379 ps, and the subsequent slower deactivation process of the triplet state. For excitation to the S2(π3s/πσ*) state at 238 nm, the population probably bifurcates into two decay channels. The dominant channel with 84 fs involves ultrafast internal conversion to the S1(ππ*) state, from which it relaxes to the electronic ground state on a 116 ps time scale. The other appears to involve motion along the S2(π3s/πσ*) potential energy surface. Our data also determine experimentally the electronic energies of S2(π3s/πσ*), S3(ππ*), and several Rydberg states in 24DFA.

Real-time detection of S(1D2) photofragments produced from the 1B2(1Σu+) state of CS2 by vacuum ultraviolet photoelectron imaging using 133 nm probe pulses

NASA Astrophysics Data System (ADS)

Horio, Takuya; Spesyvtsev, Roman; Furumido, Yu; Suzuki, Toshinori

2017-07-01

Ultrafast photodissociation dynamics from the 1B2(1Σu+) state of CS2 are studied by time-resolved photoelectron imaging using the fourth (4ω, 198 nm) and sixth (6ω, 133 nm) harmonics of a femtosecond Ti:sapphire laser. The 1B2 state of CS2 was prepared with the 4ω pulses, and subsequent dynamics were probed using the 6ω vacuum ultraviolet (VUV) pulses. The VUV pulses enabled real-time detection of S(1D2) photofragments, produced via CS2*(1B2(1Σu+)) → CS(X 1Σ+) + S(1D2). The photoionization signal of dissociating CS2*(1B2(1Σu+)) molecules starts to decrease at about 100 fs, while the S(1D2) fragments appear with a finite (ca. 400 fs) delay time after the pump pulse. Also discussed is the configuration interaction of the 1B2(1Σu+) state based on relative photoionization cross-sections to different cationic states.

Photodissociation of Small Molecules and Photoionization of Free Radicals Using the VUV Velocity-Map Imaging Photoion and Photoelectron Method

NASA Astrophysics Data System (ADS)

Gao, Hong

The tunable vacuum ultraviolet (VUV) laser generated through the two-photon resonance-enhanced four-wave mixing scheme is combined with the newly developed time-slice velocity map imaging photoion method to study the photodissociation of small molecules in the VUV region, and with the velocity map imaging photoelectron method to study the photoionization of free radicals. The photodissociation dynamics of NO in the energy region around 13.5 eV has been investigated. Branching ratios of the three lowest dissociation channels of 12C 16O that produce C(3P) + O(3P), C( 1D) + O(3P) and C(3P) + O(1D) are measured for the first time in the VUV region from 102,500 cm-1 to 110,500 cm-1, valuable information of the dissociation dynamics for this prototype system has been deduced. We demonstrated an experiment that has two independently tunable VUV lasers and a time-slice velocity map imaging setup, this provides us a global way to perform systematic state-selected photodissociation of small molecules via state-selected detection of the atomic products in the VUV region. The velocity map imaging photoelectron method was successfully used to obtain the photoelectron spectrum of the propargyl radical (C3H3) via a single VUV photoionization process. The propargyl radical is generated by the 193 nm laser photodissociation of the precursor C3H3Cl. This is the first time that the velocity map imaging photoelectron method is used to get the photoelectron spectra of free radicals, indicating that it is a powerful technique for studying the photoionization of free radicals which are always hard to be produced with high enough number densities for spectroscopic studies. This dissertation is mainly based on the following peer-reviewed journal articles: 1. Hong Gao, Yang Pan, Lei Yang, Jingang Zhou, C. Y. Ng and William M. Jackson. "Time-slice velocity-map ion imaging studies of the Photodissociation of NO in the vacuum ultraviolet region", the Journal of Chemical Physics, 136, 134302 (2012). (Chapter 2) 2. Hong Gao, Yu Song, Lei Yang, Xiaoyu Shi, Qing-Zhu Yin, C. Y. Ng and William M. Jackson. "Branching ratio measurements of the predissociation of 12C16O by time-slice velocity-map ion imaging in the energy region from 108,000 to 110,500 cm-1", the Journal of Chemical Physics, 137, 034305 (2012). (Chapter 3) 3. Hong Gao, Yu Song, Yih-Chung Chang, Xiaoyu Shi, Qing-Zhu Yin, Roger C. Wiens, William M. Jackson, C. Y. Ng, "Branching Ratio Measurements for Vacuum Ultraviolet Photodissociation of 12C16O", the Journal of Physical Chemistry A. (article online ASAP). (Chapter 4) 4. Hong Gao, Yu Song, C. Y. Ng, William M. Jackson, " Communication: State-to-state photodissociation study by the two-color VUV-VUV laser pump-probe time-slice velocity-map-imaging-photoion method", the Journal of Chemical Physics, 138, 191102(2013). (Chapter 5) 5. Hong Gao, Zhou Lu, Lei Yang, Jingang Zhou, C. Y. Ng, "Communication: A vibrational study of propargyl cation using the vacuum ultraviolet laser velocity-map imaging photoelectron method", the Journal of Chemical Physics, 137, 161101(2012). (Chapter 6)

Continuous roll-to-roll growth of graphene films by chemical vapor deposition

NASA Astrophysics Data System (ADS)

Hesjedal, Thorsten

2011-03-01

Few-layer graphene is obtained in atmospheric chemical vapor deposition on polycrystalline copper in a roll-to-roll process. Raman and x-ray photoelectron spectroscopy were employed to confirm the few-layer nature of the graphene film, to map the inhomogeneities, and to study and optimize the growth process. This continuous growth process can be easily scaled up and enables the low-cost fabrication of graphene films for industrial applications.

Ultrafast photodissociation dynamics of 1,4-diiodobenzene

NASA Astrophysics Data System (ADS)

Stankus, Brian; Zotev, Nikola; Rogers, David M.; Gao, Yan; Odate, Asami; Kirrander, Adam; Weber, Peter M.

2018-05-01

The photodissociation dynamics of 1,4-diiodobenzene is investigated using ultrafast time-resolved photoelectron spectroscopy. Following excitation by laser pulses at 271 nm, the excited-state dynamics is probed by resonance-enhanced multiphoton ionization with 405 nm probe pulses. A progression of Rydberg states, which come into resonance sequentially, provide a fingerprint of the dissociation dynamics of the molecule. The initial excitation decays with a lifetime of 33 ± 4 fs, in good agreement with a previous study. The spectrum is interpreted by reference to ab initio calculations at the CASPT2(18,14) level, including spin-orbit coupling. We propose that both the 5B1 and 6B1 states are excited initially, and based on the calculations, we identify diabatic spin-orbit coupled states corresponding to the main dissociation pathways.

Ultrafast X-Ray Spectroscopy of Conical Intersections

NASA Astrophysics Data System (ADS)

Neville, Simon P.; Chergui, Majed; Stolow, Albert; Schuurman, Michael S.

2018-06-01

Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S2(π π*) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections.

Quantum mechanics/molecular mechanics modeling of photoelectron spectra: the carbon 1s core-electron binding energies of ethanol-water solutions.

PubMed

Löytynoja, T; Niskanen, J; Jänkälä, K; Vahtras, O; Rinkevicius, Z; Ågren, H

2014-11-20

Using ethanol-water solutions as illustration, we demonstrate the capability of the hybrid quantum mechanics/molecular mechanics (QM/MM) paradigm to simulate core photoelectron spectroscopy: the binding energies and the chemical shifts. An integrated approach with QM/MM binding energy calculations coupled to preceding molecular dynamics sampling is adopted to generate binding energies averaged over the solute-solvent configurations available at a particular temperature and pressure and thus allowing for a statistical assessment with confidence levels for the final binding energies. The results are analyzed in terms of the contributions in the molecular mechanics model-electrostatic, polarization, and van der Waals-with atom or bond granulation of the corresponding MM charge and polarizability force-fields. The role of extramolecular charge transfer screening of the core-hole and explicit hydrogen bonding is studied by extending the QM core to cover the first solvation shell. The results are compared to those obtained from pure electrostatic and polarizable continuum models. Particularly, the dependence of the carbon 1s binding energies with respect to the ethanol concentration is studied. Our results indicate that QM/MM can be used as an all-encompassing model to study photoelectron binding energies and chemical shifts in solvent environments.

Attosecond-resolved photoionization of chiral molecules.

PubMed

Beaulieu, S; Comby, A; Clergerie, A; Caillat, J; Descamps, D; Dudovich, N; Fabre, B; Géneaux, R; Légaré, F; Petit, S; Pons, B; Porat, G; Ruchon, T; Taïeb, R; Blanchet, V; Mairesse, Y

2017-12-08

Chiral light-matter interactions have been investigated for two centuries, leading to the discovery of many chiroptical processes used for discrimination of enantiomers. Whereas most chiroptical effects result from a response of bound electrons, photoionization can produce much stronger chiral signals that manifest as asymmetries in the angular distribution of the photoelectrons along the light-propagation axis. We implemented self-referenced attosecond photoelectron interferometry to measure the temporal profile of the forward and backward electron wave packets emitted upon photoionization of camphor by circularly polarized laser pulses. We measured a delay between electrons ejected forward and backward, which depends on the ejection angle and reaches 24 attoseconds. The asymmetric temporal shape of electron wave packets emitted through an autoionizing state further reveals the chiral character of strongly correlated electronic dynamics. Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

Test techniques for determining laser ranging system performance

NASA Technical Reports Server (NTRS)

Zagwodzki, T. W.

1981-01-01

Procedures and results of an on going test program intended to evaluate laser ranging system performance levels in the field as well as in the laboratory are summarized. Tests show that laser ranging system design requires consideration of time biases and RMS jitters of individual system components. All simple Q switched lasers tested were found to be inadequate for 10 centimeter ranging systems. Timing discriminators operating over a typical 100:1 dynamic signal range may introduce as much as 7 to 9 centimeters of range bias. Time interval units commercially available today are capable of half centimeter performance and are adequate for all field systems currently deployed. Photomultipliers tested show typical tube time biases of one centimeter with single photoelectron transit time jitter of approximately 10 centimeters. Test results demonstrate that NASA's Mobile Laser Ranging System (MOBLAS) receiver configuration is limiting system performance below the 100 photoelectron level.

Time-dependent many-body treatment of electron-boson dynamics: Application to plasmon-accompanied photoemission

NASA Astrophysics Data System (ADS)

Schüler, M.; Berakdar, J.; Pavlyukh, Y.

2016-02-01

Recent experiments access the time-resolved photoelectron signal originating from plasmon satellites in correlated materials and address their buildup and decay in real time. Motivated by these developments, we present the Kadanoff-Baym formalism for the nonequilibrium time evolution of interacting fermions and bosons. In contrast to the fermionic case, the bosons are described by second-order differential equations. Solution of the bosonic Kadanoff-Baym equations—which is the central ingredient of this work—requires substantial modification of the usual two-times electronic propagation scheme. The solution is quite general and can be applied to a number of problems, such as the interaction of electrons with quantized photons, phonons, and other bosonic excitations. Here the formalism is applied to the photoemission from a deep core hole accompanied by plasmon excitation. We compute the time-resolved photoelectron spectra and discuss the effects of intrinsic and extrinsic electron energy losses and their interference.

Spatiotemporal interference of photoelectron wave packets and the time scale of nonadiabatic transitions in the high-frequency regime

NASA Astrophysics Data System (ADS)

Toyota, Koudai

2016-10-01

The method of the envelope Hamiltonian [K. Toyota, U. Saalmann, and J. M. Rost, New J. Phys. 17, 073005 (2015), 10.1088/1367-2630/17/7/073005] is applied to further study a detachment dynamics of a model negative ion in one dimension in the high-frequency regime. This method is based on the Floquet approach, but the time dependency of an envelope function is explicitly kept for arbitrary pulse durations. Therefore, it is capable of describing not only a photon absorption or emission, but also a nonadiabatic transition which is induced by the time-varying envelope of the pulse. It was shown that the envelope Hamiltonian accurately retrieves the results obtained by the time-dependent Schrödinger equation, and the underlying physics were well understood by the adiabatic approximation based on the envelope Hamiltonian. In this paper, we explore two more aspects of the detachment dynamics, which were not considered in our previous work. First, we determine the features of both a spatial and temporal interference of photoelectron wave packets in a photon-absorption process. We conclude that both of the interference mechanisms are universal in ionization dynamics in the high-frequency regime. Second, we extract a pulse duration which maximizes a yield of the nonadiabatic transition as a function of a pulse duration. It is shown that it becomes maximum when the pulse duration is comparable to a time scale of an electron.

Earle K. Plyler Prize Lecture: The Three Pillars of Ultrafast Molecular Science - Time, Phase, Intensity

NASA Astrophysics Data System (ADS)

Stolow, Albert

We discuss the probing and control of molecular wavepacket dynamics in the context of three main `pillars' of light-matter interaction: time, phase, intensity. Time: Using short, coherent laser pulses and perturbative matter-field interactions, we study molecular wavepackets with a focus on the ultrafast non-Born-Oppenheimer dynamics, that is, the coupling of electronic and nuclear motions. Time-Resolved Photoelectron Spectroscopy (TRPES) is a powerful ultrafast probe of these processes in polyatomic molecules because it is sensitive both electronic and vibrational dynamics. Ideally, one would like to observe these ultrafast processes from the molecule's point of view - the Molecular Frame - thereby avoiding loss of information due to orientational averaging. This can be achieved by Time-Resolved Coincidence Imaging Spectroscopy (TRCIS) which images 3D recoil vectors of both photofragments and photoelectrons, in coincidence and as a function of time, permitting direct Molecular Frame imaging of valence electronic dynamics during a molecular dynamics. Phase: Using intermediate strength non-perturbative interactions, we apply the second order (polarizability) Non-Resonant Dynamic Stark Effect (NRDSE) to control molecular dynamics without any net absorption of light. NRDSE is also the interaction underlying molecular alignment and applies to field-free 1D of linear molecules and field-free 3D alignment of general (asymmetric) molecules. Using laser alignment, we can transiently fix a molecule in space, yielding a more general approach to direct Molecular Frame imaging of valence electronic dynamics during a chemical reaction. Intensity: In strong (ionizing) laser fields, a new laser-matter physics emerges for polyatomic systems wherein both the single active electron picture and the adiabatic electron response, both implicit in the standard 3-step models, can fail dramatically. This has important consequences for all attosecond strong field spectroscopies of polyatomic molecules, including high harmonic generation (HHG). We discuss an experimental method, Channel-Resolved Above Threshold Ionization (CRATI), which directly unveils the electronic channels participating in the attosecond molecular strong field ionization response [10]. This work was supported by the National Research Council of Canada and the Natural Sciences & Engineering Research Council.

Particle Simulations of the Guard Electrode Effects on the Photoelectron Distribution Around an Electric Field Sensor

NASA Astrophysics Data System (ADS)

Miyake, Y.; Usui, H.; Kojima, H.

2010-12-01

In tenuous space plasma environment, photoelectrons emitted due to solar illumination produce a high-density photoelectron cloud localized in the vicinity of a spacecraft body and an electric field sensor. The photoelectron current emitted from the sensor has also received considerable attention because it becomes a primary factor in determining floating potentials of the sunlit spacecraft and sensor bodies. Considering the fact that asymmetric photoelectron distribution between sunlit and sunless sides of the spacecraft occasionally causes a spurious sunward electric field, we require quantitative evaluation of the photoelectron distribution around the spacecraft and its influence on electric field measurements by means of a numerical approach. In the current study, we applied the Particle-in-Cell plasma simulation to the analysis of the photoelectron environment around spacecraft. By using the PIC modeling, we can self-consistently consider the plasma kinetics. This enables us to simulate the formation of the photoelectron cloud as well as the spacecraft and sensor charging in a self-consistent manner. We report the progress of an analysis on photoelectron environment around MEFISTO, which is an electric field instrument for the BepiColombo/MMO spacecraft to Mercury’s magnetosphere. The photoelectron guard electrode is a key technology for ensuring an optimum photoelectron environment. We show some simulation results on the guard electrode effects on surrounding photoelectrons and discuss a guard operation condition for producing the optimum photoelectron environment. We also deal with another important issue, that is, how the guard electrode can mitigate an undesirable influence of an asymmetric photoelectron distribution on electric field measurements.

Electrochemical synthesis of self-organized TiO2 crystalline nanotubes without annealing

NASA Astrophysics Data System (ADS)

Giorgi, Leonardo; Dikonimos, Theodoros; Giorgi, Rossella; Buonocore, Francesco; Faggio, Giuliana; Messina, Giacomo; Lisi, Nicola

2018-03-01

This work demonstrates that upon anodic polarization in an aqueous fluoride-containing electrolyte, TiO2 nanotube array films can be formed with a well-defined crystalline phase, rather than an amorphous one. The crystalline phase was obtained avoiding any high temperature annealing. We studied the formation of nanotubes in an HF/H2O medium and the development of crystalline grains on the nanotube wall, and we found a facile way to achieve crystalline TiO2 nanotube arrays through a one-step anodization. The crystallinity of the film was influenced by the synthesis parameters, and the optimization of the electrolyte composition and anodization conditions (applied voltage and time) were carried out. For comparison purposes, crystalline anatase TiO2 nanotubes were also prepared by thermal treatment of amorphous nanotubes grown in an organic bath (ethylene glycol/NH4F/H2O). The morphology and the crystallinity of the nanotubes were studied by field emission gun-scanning electron microscopy (FEG-SEM) and Raman spectroscopy, whereas the electrochemical and semiconducting properties were analyzed by means of linear sweep voltammetry, impedance spectroscopy, and Mott-Schottky plots. X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS) allowed us to determine the surface composition and the electronic structure of the samples and to correlate them with the electrochemical data. The optimal conditions to achieve a crystalline phase with high donor concentration are defined.

X-Ray Photoelectron Spectroscopy and Ultrahigh Vacuum Contactless Capacitance-Voltage Characterization of Novel Oxide-Free InP Passivation Process Using a Silicon Surface Quantum Well

NASA Astrophysics Data System (ADS)

Takahashi, Hiroshi; Hashizume, Tamotsu; Hasegawa, Hideki

1999-02-01

In order to understand and optimize a novel oxide-free InP passivation process using a silicon surface quantum well, a detailed in situ X-ray photoelectron spectroscopy (XPS) and ultrahigh vacuum (UHV) contactless capacitance-voltage (C-V) study of the interface was carried out. Calculation of quantum levels in the silicon quantum well was performed on the basis of the band lineup of the strained Si3N4/Si/InP interface and the result indicated that the interface should become free of gap states when the silicon layer thickness is below 5 Å. Experimentally, such a delicate Si3N4/Si/InP structure was realized by partial nitridation of a molecular beam epitaxially (MBE) grown pseudomorphic silicon layer using an electron cyclotron resonance (ECR) N2 plasma. The progress of nitridation was investigated in detail by angle-resolved XPS. A newly developed UHV contactless C-V method realized in situ characterization of surface electronic properties of InP at each processing step for passivation. It was found that the interface state density decreased substantially into the 1010 cm-2 eV-1 range by optimizing the nitridation process of the silicon layer. It was concluded that both the surface bond termination and state removal by quantum confinement are responsible for the NSS reduction.

Precision analysis of the photomultiplier response to ultra low signals

NASA Astrophysics Data System (ADS)

Degtiarenko, Pavel

2017-11-01

A new computational model for the description of the photon detector response functions measured in conditions of low light is presented, together with examples of the observed photomultiplier signal amplitude distributions, successfully described using the parameterized model equation. In extension to the previously known approximations, the new model describes the underlying discrete statistical behavior of the photoelectron cascade multiplication processes in photon detectors with complex non-uniform gain structure of the first dynode. Important features of the model include the ability to represent the true single-photoelectron spectra from different photomultipliers with a variety of parameterized shapes, reflecting the variability in the design and in the individual parameters of the detectors. The new software tool is available for evaluation of the detectors' performance, response, and efficiency parameters that may be used in various applications including the ultra low background experiments such as the searches for Dark Matter and rare decays, underground neutrino studies, optimizing operations of the Cherenkov light detectors, help in the detector selection procedures, and in the experiment simulations.

Dynamic Optimization

NASA Technical Reports Server (NTRS)

Laird, Philip

1992-01-01

We distinguish static and dynamic optimization of programs: whereas static optimization modifies a program before runtime and is based only on its syntactical structure, dynamic optimization is based on the statistical properties of the input source and examples of program execution. Explanation-based generalization is a commonly used dynamic optimization method, but its effectiveness as a speedup-learning method is limited, in part because it fails to separate the learning process from the program transformation process. This paper describes a dynamic optimization technique called a learn-optimize cycle that first uses a learning element to uncover predictable patterns in the program execution and then uses an optimization algorithm to map these patterns into beneficial transformations. The technique has been used successfully for dynamic optimization of pure Prolog.

Band Offsets at the Interface between Crystalline and Amorphous Silicon from First Principles

NASA Astrophysics Data System (ADS)

Jarolimek, K.; Hazrati, E.; de Groot, R. A.; de Wijs, G. A.

2017-07-01

The band offsets between crystalline and hydrogenated amorphous silicon (a -Si ∶H ) are key parameters governing the charge transport in modern silicon heterojunction solar cells. They are an important input for macroscopic simulators that are used to further optimize the solar cell. Past experimental studies, using x-ray photoelectron spectroscopy (XPS) and capacitance-voltage measurements, have yielded conflicting results on the band offset. Here, we present a computational study on the band offsets. It is based on atomistic models and density-functional theory (DFT). The amorphous part of the interface is obtained by relatively long DFT first-principles molecular-dynamics runs at an elevated temperature on 30 statistically independent samples. In order to obtain a realistic conduction-band position the electronic structure of the interface is calculated with a hybrid functional. We find a slight asymmetry in the band offsets, where the offset in the valence band (0.29 eV) is larger than in the conduction band (0.17 eV). Our results are in agreement with the latest XPS measurements that report a valence-band offset of 0.3 eV [M. Liebhaber et al., Appl. Phys. Lett. 106, 031601 (2015), 10.1063/1.4906195].

Ultrafast High Harmonic, Soft X-Ray Probing of Molecular Dynamics

DTIC Science & Technology

2013-04-30

590 L/s scroll pump and a titanium sublimation pump . A TOF-PES has been designed and constructed to analyze the energy of the photoelectrons...are studied using the quasi-continuous vacuum ultraviolet light of the Advanced Light Source at Lawrence Berkeley National Laboratory. The molecular...34), the method of high order harmonic generation of ultrashort vacuum ultraviolet pulses was used to investigate molecular photodissociation, ultrafast

Ionization heating in rare-gas clusters under intense XUV laser pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arbeiter, Mathias; Fennel, Thomas

The interaction of intense extreme ultraviolet (XUV) laser pulses ({lambda}=32 nm, I=10{sup 11}-10{sup 14} W/cm{sup 2}) with small rare-gas clusters (Ar{sub 147}) is studied by quasiclassical molecular dynamics simulations. Our analysis supports a very general picture of the charging and heating dynamics in finite samples under short-wavelength radiation that is of relevance for several applications of free-electron lasers. First, up to a certain photon flux, ionization proceeds as a series of direct photoemission events producing a jellium-like cluster potential and a characteristic plateau in the photoelectron spectrum as observed in Bostedt et al. [Phys. Rev. Lett. 100, 133401 (2008)]. Second,more » beyond the onset of photoelectron trapping, nanoplasma formation leads to evaporative electron emission with a characteristic thermal tail in the electron spectrum. A detailed analysis of this transition is presented. Third, in contrast to the behavior in the infrared or low vacuum ultraviolet range, the nanoplasma energy capture proceeds via ionization heating, i.e., inner photoionization of localized electrons, whereas collisional heating of conduction electrons is negligible up to high laser intensities. A direct consequence of the latter is a surprising evolution of the mean energy of emitted electrons as function of laser intensity.« less

Full observation of ultrafast cascaded radiationless transitions from S{sub 2}(ππ{sup ∗}) state of pyrazine using vacuum ultraviolet photoelectron imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Horio, Takuya; Spesyvtsev, Roman; Nagashima, Kazuki

A photoexcited molecule undergoes multiple deactivation and reaction processes simultaneously or sequentially, which have been observed by combinations of various experimental methods. However, a single experimental method that enables complete observation of the photo-induced dynamics would be of great assistance for such studies. Here we report a full observation of cascaded electronic dephasing from S{sub 2}(ππ{sup *}) in pyrazine (C{sub 4}N{sub 2}H{sub 4}) by time-resolved photoelectron imaging (TRPEI) using 9.3-eV vacuum ultraviolet pulses with a sub-20 fs time duration. While we previously demonstrated a real-time observation of the ultrafast S{sub 2}(ππ{sup *}) → S{sub 1}(nπ{sup *}) internal conversion in pyrazinemore » using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S{sub 1} to S{sub 0} (internal conversion) and T{sub 1}(nπ{sup *}) (intersystem crossing). Also discussed are the role of {sup 1}A{sub u}(nπ{sup *}) in the internal conversion and the configuration interaction of the S{sub 2}(ππ{sup *}) electronic wave function.« less

Photoelectron angular distribution from free SiO2 nanoparticles as a probe of elastic electron scattering.

PubMed

Antonsson, E; Langer, B; Halfpap, I; Gottwald, J; Rühl, E

2017-06-28

In order to gain quantitative information on the surface composition of nanoparticles from X-ray photoelectron spectroscopy, a detailed understanding of photoelectron transport phenomena in these samples is needed. Theoretical results on the elastic and inelastic scattering have been reported, but a rigorous experimental verification is lacking. We report in this work on the photoelectron angular distribution from free SiO 2 nanoparticles (d = 122 ± 9 nm) after ionization by soft X-rays above the Si 2p and O 1s absorption edges, which gives insight into the relative importance of elastic and inelastic scattering channels in the sample particles. The photoelectron angular anisotropy is found to be lower for photoemission from SiO 2 nanoparticles than that expected from the theoretical values for the isolated Si and O atoms in the photoelectron kinetic energy range 20-380 eV. The reduced angular anisotropy is explained by elastic scattering of the outgoing photoelectrons from neighboring atoms, smearing out the atomic distribution. Photoelectron angular distributions yield detailed information on photoelectron elastic scattering processes allowing for a quantification of the number of elastic scattering events the photoelectrons have undergone prior to leaving the sample. The interpretation of the experimental photoelectron angular distributions is complemented by Monte Carlo simulations, which take inelastic and elastic photoelectron scattering into account using theoretical values for the scattering cross sections. The results of the simulations reproduce the experimental photoelectron angular distributions and provide further support for the assignment that elastic and inelastic electron scattering processes need to be considered.

Photoelectron Diffraction from Valence States of Oriented Molecules

NASA Astrophysics Data System (ADS)

Krüger, Peter

2018-06-01

The angular distribution of photoelectrons emitted from valence states of oriented molecules is investigated. The principles underlying the angular pattern formation are explained in terms of photoelectron wave interference, caused by initial state delocalization and final state photoelectron scattering. Computational approaches to photoelectron spectroscopy from molecules are briefly reviewed. Here a combination of molecular orbital calculations for the initial state and multiple scattering theory for the photoelectron final state is used and applied to the 3σ and 4σ orbitals of nitrogen and the highest occupied molecular orbital of pentacene. Appreciable perpendicular emission and circular dichroism in angular distributions is found, two effects that cannot be described by the popular plane wave approximation to the photoelectron final state.

Resolving Nonadiabatic Dynamics of Hydrated Electrons Using Ultrafast Photoemission Anisotropy.

PubMed

Karashima, Shutaro; Yamamoto, Yo-Ichi; Suzuki, Toshinori

2016-04-01

We have studied ultrafast nonadiabatic dynamics of excess electrons trapped in the band gap of liquid water using time- and angle-resolved photoemission spectroscopy. Anisotropic photoemission from the first excited state was discovered, which enabled unambiguous identification of nonadiabatic transition to the ground state in 60 fs in H_{2}O and 100 fs in D_{2}O. The photoelectron kinetic energy distribution exhibited a rapid spectral shift in ca. 20 fs, which is ascribed to the librational response of a hydration shell to electronic excitation. Photoemission anisotropy indicates that the electron orbital in the excited state is depolarized in less than 40 fs.

Vacuum-ultraviolet lasers and spectroscopy

NASA Astrophysics Data System (ADS)

Hollenstein, U.

2012-01-01

Single-photon ionisation of most atoms and molecules requires short-wavelength radiation, typically in the vacuum-ultraviolet (VUV, λ < 200 nm) or extreme ultraviolet (XUV, λ < 105 nm) region of the electromagnetic spectrum. The first VUV and XUV radiation sources used to study molecular photoabsorption and photoionisation spectra were light sources emitting a broad continuous spectrum, such as high pressure lamps or synchrotrons. Monochromatic VUV and XUV radiation was obtained using diffraction gratings in evacuated monochromators, which resulted in a resolving power ν/Δv of at best 106 (i. e. 0.1 cm-1 at 100 000 cm-1), but more typically in the range 104-105 . The invention of the laser and the development of nonlinear optical frequency-upconversion techniques enabled the development of table-top narrow-bandwidth, coherent VUV and XUV laser sources with which VUV photoabsorption, photoionisation and photoelectron spectra of molecules can be recorded at much higher resolution, the best sources having bandwidths better than 50 MHz. Such laser sources are ideally suited to study the structure and dynamics of electronically excited states of atoms and molecules and molecular photoionisation using photoabsorption, photoionisation and photoelectron spectroscopy. This chapter presents the general principles that are exploited to generate tunable narrow-band laser radiation below 200 nm and describes spectroscopic methods such as photoabsorption spectroscopy, photoionisation spectroscopy and threshold photoelectron spectroscopy that relay on the broad tunability and narrow-bandwidth of VUV radiation sources.

Time-resolved photoelectron imaging of iodide-nitromethane (I-·CH3NO2) photodissociation dynamics.

PubMed

Kunin, Alice; Li, Wei-Li; Neumark, Daniel M

2016-12-07

Femtosecond time-resolved photoelectron spectroscopy is used to probe the decay channels of iodide-nitromethane (I - ·CH 3 NO 2 ) binary clusters photoexcited at 3.56 eV, near the vertical detachment energy (VDE) of the cluster. The production of I - is observed, and its photoelectron signal exhibits a mono-exponential rise time of 21 ± 1 ps. Previous work has shown that excitation near the VDE of the I - ·CH 3 NO 2 complex transfers an electron from iodide to form a dipole-bound state of CH 3 NO 2 - that rapidly converts to a valence bound (VB) anion. The long appearance time for the I - fragment suggests that the VB anion decays by back transfer of the excess electron to iodide, reforming the I - ·CH 3 NO 2 anion and resulting in evaporation of iodide. Comparison of the measured lifetime to that predicted by RRKM theory suggests that the dissociation rate is limited by intramolecular vibrational energy redistribution in the re-formed anion between the high frequency CH 3 NO 2 vibrational modes and the much lower frequency intermolecular I - ·CH 3 NO 2 stretch and bends, the predominant modes involved in cluster dissociation to form I - . Evidence for a weak channel identified as HI + CH 2 NO 2 - is also observed.

Calculation of photoionization differential cross sections using complex Gauss-type orbitals.

PubMed

Matsuzaki, Rei; Yabushita, Satoshi

2017-09-05

Accurate theoretical calculation of photoelectron angular distributions for general molecules is becoming an important tool to image various chemical reactions in real time. We show in this article that not only photoionization total cross sections but also photoelectron angular distributions can be accurately calculated using complex Gauss-type orbital (cGTO) basis functions. Our method can be easily combined with existing quantum chemistry techniques including electron correlation effects, and applied to various molecules. The so-called two-potential formula is applied to represent the transition dipole moment from an initial bound state to a final continuum state in the molecular coordinate frame. The two required continuum functions, the zeroth-order final continuum state and the first-order wave function induced by the photon field, have been variationally obtained using the complex basis function method with a mixture of appropriate cGTOs and conventional real Gauss-type orbitals (GTOs) to represent the continuum orbitals as well as the remaining bound orbitals. The complex orbital exponents of the cGTOs are optimized by fitting to the outgoing Coulomb functions. The efficiency of the current method is demonstrated through the calculations of the asymmetry parameters and molecular-frame photoelectron angular distributions of H2+ and H2 . In the calculations of H2 , the static exchange and random phase approximations are employed, and the dependence of the results on the basis functions is discussed. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Breaking through the false coincidence barrier in electron–ion coincidence experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Osborn, David L.; Hayden, Carl C.; Hemberger, Patrick

Photoelectron Photoion Coincidence (PEPICO) spectroscopy holds the promise of a universal, isomer-selective, and sensitive analytical technique for time-resolved quantitative analysis of bimolecular chemical reactions. Unfortunately, its low dynamic range of ~10 3 has largely precluded its use for this purpose, where a dynamic range of at least 10 5 is generally required. This limitation is due to the false coincidence background common to all coincidence experiments, especially at high count rates. Electron/ion pairs emanating from separate ionization events but arriving within the ion time of flight (TOF) range of interest constitute the false coincidence background. Although this background has uniformmore » intensity at every m/z value, the Poisson scatter in the false coincidence background obscures small signals. In this paper, temporal ion deflection coupled with a position-sensitive ion detector enables suppression of the false coincidence background, increasing the dynamic range in the PEPICO TOF mass spectrum by 2–3 orders of magnitude. The ions experience a time-dependent electric deflection field at a well-defined fraction of their time of flight. This deflection defines an m/z- and ionization-time dependent ion impact position for true coincidences, whereas false coincidences appear randomly outside this region and can be efficiently suppressed. When cold argon clusters are ionized, false coincidence suppression allows us to observe species up to Ar 9 +, whereas Ar 4 + is the largest observable cluster under traditional operation. As a result, this advance provides mass-selected photoelectron spectra for fast, high sensitivity quantitative analysis of reacting systems.« less

Breaking through the false coincidence barrier in electron–ion coincidence experiments

DOE PAGES

Osborn, David L.; Hayden, Carl C.; Hemberger, Patrick; ...

2016-10-31

Photoelectron Photoion Coincidence (PEPICO) spectroscopy holds the promise of a universal, isomer-selective, and sensitive analytical technique for time-resolved quantitative analysis of bimolecular chemical reactions. Unfortunately, its low dynamic range of ~10 3 has largely precluded its use for this purpose, where a dynamic range of at least 10 5 is generally required. This limitation is due to the false coincidence background common to all coincidence experiments, especially at high count rates. Electron/ion pairs emanating from separate ionization events but arriving within the ion time of flight (TOF) range of interest constitute the false coincidence background. Although this background has uniformmore » intensity at every m/z value, the Poisson scatter in the false coincidence background obscures small signals. In this paper, temporal ion deflection coupled with a position-sensitive ion detector enables suppression of the false coincidence background, increasing the dynamic range in the PEPICO TOF mass spectrum by 2–3 orders of magnitude. The ions experience a time-dependent electric deflection field at a well-defined fraction of their time of flight. This deflection defines an m/z- and ionization-time dependent ion impact position for true coincidences, whereas false coincidences appear randomly outside this region and can be efficiently suppressed. When cold argon clusters are ionized, false coincidence suppression allows us to observe species up to Ar 9 +, whereas Ar 4 + is the largest observable cluster under traditional operation. As a result, this advance provides mass-selected photoelectron spectra for fast, high sensitivity quantitative analysis of reacting systems.« less

The dynamic range of LZ

NASA Astrophysics Data System (ADS)

Yin, J.

2016-02-01

The electronics of the LZ experiment, the 7-tonne dark matter detector to be installed at the Sanford Underground Research Facility (SURF), is designed to permit studies of physics where the energies deposited range from 1 keV of nuclear-recoil energy up to 3,000 keV of electron-recoil energy. The system is designed to provide a 70% efficiency for events that produce three photoelectrons in the photomultiplier tubes (PMTs). This corresponds approximately to the lowest energy threshold achievable in multi-tonne time-projection chambers, and drives the noise specifications for the front end. The upper limit of the LZ dynamic range is defined to accommodate the electroluminescence (S2) signals. The low-energy channels of the LZ amplifiers provide the dynamic range required for the tritium and krypton calibrations. The high-energy channels provide the dynamic range required to measure the activated Xe lines.

The Dynamic Range of LZ

NASA Astrophysics Data System (ADS)

Yin, Jun; LZ Collaboration

2015-10-01

The electronics of the LZ experiment, the 7-ton dark matter detector to be installed at the Sanford Underground Research Facility (SURF), is designed to provide a 70% efficiency for events that produce three photoelectrons in the photomultiplier tubes (PMTs). This corresponds approximately to the lowest energy threshold achievable in such a detector, and drives the noise specifications for the front end. The upper limit of the LZ dynamic range is defined by the electroluminescence (S2) signals. The low-energy channels of the LZ amplifiers provide the dynamic range required for the tritium and krypton calibrations. The high-energy channels provide the dynamic range required to measure the activated Xe lines. S2 signals induced by alpha particles from radon decay will saturate one or more channels of the top PMT array but techniques are being developed to recover the information lost due to saturation. This work was supported by the Department of Energy, Grant DE-SC0006605.

Ultrafast quantum control of ionization dynamics in krypton.

PubMed

Hütten, Konrad; Mittermair, Michael; Stock, Sebastian O; Beerwerth, Randolf; Shirvanyan, Vahe; Riemensberger, Johann; Duensing, Andreas; Heider, Rupert; Wagner, Martin S; Guggenmos, Alexander; Fritzsche, Stephan; Kabachnik, Nikolay M; Kienberger, Reinhard; Bernhardt, Birgitta

2018-02-19

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.

Non-radiative relaxation dynamics of pyrrole following excitation in the range 249.5-200 nm

NASA Astrophysics Data System (ADS)

Kirkby, Oliver M.; Parkes, Michael A.; Neville, Simon P.; Worth, Graham A.; Fielding, Helen H.

2017-09-01

The non-radiative relaxation dynamics of pyrrole have been investigated using time-resolved photoelectron spectroscopy and quantum dynamics simulations. Following excitation of the A2 (11 πσ∗) state, we observe population flow out of the Franck-Condon region on a ≲ 50 fs timescale. Following excitation of the B2 (21 ππ∗) state, we observe population being transferred to the A2 (11 πσ∗) state on a <50 fs timescale and subsequently out of the Franck-Condon region, also on a <50 fs timescale. Quantum dynamics calculations suggest that population is transferred from the B2 (21 ππ∗) state through the A2 (1 π 3pz) state to the B1 (21 πσ∗) state before being transferred to the A2 (11 πσ∗) state.

Dynamics of a pulsed laser generated tin plasma expanding in an oxygen atmosphere

NASA Astrophysics Data System (ADS)

Barreca, F.; Fazio, E.; Neri, F.; Barletta, E.; Trusso, S.; Fazio, B.

2005-10-01

Semiconducting tin oxide can be successfully deposited by means of the laser ablation technique. In particular by ablating metallic tin in a controlled oxygen atmosphere, thin films of SnOx have been deposited. The partial oxygen pressure at which the films are deposited strongly influences both the stoichiometry and the structural properties of the films. In this work, we present a study of the expansion dynamics of the plasma generated by ablating a tin target by means of a pulsed laser using time and space resolved optical emission spectroscopy and fast photography imaging of the expanding plasma. Both Sn I and Sn II optical emission lines have been observed from the time-integrated spectroscopy. Time resolved-measurements revealed the dynamics of the expanding plasma in the ambient oxygen atmosphere. Stoichiometry of the films has been determined by means of X-ray photoelectron spectroscopy and correlated to the expansion dynamics of the plasma.

Control of photodissociation and photoionization of the NaI molecule by dynamic Stark effect.

PubMed

Han, Yong-Chang; Yuan, Kai-Jun; Hu, Wen-Hui; Cong, Shu-Lin

2009-01-28

The diabatic photodissociation and photoionization processes of the NaI molecule are studied theoretically using the quantum wave packet method. A pump laser pulse is used to prepare a dissociation wave packet that propagates through both the ionic channel (NaI-->Na(+)+I(-)) and the covalent channel (NaI-->Na+I). A Stark pulse is used to control the diabatic dissociation dynamics and a probe pulse is employed to ionize the products from the two channels. Based on the first order nonresonant nonperturbative dynamic Stark effect, the dissociation probabilities and the branching ratio of the products from the two channels can be controlled. Moreover the final photoelectron kinetic energy distribution can also be affected by the Stark pulse. The influences of the delay time, intensity, frequency, and carrier-envelope phase of the Stark pulse on the dissociation and ionization dynamics of the NaI molecule are discussed in detail.

COMPARISON OF NONLINEAR DYNAMICS OPTIMIZATION METHODS FOR APS-U

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sun, Y.; Borland, Michael

Many different objectives and genetic algorithms have been proposed for storage ring nonlinear dynamics performance optimization. These optimization objectives include nonlinear chromaticities and driving/detuning terms, on-momentum and off-momentum dynamic acceptance, chromatic detuning, local momentum acceptance, variation of transverse invariant, Touschek lifetime, etc. In this paper, the effectiveness of several different optimization methods and objectives are compared for the nonlinear beam dynamics optimization of the Advanced Photon Source upgrade (APS-U) lattice. The optimized solutions from these different methods are preliminarily compared in terms of the dynamic acceptance, local momentum acceptance, chromatic detuning, and other performance measures.

Extraction of ochratoxin A in red wine with dopamine-coated magnetic multi-walled carbon nanotubes.

PubMed

Wan, Hong; Zhang, Bo; Bai, Xiao-Lin; Zhao, Yan; Xiao, Meng-Wei; Liao, Xun

2017-10-01

A new, rapid, green, and cost-effective magnetic solid-phase extraction of ochratoxin A from red wine samples was developed using polydopamine-coated magnetic multi-walled carbon nanotubes as the absorbent. The polydopamine-coated magnetic multi-walled carbon nanotubes were fabricated with magnetic multi-walled carbon nanotubes and dopamine by an in situ oxidative self-polymerization approach. Transmission electron microscopy, dynamic light scattering, X-ray photoelectron spectroscopy and vibrating sample magnetometry were used to characterize the absorbents. Ochratoxin A was quantified with high-performance liquid chromatography coupled with fluorescence detection, with excitation and emission wavelengths of 338 and 455 nm, respectively. The conditions affecting the magnetic solid-phase extraction procedure, such as pH, extraction solution, extraction time, absorbent amount, desorption solution and desorption time were investigated to obtain the optimal extraction conditions. Under the optimized conditions, the extraction recovery was 91.8-104.5% for ochratoxin A. A linear calibration curve was obtained in the range of 0.1-2.0 ng/mL. The limit of detection was 0.07 ng/mL, and the limit of quantitation was 0.21 ng/mL. The recoveries of ochratoxin A for spiked red wine sample ranged from 95.65 to 100.65% with relative standard deviation less than 8%. The polydopamine-coated magnetic multi-walled carbon nanotubes showed a high affinity toward ochratoxin A, allowing selective extraction and quantification of ochratoxin A from complex sample matrixes. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Vibrationally resolved photoelectron spectroscopy of electronic excited states of DNA bases: application to the ã state of thymine cation.

PubMed

Hochlaf, Majdi; Pan, Yi; Lau, Kai-Chung; Majdi, Youssef; Poisson, Lionel; Garcia, Gustavo A; Nahon, Laurent; Al Mogren, Muneerah Mogren; Schwell, Martin

2015-02-19

For fully understanding the light-molecule interaction dynamics at short time scales, recent theoretical and experimental studies proved the importance of accurate characterizations not only of the ground (D0) but also of the electronic excited states (e.g., D1) of molecules. While ground state investigations are currently straightforward, those of electronic excited states are not. Here, we characterized the à electronic state of ionic thymine (T(+)) DNA base using explicitly correlated coupled cluster ab initio methods and state-of-the-art synchrotron-based electron/ion coincidence techniques. The experimental spectrum is composed of rich and long vibrational progressions corresponding to the population of the low frequency modes of T(+)(Ã). This work challenges previous numerous works carried out on DNA bases using common synchrotron and VUV-based photoelectron spectroscopies. We provide hence a powerful theoretical and experimental framework to study the electronic structure of ionized DNA bases that could be generalized to other medium-sized biologically relevant systems.

Femtosecond Photoelectron Imaging of Dissociating and Autoionizing States in Oxygen

NASA Astrophysics Data System (ADS)

Plunkett, Alexander; Sandhu, Arvinder

2017-04-01

Time-resolved photoelectron spectra from molecular oxygen have been recorded with high energy and time resolution using a velocity map imaging (VMI) spectrometer. High harmonics were used to prepare neutral Rydberg states converging to the c4Σu- ionic state. These states display both autoionization and predissociation. A femtosecond laser pulse centered at 780 nm was used to probe the system, ionizing both the excited molecular states and the predissociated neutral atomic fragments. Electrons were collected in the 0-3 eV range using a VMI spectrometer and their spectra were reconstructed using a Fast Onion-peeling algorithm. By looking at IR modification to the electron spectrum, new features are observed which could originate from long-range columbic interactions or previously unobserved molecular decay channels. Ongoing studies extend this technique to other systems exhibiting non-adiabatic dynamics. This work was supported by the U. S. Army Research Laboratory and the U. S. Army Research Office under Grant No. W911NF-14-1-0383.

Polar Wind Measurements with TIDE/PSI and HYDRA on the Polar Spacecraft

NASA Technical Reports Server (NTRS)

Su, Y. J.; Horwitz, J. L.; Moore, Thomas E.; Giles, Barbara L.; Chandler, Michael O.; Craven, Paul D.; Chang, S.-W.; Scudder, J.

1998-01-01

The Thermal Ion Dynamics Experiment (TIDE) on the POLAR spacecraft has allowed sampling of the three-dimensional ion distributions with excellent energy, angular, and mass resolution. The companion Plasma Source Instrument, when operated, allows sufficient diminution of the electric potential to observe the polar wind at very high altitudes. In this presentation, we will describe the results of polar wind characteristics H+, He+, and 0+ as observed by TIDE at 5000 km and 8 RE altitudes. The relationship of the polar wind parameters with the solar zenith angle and with the day-night distance in the Solar Magnetic coordinate system will also be presented. We will compare these measurements with recent simulations of the photoelectron-driven polar wind using a couple fluid-semikinetic model. In addition, we will compare these polar wind observations with low-energy electrons sampled by the HYDRA experiment on POLAR to examine possible effects of the polar rain and photoelectrons and hopefully explain the large ion outflow velocity variations at POLAR apogee.

Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory.

PubMed

De Giovannini, Umberto; Brunetto, Gustavo; Castro, Alberto; Walkenhorst, Jessica; Rubio, Angel

2013-05-10

Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experiment, provide additional information about electronic structure and dynamics that improve characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Photoelectron imaging using an ellipsoidal display analyzer

NASA Astrophysics Data System (ADS)

Dütemeyer, T.; Quitmann, C.; Kitz, M.; Dörnemann, K.; Johansson, L. S. O.; Reihl, B.

2001-06-01

We have built an ellipsoidal display analyzer (EDA) for angle-resolved photoelectron spectroscopy and related techniques. The instrument is an improved version of a design by Eastman et al. [Nucl. Instrum. Methods 172, 327 (1980)] and measures the angle-resolved intensity distribution of photoelectrons at fixed energy I(θ,φ)|E=const.. Such two-dimensional cuts through the Brillouin zone are recorded using a position-sensitive detector. The large acceptance angle (Δθ=43° in the polar direction and Δφ=360° in the azimuthal direction) leads to a collection efficiency which exceeds that of conventional hemispherical analyzers by a factor of about 3000. Using ray-tracing calculations we analyze the electron optical properties of the various analyzer components and optimize their arrangement. This minimizes distortions and aberrations in the recorded images and greatly improves the performance compared to previous realizations of this analyzer. We present examples demonstrating the performance of the analyzer and its versatility. Using a commercial He-discharge lamp we are able to measure complete angular distribution patterns in less than 5 s. The energy and angular resolution are ΔEEDA=85 meV and Δθ=1.2°, respectively. Complete stacks of such cuts through the Brillouin zone at different kinetic energies E can be acquired automatically using custom software. The raw data are processed leading to a three-dimensional set (I(EB,k∥) of photoelectron intensity versus binding energy E and wave vector k∥. From this all relevant information, like the dispersion relations EB(k∥) along arbitrary directions of the Brillouin zone or Fermi-surface maps, can then be computed. An additional electron gun enables low-energy electron diffraction, Auger electron spectroscopy, and electron energy-loss spectroscopy. Switching between electrons and photons as the excitation source is possible without any movement of the sample or analyzer. Because of the high acquisition speed it is possible to study the electronic structure of solids as a function of an external parameter (i.e., temperature) or to make animated movies showing, for example, the evolution of electronic states in reciprocal space. After installation of this EDA at a synchrotron providing tunable photon energy, the full power of the instrument will come into play by adding techniques like constant final state or constant initial state spectroscopy, and x-ray photoelectron diffraction.

Ultrafast Structural Dynamics in Combustion Relevant Model Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weber, Peter M.

2014-03-31

The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energymore » of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or excited valence states is measured by inducing the dynamics using a near UV laser pulse, and employing a multi-photon ionization scheme via the Rydberg states as a probe process. Thus, the technique is capable of measuring the reaction dynamics in any electronic state of neutral molecules.« less

A novel comprehensive learning artificial bee colony optimizer for dynamic optimization biological problems.

PubMed

Su, Weixing; Chen, Hanning; Liu, Fang; Lin, Na; Jing, Shikai; Liang, Xiaodan; Liu, Wei

2017-03-01

There are many dynamic optimization problems in the real world, whose convergence and searching ability is cautiously desired, obviously different from static optimization cases. This requires an optimization algorithm adaptively seek the changing optima over dynamic environments, instead of only finding the global optimal solution in the static environment. This paper proposes a novel comprehensive learning artificial bee colony optimizer (CLABC) for optimization in dynamic environments problems, which employs a pool of optimal foraging strategies to balance the exploration and exploitation tradeoff. The main motive of CLABC is to enrich artificial bee foraging behaviors in the ABC model by combining Powell's pattern search method, life-cycle, and crossover-based social learning strategy. The proposed CLABC is a more bee-colony-realistic model that the bee can reproduce and die dynamically throughout the foraging process and population size varies as the algorithm runs. The experiments for evaluating CLABC are conducted on the dynamic moving peak benchmarks. Furthermore, the proposed algorithm is applied to a real-world application of dynamic RFID network optimization. Statistical analysis of all these cases highlights the significant performance improvement due to the beneficial combination and demonstrates the performance superiority of the proposed algorithm.

Equilibration kinetics in isolated and membrane-bound photosynthetic reaction centers upon illumination: a method to determine the photoexcitation rate.

PubMed

Manzo, Anthony J; Goushcha, Alexander O; Barabash, Yuri M; Kharkyanen, Valery N; Scott, Gary W

2009-07-01

Kinetics of electron transfer, following variation of actinic light intensity, for photosynthetic reaction centers (RCs) of purple bacteria (isolated and membrane-bound) were analyzed by measuring absorbance changes in the primary photoelectron donor absorption band at 865 nm. The bleaching of the primary photoelectron donor absorption band in RCs, following a sudden increase of illumination from the dark to an actinic light intensity of I(exp), obeys a simple exponential law with the rate constant alphaI(exp) + k(rec), in which alpha is a parameter relating the light intensity, measured in mW/cm(2), to a corresponding theoretical rate in units of reciprocal seconds, and k(rec) is the effective rate constant of the charge recombination in the photosynthetic RCs. In this work, a method for determining the alpha parameter value is developed and experimentally verified for isolated and membrane-bound RCs, allowing for rigorous modeling of RC macromolecule dynamics under varied photoexcitation conditions. Such modeling is necessary for RCs due to alterations of the forward photoexcitation rates and relaxation rates caused by illumination history and intramolecular structural dynamics effects. It is demonstrated that the classical Bouguer-Lambert-Beer formalism can be applied for the samples with relatively low scattering, which is not necessarily the case with strongly scattering media or high light intensity excitation.

Molecular dynamics simulation, ab initio calculation, and size-selected anion photoelectron spectroscopy study of initial hydration processes of calcium chloride.

PubMed

He, Zhili; Feng, Gang; Yang, Bin; Yang, Lijiang; Liu, Cheng-Wen; Xu, Hong-Guang; Xu, Xi-Ling; Zheng, Wei-Jun; Gao, Yi Qin

2018-06-14

To understand the initial hydration processes of CaCl 2 , we performed molecular simulations employing the force field based on the theory of electronic continuum correction with rescaling. Integrated tempering sampling molecular dynamics were combined with ab initio calculations to overcome the sampling challenge in cluster structure search and refinement. The calculated vertical detachment energies of CaCl 2 (H 2 O) n - (n = 0-8) were compared with the values obtained from photoelectron spectra, and consistency was found between the experiment and computation. Separation of the Cl-Ca ion pair is investigated in CaCl 2 (H 2 O) n - anions, where the first Ca-Cl ionic bond required 4 water molecules, and both Ca-Cl bonds are broken when the number of water molecules is larger than 7. For neutral CaCl 2 (H 2 O) n clusters, breaking of the first Ca-Cl bond starts at n = 5, and 8 water molecules are not enough to separate the two ion pairs. Comparing with the observations on magnesium chloride, it shows that separating one ion pair in CaCl 2 (H 2 O) n requires fewer water molecules than those for MgCl 2 (H 2 O) n . Coincidentally, the solubility of calcium chloride is higher than that of magnesium chloride in bulk solutions.

Molecular dynamics simulation, ab initio calculation, and size-selected anion photoelectron spectroscopy study of initial hydration processes of calcium chloride

NASA Astrophysics Data System (ADS)

He, Zhili; Feng, Gang; Yang, Bin; Yang, Lijiang; Liu, Cheng-Wen; Xu, Hong-Guang; Xu, Xi-Ling; Zheng, Wei-Jun; Gao, Yi Qin

2018-06-01

To understand the initial hydration processes of CaCl2, we performed molecular simulations employing the force field based on the theory of electronic continuum correction with rescaling. Integrated tempering sampling molecular dynamics were combined with ab initio calculations to overcome the sampling challenge in cluster structure search and refinement. The calculated vertical detachment energies of CaCl2(H2O)n- (n = 0-8) were compared with the values obtained from photoelectron spectra, and consistency was found between the experiment and computation. Separation of the Cl—Ca ion pair is investigated in CaCl2(H2O)n- anions, where the first Ca—Cl ionic bond required 4 water molecules, and both Ca—Cl bonds are broken when the number of water molecules is larger than 7. For neutral CaCl2(H2O)n clusters, breaking of the first Ca—Cl bond starts at n = 5, and 8 water molecules are not enough to separate the two ion pairs. Comparing with the observations on magnesium chloride, it shows that separating one ion pair in CaCl2(H2O)n requires fewer water molecules than those for MgCl2(H2O)n. Coincidentally, the solubility of calcium chloride is higher than that of magnesium chloride in bulk solutions.

Characterization of fast photoelectron packets in weak and strong laser fields in ultrafast electron microscopy.

PubMed

Plemmons, Dayne A; Tae Park, Sang; Zewail, Ahmed H; Flannigan, David J

2014-11-01

The development of ultrafast electron microscopy (UEM) and variants thereof (e.g., photon-induced near-field electron microscopy, PINEM) has made it possible to image atomic-scale dynamics on the femtosecond timescale. Accessing the femtosecond regime with UEM currently relies on the generation of photoelectrons with an ultrafast laser pulse and operation in a stroboscopic pump-probe fashion. With this approach, temporal resolution is limited mainly by the durations of the pump laser pulse and probe electron packet. The ability to accurately determine the duration of the electron packets, and thus the instrument response function, is critically important for interpretation of dynamics occurring near the temporal resolution limit, in addition to quantifying the effects of the imaging mode. Here, we describe a technique for in situ characterization of ultrashort electron packets that makes use of coupling with photons in the evanescent near-field of the specimen. We show that within the weakly-interacting (i.e., low laser fluence) regime, the zero-loss peak temporal cross-section is precisely the convolution of electron packet and photon pulse profiles. Beyond this regime, we outline the effects of non-linear processes and show that temporal cross-sections of high-order peaks explicitly reveal the electron packet profile, while use of the zero-loss peak becomes increasingly unreliable. Copyright © 2014 Elsevier B.V. All rights reserved.

Vibronic relaxation dynamics of o-dichlorobenzene in its lowest excited singlet state

NASA Astrophysics Data System (ADS)

Liu, Benkang; Zhao, Haiyan; Lin, Xiang; Li, Xinxin; Gao, Mengmeng; Wang, Li; Wang, Wei

2018-01-01

Vibronic dynamics of o-dichlorobenzene in its lowest excited singlet state, S1, is investigated in real time by using femtosecond pump-probe method, combined with time-of-flight mass spectroscopy and photoelectron velocity mapping technique. Relaxation processes for the excitation in the range of 276-252 nm can be fitted by single exponential decay model, while in the case of wavelength shorter than 252 nm two-exponential decay model must be adopted for simulating transient profiles. Lifetime constants of the vibrationally excited S1 states change from 651 ± 10 ps for 276 nm excitation to 61 ± 1 ps for 242 nm excitation. Both the internal conversion from the S1 to the highly vibrationally excited ground state S0 and the intersystem crossing from the S1 to the triplet state are supposed to play important roles in de-excitation processes. Exponential fitting of the de-excitation rates on the excitation energy implies such de-excitation process starts from the highly vibrationally excited S0 state, which is validated, by probing the relaxation following photoexcitation at 281 nm, below the S1 origin. Time-dependent photoelectron kinetic energy distributions have been obtained experimentally. As the excitation wavelength changes from 276 nm to 242 nm, different cationic vibronic vibrations can be populated, determined by the Franck-Condon factors between the large geometry distorted excited singlet states and final cationic states.

The optimal dynamic immunization under a controlled heterogeneous node-based SIRS model

NASA Astrophysics Data System (ADS)

Yang, Lu-Xing; Draief, Moez; Yang, Xiaofan

2016-05-01

Dynamic immunizations, under which the state of the propagation network of electronic viruses can be changed by adjusting the control measures, are regarded as an alternative to static immunizations. This paper addresses the optimal dynamical immunization under the widely accepted SIRS assumption. First, based on a controlled heterogeneous node-based SIRS model, an optimal control problem capturing the optimal dynamical immunization is formulated. Second, the existence of an optimal dynamical immunization scheme is shown, and the corresponding optimality system is derived. Next, some numerical examples are given to show that an optimal immunization strategy can be worked out by numerically solving the optimality system, from which it is found that the network topology has a complex impact on the optimal immunization strategy. Finally, the difference between a payoff and the minimum payoff is estimated in terms of the deviation of the corresponding immunization strategy from the optimal immunization strategy. The proposed optimal immunization scheme is justified, because it can achieve a low level of infections at a low cost.

SILAR BiOI-Sensitized TiO2 Films for Visible-Light Photocatalytic Degradation of Rhodamine B and 4-Chlorophenol.

PubMed

Odling, Gylen; Robertson, Neil

2017-04-05

BiOI nanoplates were deposited upon a film of TiO 2 nanoparticles derived from a commercial source using a simple room temperature sequential ionic layer adsorption and reaction (SILAR) method. X-ray diffraction, X-ray photoelectron spectroscopy and electron microscopies have been used to confirm the crystal phase, chemical states of key elements and morphology of the BiOI nanoplate-TiO 2 composites. Using both valence band X-ray photoelectron spectroscopy and UV/Vis diffuse reflectance measurements the band structure of the composites is determined to be that of a type II heterojunction. Through initial screening of the photocatalytic activity of the SILAR-modified films it was determined that five SILAR cycles are optimal in the photocatalytic degradation of rhodamine B. The visible-light sensitisation effect of BiOI was then proven by examination of the photocatalytic degradation of the colourless organic pollutant 4-chlorophenol, showing a large enhancement over an equivalent TiO 2 film. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

A multi-plate velocity-map imaging design for high-resolution photoelectron spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kregel, Steven J.; Thurston, Glen K.; Zhou, Jia

A velocity map imaging (VMI) setup consisting of multiple electrodes with three adjustable voltage parameters, designed for slow electron velocity map imaging applications, is presented. The motivations for this design are discussed in terms of parameters that influence the VMI resolution and functionality. Particularly, this VMI has two tunable potentials used to adjust for optimal focus, yielding good VMI focus across a relatively large energy range. It also allows for larger interaction volumes without significant sacrifice to the resolution via a smaller electric gradient at the interaction region. All the electrodes in this VMI have the same dimensions for practicalitymore » and flexibility, allowing for relatively easy modifications to suit different experimental needs. We have coupled this VMI to a cryogenic ion trap mass spectrometer that has a flexible source design. The performance is demonstrated with the photoelectron spectra of S- and CS 2 -. The latter has a long vibrational progression in the ground state, and the temperature dependence of the vibronic features is probed by changing the temperature of the ion trap.« less

Precision analysis of the photomultiplier response to ultra low signals

DOE PAGES

Degtiarenko, Pavel

2017-08-05

Here, a new computational model for the description of the photon detector response functions measured in conditions of low light is presented, together with examples of the observed photomultiplier signal amplitude distributions, successfully described using the parameterized model equation. In extension to the previously known approximations, the new model describes the underlying discrete statistical behavior of the photoelectron cascade multiplication processes in photon detectors with complex non-uniform gain structure of the first dynode. Important features of the model include the ability to represent the true single-photoelectron spectra from different photomultipliers with a variety of parameterized shapes, reflecting the variability inmore » the design and in the individual parameters of the detectors. The new software tool is available for evaluation of the detectors’ performance, response, and efficiency parameters that may be used in various applications including the ultra low background experiments such as the searches for Dark Matter and rare decays, underground neutrino studies, optimizing operations of the Cherenkov light detectors, help in the detector selection procedures, and in the experiment simulations.« less

A multi-plate velocity-map imaging design for high-resolution photoelectron spectroscopy

DOE PAGES

Kregel, Steven J.; Thurston, Glen K.; Zhou, Jia; ...

2017-09-01

A velocity map imaging (VMI) setup consisting of multiple electrodes with three adjustable voltage parameters, designed for slow electron velocity map imaging applications, is presented. The motivations for this design are discussed in terms of parameters that influence the VMI resolution and functionality. Particularly, this VMI has two tunable potentials used to adjust for optimal focus, yielding good VMI focus across a relatively large energy range. It also allows for larger interaction volumes without significant sacrifice to the resolution via a smaller electric gradient at the interaction region. All the electrodes in this VMI have the same dimensions for practicalitymore » and flexibility, allowing for relatively easy modifications to suit different experimental needs. We have coupled this VMI to a cryogenic ion trap mass spectrometer that has a flexible source design. The performance is demonstrated with the photoelectron spectra of S- and CS 2 -. The latter has a long vibrational progression in the ground state, and the temperature dependence of the vibronic features is probed by changing the temperature of the ion trap.« less

Data Analysis And Polarization Measurements With GEMS

NASA Technical Reports Server (NTRS)

Stohmayer, Tod

2011-01-01

The Gravity and Extreme Magnetism SMEX (GEMS) mission was selected by NASA for flight in 2014. GEMS will make the first sensitive survey of X-ray polarization across a wide range of source classes including black hole and neutron star binaries, AGN of different types, rotation and accretion-powered pulsars, magnetars, shell supernova remnants and pulsar wind nebulae. GEMS employs grazing-incidence foil mirrors and novel time-projection chamber (TPC) polarimeters leveraging the photoelectric effect. The GEMS detectors image the charge tracks of photoelectrons produced by 2 - 10 keV X-rays. The initial direction of the photoelectron is determined by the linear polarization of the photon. We present an overview of the data analysis challenges and methods for GEMS, including procedures for producing optimally filtered images of the charge tracks and estimating their initial directions. We illustrate our methods using laboratory measurements of polarized and unpolarized X-rays with flight-like detectors as well as from simulated tracks. We also present detailed simulations exploring the statistics of polarization measurements appropriate for GEMS, and make comparisons with previous work.

X-ray photoelectron spectroscopy characterization of composite TiO 2-poly(vinylidenefluoride) films synthesised for applications in pesticide photocatalytic degradation

NASA Astrophysics Data System (ADS)

Losito, I.; Amorisco, A.; Palmisano, F.; Zambonin, P. G.

2005-02-01

X-ray photoelectron spectroscopy (XPS) was adopted for the analytical characterization of composite titanium dioxide-poly(vinylidenefluoride) (TiO 2-PVDF) films developed for applications in the photocatalytic degradation of pollutants. The composites were deposited on glass substrates by casting or spin coating from TiO 2-PVDF suspensions in dimethylformamide (DMF). XPS data on the TiO 2-PVDF surface composition were used to optimize preparation conditions (composition of the TiO 2/PVDF suspension, deposition technique) in terms of titanium dioxide surface amount and film stability. The use of spin-coating deposition and the increase of TiO 2 amount in the DMF suspensions were found to improve the titanium surface content, although high TiO 2/PVDF ratios led to film instability. PVDF-TiO 2 films were also used in preliminary photocatalytic degradation tests on isoproturon, a phenylurea herbicide, under solar UV irradiation; the results were compared to direct photolysis to evaluate the catalytic efficiency of immobilized TiO 2 and the role played by the PVDF film during the degradation process.

Analysis of photoelectron effect on the antenna impedance via Particle-In-Cell simulation

NASA Astrophysics Data System (ADS)

Miyake, Y.; Usui, H.

2008-08-01

We present photoelectron effects on the impedance of electric field antennas used for plasma wave investigations. To illustrate the photoelectron effects, we applied electromagnetic Particle-In-Cell simulation to the self-consistent antenna impedance analysis. We confirmed the formation of a dense photoelectron region around the sunlit surfaces of the antenna and the spacecraft. The dense photoelectrons enhance the real part, and decrease the absolute value of the imaginary part, of antenna impedance at low frequencies. We also showed that the antenna conductance can be analytically calculated from simulation results of the electron current flowing into or out of the antenna. The antenna impedance in the photoelectron environment is represented by a parallel equivalent circuit consisting of a capacitance and a resistance, which is consistent with empirical knowledge. The results also imply that the impedance varies with the spin of the spacecraft, which causes the variation of the photoelectron density around the antenna.

A technique for estimating the absolute gain of a photomultiplier tube

NASA Astrophysics Data System (ADS)

Takahashi, M.; Inome, Y.; Yoshii, S.; Bamba, A.; Gunji, S.; Hadasch, D.; Hayashida, M.; Katagiri, H.; Konno, Y.; Kubo, H.; Kushida, J.; Nakajima, D.; Nakamori, T.; Nagayoshi, T.; Nishijima, K.; Nozaki, S.; Mazin, D.; Mashuda, S.; Mirzoyan, R.; Ohoka, H.; Orito, R.; Saito, T.; Sakurai, S.; Takeda, J.; Teshima, M.; Terada, Y.; Tokanai, F.; Yamamoto, T.; Yoshida, T.

2018-06-01

Detection of low-intensity light relies on the conversion of photons to photoelectrons, which are then multiplied and detected as an electrical signal. To measure the actual intensity of the light, one must know the factor by which the photoelectrons have been multiplied. To obtain this amplification factor, we have developed a procedure for estimating precisely the signal caused by a single photoelectron. The method utilizes the fact that the photoelectrons conform to a Poisson distribution. The average signal produced by a single photoelectron can then be estimated from the number of noise events, without requiring analysis of the distribution of the signal produced by a single photoelectron. The signal produced by one or more photoelectrons can be estimated experimentally without any assumptions. This technique, and an example of the analysis of a signal from a photomultiplier tube, are described in this study.

Effects of oxidation potential and retention time on electrochromic stability of poly (3-hexyl thiophene) films

NASA Astrophysics Data System (ADS)

Kim, Tae-Ho; Hyun Song, Seok; Kim, Hyo-Jae; Oh, Seong-Hyeon; Han, Song-Yi; Kim, Goung; Nah, Yoon-Chae

2018-06-01

Herein, we report the effects of applied voltage on the electrochromic (EC) stability of poly(3-hexylthiophene) (P3HT) films during EC reactions. The transmittance difference and cycling stability of these films were monitored to optimize the oxidation voltage, and their chemical compositions were analyzed by X-ray photoelectron spectroscopy after long-term electrochemical cycling. High oxidation voltages increased the color contrast of P3HT films but decreased their cycling stability due to facilitating chemical degradation. Furthermore, at an optimized oxidation voltage, the retention time during potential pulsing was adjusted utilizing the optical memory of P3HT, revealing that the decreased voltage application time reduced power consumption by 9.6% and enhanced EC stability without loss of color contrast.

X-ray Photoelectron Spectroscopy Database (Version 4.1)

National Institute of Standards and Technology Data Gateway

SRD 20 X-ray Photoelectron Spectroscopy Database (Version 4.1) (Web, free access)   The NIST XPS Database gives access to energies of many photoelectron and Auger-electron spectral lines. The database contains over 22,000 line positions, chemical shifts, doublet splittings, and energy separations of photoelectron and Auger-electron lines.

Cadmium sulfide mediated photoelectric effects in bilayer lipid membranes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baral, S.; Fendler, J.H.

1989-03-01

Development of semiconductor- and magnetic-particle-containing bilayer lipid membranes (BLMs) has been prompted by the mimetic relevance of these systems. In particular, the authors have been interested for some times in artificial photosynthesis. Optimization of a given system requires an understanding of the mechanisms of photoelectron transfers in the environments of, and across, mimetic membranes. They have undertaken, therefore, a systematic study of semiconductor-mediated photoelectric effects in BLMs. The present article reports results on steady-state and time-resolved, cadmium sulfide mediated photovoltage and photocurrent measurements in glyceryl monooleate BLMs.

CRF-PEPICO: Double velocity map imaging photoelectron photoion coincidence spectroscopy for reaction kinetics studies

NASA Astrophysics Data System (ADS)

Sztáray, Bálint; Voronova, Krisztina; Torma, Krisztián G.; Covert, Kyle J.; Bodi, Andras; Hemberger, Patrick; Gerber, Thomas; Osborn, David L.

2017-07-01

Photoelectron photoion coincidence (PEPICO) spectroscopy could become a powerful tool for the time-resolved study of multi-channel gas phase chemical reactions. Toward this goal, we have designed and tested electron and ion optics that form the core of a new PEPICO spectrometer, utilizing simultaneous velocity map imaging for both cations and electrons, while also achieving good cation mass resolution through space focusing. These optics are combined with a side-sampled, slow-flow chemical reactor for photolytic initiation of gas-phase chemical reactions. Together with a recent advance that dramatically increases the dynamic range in PEPICO spectroscopy [D. L. Osborn et al., J. Chem. Phys. 145, 164202 (2016)], the design described here demonstrates a complete prototype spectrometer and reactor interface to carry out time-resolved experiments. Combining dual velocity map imaging with cation space focusing yields tightly focused photoion images for translationally cold neutrals, while offering good mass resolution for thermal samples as well. The flexible optics design incorporates linear electric fields in the ionization region, surrounded by dual curved electric fields for velocity map imaging of ions and electrons. Furthermore, the design allows for a long extraction stage, which makes this the first PEPICO experiment to combine ion imaging with the unimolecular dissociation rate constant measurements of cations to detect and account for kinetic shifts. Four examples are shown to illustrate some capabilities of this new design. We recorded the threshold photoelectron spectrum of the propargyl and the iodomethyl radicals. While the former agrees well with a literature threshold photoelectron spectrum, we have succeeded in resolving the previously unobserved vibrational structure in the latter. We have also measured the bimolecular rate constant of the CH2I + O2 reaction and observed its product, the smallest Criegee intermediate, CH2OO. Finally, the second dissociative photoionization step of iodocyclohexane ions, the loss of ethylene from the cyclohexyl cation, is slow at threshold, as illustrated by the asymmetric threshold photoionization time-of-flight distributions.

Perspective: Electrospray photoelectron spectroscopy: From multiply-charged anions to ultracold anions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Lai-Sheng, E-mail: Lai-Sheng-Wang@brown.edu

2015-07-28

Electrospray ionization (ESI) has become an essential tool in chemical physics and physical chemistry for the production of novel molecular ions from solution samples for a variety of spectroscopic experiments. ESI was used to produce free multiply-charged anions (MCAs) for photoelectron spectroscopy (PES) in the late 1990 s, allowing many interesting properties of this class of exotic species to be investigated. Free MCAs are characterized by strong intramolecular Coulomb repulsions, which create a repulsive Coulomb barrier (RCB) for electron emission. The RCB endows many fascinating properties to MCAs, giving rise to meta-stable anions with negative electron binding energies. Recent developmentmore » in the PES of MCAs includes photoelectron imaging to examine the influence of the RCB on the electron emission dynamics, pump-probe experiments to examine electron tunneling through the RCB, and isomer-specific experiments by coupling PES with ion mobility for biological MCAs. The development of a cryogenically cooled Paul trap has led to much better resolved PE spectra for MCAs by creating vibrationally cold anions from the room temperature ESI source. Recent advances in coupling the cryogenic Paul trap with PE imaging have allowed high-resolution PE spectra to be obtained for singly charged anions produced by ESI. In particular, the observation of dipole-bound excited states has made it possible to conduct vibrational autodetachment spectroscopy and resonant PES, which yield much richer vibrational spectroscopic information for dipolar free radicals than traditional PES.« less

Synthesis and in vitro cellular interactions of superparamagnetic iron nanoparticles with a crystalline gold shell

NASA Astrophysics Data System (ADS)

Bandyopadhyay, Sulalit; Singh, Gurvinder; Sandvig, Ioanna; Sandvig, Axel; Mathieu, Roland; Anil Kumar, P.; Glomm, Wilhelm Robert

2014-10-01

Fe@Au core-shell nanoparticles (NPs) exhibit multiple functionalities enabling their effective use in applications such as medical imaging and drug delivery. In this work, a novel synthetic method was developed and optimized for the synthesis of highly stable, monodisperse Fe@Au NPs of average diameter ∼24 nm exhibiting magneto-plasmonic characteristics. Fe@Au NPs were characterized by a wide range of experimental techniques, including scanning (transmission) electron microscopy (S(T)EM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), dynamic light scattering (DLS) and UV-vis spectroscopy. The formed particles comprise an amorphous iron core with a crystalline Au shell of tunable thickness, and retain the superparamagnetic properties at room temperature after formation of a crystalline Au shell. After surface modification, PEGylated Fe@Au NPs were used for in vitro studies on olfactory ensheathing cells (OECs) and human neural stem cells (hNSCs). No adverse effects of the Fe@Au particles were observed post-labeling, both cell types retaining normal morphology, viability, proliferation, and motility. It can be concluded that no appreciable toxic effects on both cell types, coupled with multifunctionality and chemical stability make them ideal candidates for therapeutic as well as diagnostic applications.

Studies of atomic and molecular dynamics using photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Canton, Sophie E.

Photoexcitation and photoionization studies of free atoms and molecules in the gas phase provide a unique view into various aspects of radiation-matter interactions that are used as basic building blocks in many branches of physics, such as Solid State, Plasma Physics, Photochemistry or Astrophysics. With the advent of third generation synchrotron light sources delivering high photon flux (>1015 photons/s) with unprecedented resolving power over a broad energy range, it has become possible to investigate in great detail not only the internal structure of the targets, but also the dynamics of the process. Born in the 1960s, photoelectron spectroscopy specifically analyzes the kinetic energy and emission angle of the ionized electrons. It is now coming to maturity with the availability of spectrometers designed to achieve high performances. This thesis work presents three examples of experiments made possible by the combination of the radiation from the Advanced Light Source with state of the art spectrometers. First, the measurements of the partial photoionization cross sections below the second ionization potential in argon and neon have uncovered weak and narrow resonances. Their mirroring profiles in the two open channels, which had prevented them from being detected in non-differential measurements, have been explained by their LS-forbidden nature. Second, the Auger spectra produced by decay of core-excited HF have revealed specific nuclear wavepacket interferences that occur when the electronic lifetime, the nuclear dynamics and the excitation prolongation, defined as the inverse of the photon bandwidth, have comparable time scales. Third, the analysis of the underlying structure in the first ionization band for free C60 has allowed the vibronic coupling of the singly charged molecular ion to be characterized.

Sixth International Workshop on Laser Physics (LPHYS 97) Volume 8, No. 1

DTIC Science & Technology

1998-01-01

solution of the problem concerning the action of an ultrashort laser pulse on an elementary molecular sys- tem—molecular hydrogen ion H2—is of...2 summarize the dynamics of the system for a peak pulse intensity / = 1.3 x 1016 W/cm2. First, Fig. 2a shows the Coulomb explosion of a molecule. It...Ionization of He in Intense Laser Fields A. Becker and F H. M. Faisal 69 Coulomb Correction to the Volkov Solution J. Bauer 76 Photoelectron

A formula for calculating theoretical photoelectron fluxes resulting from the He/+/ 304 A solar spectral line

NASA Technical Reports Server (NTRS)

Richards, P. G.; Torr, D. G.

1981-01-01

A simplified method for the evaluation of theoretical photoelectron fluxes in the upper atmosphere resulting from the solar radiation at 304 A is presented. The calculation is based on considerations of primary and cascade (secondary) photoelectron production in the two-stream model, where photoelectron transport is described by two electron streams, one moving up and one moving down, and of loss rates due to collisions with neutral gases and thermal electrons. The calculation is illustrated for the case of photoelectrons at an energy of 24.5 eV, and it is noted that the 24.5-eV photoelectron flux may be used to monitor variations in the solar 304 A flux. Theoretical calculations based on various ionization and excitation cross sections of Banks et al. (1974) are shown to be in generally good agreement with AE-E measurements taken between 200 and 235 km, however the use of more recent, larger cross sections leads to photoelectron values a factor of two smaller than observations but in agreement with previous calculations. It is concluded that a final resolution of the photoelectron problem may depend on a reevaluation of the inelastic electron collision cross sections.

Peculiarities of Spacecraft Photoelectron Shield Formation in Magnetic Field

NASA Astrophysics Data System (ADS)

Veselov, Mikhail; Chugunin, Dmitriy

Traditionally, the current balance equations for a spacecraft in space plasma rely on the electric field of positively charged spacecraft. Equilibrium potential V is derived from currents outward and toward the spacecraft body. The currents are in turn functions of V. However, in reality photoelectrons move in both the electric field of the spacecraft and the Earth or the interplanetary magnetic field. This causes an anisotropic distribution of photoelectrons along a magnetic field line with the characteristic size of the order of several photoelectron gyro-radii. As a result, confinement of photoelectrons in the spacecraft-related electric field is much longer. Thus, a fraction of returned photoelectrons in the electron current toward the spacecraft can be rather great and may even dominate several times over the ambient electrons’ fraction. Modeled ph-electron trajectories as well as general photoelectron shield distribution around spacecraft are represented, and comparison of experimental data on the electron density with the magnetic flux tube model is discussed.

Effects of anisotropic electron-ion interactions in atomic photoelectron angular distributions

NASA Technical Reports Server (NTRS)

Dill, D.; Starace, A. F.; Manson, S. T.

1974-01-01

The photoelectron asymmetry parameter beta in LS-coupling is obtained as an expansion into contributions from alternative angular momentum transfers j sub t. The physical significance of this expansion of beta is shown to be that: (1) the electric dipole interaction transfers to the atom a charcteristic single angular momentum j sub t = sub o, where sub o is the photoelectron's initial orbital momentum; and (2) angular momentum transfers indicate the presence of anisotropic interaction of the outgoing photoelectron with the residual ion. For open shell atoms the photoelectron-ion interaction is generally anisotropic; photoelectron phase shifts and electric dipole matrix elements depend on both the multiplet term of the residual ion and the total orbital momentum of the ion-photoelectron final state channel. Consequently beta depends on the term levels of the residual ion and contains contributions from all allowed values of j sub t. Numerical calculations of the asymmetry parameters and partial cross sections for photoionization of atomic sulfur are presented.

Fast engineering optimization: A novel highly effective control parameterization approach for industrial dynamic processes.

PubMed

Liu, Ping; Li, Guodong; Liu, Xinggao

2015-09-01

Control vector parameterization (CVP) is an important approach of the engineering optimization for the industrial dynamic processes. However, its major defect, the low optimization efficiency caused by calculating the relevant differential equations in the generated nonlinear programming (NLP) problem repeatedly, limits its wide application in the engineering optimization for the industrial dynamic processes. A novel highly effective control parameterization approach, fast-CVP, is first proposed to improve the optimization efficiency for industrial dynamic processes, where the costate gradient formulae is employed and a fast approximate scheme is presented to solve the differential equations in dynamic process simulation. Three well-known engineering optimization benchmark problems of the industrial dynamic processes are demonstrated as illustration. The research results show that the proposed fast approach achieves a fine performance that at least 90% of the computation time can be saved in contrast to the traditional CVP method, which reveals the effectiveness of the proposed fast engineering optimization approach for the industrial dynamic processes. Copyright © 2015 ISA. Published by Elsevier Ltd. All rights reserved.

Combustion synthesized TiO{sub 2} for enhanced photocatalytic activity under the direct sunlight-optimization of titanylnitrate synthesis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Daya Mani, A.; Laporte, V.; Ghosal, P.

2012-09-15

Graphical abstract: Effect of oxidant on the combustion synthesis of TiO{sub 2} has been studied by preparing titanylnitrate in four different ways from Ti(IV) iso-propoxide. It is observed that oxidant preparation method has a significant effect on physico-chemical as well as photocatalytic properties of TiO{sub 2}. All the catalysts showed excellent photocatalytic activity than Degussa P-25 under direct sunlight for the degradation of a textile dye (methylene blue), without the need of external light sources, oxygen supply and reactor systems. Highlights: ► Optimized synthesis of titanylnitrate. ► Influence of titanylnitrate synthesis on the physico-chemical properties of TiO{sub 2} prepared bymore » combustion synthesis. ► Development of highly efficient TiO{sub 2} photocatalysts those are active under the direct sunlight in open atmosphere. ► Degradation of the textile dye (methylene blue) under direct sunlight. -- Abstract: Optimized synthesis of Ti-precursor ‘titanylnitrate’ for one step combustion synthesis of N- and C-doped TiO{sub 2} catalysts were reported and characterized by using powder X-ray diffraction (XRD), transmission electron microscopy (TEM), diffused reflectance UV–vis spectroscopy, N{sub 2} adsorption and X-ray photoelectron spectroscopy (XPS). XRD confirmed the formation of TiO{sub 2} anatase and nano-crystallite size which was further confirmed by TEM. UV-DRS confirmed the decrease in the band gap to less than 3.0 eV, which was assigned due to the presence of C and N in the framework of TiO{sub 2} as confirmed by X-ray photoelectron spectroscopy. Degradation of methylene blue in aqueous solution under the direct sunlight was carried out and typical results indicated the better performance of the synthesized catalysts than Degussa P-25.« less

Statistical observations of martian 20-30 eV photoelectrons by MAVEN/SWEA

NASA Astrophysics Data System (ADS)

Garnier, P.; Steckiewicz, M.; Andre, N.; Mazelle, C. X.; Sauvaud, J. A.; Sakai, S.; Cravens, T.; Mitchell, D. L.; Lillis, R. J.; Espley, J. R.; Brain, D.; Andersson, L.; Jakosky, B. M.

2016-12-01

Photoelectron peaks in the 20-30 eV energy range are commonly observed in planetary atmospheres, produced by intense photoionization from solar 30.4 nm photons. At Mars, these photoelectrons are known to escape the planet down its tail (Frahm et al., 2006). Assuming overall charge neutrality, the number of corresponding electrons must be identical to the number of ion charges escaping the planet. Studying the photoelectrons is thus important to understand and quantify the erosion of the martian atmosphere. Moreover, the photoelectrons also play a significant role for the heating and ionization of the atmosphere. The MAVEN (Mars Atmosphere and Volatile EvolutioN) spacecraft has provided detailed observations of the Martian environment for the last two years thanks to its unique orbital coverage and comprehensive plasma instrument suite. The low periapsis altitudes (down to 125 km altitude) and combined presence of an electron spectrometer (Solar Wind Electron Analyzer, SWEA) and of a magnetometer (MAG) provide a unique opportunity to investigate the source region of the photoelectrons and their transport and escape down the tail. We will present statistical results of an automatic detection of 20-30 eV photoelectrons at Mars, based on a simple algorithm using three levels of confidence. More than 150,000 spectra (each averaged over 30s) revealed clear photoelectron peaks from October 2014 to May 2016. The analysis reveals several interesting features such as: the evolution of the peak shape from their source region to higher altitudes, the influence of the magnetic field topology on photoelectron transport, a clear dusk-dawn asymmetry in agreement with the recently-discovered neutral density asymmetry, the statistical influence of the EUV and solar wind parameters and the location of the photoelectron boundary. These results will also be compared with an electron transport code (Sakai et al., 2015, 2016) to better constrain the photoelectron production and transport.

Band alignment and interfacial chemical structure of the HfLaO/InGaZnO4 heterojunction investigated by x-ray photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Qian, Ling-Xuan; Wu, Ze-Han; Zhang, Yi-Yu; Liu, Yuan; Song, Jia-Qi; Liu, Xing-Zhao; Li, Yan-Rong

2017-04-01

Amorphous InGaZnO4 thin film transistors (a-IGZO TFTs) with HfLaO gate dielectrics have been widely demonstrated to possess extremely excellent electrical characteristics, and thus show great potential for applications in various next-generation electronic products. Nevertheless, the in-depth understanding of HfLaO/IGZO interfacial features is still lacking, which makes further device optimization lack clear guidance. In this work, the band alignment and interfacial chemical structure of a sputtering-prepared HfLaO/IGZO heterojunction was investigated through x-ray photoelectron spectroscopy. The valence and conduction band offsets (ΔE v and ΔE c) at the interface were determined to be 0.57 eV and 1.48 eV, respectively. The relatively large ΔE v is mainly attributed to the formation of the interfacial layer (IL) and thus the upward band bending from IGZO to the surface of HfLaO. Furthermore, it was found that the oxygen vacancies on the surface of IGZO were significantly suppressed upon the deposition of HfLaO, which not only explained the previously reported ultrahigh performance of a-IGZO/HfLaO TFTs to some extent, but also additionally validated the formation of the IL. Our findings have successfully revealed the importance of ILs in modifying the band alignment and interfacial trap states of HfLaO/IGZO heterojunctions, thus suggesting a potential route to further optimizing a-IGZO/HfLaO TFTs so as to satisfy the requirements of next-generation technologies.

Robust Dynamic Multi-objective Vehicle Routing Optimization Method.

PubMed

Guo, Yi-Nan; Cheng, Jian; Luo, Sha; Gong, Dun-Wei

2017-03-21

For dynamic multi-objective vehicle routing problems, the waiting time of vehicle, the number of serving vehicles, the total distance of routes were normally considered as the optimization objectives. Except for above objectives, fuel consumption that leads to the environmental pollution and energy consumption was focused on in this paper. Considering the vehicles' load and the driving distance, corresponding carbon emission model was built and set as an optimization objective. Dynamic multi-objective vehicle routing problems with hard time windows and randomly appeared dynamic customers, subsequently, were modeled. In existing planning methods, when the new service demand came up, global vehicle routing optimization method was triggered to find the optimal routes for non-served customers, which was time-consuming. Therefore, robust dynamic multi-objective vehicle routing method with two-phase is proposed. Three highlights of the novel method are: (i) After finding optimal robust virtual routes for all customers by adopting multi-objective particle swarm optimization in the first phase, static vehicle routes for static customers are formed by removing all dynamic customers from robust virtual routes in next phase. (ii)The dynamically appeared customers append to be served according to their service time and the vehicles' statues. Global vehicle routing optimization is triggered only when no suitable locations can be found for dynamic customers. (iii)A metric measuring the algorithms' robustness is given. The statistical results indicated that the routes obtained by the proposed method have better stability and robustness, but may be sub-optimum. Moreover, time-consuming global vehicle routing optimization is avoided as dynamic customers appear.

Highly Resolved Studies of Vacuum Ultraviolet Photoionization Dynamics

NASA Astrophysics Data System (ADS)

Kakar, Sandeep

We use measurements of dispersed fluorescence from electronically excited photoions to study fundamental aspects of intramolecular dynamics. Our experimental innovations make it possible to obtain highly resolved photoionization data that offer qualitative insights into molecular scattering. In particular, we obtain vibrationally resolved data to probe coupling between the electronic and nuclear degrees of freedom by studying the distribution of vibrational energy among photoions. Vibrationally resolved branching ratios are measured over a broad spectral range of excitation energy and their non-Franck-Condon behavior is used as a tool to investigate two diverse aspects of shape resonant photoionization. First, vibrational branching ratios are obtained for the SiF_4 5a _1^{-1} and CS_2 5sigma_{rm u} ^{-1} photoionization channels to help elucidate the microscopic aspects of shape resonant wavefunction for polyatomic molecules. It is shown that in such molecules the shape resonant wavefunction is not necessarily attributable to a specific bond in the molecule. Second, the multichannel aspect of shape resonant photoionization dynamics, reflected in continuum channel coupling, is investigated by obtaining vibrational branching ratios for the 2 sigma_{rm u}^{ -1} and 4sigma^{ -1} photoionization of the isoelectronic molecules N_2 and CO, respectively. These data indicate that effects of continuum coupling may be widespread. We also present the first set of rotationally resolved data over a wide energy range for the 2 sigma_{rm u}^{ -1} photoionization of N_2. These data probe the partitioning of the angular momentum between the photoelectron and photoion, and highlight the multicenter nature of the molecular potential. These case studies illustrate the utility of dispersed fluorescence measurements as a complement to photoelectron spectroscopy for obtaining highly resolved data for molecular photoionization. These measurements makes it possible to probe intrinsically molecular aspects, such as the vibration and rotation, of photoionization dynamics over an extended spectral range when used in conjunction with synchrotron radiation as the exciting source. Furthermore, the high resolution made possible by this technique provides high selectivity for accessing weaker ionization channels which are the ones strongly affected by resonant activity, and the present study repeatedly stresses the importance of this capability in discovering and deciphering new trends in resonant molecular ionization dynamics.

Electronic-structure theory of plutonium chalcogenides

NASA Astrophysics Data System (ADS)

Shick, Alexander; Havela, Ladislav; Gouder, Thomas; Rebizant, Jean

2009-03-01

The correlated band theory methods, the around-mean-field LDA + U and dynamical LDA + HIA (Hubbard-I), are applied to investigate the electronic structure of Pu chalcogenides. The LDA + U calculations for PuX (X = S, Se, Te) provide non-magnetic ground state in agreement with the experimental data. Non-integer filling of 5 f-manifold (from approx. 5.6 in PuS to 5.7 PuTe). indicates a mixed valence ground state which combines f5 and f6 multiplets. Making use of the dynamical LDA+HIA method the photoelectron spectra are calculated in good agreement with experimental data. The three-peak feature near EF attributed to 5 f-manifold is well reproduced by LDA + HIA, and follows from mixed valence character of the ground state.

Interactions of gaseous molecules with X-ray photons and photoelectrons in AP-XPS study of solid surface in gas phase.

PubMed

Tao, Franklin Feng; Nguyen, Luan

2018-04-18

Studies of the surface of a catalyst in the gas phase via photoelectron spectroscopy is an important approach to establish a correlation between the surface of a catalyst under reaction conditions or during catalysis and its corresponding catalytic performance. Unlike the well understood interactions between photoelectrons and the atomic layers of a surface in ultrahigh vacuum (UHV) and the well-developed method of quantitative analysis of a solid surface in UHV, a fundamental understanding of the interactions between X-ray photons and gaseous molecules and between photoelectrons and molecules of the gas phase in ambient pressure X-ray photoelectron spectroscopy (AP-XPS) is lacking. Through well designed experiments, here the impact of the interactions between photoelectrons and gaseous molecules and interactions between X-ray photons and gaseous molecules on the intensity of the collected photoelectrons have been explored. How the changes in photoelectron intensity resulting from these interactions influence measurement of the authentic atomic ratio of element M to A of a solid surface has been discussed herein, and methods to correct the measured nominal atomic ratio of two elements of a solid surface upon travelling through a gas phase to its authentic atomic ratio have been developed.

High rate dry etching of (BiSb)2Te3 film by CH4/H2-based plasma

NASA Astrophysics Data System (ADS)

Song, Junqiang; Shi, Xun; Chen, Lidong

2014-10-01

Etching characteristics of p-type (BiSb)2Te3 films were studied with CH4/H2/Ar gas mixture using an inductively coupled plasma (ICP)-reactive ion etching (RIE) system. The effects of gas mixing ratio, working pressure and gas flow rate on the etch rate and the surface morphology were investigated. The vertical etched profile with the etch rate of 600 nm/min was achieved at the optimized processing parameters. X-ray photoelectron spectroscopy (XPS) analysis revealed the non-uniform etching of (BiSb)2Te3 films due to disparate volatility of the etching products. Micro-masking effects caused by polymer deposition and Bi-rich residues resulted in roughly etched surfaces. Smooth surfaces can be obtained by optimizing the CH4/H2/Ar mixing ratio.

Imprints of the Molecular Electronic Structure in the Photoelectron Spectra of Strong-Field Ionized Asymmetric Triatomic Model Molecules

NASA Astrophysics Data System (ADS)

Paul, Matthias; Yue, Lun; Gräfe, Stefanie

2018-06-01

We examine the circular dichroism in the angular distribution of photoelectrons of triatomic model systems ionized by strong-field ionization. Following our recent work on this effect [Paul, Yue, and Gräfe, J. Mod. Opt. 64, 1104 (2017), 10.1080/09500340.2017.1299883], we demonstrate how the symmetry and electronic structure of the system is imprinted into the photoelectron momentum distribution. We use classical trajectories to reveal the origin of the threefolded pattern in the photoelectron momentum distribution, and show how an asymmetric nuclear configuration of the triatomic system effects the photoelectron spectra.

Mapping the Complete Reaction Path of a Complex Photochemical Reaction.

PubMed

Smith, Adam D; Warne, Emily M; Bellshaw, Darren; Horke, Daniel A; Tudorovskya, Maria; Springate, Emma; Jones, Alfred J H; Cacho, Cephise; Chapman, Richard T; Kirrander, Adam; Minns, Russell S

2018-05-04

We probe the dynamics of dissociating CS_{2} molecules across the entire reaction pathway upon excitation. Photoelectron spectroscopy measurements using laboratory-generated femtosecond extreme ultraviolet pulses monitor the competing dissociation, internal conversion, and intersystem crossing dynamics. Dissociation occurs either in the initially excited singlet manifold or, via intersystem crossing, in the triplet manifold. Both product channels are monitored and show that, despite being more rapid, the singlet dissociation is the minor product and that triplet state products dominate the final yield. We explain this by a consideration of accurate potential energy curves for both the singlet and triplet states. We propose that rapid internal conversion stabilizes the singlet population dynamically, allowing for singlet-triplet relaxation via intersystem crossing and the efficient formation of spin-forbidden dissociation products on longer timescales. The study demonstrates the importance of measuring the full reaction pathway for defining accurate reaction mechanisms.

Mapping the Complete Reaction Path of a Complex Photochemical Reaction

NASA Astrophysics Data System (ADS)

Smith, Adam D.; Warne, Emily M.; Bellshaw, Darren; Horke, Daniel A.; Tudorovskya, Maria; Springate, Emma; Jones, Alfred J. H.; Cacho, Cephise; Chapman, Richard T.; Kirrander, Adam; Minns, Russell S.

2018-05-01

We probe the dynamics of dissociating CS2 molecules across the entire reaction pathway upon excitation. Photoelectron spectroscopy measurements using laboratory-generated femtosecond extreme ultraviolet pulses monitor the competing dissociation, internal conversion, and intersystem crossing dynamics. Dissociation occurs either in the initially excited singlet manifold or, via intersystem crossing, in the triplet manifold. Both product channels are monitored and show that, despite being more rapid, the singlet dissociation is the minor product and that triplet state products dominate the final yield. We explain this by a consideration of accurate potential energy curves for both the singlet and triplet states. We propose that rapid internal conversion stabilizes the singlet population dynamically, allowing for singlet-triplet relaxation via intersystem crossing and the efficient formation of spin-forbidden dissociation products on longer timescales. The study demonstrates the importance of measuring the full reaction pathway for defining accurate reaction mechanisms.

Ultrafast electron dynamics reveal the high potential of InSe for hot-carrier optoelectronics

NASA Astrophysics Data System (ADS)

Chen, Zhesheng; Giorgetti, Christine; Sjakste, Jelena; Cabouat, Raphael; Véniard, Valérie; Zhang, Zailan; Taleb-Ibrahimi, Amina; Papalazarou, Evangelos; Marsi, Marino; Shukla, Abhay; Peretti, Jacques; Perfetti, Luca

2018-06-01

We monitor the dynamics of hot carriers in InSe by means of two-photon photoelectron spectroscopy (2PPE). The electrons excited by photons of 3.12 eV experience a manifold relaxation. First, they thermalize to electronic states degenerate with the M ¯ valley. Subsequently, the electronic cooling is dictated by Fröhlich coupling with phonons of small momentum transfer. Ab initio calculations predict cooling rates that are in good agreement with the observed dynamics. We argue that electrons accumulating in states degenerate with the M ¯ valley could travel through a multilayer flake of InSe with a lateral size of 1 μ m . The hot carriers pave a viable route to the realization of below-band-gap photodiodes and Gunn oscillators. Our results indicate that these technologies may find a natural implementation in future devices based on layered chalcogenides.

Optimized permeation and antifouling of PVDF hybrid ultrafiltration membranes: synergistic effect of dispersion and migration for fluorinated graphene oxide

NASA Astrophysics Data System (ADS)

Li, Mingming; Shi, Jie; Chen, Cheng; Li, Nan; Xu, Zhiwei; Li, Jing; Lv, Hanming; Qian, Xiaoming; Jiao, Xiaoning

2017-03-01

Nanoparticles may have suffered from low modification efficiency in hybrid membranes due to embedding and aggregating in polymer matrix. In order to analyze the modification mechanisms of nanoparticle migration and dispersion on the properties of hybrid membranes, we designed different F/ O ratios ( R F/ O ) of fluorinated graphene oxide (FGO, diameter = 1.5 17.5 μm) by carbon tetrafluoride (CF4) plasma treatment GO for 3, 5, 10, 15, and 20 min and successfully prepared novel PVDF hybrid membranes containing FGO via the phase inversion method. After a prolonged plasma treatment, the R F/ O of FGO was enhanced sharply, indicating an increasing compatibility of FGO with the matrix, especially FGO-20 (GO treated for 20 min). FGO contents in the top layer, sublayer, and the whole of membranes were probed by X-ray photoelectron spectroscopy, energy-dispersive spectrometer, and indirect computation, respectively. In the top layer of membranes, FGO contents declined from 13.14 wt% (PVDF/GO) to 4.00 wt% (PVDF/FGO-10) and 1.96 wt% (PVDF/FGO-20) due to the reduced migration ability of FGO. It is worth mentioning that PVDF/FGO-10 membranes exhibited an excellent water flux and flux recovery rate (up to 406.90 L m-2 h-1 and 88.9%), which were improved by 67.3% and 14.6% and 52.5% and 24.0% compared with those of PVDF/GO and PVDF/FGO-20 membranes, respectively, although the dispersion and migration ability of FGO-10 was maintained at a moderate level. It indicated that the migration and dispersion of FGO in membranes could result in dynamic equilibrium, which played a key role in making the best use of nanomaterials to optimize membrane performance.

Online optimization of storage ring nonlinear beam dynamics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huang, Xiaobiao; Safranek, James

2015-08-01

We propose to optimize the nonlinear beam dynamics of existing and future storage rings with direct online optimization techniques. This approach may have crucial importance for the implementation of diffraction limited storage rings. In this paper considerations and algorithms for the online optimization approach are discussed. We have applied this approach to experimentally improve the dynamic aperture of the SPEAR3 storage ring with the robust conjugate direction search method and the particle swarm optimization method. The dynamic aperture was improved by more than 5 mm within a short period of time. Experimental setup and results are presented.

Correlation between dynamic wetting behavior and chemical components of thermally modified wood

NASA Astrophysics Data System (ADS)

Wang, Wang; Zhu, Yuan; Cao, Jinzhen; Sun, Wenjing

2015-01-01

In order to investigate the dynamic wetting behavior of thermally modified wood, Cathay poplar (Populus cathayana Rehd.) and Scots pine (Pinus sylvestris L.) samples were thermally modified in an oven at 160, 180, 200, 220 or 240 °C for 4 h in this study. The dynamic contact angles and droplet volumes of water droplets on modified and unmodified wood surfaces were measured by sessile drop method, and their changing rates (expression index: K value and wetting slope) calculated by wetting models were illustrated for mapping the dynamic wetting process. The surface chemical components were also measured by X-ray photoelectron spectroscopy analysis (XPS), thus the relationship between dynamic wetting behavior and chemical components of thermally modified wood were determined. The results indicated that thermal modification was capable of decreasing the dynamic wettability of wood, expressed in lowing spread and penetration speed of water droplets on wood surfaces. This change was more obvious with the increased heating temperature. The K values varied linearly with the chemical components parameter (mass loss, O/C ratio, and C1/C2 ratio), indicating a strong correlation between dynamic wetting behavior and chemical components of thermally modified wood.

An inverse dynamics approach to trajectory optimization and guidance for an aerospace plane

NASA Technical Reports Server (NTRS)

Lu, Ping

1992-01-01

The optimal ascent problem for an aerospace planes is formulated as an optimal inverse dynamic problem. Both minimum-fuel and minimax type of performance indices are considered. Some important features of the optimal trajectory and controls are used to construct a nonlinear feedback midcourse controller, which not only greatly simplifies the difficult constrained optimization problem and yields improved solutions, but is also suited for onboard implementation. Robust ascent guidance is obtained by using combination of feedback compensation and onboard generation of control through the inverse dynamics approach. Accurate orbital insertion can be achieved with near-optimal control of the rocket through inverse dynamics even in the presence of disturbances.

Synchrotron radiation x-ray photoelectron spectroscopy study on the interface chemistry of high-k PrxAl2-xO3 (x=0-2) dielectrics on TiN for dynamic random access memory applications

NASA Astrophysics Data System (ADS)

Schroeder, T.; Lupina, G.; Sohal, R.; Lippert, G.; Wenger, Ch.; Seifarth, O.; Tallarida, M.; Schmeisser, D.

2007-07-01

Engineered dielectrics combined with compatible metal electrodes are important materials science approaches to scale three-dimensional trench dynamic random access memory (DRAM) cells. Highly insulating dielectrics with high dielectric constants were engineered in this study on TiN metal electrodes by partly substituting Al in the wide band gap insulator Al2O3 by Pr cations. High quality PrAlO3 metal-insulator-metal capacitors were processed with a dielectric constant of 19, three times higher than in the case of Al2O3 reference cells. As a parasitic low dielectric constant interface layer between PrAlO3 and TiN limits the total performance gain, a systematic nondestructive synchrotron x-ray photoelectron spectroscopy study on the interface chemistry of PrxAl2-xO3 (x =0-2) dielectrics on TiN layers was applied to unveil its chemical origin. The interface layer results from the decreasing chemical reactivity of PrxAl2-xO3 dielectrics with increasing Pr content x to reduce native Ti oxide compounds present on unprotected TiN films. Accordingly, PrAlO3 based DRAM capacitors require strict control of the surface chemistry of the TiN electrode, a parameter furthermore of importance to engineer the band offsets of PrxAl2-xO3/TiN heterojunctions.

Theory and Application of Auger and Photoelectron Diffraction and Holography

NASA Astrophysics Data System (ADS)

Chen, Xiang

This dissertation addresses the theories and applications of three important surface analysis techniques: Auger electron diffraction (AED), x-ray photoelectron diffraction (XPD), and Auger and photoelectron holography. A full multiple-scattering scheme for the calculations of XPD, AED, and Kikuchi electron diffraction pattern from a surface cluster is described. It is used to simulate 64 eV M_{2,3}VV and 913 eV L_3VV AED patterns from Cu(001) surfaces, in order to test assertions in the literature that they are explicable by a classical "blocking" and channeling model. We find that this contention is not valid, and that only a quantum mechanical multiple-scattering calculation is able to simulate these patterns well. The same multiple scattering simulation scheme is also used to investigate the anomalous phenomena of peak shifts off the forward-scattering directions in photo -electron diffraction patterns of Mg KLL (1180 eV) and O 1s (955 eV) from MgO(001) surfaces. These shifts are explained by calculations assuming a short electron mean free path. Similar simulations of XPD from a CoSi_2(111) surface for Co-3p and Si-2p normal emission agree well with experimental diffraction patterns. A filtering process aimed at eliminating the self -interference effect in photoelectron holography is developed. A better reconstructed image from Si-2p XPD from a Si(001) (2 times 1) surface is seen at atomic resolution. A reconstruction algorithm which corrects for the anisotropic emitter waves as well as the anisotropic atomic scattering factors is used for holographic reconstruction from a Co-3p XPD pattern from a CoSi_2 surface. This new algorithm considerably improves the reconstructed image. Finally, a new reconstruction algorithm called "atomic position recovery by iterative optimization of reconstructed intensities" (APRIORI), which takes account of the self-interference terms omitted by the other holographic algorithms, is developed. Tests on a Ni-C-O chain and Si(111)(sqrt{3} times sqrt{3})B surface suggest that this new method may overcome the twin image problem in the traditional holographic methods, reduce the artifacts in real space, and even separately identify the chemical species of the scatterers.

Extracting conformational structure information of benzene molecules via laser-induced electron diffraction

DOE PAGES

Ito, Yuta; Wang, Chuncheng; Le, Anh-Thu; ...

2016-05-01

Here, we have measured the angular distributions of high energy photoelectrons of benzene molecules generated by intense infrared femtosecond laser pulses. These electrons arise from the elastic collisions between the benzene ions with the previously tunnel-ionized electrons that have been driven back by the laser field. Theory shows that laser-free elastic differential cross sections (DCSs) can be extracted from these photoelectrons, and the DCS can be used to retrieve the bond lengths of gas-phase molecules similar to the conventional electron diffraction method. From our experimental results, we have obtained the C-C and C-H bond lengths of benzene with a spatialmore » resolution of about 10 pm. Our results demonstrate that laser induced electron diffraction (LIED) experiments can be carried out with the present-day ultrafast intense lasers already. Looking ahead, with aligned or oriented molecules, more complete spatial information of the molecule can be obtained from LIED, and applying LIED to probe photo-excited molecules, a “molecular movie” of the dynamic system may be created with sub-A°ngstrom spatial and few-ten femtosecond temporal resolutions.« less

Electronic structure of ferromagnetic heavy fermion, YbPdSi, YbPdGe, and YbPtGe studied by photoelectron spectroscopy, x-ray emission spectroscopy, and DFT + DMFT calculations

DOE PAGES

Yamaoka, Hitoshi; Thunstrom, Patrik; Tsujii, Naohito; ...

2017-11-02

Here, the electronic structures of ferromagnetic heavy fermion Yb compounds of YbPdSi, YbPdGe, and YbPtGe are studied by photoelectron spectroscopy around the Yb 4d–4f resonance, resonant x-ray emission spectroscopy at the Yb L 3 absorption edge, and density functional theory combined with dynamical mean field theory calculations. These compounds all have a temperature-independent intermediate Yb valence with largemore » $${\\rm Yb}^{3+}$$ and small $${\\rm Yb}^{2+}$$ components. The magnitude of the Yb valence is evaluated to be YbPtGe $<$ YbPdGe $$\\lesssim $$ YbPdSi, suggesting that YbPtGe is the closest to the quantum critical point among the three Yb compounds. Our results support the scenario of the coexistence of heavy fermion behavior and ferromagnetic ordering which is described by a magnetically-ordered Kondo lattice where the magnitude of the Kondo effect and the RKKY interaction are comparable.« less

Influence of polymolybdate adsorbates on electrooxidation of ethanol at PtRu nanoparticles: Combined electrochemical, mass spectrometric and X-ray photoelectron spectroscopic studies

NASA Astrophysics Data System (ADS)

Gralec, Barbara; Lewera, Adam; Kulesza, Pawel J.

2016-05-01

The role Keggin-type phosphomolybdate (PMo12O403-) ions (adsorbed on carbon-supported PtRu, PtRu/C) on electrooxidation of ethanol is addressed here. The combined results obtained using Differential Electrochemical Mass Spectrometry, X-ray Photoelectron Spectroscopy and Cyclic Voltammetry are consistent with the view that presence of the Keggin-type polyoxometallate, phosphomolybdate, ions (adsorbates) leads to enlargement of the current densities associated with electrooxidation of ethanol at potentials greater than 700 mV vs. RHE. This increase of the anodic currents is correlated with the higher acetaldehyde yield which is likely to reflect changes in the reaction kinetics (e.g. more dynamic dehydrogenation of ethanol leading to acetaldehyde) or in the reaction mechanism defined by the preferential surface modification resulting not only in faster kinetics but also in higher selectivity with respect to acetaldehyde production. It is apparent from the spectroscopic data that modification of PtRu/C nanoparticles with phosphomolybdate ions leads to suppression of the formation of Ru surface oxides.

Electronic structure of ferromagnetic heavy fermion, YbPdSi, YbPdGe, and YbPtGe studied by photoelectron spectroscopy, x-ray emission spectroscopy, and DFT + DMFT calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yamaoka, Hitoshi; Thunstrom, Patrik; Tsujii, Naohito

Here, the electronic structures of ferromagnetic heavy fermion Yb compounds of YbPdSi, YbPdGe, and YbPtGe are studied by photoelectron spectroscopy around the Yb 4d–4f resonance, resonant x-ray emission spectroscopy at the Yb L 3 absorption edge, and density functional theory combined with dynamical mean field theory calculations. These compounds all have a temperature-independent intermediate Yb valence with largemore » $${\\rm Yb}^{3+}$$ and small $${\\rm Yb}^{2+}$$ components. The magnitude of the Yb valence is evaluated to be YbPtGe $<$ YbPdGe $$\\lesssim $$ YbPdSi, suggesting that YbPtGe is the closest to the quantum critical point among the three Yb compounds. Our results support the scenario of the coexistence of heavy fermion behavior and ferromagnetic ordering which is described by a magnetically-ordered Kondo lattice where the magnitude of the Kondo effect and the RKKY interaction are comparable.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ito, Yuta; Wang, Chuncheng; Le, Anh-Thu

Here, we have measured the angular distributions of high energy photoelectrons of benzene molecules generated by intense infrared femtosecond laser pulses. These electrons arise from the elastic collisions between the benzene ions with the previously tunnel-ionized electrons that have been driven back by the laser field. Theory shows that laser-free elastic differential cross sections (DCSs) can be extracted from these photoelectrons, and the DCS can be used to retrieve the bond lengths of gas-phase molecules similar to the conventional electron diffraction method. From our experimental results, we have obtained the C-C and C-H bond lengths of benzene with a spatialmore » resolution of about 10 pm. Our results demonstrate that laser induced electron diffraction (LIED) experiments can be carried out with the present-day ultrafast intense lasers already. Looking ahead, with aligned or oriented molecules, more complete spatial information of the molecule can be obtained from LIED, and applying LIED to probe photo-excited molecules, a “molecular movie” of the dynamic system may be created with sub-A°ngstrom spatial and few-ten femtosecond temporal resolutions.« less

Femtosecond Electron Wave Packet Propagation and Diffraction: Towards Making the ``Molecular Movie"

NASA Astrophysics Data System (ADS)

Miller, R. J. Dwayne

2003-03-01

Time-resolved electron diffraction harbors great promise for achieving atomic resolution of the fastest chemical processes. The generation of sufficiently short electron pulses to achieve this real time view of a chemical reaction has been limited by problems in maintaining short electron pulses with realistic electron densities to the sample. The propagation dynamics of femtosecond electron packets in the drift region of a photoelectron gun are investigated with an N-body numerical simulation and mean-field model. This analyis shows that the redistribution of electrons inside the packet, arising from space-charge and dispersion contributions, changes the pulse envelope and leads to the development of a spatially linear axial velocity distribution. These results have been used in the design of femtosecond photoelectron guns with higher time resolution and novel electron-optical methods of pulse characterization that are approaching 100 fs timescales. Time-resolved diffraction studies with electron pulses of approximately 500 femtoseconds have focused on solid-liquid phase transitions under far from equilibrium conditions. This work gives a microscopic description of the melting process and illustrates the promise of atomically resolving transition state processes.

X-ray position detector and implementation in a mirror pointing servo system

DOEpatents

Rabedeau, Thomas A.; Van Campen, Douglas G.; Stefan, Peter M.

2016-04-05

An X-ray beam position and stability detector is provided having a first metal blade collinear with a second metal blade, where an edge of the first metal blade is opposite an edge of the second metal blade, where the first metal blade edge and the second metal blade edge are disposed along a centerline with respect to each other, where the metal blades are capable of photoelectron emission when exposed to an x-ray beam, a metal coating on the metal blades that is capable of enhancing the photoelectron emission, or suppressing energy-resonant contaminants, or enhancing the photoelectron emission and suppressing energy-resonant contaminants, a background shielding element having an electrode capable of suppressing photoelectron emission from spurious x-rays not contained in an x-ray beam of interest, and a photoelectron emission detector having an amplifier capable of detecting the photoelectron emission as a current signal.

Photoelectron spectrometer for attosecond spectroscopy of liquids and gases

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jordan, I.; Huppert, M.; Wörner, H. J., E-mail: hwoerner@ethz.ch

2015-12-15

A new apparatus for attosecond time-resolved photoelectron spectroscopy of liquids and gases is described. It combines a liquid microjet source with a magnetic-bottle photoelectron spectrometer and an actively stabilized attosecond beamline. The photoelectron spectrometer permits venting and pumping of the interaction chamber without affecting the low pressure in the flight tube. This pressure separation has been realized through a sliding skimmer plate, which effectively seals the flight tube in its closed position and functions as a differential pumping stage in its open position. A high-harmonic photon spectrometer, attached to the photoelectron spectrometer, exit port is used to acquire photon spectramore » for calibration purposes. Attosecond pulse trains have been used to record photoelectron spectra of noble gases, water in the gas and liquid states as well as solvated species. RABBIT scans demonstrate the attosecond resolution of this setup.« less

Recent advances in integrated multidisciplinary optimization of rotorcraft

NASA Technical Reports Server (NTRS)

Adelman, Howard M.; Walsh, Joanne L.; Pritchard, Jocelyn I.

1992-01-01

A joint activity involving NASA and Army researchers at NASA LaRC to develop optimization procedures to improve the rotor blade design process by integrating appropriate disciplines and accounting for all of the important interactions among the disciplines is described. The disciplines involved include rotor aerodynamics, rotor dynamics, rotor structures, airframe dynamics, and acoustics. The work is focused on combining these five key disciplines in an optimization procedure capable of designing a rotor system to satisfy multidisciplinary design requirements. Fundamental to the plan is a three-phased approach. In phase 1, the disciplines of blade dynamics, blade aerodynamics, and blade structure are closely coupled while acoustics and airframe dynamics are decoupled and are accounted for as effective constraints on the design for the first three disciplines. In phase 2, acoustics is integrated with the first three disciplines. Finally, in phase 3, airframe dynamics is integrated with the other four disciplines. Representative results from work performed to date are described. These include optimal placement of tuning masses for reduction of blade vibratory shear forces, integrated aerodynamic/dynamic optimization, and integrated aerodynamic/dynamic/structural optimization. Examples of validating procedures are described.

Recent advances in multidisciplinary optimization of rotorcraft

NASA Technical Reports Server (NTRS)

Adelman, Howard M.; Walsh, Joanne L.; Pritchard, Jocelyn I.

1992-01-01

A joint activity involving NASA and Army researchers at NASA LaRC to develop optimization procedures to improve the rotor blade design process by integrating appropriate disciplines and accounting for all of the important interactions among the disciplines is described. The disciplines involved include rotor aerodynamics, rotor dynamics, rotor structures, airframe dynamics, and acoustics. The work is focused on combining these five key disciplines in an optimization procedure capable of designing a rotor system to satisfy multidisciplinary design requirements. Fundamental to the plan is a three-phased approach. In phase 1, the disciplines of blade dynamics, blade aerodynamics, and blade structure are closely coupled while acoustics and airframe dynamics are decoupled and are accounted for as effective constraints on the design for the first three disciplines. In phase 2, acoustics is integrated with the first three disciplines. Finally, in phase 3, airframe dynamics is integrated with the other four disciplines. Representative results from work performed to date are described. These include optimal placement of tuning masses for reduction of blade vibratory shear forces, integrated aerodynamic/dynamic optimization, and integrated aerodynamic/dynamic/structural optimization. Examples of validating procedures are described.

Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts

DOE PAGES

Zugic, Branko; Wang, Lucun; Heine, Christian; ...

2016-12-19

Bimetallic, nanostructured materials hold promise for improving catalyst activity and selectivity, yet little is known about the dynamic compositional and structural changes that these systems undergo during pretreatment that leads to efficient catalyst function. Here we use ozone-activated silver–gold alloys in the form of nanoporous gold as a case study to demonstrate the dynamic behaviour of bimetallic systems during activation to produce a functioning catalyst. We show that it is these dynamic changes that give rise to the observed catalytic activity. Advanced in situ electron microscopy and X-ray photoelectron spectroscopy are used to demonstrate that major restructuring and compositional changesmore » occur along the path to catalytic function for selective alcohol oxidation. Transient kinetic measurements correlate the restructuring to three types of oxygen on the surface. The direct influence of changes in surface silver concentration and restructuring at the nanoscale on oxidation activity is demonstrated. Finally, our results demonstrate that characterization of these dynamic changes is necessary to unlock the full potential of bimetallic catalytic materials.« less

Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zugic, Branko; Wang, Lucun; Heine, Christian

Bimetallic, nanostructured materials hold promise for improving catalyst activity and selectivity, yet little is known about the dynamic compositional and structural changes that these systems undergo during pretreatment that leads to efficient catalyst function. Here we use ozone-activated silver–gold alloys in the form of nanoporous gold as a case study to demonstrate the dynamic behaviour of bimetallic systems during activation to produce a functioning catalyst. We show that it is these dynamic changes that give rise to the observed catalytic activity. Advanced in situ electron microscopy and X-ray photoelectron spectroscopy are used to demonstrate that major restructuring and compositional changesmore » occur along the path to catalytic function for selective alcohol oxidation. Transient kinetic measurements correlate the restructuring to three types of oxygen on the surface. The direct influence of changes in surface silver concentration and restructuring at the nanoscale on oxidation activity is demonstrated. Finally, our results demonstrate that characterization of these dynamic changes is necessary to unlock the full potential of bimetallic catalytic materials.« less

Ultrafast Dynamics of 1,3-Cyclohexadiene in Highly Excited States

DOE PAGES

Bühler, Christine C.; Minitti, Michael P.; Deb, Sanghamitra; ...

2011-01-01

The ultrafast dynamics of 1,3-cyclohexadiene has been investigated via structurally sensitive Rydberg electron binding energies and shown to differ upon excitation to the 1B state and the 3p Rydberg state. Excitation of the molecule with 4.63 eV photons into the ultrashort-lived 1B state yields the well-known ring opening to 1,3,5-hexatriene, while a 5.99 eV photon lifts the molecule directly into the 3p-Rydberg state. Excitation to 3p does not induce ring opening. In both experiments, time-dependent shifts of the Rydberg electron binding energy reflect the structural dynamics of the molecular core. Structural distortions associated with 3p-excitation cause a dynamical shift in the -more » and -binding energies by 10 and 26 meV/ps, respectively, whereas after excitation into 1B, more severe structural transformations along the ring-opening coordinate produce shifts at a rate of 40 to 60 meV/ps. The experiment validates photoionization-photoelectron spectroscopy via Rydberg states as a powerful technique to observe structural dynamics of polyatomic molecules.« less

Single photon detection with self-quenching multiplication

NASA Technical Reports Server (NTRS)

Zheng, Xinyu (Inventor); Cunningham, Thomas J. (Inventor); Pain, Bedabrata (Inventor)

2011-01-01

A photoelectronic device and an avalanche self-quenching process for a photoelectronic device are described. The photoelectronic device comprises a nanoscale semiconductor multiplication region and a nanoscale doped semiconductor quenching structure including a depletion region and an undepletion region. The photoelectronic device can act as a single photon detector or a single carrier multiplier. The avalanche self-quenching process allows electrical field reduction in the multiplication region by movement of the multiplication carriers, thus quenching the avalanche.

Photoelectron Effects on the Self-Consistent Potential in the Collisionless Polar Wind

NASA Technical Reports Server (NTRS)

Khazanov, G. V.; Liemohn, M. W.; Moore, T. E.

1997-01-01

The presence of unthermalized photoelectrons in the sunlit polar cap leads to an enhanced ambipolar potential drop and enhanced upward ion acceleration. Observations in the topside ionosphere have led to the conclusion that large-scale electrostatic potential drops exist above the spacecraft along polar magnetic field lines connected to regions of photoelectron production. A kinetic approach is used for the O(+), H(+), and photoelectron (p) distributions, while a fluid approach is used to describe the thermal electrons (e) and self-consistent electric field (E(sub II)) electrons are allowed to carry a flux that compensates for photoelectron escape, a critical assumption. Collisional processes are excluded, leading to easier escape of polar wind particles and therefore to the formation of the largest potential drop consistent with this general approach. We compute the steady state electric field enhancement and net potential drop expected in the polar wind due to the presence of photoelectrons as a function of the fractional photoelectron content and the thermal plasma characteristics. For a set of low-altitude boundary conditions typical of the polar wind ionosphere, including 0.1% photoelectron content, we found a potential drop from 500 km to 5 R(sub E) of 6.5 V and a maximum thermal electron temperature of 8800 K. The reasonable agreement of our results with the observed polar wind suggests that the assumptions of this approach are valid.

Regulation of Dynamical Systems to Optimal Solutions of Semidefinite Programs: Algorithms and Applications to AC Optimal Power Flow

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dall'Anese, Emiliano; Dhople, Sairaj V.; Giannakis, Georgios B.

2015-07-01

This paper considers a collection of networked nonlinear dynamical systems, and addresses the synthesis of feedback controllers that seek optimal operating points corresponding to the solution of pertinent network-wide optimization problems. Particular emphasis is placed on the solution of semidefinite programs (SDPs). The design of the feedback controller is grounded on a dual e-subgradient approach, with the dual iterates utilized to dynamically update the dynamical-system reference signals. Global convergence is guaranteed for diminishing stepsize rules, even when the reference inputs are updated at a faster rate than the dynamical-system settling time. The application of the proposed framework to the controlmore » of power-electronic inverters in AC distribution systems is discussed. The objective is to bridge the time-scale separation between real-time inverter control and network-wide optimization. Optimization objectives assume the form of SDP relaxations of prototypical AC optimal power flow problems.« less

Dynamics of dipole- and valence bound anions in iodide-adenine binary complexes: A time-resolved photoelectron imaging and quantum mechanical investigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stephansen, Anne B.; King, Sarah B.; Li, Wei-Li

2015-09-14

Dipole bound (DB) and valence bound (VB) anions of binary iodide-adenine complexes have been studied using one-color and time-resolved photoelectron imaging at excitation energies near the vertical detachment energy. The experiments are complemented by quantum chemical calculations. One-color spectra show evidence for two adenine tautomers, the canonical, biologically relevant A9 tautomer and the A3 tautomer. In the UV-pump/IR-probe time-resolved experiments, transient adenine anions can be formed by electron transfer from the iodide. These experiments show signals from both DB and VB states of adenine anions formed on femto- and picosecond time scales, respectively. Analysis of the spectra and comparison withmore » calculations suggest that while both the A9 and A3 tautomers contribute to the DB signal, only the DB state of the A3 tautomer undergoes a transition to the VB anion. The VB anion of A9 is higher in energy than both the DB anion and the neutral, and the VB anion is therefore not accessible through the DB state. Experimental evidence of the metastable A9 VB anion is instead observed as a shape resonance in the one-color photoelectron spectra, as a result of UV absorption by A9 and subsequent electron transfer from iodide into the empty π-orbital. In contrast, the iodide-A3 complex constitutes an excellent example of how DB states can act as doorway state for VB anion formation when the VB state is energetically available.« less

Vibrationally-resolved Photoelectron Spectroscopy of the Model GFP Chromophore Anion Revealing the Photoexcited S-1 State being both Vertically and Adiabatically Bound against the Photodetached D-0 Continuum

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deng, Shihu; Kong, Xiangyu; Zhang, GuanXin

2014-06-19

The first excited state of the model green fluorescence protein (GFP) chromophore anion (S1) and its energy level against the electron-detached neutral radical, D0 state are crucial in determining the photophysics and the photo-induced dynamics of GFP. Extensive experimental and theoretical studies, particularly several very recent gas phase investigations concluded that S1 is a bound state in the Franck-Condon vertical region with respect to D0. However, what remains unknown and challenging is if S1 is bound adiabatically, primarily due to lack of accurate experimental measurements, as well as due to close proximity in energy for these two states that evenmore » sophisticated high-level ab initio calculations can’t reliably predict. Here, we report a negative ion photoelectron spectroscopy study on the model GFP chromophore anion, the deprotonated p-hydroxybenzylidene-2,3-dimethylimidazolinone anion (HBDI–). Despite the considerable size and low symmetry of the molecule, well resolved vibrational structures were obtained with the 0–0 transition being the most intense peak. The adiabatic (ADE) and vertical detachment energy (VDE) therefore are determined, both to be 2.73 ± 0.01 eV, indicating the detached D0 state is 0.16 eV higher in energy than the photon excited S1 state. The accurate ADE and VDE values and the well-resolved photoelectron spectra reported here provide much needed, robust benchmarks for future theoretical investigations.« less

Sorption isotherms, kinetic and optimization process of amino acid proline based polymer nanocomposite for the removal of selected textile dyes from industrial wastewater.

PubMed

Raghunath, Sharista; Anand, K; Gengan, R M; Nayunigari, Mithil Kumar; Maity, Arjun

2016-12-01

In this article, adsorption and kinetic studies were carried out on three textile dyes, namely Reactive Blue 222 (RB 222), Reactive Red 195 (RR 195) and Reactive Yellow 145 (RY 145). The dyes studied in a mixture were adsorbed under various conditions onto PRO-BEN, a bentonite modified with a new cationic proline polymer (l-proline-epichlorohydrin polymer). The proline polymer was characterized by 1 H NMR, Fourier transform infrared spectroscopy (FT-IR), dynamic light scattering (DLS) and TEM. The PRO-BEN composite was characterized by FT-IR, dynamic light scattering (DLS) (zeta potential), TEM imaging, SEM/EDX and X-ray photoelectron spectroscopy (characterize the binding energy). During adsorption studies, factors involving pH, temperature, the initial concentrations of the dyes and the quantity of PRO-BEN used during adsorption were established. The results revealed that the adsorption mechanism was categorized by the Langmuir type 1 isotherm. The adsorption data followed the pseudo-second order kinetic model. The intraparticle diffusion model indicated that adsorption did not only depend on the intraparticle diffusion of the dyes. The thermodynamic parameters verified that the adsorption process was spontaneous and exothermic. The Gibbs free energy values indicated that physisorption had occurred. Successful adsorption of dyes from an industrial effluent was achieved. Desorption studies concluded that PRO-BEN desorbed the dyes better than alumina. This can thereby be viewed as a recyclable remediation material. The PRO-BEN composite could be a cost efficient alternative towards the removal of organic dyes in wastewater treatment. Copyright © 2016 Elsevier B.V. All rights reserved.

Fully integrated aerodynamic/dynamic optimization of helicopter rotor blades

NASA Technical Reports Server (NTRS)

Walsh, Joanne L.; Lamarsh, William J., II; Adelman, Howard M.

1992-01-01

This paper describes a fully integrated aerodynamic/dynamic optimization procedure for helicopter rotor blades. The procedure combines performance and dynamics analyses with a general purpose optimizer. The procedure minimizes a linear combination of power required (in hover, forward flight, and maneuver) and vibratory hub shear. The design variables include pretwist, taper initiation, taper ratio, root chord, blade stiffnesses, tuning masses, and tuning mass locations. Aerodynamic constraints consist of limits on power required in hover, forward flight and maneuver; airfoil section stall; drag divergence Mach number; minimum tip chord; and trim. Dynamic constraints are on frequencies, minimum autorotational inertia, and maximum blade weight. The procedure is demonstrated for two cases. In the first case the objective function involves power required (in hover, forward flight, and maneuver) and dynamics. The second case involves only hover power and dynamics. The designs from the integrated procedure are compared with designs from a sequential optimization approach in which the blade is first optimized for performance and then for dynamics. In both cases, the integrated approach is superior.

Fully integrated aerodynamic/dynamic optimization of helicopter rotor blades

NASA Technical Reports Server (NTRS)

Walsh, Joanne L.; Lamarsh, William J., II; Adelman, Howard M.

1992-01-01

A fully integrated aerodynamic/dynamic optimization procedure is described for helicopter rotor blades. The procedure combines performance and dynamic analyses with a general purpose optimizer. The procedure minimizes a linear combination of power required (in hover, forward flight, and maneuver) and vibratory hub shear. The design variables include pretwist, taper initiation, taper ratio, root chord, blade stiffnesses, tuning masses, and tuning mass locations. Aerodynamic constraints consist of limits on power required in hover, forward flight and maneuvers; airfoil section stall; drag divergence Mach number; minimum tip chord; and trim. Dynamic constraints are on frequencies, minimum autorotational inertia, and maximum blade weight. The procedure is demonstrated for two cases. In the first case, the objective function involves power required (in hover, forward flight and maneuver) and dynamics. The second case involves only hover power and dynamics. The designs from the integrated procedure are compared with designs from a sequential optimization approach in which the blade is first optimized for performance and then for dynamics. In both cases, the integrated approach is superior.

Measurements of the ambient photoelectron spectrum from Atmosphere Explorer. I - AE-E measurements below 300 km during solar minimum conditions. II - AE-E measurements from 300 to 1000 km during solar minimum conditions

NASA Technical Reports Server (NTRS)

Lee, J. S.; Doering, J. P.; Potemra, T. A.; Brace, L. H.

1980-01-01

A study is presented of the ambient photoelectron spectrum below 300 km which includes 500 AE-E orbits observed from Dec. 13, 1975 to Feb. 24, 1976. The daytime photoelectron spectrum from 1 to 100 eV was illustrated by several spectra; high resolution 10-32 eV spectra show the widths of the photoelectron lines and the variation of the linewidth and intensity with altitude. The photoelectron flux below 300 km is constant over a period of several months; the photoelectron lines between 20 and 30 eV are very sharp when the total plasma density is low, but broaden at high altitudes as the plasma density builds up during the day. The photo-electron flux above 300 km had an intensity and energy spectrum characteristic of the 250-300 km region only in the presence of low plasma density at the satellite altitude. The flux at high altitudes was extremely variable 3 h after sunrise as a result of attenuation and energy loss to thermal plasma along the path of escaping electrons.

Optimization of fuel-cell tram operation based on two dimension dynamic programming

NASA Astrophysics Data System (ADS)

Zhang, Wenbin; Lu, Xuecheng; Zhao, Jingsong; Li, Jianqiu

2018-02-01

This paper proposes an optimal control strategy based on the two-dimension dynamic programming (2DDP) algorithm targeting at minimizing operation energy consumption for a fuel-cell tram. The energy consumption model with the tram dynamics is firstly deduced. Optimal control problem are analyzed and the 2DDP strategy is applied to solve the problem. The optimal tram speed profiles are obtained for each interstation which consist of three stages: accelerate to the set speed with the maximum traction power, dynamically adjust to maintain a uniform speed and decelerate to zero speed with the maximum braking power at a suitable timing. The optimal control curves of all the interstations are connected with the parking time to form the optimal control method of the whole line. The optimized speed profiles are also simplified for drivers to follow.

Optimal Strategy for Integrated Dynamic Inventory Control and Supplier Selection in Unknown Environment via Stochastic Dynamic Programming

NASA Astrophysics Data System (ADS)

Sutrisno; Widowati; Solikhin

2016-06-01

In this paper, we propose a mathematical model in stochastic dynamic optimization form to determine the optimal strategy for an integrated single product inventory control problem and supplier selection problem where the demand and purchasing cost parameters are random. For each time period, by using the proposed model, we decide the optimal supplier and calculate the optimal product volume purchased from the optimal supplier so that the inventory level will be located at some point as close as possible to the reference point with minimal cost. We use stochastic dynamic programming to solve this problem and give several numerical experiments to evaluate the model. From the results, for each time period, the proposed model was generated the optimal supplier and the inventory level was tracked the reference point well.

Application of numerical optimization techniques to control system design for nonlinear dynamic models of aircraft

NASA Technical Reports Server (NTRS)

Lan, C. Edward; Ge, Fuying

1989-01-01

Control system design for general nonlinear flight dynamic models is considered through numerical simulation. The design is accomplished through a numerical optimizer coupled with analysis of flight dynamic equations. The general flight dynamic equations are numerically integrated and dynamic characteristics are then identified from the dynamic response. The design variables are determined iteratively by the optimizer to optimize a prescribed objective function which is related to desired dynamic characteristics. Generality of the method allows nonlinear effects to aerodynamics and dynamic coupling to be considered in the design process. To demonstrate the method, nonlinear simulation models for an F-5A and an F-16 configurations are used to design dampers to satisfy specifications on flying qualities and control systems to prevent departure. The results indicate that the present method is simple in formulation and effective in satisfying the design objectives.

A parameters optimization method for planar joint clearance model and its application for dynamics simulation of reciprocating compressor

NASA Astrophysics Data System (ADS)

Hai-yang, Zhao; Min-qiang, Xu; Jin-dong, Wang; Yong-bo, Li

2015-05-01

In order to improve the accuracy of dynamics response simulation for mechanism with joint clearance, a parameter optimization method for planar joint clearance contact force model was presented in this paper, and the optimized parameters were applied to the dynamics response simulation for mechanism with oversized joint clearance fault. By studying the effect of increased clearance on the parameters of joint clearance contact force model, the relation of model parameters between different clearances was concluded. Then the dynamic equation of a two-stage reciprocating compressor with four joint clearances was developed using Lagrange method, and a multi-body dynamic model built in ADAMS software was used to solve this equation. To obtain a simulated dynamic response much closer to that of experimental tests, the parameters of joint clearance model, instead of using the designed values, were optimized by genetic algorithms approach. Finally, the optimized parameters were applied to simulate the dynamics response of model with oversized joint clearance fault according to the concluded parameter relation. The dynamics response of experimental test verified the effectiveness of this application.

miRNA purification with an optimized PDMS microdevice: Toward the direct purification of low abundant circulating biomarkers.

PubMed

Santini, G C; Potrich, C; Lunelli, L; Vanzetti, L; Marasso, S L; Cocuzza, M; Pirri, F C; Pederzolli, C

2017-10-01

A reliable clinical assay based on circulating microRNAs (miRNAs) as biomarkers is highly required. Microdevices offer an attractive solution as a fast and inexpensive way of concentrating these biomarkers from a low sample volume. A previously developed polydimethylsiloxane (PDMS) microdevice able to purify and detect circulating miRNAs was here optimized. The optimization of the morphological and chemical surface properties by nanopatterning and functionalization is presented. Surfaces were firstly characterized by atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), fluorescamine assay and s-SDTB (sulphosuccinimidyl-4-o-(4,4-dimethoxytrityl) butyrate) assay and subsequently tested for their capacity to adsorb a fluorescent miRNA. From our analysis, modification of surface charge with 0.1% APTMS ((3-Aminopropyl)trimethoxysilane) and 0.9% PEG-s (2-[Methoxy-(polyethyleneoxy)propyl]trimethoxysilane) performed at 60°C for 10min was identified as the best purification condition. Our optimized microdevice integrated with real-time PCR detection, was demonstrated to selectively purify both synthetic and natural circulating miRNAs with a sensitivity of 0.01pM. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches.

PubMed

Antipov, Sergey V; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2017-11-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research "Molecular Ultrafast Science and Technology," are presented: These include Bohmian dynamics description of the collision of H with H 2 , local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches

PubMed Central

Antipov, Sergey V.; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2018-01-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research “Molecular Ultrafast Science and Technology,” are presented: These include Bohmian dynamics description of the collision of H with H2, local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase. PMID:29376107

Surveys of research in the Chemistry Division, Argonne National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grazis, B.M.

1992-01-01

Research reports are presented on reactive intermediates in condensed phase (radiation chemistry, photochemistry), electron transfer and energy conversion, photosynthesis and solar energy conversion, metal cluster chemistry, chemical dynamics in gas phase, photoionization-photoelectrons, characterization and reactivity of coal and coal macerals, premium coal sample program, chemical separations, heavy elements coordination chemistry, heavy elements photophysics/photochemistry, f-electron interactions, radiation chemistry of high-level wastes (gas generation in waste tanks), ultrafast molecular electronic devices, and nuclear medicine. Separate abstracts have been prepared. Accelerator activites and computer system/network services are also reported.

Surveys of research in the Chemistry Division, Argonne National Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grazis, B.M.

1992-11-01

Research reports are presented on reactive intermediates in condensed phase (radiation chemistry, photochemistry), electron transfer and energy conversion, photosynthesis and solar energy conversion, metal cluster chemistry, chemical dynamics in gas phase, photoionization-photoelectrons, characterization and reactivity of coal and coal macerals, premium coal sample program, chemical separations, heavy elements coordination chemistry, heavy elements photophysics/photochemistry, f-electron interactions, radiation chemistry of high-level wastes (gas generation in waste tanks), ultrafast molecular electronic devices, and nuclear medicine. Separate abstracts have been prepared. Accelerator activites and computer system/network services are also reported.

Intense Vibronic Modulation of the Chiral Photoelectron Angular Distribution Generated by Photoionization of Limonene Enantiomers with Circularly Polarized Synchrotron Radiation.

PubMed

Rafiee Fanood, Mohammad M; Ganjitabar, Hassan; Garcia, Gustavo A; Nahon, Laurent; Turchini, Stefano; Powis, Ivan

2018-04-17

Photoionization of the chiral monoterpene limonene has been investigated using polarized synchrotron radiation between the adiabatic ionization threshold, 8.505 and 23.5 eV. A rich vibrational structure is seen in the threshold photoelectron spectrum and is interpreted using a variety of computational methods. The corresponding photoelectron circular dichroism-measured in the photoelectron angular distribution as a forward-backward asymmetry with respect to the photon direction-was found to be strongly dependent on the vibronic structure appearing in the photoelectron spectra, with the observed asymmetry even switching direction in between the major vibrational peaks. This effect can be ultimately attributed to the sensitivity of this dichroism to small phase shifts between adjacent partial waves of the outgoing photoelectron. These observations have implications for potential applications of this chiroptical technique, where the enantioselective analysis of monoterpene components is of particular interest. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Supercomputer optimizations for stochastic optimal control applications

NASA Technical Reports Server (NTRS)

Chung, Siu-Leung; Hanson, Floyd B.; Xu, Huihuang

1991-01-01

Supercomputer optimizations for a computational method of solving stochastic, multibody, dynamic programming problems are presented. The computational method is valid for a general class of optimal control problems that are nonlinear, multibody dynamical systems, perturbed by general Markov noise in continuous time, i.e., nonsmooth Gaussian as well as jump Poisson random white noise. Optimization techniques for vector multiprocessors or vectorizing supercomputers include advanced data structures, loop restructuring, loop collapsing, blocking, and compiler directives. These advanced computing techniques and superconducting hardware help alleviate Bellman's curse of dimensionality in dynamic programming computations, by permitting the solution of large multibody problems. Possible applications include lumped flight dynamics models for uncertain environments, such as large scale and background random aerospace fluctuations.

Ab Initio Theory of Dynamical Core-Hole Screening in Graphite from X-Ray Absorption Spectra

NASA Astrophysics Data System (ADS)

Wessely, O.; Katsnelson, M. I.; Eriksson, O.

2005-04-01

We have implemented the effect of dynamical core-hole screening, as given by Mahan, Nozières, and De Dominicis, in a first-principles based method and applied the theory to the x-ray absorption (XA) spectrum of graphite. It turns out that two of the conspicuous peaks of graphite are well described, both regarding the position, shape, and relative intensity, whereas one peak is absent in the theory. Only by incorporation of both excitonic and delocalized processes can a full account of the experimental spectrum be obtained theoretically, and we interpret the XA spectrum in graphite to be the result of a well screened and a poor screened process, much in the same way as is done for core level x-ray photoelectron spectroscopy.

Photoelectron Imaging as a Quantum Chemistry Visualization Tool

ERIC Educational Resources Information Center

Grumbling, Emily R.; Pichugin, Kostyantyn; Mabbs, Richard; Sanov, Andrei

2011-01-01

An overview and simple example of photoelectron imaging is presented, highlighting its efficacy as a pedagogical tool for visualizing quantum phenomena. Specifically, photoelectron imaging of H[superscript -] (the simplest negative ion) is used to demonstrate several quantum mechanical principles. This example could be incorporated into an…

High-resolution soft X-ray beamline ADRESS at the Swiss Light Source for resonant inelastic X-ray scattering and angle-resolved photoelectron spectroscopies

PubMed Central

Strocov, V. N.; Schmitt, T.; Flechsig, U.; Schmidt, T.; Imhof, A.; Chen, Q.; Raabe, J.; Betemps, R.; Zimoch, D.; Krempasky, J.; Wang, X.; Grioni, M.; Piazzalunga, A.; Patthey, L.

2010-01-01

The concepts and technical realisation of the high-resolution soft X-ray beamline ADRESS operating in the energy range from 300 to 1600 eV and intended for resonant inelastic X-ray scattering (RIXS) and angle-resolved photoelectron spectroscopy (ARPES) are described. The photon source is an undulator of novel fixed-gap design where longitudinal movement of permanent magnetic arrays controls not only the light polarization (including circular and 0–180° rotatable linear polarizations) but also the energy without changing the gap. The beamline optics is based on the well established scheme of plane-grating monochromator operating in collimated light. The ultimate resolving power E/ΔE is above 33000 at 1 keV photon energy. The choice of blazed versus lamellar gratings and optimization of their profile parameters is described. Owing to glancing angles on the mirrors as well as optimized groove densities and profiles of the gratings, the beamline is capable of delivering high photon flux up to 1 × 1013 photons s−1 (0.01% BW)−1 at 1 keV. Ellipsoidal refocusing optics used for the RIXS endstation demagnifies the vertical spot size down to 4 µm, which allows slitless operation and thus maximal transmission of the high-resolution RIXS spectrometer delivering E/ΔE > 11000 at 1 keV photon energy. Apart from the beamline optics, an overview of the control system is given, the diagnostics and software tools are described, and strategies used for the optical alignment are discussed. An introduction to the concepts and instrumental realisation of the ARPES and RIXS endstations is given. PMID:20724785

Mystic: Implementation of the Static Dynamic Optimal Control Algorithm for High-Fidelity, Low-Thrust Trajectory Design

NASA Technical Reports Server (NTRS)

Whiffen, Gregory J.

2006-01-01

Mystic software is designed to compute, analyze, and visualize optimal high-fidelity, low-thrust trajectories, The software can be used to analyze inter-planetary, planetocentric, and combination trajectories, Mystic also provides utilities to assist in the operation and navigation of low-thrust spacecraft. Mystic will be used to design and navigate the NASA's Dawn Discovery mission to orbit the two largest asteroids, The underlying optimization algorithm used in the Mystic software is called Static/Dynamic Optimal Control (SDC). SDC is a nonlinear optimal control method designed to optimize both 'static variables' (parameters) and dynamic variables (functions of time) simultaneously. SDC is a general nonlinear optimal control algorithm based on Bellman's principal.

Initial state-specific photodissociation dynamics of pyrrole via 1 π σ ∗/ S 0 conical intersection initiated with optimally controlled UV-laser pulses

NASA Astrophysics Data System (ADS)

Nandipati, K. R.; Kanakati, Arun Kumar; Singh, H.; Lan, Z.; Mahapatra, S.

2017-09-01

Optimal initiation of quantum dynamics of N-H photodissociation of pyrrole on the S0-1πσ∗(1A2) coupled electronic states by UV-laser pulses in an effort to guide the subsequent dynamics to dissociation limits is studied theoretically. Specifically, the task of designing optimal laser pulses that act on initial vibrational states of the system for an effective UV-photodissociation is considered by employing optimal control theory. The associated control mechanism(s) for the initial state dependent photodissociation dynamics of pyrrole in the presence of control pulses is examined and discussed in detail. The initial conditions determine implicitly the variation in the dissociation probabilities for the two channels, upon interaction with the field. The optimal pulse corresponds to the objective fixed as maximization of overall reactive flux subject to constraints of reasonable fluence and quantum dynamics. The simple optimal pulses obtained by the use of genetic algorithm based optimization are worth an experimental implementation given the experimental relevance of πσ∗-photochemistry in recent times.

An experimental and theoretical study of the valence shell photoelectron spectra of 2-chloropyridine and 3-chloropyridine

NASA Astrophysics Data System (ADS)

Holland, D. M. P.; Powis, I.; Trofimov, A. B.; Menzies, R. C.; Potts, A. W.; Karlsson, L.; Badsyuk, I. L.; Moskovskaya, T. E.; Gromov, E. V.; Schirmer, J.

2017-10-01

The valence shell photoelectron spectra of 2-chloropyridine and 3-chloropyridine have been studied both experimentally and theoretically. Synchrotron radiation has been employed to record angle resolved photoelectron spectra in the photon energy range 20-100 eV, and these have enabled anisotropy parameters and branching ratios to be derived. The experimental results have been compared with theoretical predictions obtained using the continuum multiple scattering Xα approach. This comparison shows that the anisotropy parameter associated with the nominally chlorine lone-pair orbital lying in the molecular plane is strongly affected by the atomic Cooper minimum. In contrast, the photoionization dynamics of the second lone-pair orbital, orientated perpendicular to the molecular plane, seem relatively unaffected by this atomic phenomenon. The outer valence ionization has been studied theoretically using the third-order algebraic-diagrammatic construction (ADC(3)) approximation scheme for the one-particle Green's function, the outer valence Green's function method, and the equation-of-motion (EOM) coupled cluster (CC) theory at the level of the EOM-IP-CCSD and EOM-EE-CC3 models. The convergence of the results to the complete basis set limit has been investigated. The ADC(3) method has been employed to compute the complete valence shell ionization spectra of 2-chloropyridine and 3-chloropyridine. The relaxation mechanism for ionization of the nitrogen σ-type lone-pair orbital (σN LP) has been found to be different to that for the corresponding chlorine lone-pair (σCl LP). For the σN LP orbital, π-π* excitations play the main role in the screening of the lone-pair hole. In contrast, excitations localized at the chlorine site involving the chlorine πCl LP lone-pair and the Cl 4p Rydberg orbital are the most important for the σCl LP orbital. The calculated photoelectron spectra have allowed assignments to be proposed for most of the structure observed in the experimental spectra. The theoretical work also highlights the formation of satellite states, due to the breakdown of the single particle model of ionization, in the inner valence region.

Ultrafast photoelectron spectroscopy of small molecule organic films

NASA Astrophysics Data System (ADS)

Read, Kendall Laine

As research in the field of ultrafast optics has produced shorter and shorter pulses, at an ever-widening range of frequencies, ultrafast spectroscopy has grown correspondingly. In particular, ultrafast photoelectron spectroscopy allows direct observation of electrons in transient or excited states, regardless of the eventual relaxation mechanisms. High-harmonic conversion of 800nm, femtosecond, Ti:sapphire laser pulses allows excite/probe spectroscopy down into atomic core level states. To this end, an ultrafast, X-UV photoelectron spectroscopic system is described, including design considerations for the high-harmonic generation line, the time of flight detector, and the subsequent data collection electronics. Using a similar experimental setup, I have performed several ultrafast, photoelectron excited state decay studies at the IBM, T. J. Watson Research Center. All of the observed materials were electroluminescent thin film organics, which have applications as the emitter layer in organic light emitting devices. The specific materials discussed are: Alq, BAlq, DPVBi, and Alq doped with DCM or DMQA. Alq:DCM is also known to lase at low photoexcitation thresholds. A detailed understanding of the involved relaxation mechanisms is beneficial to both applications. Using 3.14 eV excite, and 26.7 eV probe, 90 fs laser pulses, we have observed the lowest unoccupied molecular orbital (LUMO) decay rate over the first 200 picoseconds. During this time, diffusion is insignificant, and all dynamics occur in the absence of electron transport. With excitation intensities in the range of 100μJ/cm2, we have modeled the Alq, BAlq, and DPVBi decays via bimolecular singlet-singlet annihilation. At similar excitations, we have modeled the Alq:DCM decay via Förster transfer, stimulated emission, and excimeric formation. Furthermore, the Alq:DCM occupied to unoccupied molecular orbital energy gap was seen to shrink as a function of excite-to-probe delay, in accordance with the expected relaxation within the excited states. Stable, shorter pulses allow finer temporal resolution and more efficient high-harmonic generation. This work therefore concludes by discussing a method for further shortening 25 femtosecond pulses via self-phase modulation, using filamentation in air and subsequent fiber channeling.

An experimental and theoretical study of the valence shell photoelectron spectra of 2-chloropyridine and 3-chloropyridine.

PubMed

Holland, D M P; Powis, I; Trofimov, A B; Menzies, R C; Potts, A W; Karlsson, L; Badsyuk, I L; Moskovskaya, T E; Gromov, E V; Schirmer, J

2017-10-28

The valence shell photoelectron spectra of 2-chloropyridine and 3-chloropyridine have been studied both experimentally and theoretically. Synchrotron radiation has been employed to record angle resolved photoelectron spectra in the photon energy range 20-100 eV, and these have enabled anisotropy parameters and branching ratios to be derived. The experimental results have been compared with theoretical predictions obtained using the continuum multiple scattering Xα approach. This comparison shows that the anisotropy parameter associated with the nominally chlorine lone-pair orbital lying in the molecular plane is strongly affected by the atomic Cooper minimum. In contrast, the photoionization dynamics of the second lone-pair orbital, orientated perpendicular to the molecular plane, seem relatively unaffected by this atomic phenomenon. The outer valence ionization has been studied theoretically using the third-order algebraic-diagrammatic construction (ADC(3)) approximation scheme for the one-particle Green's function, the outer valence Green's function method, and the equation-of-motion (EOM) coupled cluster (CC) theory at the level of the EOM-IP-CCSD and EOM-EE-CC3 models. The convergence of the results to the complete basis set limit has been investigated. The ADC(3) method has been employed to compute the complete valence shell ionization spectra of 2-chloropyridine and 3-chloropyridine. The relaxation mechanism for ionization of the nitrogen σ-type lone-pair orbital (σ N LP ) has been found to be different to that for the corresponding chlorine lone-pair (σ Cl LP ). For the σ N LP orbital, π-π* excitations play the main role in the screening of the lone-pair hole. In contrast, excitations localized at the chlorine site involving the chlorine π Cl LP lone-pair and the Cl 4p Rydberg orbital are the most important for the σ Cl LP orbital. The calculated photoelectron spectra have allowed assignments to be proposed for most of the structure observed in the experimental spectra. The theoretical work also highlights the formation of satellite states, due to the breakdown of the single particle model of ionization, in the inner valence region.

75 FR 63810 - Grant of Authority for Subzone Status; SICK, Inc. (Photo-Electronic Industrial Sensors...

Federal Register 2010, 2011, 2012, 2013, 2014

2010-10-18

... Status; SICK, Inc. (Photo- Electronic Industrial Sensors); Bloomington, MN Pursuant to its authority... to establish a special- purpose subzone at the photo-electronic industrial sensor manufacturing and... manufacturing and distribution of photo-electronic industrial sensors at the SICK, Inc., facility located in...

Photoelectron energy-loss study of the Bi2CaSr2Cu2O8 superconductor

NASA Astrophysics Data System (ADS)

Shen, Z.-X.; Lindberg, P. A. P.; Dessau, D. S.; Lindau, I.; Spicer, W. E.; Mitzi, D. B.; Bozovic, I.; Kapitulnik, A.

1989-03-01

Using energy-loss spectroscopy of photoelectrons from a single crystal of Bi2CaSr2Cu2O8, we show that the electronic structure of the near-surface region is the same as that of the bulk. Utilizing the fact that photoelectrons of different elements are excited at different locations in the unit cell, we identify the energy-loss features as due to valence plasmon excitations, and one-electron excitations by comparing the photoelectron energy-loss spectra of the different elements.

Renner-Teller effects in the photoelectron spectra of CNC, CCN, and HCCN.

PubMed

Coudert, Laurent H; Gans, Bérenger; Garcia, Gustavo A; Loison, Jean-Christophe

2018-02-07

The line intensity of photoelectron spectra when either the neutral or cationic species display a Renner-Teller coupling is derived and applied to the modeling of the photoelectron spectra of CNC, CCN, and HCCN. The rovibronic energy levels of these three radicals and of their cations are investigated starting from ab initio results. A model treating simultaneously the bending mode and the overall rotation is developed to deal with the quasilinearity problem in CNC + , CCN + , and HCCN and accounts for the large amplitude nature of their bending mode. This model is extended to treat the Renner-Teller coupling in CNC, CCN, and HCCN + . Based on the derived photoelectron line intensity, the photoelectron spectra of all three molecules are calculated and compared to the experimental ones.

C-learning: A new classification framework to estimate optimal dynamic treatment regimes.

PubMed

Zhang, Baqun; Zhang, Min

2017-12-11

A dynamic treatment regime is a sequence of decision rules, each corresponding to a decision point, that determine that next treatment based on each individual's own available characteristics and treatment history up to that point. We show that identifying the optimal dynamic treatment regime can be recast as a sequential optimization problem and propose a direct sequential optimization method to estimate the optimal treatment regimes. In particular, at each decision point, the optimization is equivalent to sequentially minimizing a weighted expected misclassification error. Based on this classification perspective, we propose a powerful and flexible C-learning algorithm to learn the optimal dynamic treatment regimes backward sequentially from the last stage until the first stage. C-learning is a direct optimization method that directly targets optimizing decision rules by exploiting powerful optimization/classification techniques and it allows incorporation of patient's characteristics and treatment history to improve performance, hence enjoying advantages of both the traditional outcome regression-based methods (Q- and A-learning) and the more recent direct optimization methods. The superior performance and flexibility of the proposed methods are illustrated through extensive simulation studies. © 2017, The International Biometric Society.

An experimental and theoretical study of the adsorption removal of toluene and chlorobenzene on coconut shell derived carbon.

PubMed

Zhao, Xiaoyan; Zeng, Xiaolan; Qin, Yu; Li, Xiang; Zhu, Tianle; Tang, Xiaolong

2018-04-26

The adsorption performance of toluene and chlorobenzene on prepared coconut shell derived carbon (CDC) is investigated and compared with commercial activated carbon (CAC) by experiment and theory calculation. Textural properties of prepared adsorbents are characterized by N 2 adsorption, infrared spectra (FT-IR), Raman spectra and X-ray photoelectron spectra (XPS). Adsorption isotherms of toluene and chlorobenzene are obtained and fitted using structure optimizations, Grand Canonical Monte Carlo (GCMC) simulation and thermodynamic models. The results indicate that CDC shows better volatile organic compounds (VOCs) removal performance than CAC, and chlorobenzene is easily adsorbed than toluene. On the aspect of textural characteristics, CDC possesses more micropores ratio and narrower pore size distribution than CAC. Furthermore, amounts of electron-withdrawing carbonyl groups on the CAC surface reduce the electron density of adsorbents, thus weakening the interaction between VOCs and adsorbents. On the aspect of model fitting, the Yoon and Nelson (Y-N) and Dubinin-Astakhov (D-A) models can well describe the dynamic adsorption and the adsorption equilibrium of toluene and chlorobenzene on CDC respectively. It is believed that substituent groups of adsorbates, making the charge distribution deviate, lead to adsorption potentials of chlorobenzene larger than toluene. In general, both the pore structure and the surface property of adsorbents affect the VOCs adsorption behaviors on CDC. Copyright © 2018. Published by Elsevier Ltd.

High Dielectric Performance of Solution-Processed Aluminum Oxide-Boron Nitride Composite Films

NASA Astrophysics Data System (ADS)

Yu, Byoung-Soo; Ha, Tae-Jun

2018-04-01

The material compositions of oxide films have been extensively investigated in an effort to improve the electrical characteristics of dielectrics which have been utilized in various electronic devices such as field-effect transistors, and storage capacitors. Significantly, solution-based compositions have attracted considerable attention as a highly effective and practical technique to replace vacuum-based process in large-area. Here, we demonstrate solution-processed composite films consisting of aluminum oxide (Al2O3) and boron nitride (BN), which exhibit remarkable dielectric properties through the optimization process. The leakage current of the optimized Al2O3-BN thin films was decreased by a factor of 100 at 3V, compared to pristine Al2O3 thin film without a loss of the dielectric constant or degradation of the morphological roughness. The characterization by X-ray photoelectron spectroscopy measurements revealed that the incorporation of BN with an optimized concentration into the Al2O3 dielectric film reduced the density of oxygen vacancies which act as defect states, thereby improving the dielectric characteristics.

Removal of mercury (II), elemental mercury and arsenic from simulated flue gas by ammonium sulphide.

PubMed

Ning, Ping; Guo, Xiaolong; Wang, Xueqian; Wang, Ping; Ma, Yixing; Lan, Yi

2015-01-01

A tubular resistance furnace was used as a reactor to simulate mercury and arsenic in smelter flue gases by heating mercury and arsenic compounds. The flue gas containing Hg(2+), Hg(0) and As was treated with ammonium sulphide. The experiment was conducted to investigate the effects of varying the concentration of ammonium sulphide, the pH value of ammonium sulphide, the temperature of ammonium sulphide, the presence of SO2 and the presence of sulphite ion on removal efficiency. The prepared adsorption products were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and scanning electron microscopy. The results showed that the optimal concentration of ammonium sulphide was 0.8 mol/L. The optimal pH value of ammonium sulphide was 10, and the optimal temperature of ammonium sulphide was 20°C.Under the optimum conditions, the removal efficiency of Hg(2+), Hg(0) and As could reach 99%, 88.8%, 98%, respectively. In addition, SO2 and sulphite ion could reduce the removal efficiency of mercury and arsenic from simulated flue gas.

Dynamic optimization of metabolic networks coupled with gene expression.

PubMed

Waldherr, Steffen; Oyarzún, Diego A; Bockmayr, Alexander

2015-01-21

The regulation of metabolic activity by tuning enzyme expression levels is crucial to sustain cellular growth in changing environments. Metabolic networks are often studied at steady state using constraint-based models and optimization techniques. However, metabolic adaptations driven by changes in gene expression cannot be analyzed by steady state models, as these do not account for temporal changes in biomass composition. Here we present a dynamic optimization framework that integrates the metabolic network with the dynamics of biomass production and composition. An approximation by a timescale separation leads to a coupled model of quasi-steady state constraints on the metabolic reactions, and differential equations for the substrate concentrations and biomass composition. We propose a dynamic optimization approach to determine reaction fluxes for this model, explicitly taking into account enzyme production costs and enzymatic capacity. In contrast to the established dynamic flux balance analysis, our approach allows predicting dynamic changes in both the metabolic fluxes and the biomass composition during metabolic adaptations. Discretization of the optimization problems leads to a linear program that can be efficiently solved. We applied our algorithm in two case studies: a minimal nutrient uptake network, and an abstraction of core metabolic processes in bacteria. In the minimal model, we show that the optimized uptake rates reproduce the empirical Monod growth for bacterial cultures. For the network of core metabolic processes, the dynamic optimization algorithm predicted commonly observed metabolic adaptations, such as a diauxic switch with a preference ranking for different nutrients, re-utilization of waste products after depletion of the original substrate, and metabolic adaptation to an impending nutrient depletion. These examples illustrate how dynamic adaptations of enzyme expression can be predicted solely from an optimization principle. Copyright © 2014 Elsevier Ltd. All rights reserved.

Acicular photomultiplier photocathode structure

DOEpatents

Craig, Richard A.; Bliss, Mary

2003-09-30

A method and apparatus for increasing the quantum efficiency of a photomultiplier tube by providing a photocathode with an increased surface-to-volume ratio. The photocathode includes a transparent substrate, upon one major side of which is formed one or more large aspect-ratio structures, such as needles, cones, fibers, prisms, or pyramids. The large aspect-ratio structures are at least partially composed of a photoelectron emitting material, i.e., a material that emits a photoelectron upon absorption of an optical photon. The large aspect-ratio structures may be substantially composed of the photoelectron emitting material (i.e., formed as such upon the surface of a relatively flat substrate) or be only partially composed of a photoelectron emitting material (i.e., the photoelectron emitting material is coated over large aspect-ratio structures formed from the substrate material itself.) The large aspect-ratio nature of the photocathode surface allows for an effective increase in the thickness of the photocathode relative the absorption of optical photons, thereby increasing the absorption rate of incident photons, without substantially increasing the effective thickness of the photocathode relative the escape incidence of the photoelectrons.

Modelling Photoelectron Production in the Enceladus Plume and Comparison with Observations by CAPS-ELS

NASA Astrophysics Data System (ADS)

Taylor, S. A.; Coates, A. J.; Jones, G.; Wellbrock, A.; Waite, J. H., Jr.

2016-12-01

The Electron Spectrometer (ELS) of the Cassini Plasma Spectrometer (CAPS) measures electrons in the energy range 0.6-28,000 eV with an energy resolution of 16.7%. ELS has observed photoelectrons produced in the plume of Enceladus. These photoelectrons are found during Enceladus encounters in the energetic particle shadow where the spacecraft is shielded from penetrating radiation by the moon [Coates et al, 2013]. Observable is a population of photoelectrons at 20-30eV, which are seen at other bodies in the solar system and are usually associated with ionisation by the strong solar He II (30.4 nm) line. We have identified secondary peaks at 40-50eV detected by ELS which are also interpreted as a warmer population of photoelectrons created through the ionisation of neutrals in the Enceladus torus. We have constructed a model of photoelectron production in the plume and compared it with ELS Enceladus flyby data using automated fitting procedures. This has yielded estimates for electron temperature and density as well as a spacecraft potential estimate which is corrected for.

Dynamical photo-induced electronic properties of molecular junctions

NASA Astrophysics Data System (ADS)

Beltako, K.; Michelini, F.; Cavassilas, N.; Raymond, L.

2018-03-01

Nanoscale molecular-electronic devices and machines are emerging as promising functional elements, naturally flexible and efficient, for next-generation technologies. A deeper understanding of carrier dynamics in molecular junctions is expected to benefit many fields of nanoelectronics and power devices. We determine time-resolved charge current flowing at the donor-acceptor interface in molecular junctions connected to metallic electrodes by means of quantum transport simulations. The current is induced by the interaction of the donor with a Gaussian-shape femtosecond laser pulse. Effects of the molecular internal coupling, metal-molecule tunneling, and light-donor coupling on photocurrent are discussed. We then define the time-resolved local density of states which is proposed as an efficient tool to describe the absorbing molecule in contact with metallic electrodes. Non-equilibrium reorganization of hybridized molecular orbitals through the light-donor interaction gives rise to two phenomena: the dynamical Rabi shift and the appearance of Floquet-like states. Such insights into the dynamical photoelectronic structure of molecules are of strong interest for ultrafast spectroscopy and open avenues toward the possibility of analyzing and controlling the internal properties of quantum nanodevices with pump-push photocurrent spectroscopy.

Characterization of gigahertz (GHz) bandwidth photomultipliers

NASA Technical Reports Server (NTRS)

Abshire, J. B.; Rowe, H. E.

1977-01-01

The average impulse response, root-mean-square times jitter as a function of signal level, single photoelectron distribution, and multiphotoelectron dark-count distribution have been measured for two static crossed-field and five electrostatic photomultipliers. The optical signal source for the first three of these tests was a 30 picosecond mode-locked laser pulse at 0.53 micron. The static crossed-field detectors had 2-photoelectron resolution, less than 200 ps rise times, and rms time jitters of 30 ps at the single photoelectron level. The electrostatic photomultipliers had rise times from 1 to 2.5 nanoseconds, and rms time jitters from 160 to 650 ps at the same signal level. The two static crossed-field photomultipliers had ion-feedback-generated dark pulses to the 50-photoelectron level, whereas one electrostatic photomultiplier had dark pulses to the 30-photoelectron level.

Optimal blood glucose level control using dynamic programming based on minimal Bergman model

NASA Astrophysics Data System (ADS)

Rettian Anggita Sari, Maria; Hartono

2018-03-01

The purpose of this article is to simulate the glucose dynamic and the insulin kinetic of diabetic patient. The model used in this research is a non-linear Minimal Bergman model. Optimal control theory is then applied to formulate the problem in order to determine the optimal dose of insulin in the treatment of diabetes mellitus such that the glucose level is in the normal range for some specific time range. The optimization problem is solved using dynamic programming. The result shows that dynamic programming is quite reliable to represent the interaction between glucose and insulin levels in diabetes mellitus patient.

Analysis of femtosecond pump-probe photoelectron-photoion coincidence measurements applying Bayesian probability theory

NASA Astrophysics Data System (ADS)

Rumetshofer, M.; Heim, P.; Thaler, B.; Ernst, W. E.; Koch, M.; von der Linden, W.

2018-06-01

Ultrafast dynamical processes in photoexcited molecules can be observed with pump-probe measurements, in which information about the dynamics is obtained from the transient signal associated with the excited state. Background signals provoked by pump and/or probe pulses alone often obscure these excited-state signals. Simple subtraction of pump-only and/or probe-only measurements from the pump-probe measurement, as commonly applied, results in a degradation of the signal-to-noise ratio and, in the case of coincidence detection, the danger of overrated background subtraction. Coincidence measurements additionally suffer from false coincidences, requiring long data-acquisition times to keep erroneous signals at an acceptable level. Here we present a probabilistic approach based on Bayesian probability theory that overcomes these problems. For a pump-probe experiment with photoelectron-photoion coincidence detection, we reconstruct the interesting excited-state spectrum from pump-probe and pump-only measurements. This approach allows us to treat background and false coincidences consistently and on the same footing. We demonstrate that the Bayesian formalism has the following advantages over simple signal subtraction: (i) the signal-to-noise ratio is significantly increased, (ii) the pump-only contribution is not overestimated, (iii) false coincidences are excluded, (iv) prior knowledge, such as positivity, is consistently incorporated, (v) confidence intervals are provided for the reconstructed spectrum, and (vi) it is applicable to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, the Bayesian approach allows us to run experiments at higher ionization rates, resulting in a significant reduction of data acquisition times. The probabilistic approach is thoroughly scrutinized by challenging mock data. The application to pump-probe coincidence measurements on acetone molecules enables quantitative interpretations about the molecular decay dynamics and fragmentation behavior. All results underline the superiority of a consistent probabilistic approach over ad hoc estimations.

Correlation between excited d-orbital electron lifetime in polaron dynamics and coloration of WO3 upon ultraviolet exposure

NASA Astrophysics Data System (ADS)

Lee, Young-Ahn; Han, Seung-Ik; Rhee, Hanju; Seo, Hyungtak

2018-05-01

Polarons have been suggested to explain the mechanism of the coloration of WO3 induced by UV light. However, despite the many experimental results that support small polarons as a key mechanism, direct observation of the carrier dynamics of polarons have yet to be reported. Here, we investigate the correlation between the electronic structure and the coloration of WO3 upon exposure to UV light in 5% H2/N2 gas and, more importantly, reveal photon-induced excited d-electron generation/relaxation via the W5+ oxidation state. The WO3 is fabricated by radio-frequency magnetron sputtering. X-ray diffraction patterns show that prepared WO3 is amorphous. Optical bandgap of 3.1 eV is measured by UV-vis before and after UV light. The results of Fourier transform infrared and Raman exhibit pristine WO3 is formed with surface H2O. The colored WO3 shows reduced state of W5+ state (34.3 eV) by using X-ray photoelectron spectroscopy. The valence band maximum of WO3 after UV light in H2 is shifted from mid gap to shallow donor by using ultraviolet photoelectron spectroscopy. During the exploration of the carrier dynamics, pump (700 nm)-probe (1000 nm) spectroscopy at the femtosecond scale was used. The results indicated that electron-phonon relaxation of UV-irradiated WO3, which is the origin of the polaron-induced local surface plasmonic effect, is dominant, resulting in slow decay (within a few picoseconds); in contrast, pristine WO3 shows fast decay (less than a picosecond). Accordingly, the long photoinduced carrier relaxation is ascribed to the prolonged hot-carrier lifetime in reduced oxides resulting in a greater number of free d-electrons and, therefore, more interactions with the W5+ sub-gap states.

Optimization of process factors for self-healing vanadium-based conversion coating on AZ31 magnesium alloy

NASA Astrophysics Data System (ADS)

Li, Kun; Liu, Junyao; Lei, Ting; Xiao, Tao

2015-10-01

A self-healing vanadium-based conversion coating was prepared on AZ31 magnesium alloy. The optimum operating conditions including vanadia solution concentration, pH and treating temperature for obtaining the best corrosion protective vanadia coatings and improved localized corrosion resistance to the magnesium substrate were determined by an orthogonal experiment design. Surface morphology and composition of the resultant conversion coatings were investigated by scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). The self-healing behavior of the coating was investigated by cross-cut immersion test and electrochemical impedance spectroscopy (EIS) measurements in 3.5% NaCl solution.

Time-resolved photoelectron spectroscopy of a dinuclear Pt(II) complex: Tunneling autodetachment from both singlet and triplet excited states of a molecular dianion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Winghart, Marc-Oliver, E-mail: marc-oliver.winghart@kit.edu; Unterreiner, Andreas-Neil; Yang, Ji-Ping

2016-02-07

Time-resolved pump-probe photoelectron spectroscopy has been used to study the relaxation dynamics of gaseous [Pt{sub 2}(μ-P{sub 2}O{sub 5}H{sub 2}){sub 4} + 2H]{sup 2−} after population of its first singlet excited state by 388 nm femtosecond laser irradiation. In contrast to the fluorescence and phosphorescence observed in condensed phase, a significant fraction of the photoexcited isolated dianions decays by electron loss to form the corresponding monoanions. Our transient photoelectron data reveal an ultrafast decay of the initially excited singlet {sup 1}A{sub 2u} state and concomitant rise in population of the triplet {sup 3}A{sub 2u} state, via sub-picosecond intersystem crossing (ISC). Wemore » find that both of the electronically excited states are metastably bound behind a repulsive Coulomb barrier and can decay via delayed autodetachment to yield electrons with characteristic kinetic energies. While excited state tunneling detachment (ESETD) from the singlet {sup 1}A{sub 2u} state takes only a few picoseconds, ESETD from the triplet {sup 3}A{sub 2u} state is much slower and proceeds on a time scale of hundreds of nanoseconds. The ISC rate in the gas phase is significantly higher than in solution, which can be rationalized in terms of changes to the energy dissipation mechanism in the absence of solvent molecules. [Pt{sub 2}(μ-P{sub 2}O{sub 5}H{sub 2}){sub 4} + 2H]{sup 2−} is the first example of a photoexcited multianion for which ESETD has been observed following ISC.« less

SUPRATHERMAL ELECTRONS IN TITAN’S SUNLIT IONOSPHERE: MODEL–OBSERVATION COMPARISONS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vigren, E.; Edberg, N. J. T.; Wahlund, J.-E.

2016-08-01

The dayside ionosphere of the Saturnian satellite Titan is generated mainly from photoionization of N{sub 2} and CH{sub 4}. We compare model-derived suprathermal electron intensities with spectra measured by the Cassini Plasma Spectrometer/Electron Spectrometer (CAPS/ELS) in Titan's sunlit ionosphere (altitudes of 970–1250 km) focusing on the T40, T41, T42, and T48 Titan flybys by the Cassini spacecraft. The model accounts only for photoelectrons and associated secondary electrons, with a main input being the impinging solar EUV spectra as measured by the Thermosphere Ionosphere Mesosphere Energy and Dynamics/Solar EUV Experiment and extrapolated to Saturn. Associated electron-impact electron production rates have beenmore » derived from ambient number densities of N{sub 2} and CH{sub 4} (measured by the Ion Neutral Mass Spectrometer/Closed Source Neutral mode) and related energy-dependent electron-impact ionization cross sections. When integrating up to electron energies of 60 eV, covering the bulk of the photoelectrons, the model-based values exceed the observationally based values typically by factors of ∼3 ± 1. This finding is possibly related to current difficulties in accurately reproducing the observed electron number densities in Titan's dayside ionosphere. We compare the utilized dayside CAPS/ELS spectra with ones measured in Titan's nightside ionosphere during the T55–T59 flybys. The investigated nightside locations were associated with higher fluxes of high-energy (>100 eV) electrons than the dayside locations. As expected, for similar neutral number densities, electrons with energies <60 eV give a higher relative contribution to the total electron-impact ionization rates on the dayside (due to the contribution from photoelectrons) than on the nightside.« less

Dynamic regime marginal structural mean models for estimation of optimal dynamic treatment regimes, Part II: proofs of results.

PubMed

Orellana, Liliana; Rotnitzky, Andrea; Robins, James M

2010-03-03

In this companion article to "Dynamic Regime Marginal Structural Mean Models for Estimation of Optimal Dynamic Treatment Regimes, Part I: Main Content" [Orellana, Rotnitzky and Robins (2010), IJB, Vol. 6, Iss. 2, Art. 7] we present (i) proofs of the claims in that paper, (ii) a proposal for the computation of a confidence set for the optimal index when this lies in a finite set, and (iii) an example to aid the interpretation of the positivity assumption.

A framework for modeling and optimizing dynamic systems under uncertainty

DOE PAGES

Nicholson, Bethany; Siirola, John

2017-11-11

Algebraic modeling languages (AMLs) have drastically simplified the implementation of algebraic optimization problems. However, there are still many classes of optimization problems that are not easily represented in most AMLs. These classes of problems are typically reformulated before implementation, which requires significant effort and time from the modeler and obscures the original problem structure or context. In this work we demonstrate how the Pyomo AML can be used to represent complex optimization problems using high-level modeling constructs. We focus on the operation of dynamic systems under uncertainty and demonstrate the combination of Pyomo extensions for dynamic optimization and stochastic programming.more » We use a dynamic semibatch reactor model and a large-scale bubbling fluidized bed adsorber model as test cases.« less

A framework for modeling and optimizing dynamic systems under uncertainty

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nicholson, Bethany; Siirola, John

Algebraic modeling languages (AMLs) have drastically simplified the implementation of algebraic optimization problems. However, there are still many classes of optimization problems that are not easily represented in most AMLs. These classes of problems are typically reformulated before implementation, which requires significant effort and time from the modeler and obscures the original problem structure or context. In this work we demonstrate how the Pyomo AML can be used to represent complex optimization problems using high-level modeling constructs. We focus on the operation of dynamic systems under uncertainty and demonstrate the combination of Pyomo extensions for dynamic optimization and stochastic programming.more » We use a dynamic semibatch reactor model and a large-scale bubbling fluidized bed adsorber model as test cases.« less

Dynamic optimization case studies in DYNOPT tool

NASA Astrophysics Data System (ADS)

Ozana, Stepan; Pies, Martin; Docekal, Tomas

2016-06-01

Dynamic programming is typically applied to optimization problems. As the analytical solutions are generally very difficult, chosen software tools are used widely. These software packages are often third-party products bound for standard simulation software tools on the market. As typical examples of such tools, TOMLAB and DYNOPT could be effectively applied for solution of problems of dynamic programming. DYNOPT will be presented in this paper due to its licensing policy (free product under GPL) and simplicity of use. DYNOPT is a set of MATLAB functions for determination of optimal control trajectory by given description of the process, the cost to be minimized, subject to equality and inequality constraints, using orthogonal collocation on finite elements method. The actual optimal control problem is solved by complete parameterization both the control and the state profile vector. It is assumed, that the optimized dynamic model may be described by a set of ordinary differential equations (ODEs) or differential-algebraic equations (DAEs). This collection of functions extends the capability of the MATLAB Optimization Tool-box. The paper will introduce use of DYNOPT in the field of dynamic optimization problems by means of case studies regarding chosen laboratory physical educational models.

Soft X-ray spectroscopy of nanoparticles by velocity map imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kostko, O.; Xu, B.; Jacobs, M. I.

Velocity map imaging (VMI), a technique traditionally used to study chemical dynamics in the gas phase, is applied to study X-ray photoemission from aerosol nanoparticles. Soft X-rays from the Advanced Light Source synchrotron, probe a beam of nanoparticles, and the resulting photoelectrons are velocity mapped to obtain their kinetic energy distributions. A new design of the VMI spectrometer is described. The spectrometer is benchmarked by measuring vacuum ultraviolet photoemission from gas phase xenon and squalene nanoparticles followed by measurements using soft X-rays. It is demonstrated that the photoelectron distribution from X-ray irradiated squalene nanoparticles is dominated by secondary electrons. Bymore » scanning the photon energies and measuring the intensities of these secondary electrons, a near edge X-ray absorption fine structure (NEXAFS) spectrum is obtained. The NEXAFS technique is used to obtain spectra of aqueous nanoparticles at the oxygen K edge. By varying the position of the aqueous nanoparticle beam relative to the incident X-ray beam, evidence is presented such that the VMI technique allows for NEXAFS spectroscopy of water in different physical states. Finally, we discuss the possibility of applying VMI methods to probe liquids and solids via X-ray spectroscopy.« less

Soft X-ray spectroscopy of nanoparticles by velocity map imaging

DOE PAGES

Kostko, O.; Xu, B.; Jacobs, M. I.; ...

2017-05-05

Velocity map imaging (VMI), a technique traditionally used to study chemical dynamics in the gas phase, is applied to study X-ray photoemission from aerosol nanoparticles. Soft X-rays from the Advanced Light Source synchrotron, probe a beam of nanoparticles, and the resulting photoelectrons are velocity mapped to obtain their kinetic energy distributions. A new design of the VMI spectrometer is described. The spectrometer is benchmarked by measuring vacuum ultraviolet photoemission from gas phase xenon and squalene nanoparticles followed by measurements using soft X-rays. It is demonstrated that the photoelectron distribution from X-ray irradiated squalene nanoparticles is dominated by secondary electrons. Bymore » scanning the photon energies and measuring the intensities of these secondary electrons, a near edge X-ray absorption fine structure (NEXAFS) spectrum is obtained. The NEXAFS technique is used to obtain spectra of aqueous nanoparticles at the oxygen K edge. By varying the position of the aqueous nanoparticle beam relative to the incident X-ray beam, evidence is presented such that the VMI technique allows for NEXAFS spectroscopy of water in different physical states. Finally, we discuss the possibility of applying VMI methods to probe liquids and solids via X-ray spectroscopy.« less

Integrated aerodynamic/dynamic/structural optimization of helicopter rotor blades using multilevel decomposition

NASA Technical Reports Server (NTRS)

Walsh, Joanne L.; Young, Katherine C.; Pritchard, Jocelyn I.; Adelman, Howard M.; Mantay, Wayne R.

1995-01-01

This paper describes an integrated aerodynamic/dynamic/structural (IADS) optimization procedure for helicopter rotor blades. The procedure combines performance, dynamics, and structural analyses with a general-purpose optimizer using multilevel decomposition techniques. At the upper level, the structure is defined in terms of global quantities (stiffness, mass, and average strains). At the lower level, the structure is defined in terms of local quantities (detailed dimensions of the blade structure and stresses). The IADS procedure provides an optimization technique that is compatible with industrial design practices in which the aerodynamic and dynamic designs are performed at a global level and the structural design is carried out at a detailed level with considerable dialog and compromise among the aerodynamic, dynamic, and structural groups. The IADS procedure is demonstrated for several examples.

Multilevel decomposition approach to integrated aerodynamic/dynamic/structural optimization of helicopter rotor blades

NASA Technical Reports Server (NTRS)

Walsh, Joanne L.; Young, Katherine C.; Pritchard, Jocelyn I.; Adelman, Howard M.; Mantay, Wayne R.

1994-01-01

This paper describes an integrated aerodynamic, dynamic, and structural (IADS) optimization procedure for helicopter rotor blades. The procedure combines performance, dynamics, and structural analyses with a general purpose optimizer using multilevel decomposition techniques. At the upper level, the structure is defined in terms of local quantities (stiffnesses, mass, and average strains). At the lower level, the structure is defined in terms of local quantities (detailed dimensions of the blade structure and stresses). The IADS procedure provides an optimization technique that is compatible with industrial design practices in which the aerodynamic and dynamic design is performed at a global level and the structural design is carried out at a detailed level with considerable dialogue and compromise among the aerodynamic, dynamic, and structural groups. The IADS procedure is demonstrated for several cases.

Evolutionary Dynamic Multiobjective Optimization Via Kalman Filter Prediction.

PubMed

Muruganantham, Arrchana; Tan, Kay Chen; Vadakkepat, Prahlad

2016-12-01

Evolutionary algorithms are effective in solving static multiobjective optimization problems resulting in the emergence of a number of state-of-the-art multiobjective evolutionary algorithms (MOEAs). Nevertheless, the interest in applying them to solve dynamic multiobjective optimization problems has only been tepid. Benchmark problems, appropriate performance metrics, as well as efficient algorithms are required to further the research in this field. One or more objectives may change with time in dynamic optimization problems. The optimization algorithm must be able to track the moving optima efficiently. A prediction model can learn the patterns from past experience and predict future changes. In this paper, a new dynamic MOEA using Kalman filter (KF) predictions in decision space is proposed to solve the aforementioned problems. The predictions help to guide the search toward the changed optima, thereby accelerating convergence. A scoring scheme is devised to hybridize the KF prediction with a random reinitialization method. Experimental results and performance comparisons with other state-of-the-art algorithms demonstrate that the proposed algorithm is capable of significantly improving the dynamic optimization performance.

A Sensor Dynamic Measurement Error Prediction Model Based on NAPSO-SVM.

PubMed

Jiang, Minlan; Jiang, Lan; Jiang, Dingde; Li, Fei; Song, Houbing

2018-01-15

Dynamic measurement error correction is an effective way to improve sensor precision. Dynamic measurement error prediction is an important part of error correction, and support vector machine (SVM) is often used for predicting the dynamic measurement errors of sensors. Traditionally, the SVM parameters were always set manually, which cannot ensure the model's performance. In this paper, a SVM method based on an improved particle swarm optimization (NAPSO) is proposed to predict the dynamic measurement errors of sensors. Natural selection and simulated annealing are added in the PSO to raise the ability to avoid local optima. To verify the performance of NAPSO-SVM, three types of algorithms are selected to optimize the SVM's parameters: the particle swarm optimization algorithm (PSO), the improved PSO optimization algorithm (NAPSO), and the glowworm swarm optimization (GSO). The dynamic measurement error data of two sensors are applied as the test data. The root mean squared error and mean absolute percentage error are employed to evaluate the prediction models' performances. The experimental results show that among the three tested algorithms the NAPSO-SVM method has a better prediction precision and a less prediction errors, and it is an effective method for predicting the dynamic measurement errors of sensors.

Slow Photoelectron Velocity-Map Imaging of Cryogenically Cooled Anions

NASA Astrophysics Data System (ADS)

Weichman, Marissa L.; Neumark, Daniel M.

2018-04-01

Slow photoelectron velocity-map imaging spectroscopy of cryogenically cooled anions (cryo-SEVI) is a powerful technique for elucidating the vibrational and electronic structure of neutral radicals, clusters, and reaction transition states. SEVI is a high-resolution variant of anion photoelectron spectroscopy based on photoelectron imaging that yields spectra with energy resolution as high as 1-2 cm‑1. The preparation of cryogenically cold anions largely eliminates hot bands and dramatically narrows the rotational envelopes of spectral features, enabling the acquisition of well-resolved photoelectron spectra for complex and spectroscopically challenging species. We review the basis and history of the SEVI method, including recent experimental developments that have improved its resolution and versatility. We then survey recent SEVI studies to demonstrate the utility of this technique in the spectroscopy of aromatic radicals, metal and metal oxide clusters, nonadiabatic interactions between excited states of small molecules, and transition states of benchmark bimolecular reactions.

Achieving Zero Current for Polar Wind Outflow on Open Flux Tubes Subjected to Large Photoelectron Fluxes

NASA Technical Reports Server (NTRS)

Wilson, G. R.; Khazanov, G.; Horwitz, J. L.

1997-01-01

In this study we investigate how the condition of zero current on open flux tubes with polar wind outflow, subjected to large photoelectron fluxes, can be achieved. We employ a steady state collisionless semikinetic model to determine the density profiles of O(+), H(+), thermal electrons and photoelectrons coming from the ionosphere along with H(+), ions and electrons coming from the magnetosphere. The model solution attains a potential distribution which both satisfies the condition of charge neutrality and zero current. For the range of parameters considered in this study we find that a 45-60 volt discontinuous potential drop may develop to reflect most of the photoelectrons back toward the ionosphere. This develops because the downward flux of electrons from the magnetosphere to the ionosphere on typical open flux tubes (e.g. the polar rain) appears to be insufficient to balance the photoelectron flux from the ionosphere.

Modeling, Analysis, and Interpretation of Photoelectron Energy Spectra at Enceladus Observed by Cassini

NASA Astrophysics Data System (ADS)

Taylor, S. A.; Coates, A. J.; Jones, G. H.; Wellbrock, A.; Fazakerley, A. N.; Desai, R. T.; Caro-Carretero, R.; Michiko, M. W.; Schippers, P.; Waite, J. H.

2018-01-01

The Electron Spectrometer (ELS) of the Cassini Plasma Spectrometer has observed photoelectrons produced in the plume of Enceladus. These photoelectrons are observed during Enceladus encounters in the energetic particle shadow where the spacecraft is largely shielded from penetrating radiation by the moon. We present a complex electron spectrum at Enceladus including evidence of two previously unidentified electron populations at 6-10 eV and 10-16 eV. We estimate that the proportion of "hot" (>15 eV) to "cold" (<15 eV) electrons during the Enceladus flybys is ≈ 0.1-0.5%. We have constructed a model of photoelectron production in the plume and compared it with ELS Enceladus flyby data by scaling and energy shifting according to spacecraft potential. We suggest that the complex structure of the electron spectrum observed can be explained entirely by photoelectron production in the plume ionosphere.

A dynamic multi-level optimal design method with embedded finite-element modeling for power transformers

NASA Astrophysics Data System (ADS)

Zhang, Yunpeng; Ho, Siu-lau; Fu, Weinong

2018-05-01

This paper proposes a dynamic multi-level optimal design method for power transformer design optimization (TDO) problems. A response surface generated by second-order polynomial regression analysis is updated dynamically by adding more design points, which are selected by Shifted Hammersley Method (SHM) and calculated by finite-element method (FEM). The updating stops when the accuracy requirement is satisfied, and optimized solutions of the preliminary design are derived simultaneously. The optimal design level is modulated through changing the level of error tolerance. Based on the response surface of the preliminary design, a refined optimal design is added using multi-objective genetic algorithm (MOGA). The effectiveness of the proposed optimal design method is validated through a classic three-phase power TDO problem.

Measurement and modeling of the refilling plasmasphere during 2001

DOE PAGES

Krall, J.; Huba, J. D.; Jordanova, V. K.; ...

2016-03-18

The Naval Research Laboratory SAMI3 (Sami3 is Also a Model of the Ionosphere) and the RAM-CPL (Ring current Atmosphere interaction Model-Cold PLasma) codes are used to model observed plasmasphere dynamics during 25 November 2001 to 1 December 2001 and 1–5 February 2001. Model results compare well to plasmasphere observations of electron and mass densities. Comparison of model results to refilling data and to each other shows good agreement, generally within a factor of 2. We find that SAMI3 plasmaspheric refilling rates and ion densities are sensitive to the composition and temperature of the thermosphere and exosphere, and to photoelectron heating.more » Furthermore, results also support our previous finding that the wind-driven dynamo significantly impacts both refilling rates and plasmasphere dynamics during quiet periods.« less

Measurement and modeling of the refilling plasmasphere during 2001

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krall, J.; Huba, J. D.; Jordanova, V. K.

The Naval Research Laboratory SAMI3 (Sami3 is Also a Model of the Ionosphere) and the RAM-CPL (Ring current Atmosphere interaction Model-Cold PLasma) codes are used to model observed plasmasphere dynamics during 25 November 2001 to 1 December 2001 and 1–5 February 2001. Model results compare well to plasmasphere observations of electron and mass densities. Comparison of model results to refilling data and to each other shows good agreement, generally within a factor of 2. We find that SAMI3 plasmaspheric refilling rates and ion densities are sensitive to the composition and temperature of the thermosphere and exosphere, and to photoelectron heating.more » Furthermore, results also support our previous finding that the wind-driven dynamo significantly impacts both refilling rates and plasmasphere dynamics during quiet periods.« less

An Improved Co-evolutionary Particle Swarm Optimization for Wireless Sensor Networks with Dynamic Deployment

PubMed Central

Wang, Xue; Wang, Sheng; Ma, Jun-Jie

2007-01-01

The effectiveness of wireless sensor networks (WSNs) depends on the coverage and target detection probability provided by dynamic deployment, which is usually supported by the virtual force (VF) algorithm. However, in the VF algorithm, the virtual force exerted by stationary sensor nodes will hinder the movement of mobile sensor nodes. Particle swarm optimization (PSO) is introduced as another dynamic deployment algorithm, but in this case the computation time required is the big bottleneck. This paper proposes a dynamic deployment algorithm which is named “virtual force directed co-evolutionary particle swarm optimization” (VFCPSO), since this algorithm combines the co-evolutionary particle swarm optimization (CPSO) with the VF algorithm, whereby the CPSO uses multiple swarms to optimize different components of the solution vectors for dynamic deployment cooperatively and the velocity of each particle is updated according to not only the historical local and global optimal solutions, but also the virtual forces of sensor nodes. Simulation results demonstrate that the proposed VFCPSO is competent for dynamic deployment in WSNs and has better performance with respect to computation time and effectiveness than the VF, PSO and VFPSO algorithms.

Preserving electron spin coherence in solids by optimal dynamical decoupling.

PubMed

Du, Jiangfeng; Rong, Xing; Zhao, Nan; Wang, Ya; Yang, Jiahui; Liu, R B

2009-10-29

To exploit the quantum coherence of electron spins in solids in future technologies such as quantum computing, it is first vital to overcome the problem of spin decoherence due to their coupling to the noisy environment. Dynamical decoupling, which uses stroboscopic spin flips to give an average coupling to the environment that is effectively zero, is a particularly promising strategy for combating decoherence because it can be naturally integrated with other desired functionalities, such as quantum gates. Errors are inevitably introduced in each spin flip, so it is desirable to minimize the number of control pulses used to realize dynamical decoupling having a given level of precision. Such optimal dynamical decoupling sequences have recently been explored. The experimental realization of optimal dynamical decoupling in solid-state systems, however, remains elusive. Here we use pulsed electron paramagnetic resonance to demonstrate experimentally optimal dynamical decoupling for preserving electron spin coherence in irradiated malonic acid crystals at temperatures from 50 K to room temperature. Using a seven-pulse optimal dynamical decoupling sequence, we prolonged the spin coherence time to about 30 mus; it would otherwise be about 0.04 mus without control or 6.2 mus under one-pulse control. By comparing experiments with microscopic theories, we have identified the relevant electron spin decoherence mechanisms in the solid. Optimal dynamical decoupling may be applied to other solid-state systems, such as diamonds with nitrogen-vacancy centres, and so lay the foundation for quantum coherence control of spins in solids at room temperature.

Minimal complexity control law synthesis

NASA Technical Reports Server (NTRS)

Bernstein, Dennis S.; Haddad, Wassim M.; Nett, Carl N.

1989-01-01

A paradigm for control law design for modern engineering systems is proposed: Minimize control law complexity subject to the achievement of a specified accuracy in the face of a specified level of uncertainty. Correspondingly, the overall goal is to make progress towards the development of a control law design methodology which supports this paradigm. Researchers achieve this goal by developing a general theory of optimal constrained-structure dynamic output feedback compensation, where here constrained-structure means that the dynamic-structure (e.g., dynamic order, pole locations, zero locations, etc.) of the output feedback compensation is constrained in some way. By applying this theory in an innovative fashion, where here the indicated iteration occurs over the choice of the compensator dynamic-structure, the paradigm stated above can, in principle, be realized. The optimal constrained-structure dynamic output feedback problem is formulated in general terms. An elegant method for reducing optimal constrained-structure dynamic output feedback problems to optimal static output feedback problems is then developed. This reduction procedure makes use of star products, linear fractional transformations, and linear fractional decompositions, and yields as a byproduct a complete characterization of the class of optimal constrained-structure dynamic output feedback problems which can be reduced to optimal static output feedback problems. Issues such as operational/physical constraints, operating-point variations, and processor throughput/memory limitations are considered, and it is shown how anti-windup/bumpless transfer, gain-scheduling, and digital processor implementation can be facilitated by constraining the controller dynamic-structure in an appropriate fashion.

Integrated aerodynamic/dynamic optimization of helicopter rotor blades

NASA Technical Reports Server (NTRS)

Chattopadhyay, Aditi; Walsh, Joanne L.; Riley, Michael F.

1989-01-01

An integrated aerodynamic/dynamic optimization procedure is used to minimize blade weight and 4 per rev vertical hub shear for a rotor blade in forward flight. The coupling of aerodynamics and dynamics is accomplished through the inclusion of airloads which vary with the design variables during the optimization process. Both single and multiple objective functions are used in the optimization formulation. The Global Criteria Approach is used to formulate the multiple objective optimization and results are compared with those obtained by using single objective function formulations. Constraints are imposed on natural frequencies, autorotational inertia, and centrifugal stress. The program CAMRAD is used for the blade aerodynamic and dynamic analyses, and the program CONMIN is used for the optimization. Since the spanwise and the azimuthal variations of loading are responsible for most rotor vibration and noise, the vertical airload distributions on the blade, before and after optimization, are compared. The total power required by the rotor to produce the same amount of thrust for a given area is also calculated before and after optimization. Results indicate that integrated optimization can significantly reduce the blade weight, the hub shear and the amplitude of the vertical airload distributions on the blade and the total power required by the rotor.

Quantitative analysis of trace levels of surface contamination by X-ray photoelectron spectroscopy Part I: statistical uncertainty near the detection limit.

PubMed

Hill, Shannon B; Faradzhev, Nadir S; Powell, Cedric J

2017-12-01

We discuss the problem of quantifying common sources of statistical uncertainties for analyses of trace levels of surface contamination using X-ray photoelectron spectroscopy. We examine the propagation of error for peak-area measurements using common forms of linear and polynomial background subtraction including the correlation of points used to determine both background and peak areas. This correlation has been neglected in previous analyses, but we show that it contributes significantly to the peak-area uncertainty near the detection limit. We introduce the concept of relative background subtraction variance (RBSV) which quantifies the uncertainty introduced by the method of background determination relative to the uncertainty of the background area itself. The uncertainties of the peak area and atomic concentration and of the detection limit are expressed using the RBSV, which separates the contributions from the acquisition parameters, the background-determination method, and the properties of the measured spectrum. These results are then combined to find acquisition strategies that minimize the total measurement time needed to achieve a desired detection limit or atomic-percentage uncertainty for a particular trace element. Minimization of data-acquisition time is important for samples that are sensitive to x-ray dose and also for laboratories that need to optimize throughput.

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources.

PubMed

Pincelli, T; Petrov, V N; Brajnik, G; Ciprian, R; Lollobrigida, V; Torelli, P; Krizmancic, D; Salvador, F; De Luisa, A; Sergo, R; Gubertini, A; Cautero, G; Carrato, S; Rossi, G; Panaccione, G

2016-03-01

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric and magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources

NASA Astrophysics Data System (ADS)

Pincelli, T.; Petrov, V. N.; Brajnik, G.; Ciprian, R.; Lollobrigida, V.; Torelli, P.; Krizmancic, D.; Salvador, F.; De Luisa, A.; Sergo, R.; Gubertini, A.; Cautero, G.; Carrato, S.; Rossi, G.; Panaccione, G.

2016-03-01

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric and magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pincelli, T., E-mail: pincelli@iom.cnr.it; Rossi, G.; Laboratorio TASC, IOM-CNR, S.S. 14 km 163.5, Basovizza, 34149 Trieste

2016-03-15

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric andmore » magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).« less

Probing the structural evolution of ruthenium doped germanium clusters: Photoelectron spectroscopy and density functional theory calculations

PubMed Central

Jin, Yuanyuan; Lu, Shengjie; Hermann, Andreas; Kuang, Xiaoyu; Zhang, Chuanzhao; Lu, Cheng; Xu, Hongguang; Zheng, Weijun

2016-01-01

We present a combined experimental and theoretical study of ruthenium doped germanium clusters, RuGen− (n = 3–12), and their corresponding neutral species. Photoelectron spectra of RuGen− clusters are measured at 266 nm. The vertical detachment energies (VDEs) and adiabatic detachment energies (ADEs) are obtained. Unbiased CALYPSO structure searches confirm the low-lying structures of anionic and neutral ruthenium doped germanium clusters in the size range of 3 ≤ n ≤ 12. Subsequent geometry optimizations using density functional theory (DFT) at PW91/LANL2DZ level are carried out to determine the relative stability and electronic properties of ruthenium doped germanium clusters. It is found that most of the anionic and neutral clusters have very similar global features. Although the global minimum structures of the anionic and neutral clusters are different, their respective geometries are observed as the low-lying isomers in either case. In addition, for n > 8, the Ru atom in RuGen−/0 clusters is absorbed endohedrally in the Ge cage. The theoretically predicted vertical and adiabatic detachment energies are in good agreement with the experimental measurements. The excellent agreement between DFT calculations and experiment enables a comprehensive evaluation of the geometrical and electronic structures of ruthenium doped germanium clusters. PMID:27439955

Tunable band alignment in two-phase-coexistence Nb3O7F nanocrystals with enhanced light harvesting and photocatalytic performance

NASA Astrophysics Data System (ADS)

Li, Zhen; Huang, Fei; Feng, Xin; Yan, Aihua; Dong, Haiming; Hu, Miao; Li, Qi

2018-06-01

A two-phase-coexistence technique offers intriguing variables to maneuver novel and enhanced functionality in a single-component material. Most importantly, new band alignment and perfect interfaces between two phases can strongly affect local photoelectronic properties. However, previous efforts to achieve two-phase coexistence were mainly restricted to specific systems and methods. Here we demonstrate a phase-transition route to acquire two-phase-coexistence niobium oxyfluoride (Nb3O7F) nanocrystals for the first time. Based on key distinguishing features of the experimental results and theoretical analysis, the phase transition of Nb3O7F involves an organic/inorganic hybrid, heat treating, Al-doping, lattice deformation and structural rearrangement. The band gap can be effectively tuned from 3.03 eV to 2.84 eV, and the VBM can be tuned from 1.49 eV to 1.69 eV according to the phase proportion. Benefiting from uniform nanocrystal size, tunable band alignment and an optimized interfacial structure, the two-phase coexistence markedly enhances visible-light harvesting and the photocatalytic performance of Nb3O7F nanocrystals. The results not only demonstrate an opportunity to explore two-phase coexistence of novel nanocrystals, but also illustrate the role of two-phase coexistence in achieving enhanced photoelectronic properties.

Tunable band alignment in two-phase-coexistence Nb3O7F nanocrystals with enhanced light harvesting and photocatalytic performance.

PubMed

Li, Zhen; Huang, Fei; Feng, Xin; Yan, Aihua; Dong, Haiming; Hu, Miao; Li, Qi

2018-06-01

A two-phase-coexistence technique offers intriguing variables to maneuver novel and enhanced functionality in a single-component material. Most importantly, new band alignment and perfect interfaces between two phases can strongly affect local photoelectronic properties. However, previous efforts to achieve two-phase coexistence were mainly restricted to specific systems and methods. Here we demonstrate a phase-transition route to acquire two-phase-coexistence niobium oxyfluoride (Nb 3 O 7 F) nanocrystals for the first time. Based on key distinguishing features of the experimental results and theoretical analysis, the phase transition of Nb 3 O 7 F involves an organic/inorganic hybrid, heat treating, Al-doping, lattice deformation and structural rearrangement. The band gap can be effectively tuned from 3.03 eV to 2.84 eV, and the VBM can be tuned from 1.49 eV to 1.69 eV according to the phase proportion. Benefiting from uniform nanocrystal size, tunable band alignment and an optimized interfacial structure, the two-phase coexistence markedly enhances visible-light harvesting and the photocatalytic performance of Nb 3 O 7 F nanocrystals. The results not only demonstrate an opportunity to explore two-phase coexistence of novel nanocrystals, but also illustrate the role of two-phase coexistence in achieving enhanced photoelectronic properties.

Propensity of bond exchange as a window into the mechanical properties of metallic glasses

NASA Astrophysics Data System (ADS)

Jiao, W.; Wang, X. L.; Lan, S.; Pan, S. P.; Lu, Z. P.

2015-02-01

We investigated the mechanical properties of Zr-Cu-Al bulk metallic glasses, by compression experiment and molecular dynamics simulations. From the simulation, we found that the large, solvent atom, Zr, has high propensity of bond exchange compared to those of the smaller solute atoms. The difference in bond exchange is consistent with the observed disparity in mechanical behaviors: Zr-rich metallic glass exhibits low elastic modulus and large plastic strain. X-ray photoelectron spectroscopy measurements suggest that the increased propensity in bond exchange is related to the softening of Zr bonds with increasing Zr content.

Application of the Lucy–Richardson Deconvolution Procedure to High Resolution Photoemission Spectra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rameau, J.; Yang, H.-B.; Johnson, P.D.

2010-07-01

Angle-resolved photoemission has developed into one of the leading probes of the electronic structure and associated dynamics of condensed matter systems. As with any experimental technique the ability to resolve features in the spectra is ultimately limited by the resolution of the instrumentation used in the measurement. Previously developed for sharpening astronomical images, the Lucy-Richardson deconvolution technique proves to be a useful tool for improving the photoemission spectra obtained in modern hemispherical electron spectrometers where the photoelectron spectrum is displayed as a 2D image in energy and momentum space.

Angular distribution of photoelectrons at 584A using polarized radiation

NASA Technical Reports Server (NTRS)

Hancock, W. H.; Samson, J. A. R.

1975-01-01

Photoelectron angular distributions for Ar, Xe, N2, O2, CO, CO2, and NH3 were obtained at 584 A by observing the photoelectrons at a fixed angle and simply rotating the plane of polarization of a highly polarized photon source. The radiation from a helium dc glow discharge source was polarized (84%) using a reflection type polarizer.

Control of wavepacket dynamics in mixed alkali metal clusters by optimally shaped fs pulses

NASA Astrophysics Data System (ADS)

Bartelt, A.; Minemoto, S.; Lupulescu, C.; Vajda, Š.; Wöste, L.

We have performed adaptive feedback optimization of phase-shaped femtosecond laser pulses to control the wavepacket dynamics of small mixed alkali-metal clusters. An optimization algorithm based on Evolutionary Strategies was used to maximize the ion intensities. The optimized pulses for NaK and Na2K converged to pulse trains consisting of numerous peaks. The timing of the elements of the pulse trains corresponds to integer and half integer numbers of the vibrational periods of the molecules, reflecting the wavepacket dynamics in their excited states.

Spacecraft charging and ion wake formation in the near-Sun environment

NASA Astrophysics Data System (ADS)

Ergun, R. E.; Malaspina, D. M.; Bale, S. D.; McFadden, J. P.; Larson, D. E.; Mozer, F. S.; Meyer-Vernet, N.; Maksimovic, M.; Kellogg, P. J.; Wygant, J. R.

2010-07-01

A three-dimensional, self-consistent code is employed to solve for the static potential structure surrounding a spacecraft in a high photoelectron environment. The numerical solutions show that, under certain conditions, a spacecraft can take on a negative potential in spite of strong photoelectron currents. The negative potential is due to an electrostatic barrier near the surface of the spacecraft that can reflect a large fraction of the photoelectron flux back to the spacecraft. This electrostatic barrier forms if (1) the photoelectron density at the surface of the spacecraft greatly exceeds the ambient plasma density, (2) the spacecraft size is significantly larger than local Debye length of the photoelectrons, and (3) the thermal electron energy is much larger than the characteristic energy of the escaping photoelectrons. All of these conditions are present near the Sun. The numerical solutions also show that the spacecraft's negative potential can be amplified by an ion wake. The negative potential of the ion wake prevents secondary electrons from escaping the part of spacecraft in contact with the wake. These findings may be important for future spacecraft missions that go nearer to the Sun, such as Solar Orbiter and Solar Probe Plus.

Ckmeans.1d.dp: Optimal k-means Clustering in One Dimension by Dynamic Programming.

PubMed

Wang, Haizhou; Song, Mingzhou

2011-12-01

The heuristic k -means algorithm, widely used for cluster analysis, does not guarantee optimality. We developed a dynamic programming algorithm for optimal one-dimensional clustering. The algorithm is implemented as an R package called Ckmeans.1d.dp . We demonstrate its advantage in optimality and runtime over the standard iterative k -means algorithm.

Optimal control of HIV/AIDS dynamic: Education and treatment

NASA Astrophysics Data System (ADS)

Sule, Amiru; Abdullah, Farah Aini

2014-07-01

A mathematical model which describes the transmission dynamics of HIV/AIDS is developed. The optimal control representing education and treatment for this model is explored. The existence of optimal Control is established analytically by the use of optimal control theory. Numerical simulations suggest that education and treatment for the infected has a positive impact on HIV/AIDS control.

Practical synchronization on complex dynamical networks via optimal pinning control

NASA Astrophysics Data System (ADS)

Li, Kezan; Sun, Weigang; Small, Michael; Fu, Xinchu

2015-07-01

We consider practical synchronization on complex dynamical networks under linear feedback control designed by optimal control theory. The control goal is to minimize global synchronization error and control strength over a given finite time interval, and synchronization error at terminal time. By utilizing the Pontryagin's minimum principle, and based on a general complex dynamical network, we obtain an optimal system to achieve the control goal. The result is verified by performing some numerical simulations on Star networks, Watts-Strogatz networks, and Barabási-Albert networks. Moreover, by combining optimal control and traditional pinning control, we propose an optimal pinning control strategy which depends on the network's topological structure. Obtained results show that optimal pinning control is very effective for synchronization control in real applications.

Optimal estimation of recurrence structures from time series

NASA Astrophysics Data System (ADS)

beim Graben, Peter; Sellers, Kristin K.; Fröhlich, Flavio; Hutt, Axel

2016-05-01

Recurrent temporal dynamics is a phenomenon observed frequently in high-dimensional complex systems and its detection is a challenging task. Recurrence quantification analysis utilizing recurrence plots may extract such dynamics, however it still encounters an unsolved pertinent problem: the optimal selection of distance thresholds for estimating the recurrence structure of dynamical systems. The present work proposes a stochastic Markov model for the recurrent dynamics that allows for the analytical derivation of a criterion for the optimal distance threshold. The goodness of fit is assessed by a utility function which assumes a local maximum for that threshold reflecting the optimal estimate of the system's recurrence structure. We validate our approach by means of the nonlinear Lorenz system and its linearized stochastic surrogates. The final application to neurophysiological time series obtained from anesthetized animals illustrates the method and reveals novel dynamic features of the underlying system. We propose the number of optimal recurrence domains as a statistic for classifying an animals' state of consciousness.

Modeling and prediction of copper removal from aqueous solutions by nZVI/rGO magnetic nanocomposites using ANN-GA and ANN-PSO.

PubMed

Fan, Mingyi; Hu, Jiwei; Cao, Rensheng; Xiong, Kangning; Wei, Xionghui

2017-12-21

Reduced graphene oxide-supported nanoscale zero-valent iron (nZVI/rGO) magnetic nanocomposites were prepared and then applied in the Cu(II) removal from aqueous solutions. Scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and superconduction quantum interference device magnetometer were performed to characterize the nZVI/rGO nanocomposites. In order to reduce the number of experiments and the economic cost, response surface methodology (RSM) combined with artificial intelligence (AI) techniques, such as artificial neural network (ANN), genetic algorithm (GA) and particle swarm optimization (PSO), has been utilized as a major tool that can model and optimize the removal processes, because a tremendous advance has recently been made on AI that may result in extensive applications. Based on RSM, ANN-GA and ANN-PSO were employed to model the Cu(II) removal process and optimize the operating parameters, e.g., operating temperature, initial pH, initial concentration and contact time. The ANN-PSO model was proven to be an effective tool for modeling and optimizing the Cu(II) removal with a low absolute error and a high removal efficiency. Furthermore, the isotherm, kinetic, thermodynamic studies and the XPS analysis were performed to explore the mechanisms of Cu(II) removal process.

Dynamic Regime Marginal Structural Mean Models for Estimation of Optimal Dynamic Treatment Regimes, Part II: Proofs of Results*

PubMed Central

Orellana, Liliana; Rotnitzky, Andrea; Robins, James M.

2010-01-01

In this companion article to “Dynamic Regime Marginal Structural Mean Models for Estimation of Optimal Dynamic Treatment Regimes, Part I: Main Content” [Orellana, Rotnitzky and Robins (2010), IJB, Vol. 6, Iss. 2, Art. 7] we present (i) proofs of the claims in that paper, (ii) a proposal for the computation of a confidence set for the optimal index when this lies in a finite set, and (iii) an example to aid the interpretation of the positivity assumption. PMID:20405047

Stability-Constrained Aerodynamic Shape Optimization with Applications to Flying Wings

NASA Astrophysics Data System (ADS)

Mader, Charles Alexander

A set of techniques is developed that allows the incorporation of flight dynamics metrics as an additional discipline in a high-fidelity aerodynamic optimization. Specifically, techniques for including static stability constraints and handling qualities constraints in a high-fidelity aerodynamic optimization are demonstrated. These constraints are developed from stability derivative information calculated using high-fidelity computational fluid dynamics (CFD). Two techniques are explored for computing the stability derivatives from CFD. One technique uses an automatic differentiation adjoint technique (ADjoint) to efficiently and accurately compute a full set of static and dynamic stability derivatives from a single steady solution. The other technique uses a linear regression method to compute the stability derivatives from a quasi-unsteady time-spectral CFD solution, allowing for the computation of static, dynamic and transient stability derivatives. Based on the characteristics of the two methods, the time-spectral technique is selected for further development, incorporated into an optimization framework, and used to conduct stability-constrained aerodynamic optimization. This stability-constrained optimization framework is then used to conduct an optimization study of a flying wing configuration. This study shows that stability constraints have a significant impact on the optimal design of flying wings and that, while static stability constraints can often be satisfied by modifying the airfoil profiles of the wing, dynamic stability constraints can require a significant change in the planform of the aircraft in order for the constraints to be satisfied.

Dynamic optimization approach for integrated supplier selection and tracking control of single product inventory system with product discount

NASA Astrophysics Data System (ADS)

Sutrisno; Widowati; Heru Tjahjana, R.

2017-01-01

In this paper, we propose a mathematical model in the form of dynamic/multi-stage optimization to solve an integrated supplier selection problem and tracking control problem of single product inventory system with product discount. The product discount will be stated as a piece-wise linear function. We use dynamic programming to solve this proposed optimization to determine the optimal supplier and the optimal product volume that will be purchased from the optimal supplier for each time period so that the inventory level tracks a reference trajectory given by decision maker with minimal total cost. We give a numerical experiment to evaluate the proposed model. From the result, the optimal supplier was determined for each time period and the inventory level follows the given reference well.

Dynamic modeling and optimization for space logistics using time-expanded networks

NASA Astrophysics Data System (ADS)

Ho, Koki; de Weck, Olivier L.; Hoffman, Jeffrey A.; Shishko, Robert

2014-12-01

This research develops a dynamic logistics network formulation for lifecycle optimization of mission sequences as a system-level integrated method to find an optimal combination of technologies to be used at each stage of the campaign. This formulation can find the optimal transportation architecture considering its technology trades over time. The proposed methodologies are inspired by the ground logistics analysis techniques based on linear programming network optimization. Particularly, the time-expanded network and its extension are developed for dynamic space logistics network optimization trading the quality of the solution with the computational load. In this paper, the methodologies are applied to a human Mars exploration architecture design problem. The results reveal multiple dynamic system-level trades over time and give recommendation of the optimal strategy for the human Mars exploration architecture. The considered trades include those between In-Situ Resource Utilization (ISRU) and propulsion technologies as well as the orbit and depot location selections over time. This research serves as a precursor for eventual permanent settlement and colonization of other planets by humans and us becoming a multi-planet species.

Tunable Stoichiometry of BCxNy Thin Films Through Multitarget Pulsed Laser Deposition Monitored via In Situ Ellipsometry (Postprint)

DTIC Science & Technology

2014-02-05

X - ray photoelectron spectroscopy (XPS), Raman spectroscopy , and atomic ...calculate thickness, n and k. X - ray photoelectron spectroscopy (XPS), Raman spectroscopy , and atomic force microscopy (AFM) were all performed on each of the... X - ray photoelectron spectroscopy (XPS) and Raman spectroscopy were used to measure and compare the composition of the films.6 In this paper,

Low-Thrust Many-Revolution Trajectory Optimization via Differential Dynamic Programming and a Sundman Transformation

NASA Astrophysics Data System (ADS)

Aziz, Jonathan D.; Parker, Jeffrey S.; Scheeres, Daniel J.; Englander, Jacob A.

2018-01-01

Low-thrust trajectories about planetary bodies characteristically span a high count of orbital revolutions. Directing the thrust vector over many revolutions presents a challenging optimization problem for any conventional strategy. This paper demonstrates the tractability of low-thrust trajectory optimization about planetary bodies by applying a Sundman transformation to change the independent variable of the spacecraft equations of motion to an orbit angle and performing the optimization with differential dynamic programming. Fuel-optimal geocentric transfers are computed with the transfer duration extended up to 2000 revolutions. The flexibility of the approach to higher fidelity dynamics is shown with Earth's J 2 perturbation and lunar gravity included for a 500 revolution transfer.

Low-Thrust Many-Revolution Trajectory Optimization via Differential Dynamic Programming and a Sundman Transformation

NASA Astrophysics Data System (ADS)

Aziz, Jonathan D.; Parker, Jeffrey S.; Scheeres, Daniel J.; Englander, Jacob A.

2018-06-01

Low-thrust trajectories about planetary bodies characteristically span a high count of orbital revolutions. Directing the thrust vector over many revolutions presents a challenging optimization problem for any conventional strategy. This paper demonstrates the tractability of low-thrust trajectory optimization about planetary bodies by applying a Sundman transformation to change the independent variable of the spacecraft equations of motion to an orbit angle and performing the optimization with differential dynamic programming. Fuel-optimal geocentric transfers are computed with the transfer duration extended up to 2000 revolutions. The flexibility of the approach to higher fidelity dynamics is shown with Earth's J 2 perturbation and lunar gravity included for a 500 revolution transfer.

Optimization of dynamic soaring maneuvers to enhance endurance of a versatile UAV

NASA Astrophysics Data System (ADS)

Mir, Imran; Maqsood, Adnan; Akhtar, Suhail

2017-06-01

Dynamic soaring is a process of acquiring energy available in atmospheric wind shears and is commonly exhibited by soaring birds to perform long distance flights. This paper aims to demonstrate a viable algorithm which can be implemented in near real time environment to formulate optimal trajectories for dynamic soaring maneuvers for a small scale Unmanned Aerial Vehicle (UAV). The objective is to harness maximum energy from atmosphere wind shear to improve loiter time for Intelligence, Surveillance and Reconnaissance (ISR) missions. Three-dimensional point-mass UAV equations of motion and linear wind gradient profile are used to model flight dynamics. Utilizing UAV states, controls, operational constraints, initial and terminal conditions that enforce a periodic flight, dynamic soaring problem is formulated as an optimal control problem. Optimized trajectories of the maneuver are subsequently generated employing pseudo spectral techniques against distant UAV performance parameters. The discussion also encompasses the requirement for generation of optimal trajectories for dynamic soaring in real time environment and the ability of the proposed algorithm for speedy solution generation. Coupled with the fact that dynamic soaring is all about immediately utilizing the available energy from the wind shear encountered, the proposed algorithm promises its viability for practical on board implementations requiring computation of trajectories in near real time.

A Sensor Dynamic Measurement Error Prediction Model Based on NAPSO-SVM

PubMed Central

Jiang, Minlan; Jiang, Lan; Jiang, Dingde; Li, Fei

2018-01-01

Dynamic measurement error correction is an effective way to improve sensor precision. Dynamic measurement error prediction is an important part of error correction, and support vector machine (SVM) is often used for predicting the dynamic measurement errors of sensors. Traditionally, the SVM parameters were always set manually, which cannot ensure the model’s performance. In this paper, a SVM method based on an improved particle swarm optimization (NAPSO) is proposed to predict the dynamic measurement errors of sensors. Natural selection and simulated annealing are added in the PSO to raise the ability to avoid local optima. To verify the performance of NAPSO-SVM, three types of algorithms are selected to optimize the SVM’s parameters: the particle swarm optimization algorithm (PSO), the improved PSO optimization algorithm (NAPSO), and the glowworm swarm optimization (GSO). The dynamic measurement error data of two sensors are applied as the test data. The root mean squared error and mean absolute percentage error are employed to evaluate the prediction models’ performances. The experimental results show that among the three tested algorithms the NAPSO-SVM method has a better prediction precision and a less prediction errors, and it is an effective method for predicting the dynamic measurement errors of sensors. PMID:29342942

A COMPARISON OF STATIC AND DYNAMIC OPTIMIZATION MUSCLE FORCE PREDICTIONS DURING WHEELCHAIR PROPULSION

PubMed Central

Morrow, Melissa M.; Rankin, Jeffery W.; Neptune, Richard R.; Kaufman, Kenton R.

2014-01-01

The primary purpose of this study was to compare static and dynamic optimization muscle force and work predictions during the push phase of wheelchair propulsion. A secondary purpose was to compare the differences in predicted shoulder and elbow kinetics and kinematics and handrim forces. The forward dynamics simulation minimized differences between simulated and experimental data (obtained from 10 manual wheelchair users) and muscle co-contraction. For direct comparison between models, the shoulder and elbow muscle moment arms and net joint moments from the dynamic optimization were used as inputs into the static optimization routine. RMS errors between model predictions were calculated to quantify model agreement. There was a wide range of individual muscle force agreement that spanned from poor (26.4 % Fmax error in the middle deltoid) to good (6.4 % Fmax error in the anterior deltoid) in the prime movers of the shoulder. The predicted muscle forces from the static optimization were sufficient to create the appropriate motion and joint moments at the shoulder for the push phase of wheelchair propulsion, but showed deviations in the elbow moment, pronation-supination motion and hand rim forces. These results suggest the static approach does not produce results similar enough to be a replacement for forward dynamics simulations, and care should be taken in choosing the appropriate method for a specific task and set of constraints. Dynamic optimization modeling approaches may be required for motions that are greatly influenced by muscle activation dynamics or that require significant co-contraction. PMID:25282075

Multiobjective Optimization of Low-Energy Trajectories Using Optimal Control on Dynamical Channels

NASA Technical Reports Server (NTRS)

Coffee, Thomas M.; Anderson, Rodney L.; Lo, Martin W.

2011-01-01

We introduce a computational method to design efficient low-energy trajectories by extracting initial solutions from dynamical channels formed by invariant manifolds, and improving these solutions through variational optimal control. We consider trajectories connecting two unstable periodic orbits in the circular restricted 3-body problem (CR3BP). Our method leverages dynamical channels to generate a range of solutions, and approximates the areto front for impulse and time of flight through a multiobjective optimization of these solutions based on primer vector theory. We demonstrate the application of our method to a libration orbit transfer in the Earth-Moon system.

Optimal dynamic pricing for deteriorating items with reference-price effects

NASA Astrophysics Data System (ADS)

Xue, Musen; Tang, Wansheng; Zhang, Jianxiong

2016-07-01

In this paper, a dynamic pricing problem for deteriorating items with the consumers' reference-price effect is studied. An optimal control model is established to maximise the total profit, where the demand not only depends on the current price, but also is sensitive to the historical price. The continuous-time dynamic optimal pricing strategy with reference-price effect is obtained through solving the optimal control model on the basis of Pontryagin's maximum principle. In addition, numerical simulations and sensitivity analysis are carried out. Finally, some managerial suggestions that firm may adopt to formulate its pricing policy are proposed.

A new upper limit to the field-aligned potential near Titan.

PubMed

Coates, Andrew J; Wellbrock, Anne; Waite, J Hunter; Jones, Geraint H

2015-06-28

Neutral particles dominate regions of the Saturn magnetosphere and locations near several of Saturn's moons. Sunlight ionizes neutrals, producing photoelectrons with characteristic energy spectra. The Cassini plasma spectrometer electron spectrometer has detected photoelectrons throughout these regions, where photoelectrons may be used as tracers of magnetic field morphology. They also enhance plasma escape by setting up an ambipolar electric field, since the relatively energetic electrons move easily along the magnetic field. A similar mechanism is seen in the Earth's polar wind and at Mars and Venus. Here we present a new analysis of Titan photoelectron data, comparing spectra measured in the sunlit ionosphere at ~1.4 Titan radii ( R T ) and at up to 6.8 R T away. This results in an upper limit on the potential of 2.95 V along magnetic field lines associated with Titan at up to 6.8 R T , which is comparable to some similar estimates for photoelectrons seen in Earth's magnetosphere.

Holographic Reconstruction of Photoelectron Diffraction and Its Circular Dichroism for Local Structure Probing

NASA Astrophysics Data System (ADS)

Matsui, Fumihiko; Matsushita, Tomohiro; Daimon, Hiroshi

2018-06-01

The local atomic structure around a specific element atom can be recorded as a photoelectron diffraction pattern. Forward focusing peaks and diffraction rings around them indicate the directions and distances from the photoelectron emitting atom to the surrounding atoms. The state-of-the-art holography reconstruction algorithm enables us to image the local atomic arrangement around the excited atom in a real space. By using circularly polarized light as an excitation source, the angular momentum transfer from the light to the photoelectron induces parallax shifts in these diffraction patterns. As a result, stereographic images of atomic arrangements are obtained. These diffraction patterns can be used as atomic-site-resolved probes for local electronic structure investigation in combination with spectroscopy techniques. Direct three-dimensional atomic structure visualization and site-specific electronic property analysis methods are reviewed. Furthermore, circular dichroism was also found in valence photoelectron and Auger electron diffraction patterns. The investigation of these new phenomena provides hints for the development of new techniques for local structure probing.

A new upper limit to the field‐aligned potential near Titan

PubMed Central

Wellbrock, Anne; Waite, J. Hunter; Jones, Geraint H.

2015-01-01

Abstract Neutral particles dominate regions of the Saturn magnetosphere and locations near several of Saturn's moons. Sunlight ionizes neutrals, producing photoelectrons with characteristic energy spectra. The Cassini plasma spectrometer electron spectrometer has detected photoelectrons throughout these regions, where photoelectrons may be used as tracers of magnetic field morphology. They also enhance plasma escape by setting up an ambipolar electric field, since the relatively energetic electrons move easily along the magnetic field. A similar mechanism is seen in the Earth's polar wind and at Mars and Venus. Here we present a new analysis of Titan photoelectron data, comparing spectra measured in the sunlit ionosphere at ~1.4 Titan radii (R T) and at up to 6.8 R T away. This results in an upper limit on the potential of 2.95 V along magnetic field lines associated with Titan at up to 6.8 R T, which is comparable to some similar estimates for photoelectrons seen in Earth's magnetosphere. PMID:27609997

Dynamic optimization and adaptive controller design

NASA Astrophysics Data System (ADS)

Inamdar, S. R.

2010-10-01

In this work I present a new type of controller which is an adaptive tracking controller which employs dynamic optimization for optimizing current value of controller action for the temperature control of nonisothermal continuously stirred tank reactor (CSTR). We begin with a two-state model of nonisothermal CSTR which are mass and heat balance equations and then add cooling system dynamics to eliminate input multiplicity. The initial design value is obtained using local stability of steady states where approach temperature for cooling action is specified as a steady state and a design specification. Later we make a correction in the dynamics where material balance is manipulated to use feed concentration as a system parameter as an adaptive control measure in order to avoid actuator saturation for the main control loop. The analysis leading to design of dynamic optimization based parameter adaptive controller is presented. The important component of this mathematical framework is reference trajectory generation to form an adaptive control measure.

Photoelectron studies of machined brass surfaces

NASA Astrophysics Data System (ADS)

Potts, A. W.; Merrison, J. P.; Tournas, A. D.; Yacoot, A.

UV photoelectron spectroscopy has been used to determine the surface composition of machined brass. The results show a considerable change between the photoelectron surface composition and the bulk composition of the same sample determined by energy-dispersive X-ray fluorescence. On the surface the lead composition is increased by ˜900 G. This is consistent with the important part that lead is believed to play in improving the machinability of this alloy.

An Optimization Framework for Dynamic Hybrid Energy Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wenbo Du; Humberto E Garcia; Christiaan J.J. Paredis

A computational framework for the efficient analysis and optimization of dynamic hybrid energy systems (HES) is developed. A microgrid system with multiple inputs and multiple outputs (MIMO) is modeled using the Modelica language in the Dymola environment. The optimization loop is implemented in MATLAB, with the FMI Toolbox serving as the interface between the computational platforms. Two characteristic optimization problems are selected to demonstrate the methodology and gain insight into the system performance. The first is an unconstrained optimization problem that optimizes the dynamic properties of the battery, reactor and generator to minimize variability in the HES. The second problemmore » takes operating and capital costs into consideration by imposing linear and nonlinear constraints on the design variables. The preliminary optimization results obtained in this study provide an essential step towards the development of a comprehensive framework for designing HES.« less

Sub-optimal control of fuzzy linear dynamical systems under granular differentiability concept.

PubMed

Mazandarani, Mehran; Pariz, Naser

2018-05-01

This paper deals with sub-optimal control of a fuzzy linear dynamical system. The aim is to keep the state variables of the fuzzy linear dynamical system close to zero in an optimal manner. In the fuzzy dynamical system, the fuzzy derivative is considered as the granular derivative; and all the coefficients and initial conditions can be uncertain. The criterion for assessing the optimality is regarded as a granular integral whose integrand is a quadratic function of the state variables and control inputs. Using the relative-distance-measure (RDM) fuzzy interval arithmetic and calculus of variations, the optimal control law is presented as the fuzzy state variables feedback. Since the optimal feedback gains are obtained as fuzzy functions, they need to be defuzzified. This will result in the sub-optimal control law. This paper also sheds light on the restrictions imposed by the approaches which are based on fuzzy standard interval arithmetic (FSIA), and use strongly generalized Hukuhara and generalized Hukuhara differentiability concepts for obtaining the optimal control law. The granular eigenvalues notion is also defined. Using an RLC circuit mathematical model, it is shown that, due to their unnatural behavior in the modeling phenomenon, the FSIA-based approaches may obtain some eigenvalues sets that might be different from the inherent eigenvalues set of the fuzzy dynamical system. This is, however, not the case with the approach proposed in this study. The notions of granular controllability and granular stabilizability of the fuzzy linear dynamical system are also presented in this paper. Moreover, a sub-optimal control for regulating a Boeing 747 in longitudinal direction with uncertain initial conditions and parameters is gained. In addition, an uncertain suspension system of one of the four wheels of a bus is regulated using the sub-optimal control introduced in this paper. Copyright © 2018 ISA. Published by Elsevier Ltd. All rights reserved.

Strong-Field Driven Dynamics of Metal and Dielectric Nanoparticles

NASA Astrophysics Data System (ADS)

Powell, Jeffrey

The motion of electrons in atoms, molecules, and solids in the presence of intense electromagnetic radiation is an important research topic in physics and physical chemistry because of its fundamental nature and numerous practical applications, ranging from precise machining of materials to optical control of chemical reactions and light-driven electronic devices. Mechanisms of light-matter interactions critically depend on the dimensions of the irradiated system and evolve significantly from single atoms or molecules to the macroscopic bulk. Nanoparticles provide the link between these two extremes. In this thesis, I take advantage of this bridge to study light-matter interactions as a function of nanoparticle size, shape, and composition. I present here three discrete, but interconnected, experiments contributing to our knowledge of nanoparticle properties and their response to intense, short-pulsed light fields. First, I investigate how individual nanoparticles interact with each other in solution, studying their temperature-dependent solubility. The interaction potential between 5.5nm gold nanoparticles, ligated by an alkanethiol was found to be -0.165eV, in reasonable agreement with a phenomenological model. The other two experiments explore ultrafast dynamics driven by intense femtosecond lasers in isolated, gas-phase metallic and dielectric nanoparticles. Photoelectron momentum imaging is applied to study the response of gold, silica, and gold-shell/silica-core nanoparticles (ranging from single to several hundred nanometers in size) with near-infrared (NIR), 25 fs laser pulses in the intensity range of 1011 - 1014 W/cm2. These measurements, which constitute the bulk of my graduate work, reveal the complex interplay between the external optical field and the induced near-field of the nanoparticle, resulting in the emission of very energetic electrons that are much faster than those emitted from isolated atoms or molecules exposed to the same light pulses. The highest photoelectron energies ("cutoffs") were measured as a function of laser intensity, nanoparticle material and size. We found that the energy cutoffs increase monotonically with laser intensity and nanoparticle size, except for the gold/silica hybrid where the plasmon resonance response modifies this behavior at low intensities. The measured photoelectron spectra for metallic nanoparticles display a large energy enhancement over silica. Finally, the last part of this thesis explores the possibility to apply time-resolved x-ray scattering as a probe of the ultrafast dynamics in isolated nanoparticles driven by very intense ( 1015 W/cm2) NIR laser radiation. To do this, I developed and built a nanoparticle source capable of injecting single, gas-phase nanoparticles with a narrow size distribution into the laser focus. We used femtosecond x-ray pulses from an x-ray free electron laser (XFEL) to map the evolution of the laser-irradiated nanoparticle. The ultrafast dynamics were observed in the single-shot x-ray diffraction patterns measured as a function of delay between the NIR and x-ray pulses, which allows for femtosecond temporal and nanometer spatial resolution. We found that the intense IR laser pulse rapidly ionizes the nanoparticle, effectively turning it into a nanoplasma within less than a picosecond, and observed signatures of the nanoparticle surface softening on a few hundred-femtosecond time scale.

An Optimization Framework for Dynamic, Distributed Real-Time Systems

NASA Technical Reports Server (NTRS)

Eckert, Klaus; Juedes, David; Welch, Lonnie; Chelberg, David; Bruggerman, Carl; Drews, Frank; Fleeman, David; Parrott, David; Pfarr, Barbara

2003-01-01

Abstract. This paper presents a model that is useful for developing resource allocation algorithms for distributed real-time systems .that operate in dynamic environments. Interesting aspects of the model include dynamic environments, utility and service levels, which provide a means for graceful degradation in resource-constrained situations and support optimization of the allocation of resources. The paper also provides an allocation algorithm that illustrates how to use the model for producing feasible, optimal resource allocations.

Integrated multidisciplinary design optimization of rotorcraft

NASA Technical Reports Server (NTRS)

Adelman, Howard M.; Mantay, Wayne R.

1989-01-01

The NASA/Army research plan for developing the logic elements for helicopter rotor design optimization by integrating appropriate disciplines and accounting for important interactions among the disciplines is discussed. The paper describes the optimization formulation in terms of the objective function, design variables, and constraints. The analysis aspects are discussed, and an initial effort at defining the interdisciplinary coupling is summarized. Results are presented on the achievements made in the rotor aerodynamic performance optimization for minimum hover horsepower, rotor dynamic optimization for vibration reduction, rotor structural optimization for minimum weight, and integrated aerodynamic load/dynamics optimization for minimum vibration and weight.

Vertically aligned N-doped CNTs growth using Taguchi experimental design

NASA Astrophysics Data System (ADS)

Silva, Ricardo M.; Fernandes, António J. S.; Ferro, Marta C.; Pinna, Nicola; Silva, Rui F.

2015-07-01

The Taguchi method with a parameter design L9 orthogonal array was implemented for optimizing the nitrogen incorporation in the structure of vertically aligned N-doped CNTs grown by thermal chemical deposition (TCVD). The maximization of the ID/IG ratio of the Raman spectra was selected as the target value. As a result, the optimal deposition configuration was NH3 = 90 sccm, growth temperature = 825 °C and catalyst pretreatment time of 2 min, the first parameter having the main effect on nitrogen incorporation. A confirmation experiment with these values was performed, ratifying the predicted ID/IG ratio of 1.42. Scanning electron microscopy (SEM) characterization revealed a uniform completely vertically aligned array of multiwalled CNTs which individually exhibit a bamboo-like structure, consisting of periodically curved graphitic layers, as depicted by high resolution transmission electron microscopy (HRTEM). The X-ray photoelectron spectroscopy (XPS) results indicated a 2.00 at.% of N incorporation in the CNTs in pyridine-like and graphite-like, as the predominant species.

Fluorine and sulfur simultaneously co-doped suspended graphene

NASA Astrophysics Data System (ADS)

Struzzi, C.; Sezen, H.; Amati, M.; Gregoratti, L.; Reckinger, N.; Colomer, J.-F.; Snyders, R.; Bittencourt, C.; Scardamaglia, M.

2017-11-01

Suspended graphene flakes are exposed simultaneously to fluorine and sulfur ions produced by the μ-wave plasma discharge of the SF6 precursor gas. The microscopic and spectroscopic analyses, performed by Raman spectroscopy, scanning electron microscopy and photoelectron spectromicroscopy, show the homogeneity in functionalization yield over the graphene flakes with F and S atoms covalently bonded to the carbon lattice. This promising surface shows potential for several applications ranging from biomolecule immobilization to lithium battery and hydrogen storage devices. The present co-doping process is an optimal strategy to engineer the graphene surface with a concurrent hydrophobic character, thanks to the fluorine atoms, and a high affinity with metal nanoparticles due to the presence of sulfur atoms.

An improved experimental scheme for simultaneous measurement of high-resolution zero electron kinetic energy (ZEKE) photoelectron and threshold photoion (MATI) spectra

NASA Astrophysics Data System (ADS)

Michels, François; Mazzoni, Federico; Becucci, Maurizio; Müller-Dethlefs, Klaus

2017-10-01

An improved detection scheme is presented for threshold ionization spectroscopy with simultaneous recording of the Zero Electron Kinetic Energy (ZEKE) and Mass Analysed Threshold Ionisation (MATI) signals. The objective is to obtain accurate dissociation energies for larger molecular clusters by simultaneously detecting the fragment and parent ion MATI signals with identical transmission. The scheme preserves an optimal ZEKE spectral resolution together with excellent separation of the spontaneous ion and MATI signals in the time-of-flight mass spectrum. The resulting improvement in sensitivity will allow for the determination of dissociation energies in clusters with substantial mass difference between parent and daughter ions.

COPS: Large-scale nonlinearly constrained optimization problems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bondarenko, A.S.; Bortz, D.M.; More, J.J.

2000-02-10

The authors have started the development of COPS, a collection of large-scale nonlinearly Constrained Optimization Problems. The primary purpose of this collection is to provide difficult test cases for optimization software. Problems in the current version of the collection come from fluid dynamics, population dynamics, optimal design, and optimal control. For each problem they provide a short description of the problem, notes on the formulation of the problem, and results of computational experiments with general optimization solvers. They currently have results for DONLP2, LANCELOT, MINOS, SNOPT, and LOQO.

Large-scale hydropower system optimization using dynamic programming and object-oriented programming: the case of the Northeast China Power Grid.

PubMed

Li, Ji-Qing; Zhang, Yu-Shan; Ji, Chang-Ming; Wang, Ai-Jing; Lund, Jay R

2013-01-01

This paper examines long-term optimal operation using dynamic programming for a large hydropower system of 10 reservoirs in Northeast China. Besides considering flow and hydraulic head, the optimization explicitly includes time-varying electricity market prices to maximize benefit. Two techniques are used to reduce the 'curse of dimensionality' of dynamic programming with many reservoirs. Discrete differential dynamic programming (DDDP) reduces the search space and computer memory needed. Object-oriented programming (OOP) and the ability to dynamically allocate and release memory with the C++ language greatly reduces the cumulative effect of computer memory for solving multi-dimensional dynamic programming models. The case study shows that the model can reduce the 'curse of dimensionality' and achieve satisfactory results.

Dynamic optimization and its relation to classical and quantum constrained systems

NASA Astrophysics Data System (ADS)

Contreras, Mauricio; Pellicer, Rely; Villena, Marcelo

2017-08-01

We study the structure of a simple dynamic optimization problem consisting of one state and one control variable, from a physicist's point of view. By using an analogy to a physical model, we study this system in the classical and quantum frameworks. Classically, the dynamic optimization problem is equivalent to a classical mechanics constrained system, so we must use the Dirac method to analyze it in a correct way. We find that there are two second-class constraints in the model: one fix the momenta associated with the control variables, and the other is a reminder of the optimal control law. The dynamic evolution of this constrained system is given by the Dirac's bracket of the canonical variables with the Hamiltonian. This dynamic results to be identical to the unconstrained one given by the Pontryagin equations, which are the correct classical equations of motion for our physical optimization problem. In the same Pontryagin scheme, by imposing a closed-loop λ-strategy, the optimality condition for the action gives a consistency relation, which is associated to the Hamilton-Jacobi-Bellman equation of the dynamic programming method. A similar result is achieved by quantizing the classical model. By setting the wave function Ψ(x , t) =e iS(x , t) in the quantum Schrödinger equation, a non-linear partial equation is obtained for the S function. For the right-hand side quantization, this is the Hamilton-Jacobi-Bellman equation, when S(x , t) is identified with the optimal value function. Thus, the Hamilton-Jacobi-Bellman equation in Bellman's maximum principle, can be interpreted as the quantum approach of the optimization problem.

Particle swarm optimization with recombination and dynamic linkage discovery.

PubMed

Chen, Ying-Ping; Peng, Wen-Chih; Jian, Ming-Chung

2007-12-01

In this paper, we try to improve the performance of the particle swarm optimizer by incorporating the linkage concept, which is an essential mechanism in genetic algorithms, and design a new linkage identification technique called dynamic linkage discovery to address the linkage problem in real-parameter optimization problems. Dynamic linkage discovery is a costless and effective linkage recognition technique that adapts the linkage configuration by employing only the selection operator without extra judging criteria irrelevant to the objective function. Moreover, a recombination operator that utilizes the discovered linkage configuration to promote the cooperation of particle swarm optimizer and dynamic linkage discovery is accordingly developed. By integrating the particle swarm optimizer, dynamic linkage discovery, and recombination operator, we propose a new hybridization of optimization methodologies called particle swarm optimization with recombination and dynamic linkage discovery (PSO-RDL). In order to study the capability of PSO-RDL, numerical experiments were conducted on a set of benchmark functions as well as on an important real-world application. The benchmark functions used in this paper were proposed in the 2005 Institute of Electrical and Electronics Engineers Congress on Evolutionary Computation. The experimental results on the benchmark functions indicate that PSO-RDL can provide a level of performance comparable to that given by other advanced optimization techniques. In addition to the benchmark, PSO-RDL was also used to solve the economic dispatch (ED) problem for power systems, which is a real-world problem and highly constrained. The results indicate that PSO-RDL can successfully solve the ED problem for the three-unit power system and obtain the currently known best solution for the 40-unit system.

Correlated electron and nuclear dynamics in strong field photoionization of H(2)(+).

PubMed

Silva, R E F; Catoire, F; Rivière, P; Bachau, H; Martín, F

2013-03-15

We present a theoretical study of H(2)(+) ionization under strong IR femtosecond pulses by using a method designed to extract correlated (2D) photoelectron and proton kinetic energy spectra. The results show two distinct ionization mechanisms-tunnel and multiphoton ionization-in which electrons and nuclei do not share the energy from the field in the same way. Electrons produced in multiphoton ionization share part of their energy with the nuclei, an effect that shows up in the 2D spectra in the form of energy-conservation fringes similar to those observed in weak-field ionization of diatomic molecules. In contrast, tunneling electrons lead to fringes whose position does not depend on the proton kinetic energy. At high intensity, the two processes coexist and the 2D plots show a very rich behavior, suggesting that the correlation between electron and nuclear dynamics in strong field ionization is more complex than one would have anticipated.

Field propagation-induced directionality of carrier-envelope phase-controlled photoemission from nanospheres

PubMed Central

Süßmann, F.; Seiffert, L.; Zherebtsov, S.; Mondes, V.; Stierle, J.; Arbeiter, M.; Plenge, J.; Rupp, P.; Peltz, C.; Kessel, A.; Trushin, S. A.; Ahn, B.; Kim, D.; Graf, C.; Rühl, E.; Kling, M. F.; Fennel, T.

2015-01-01

Near-fields of non-resonantly laser-excited nanostructures enable strong localization of ultrashort light fields and have opened novel routes to fundamentally modify and control electronic strong-field processes. Harnessing spatiotemporally tunable near-fields for the steering of sub-cycle electron dynamics may enable ultrafast optoelectronic devices and unprecedented control in the generation of attosecond electron and photon pulses. Here we utilize unsupported sub-wavelength dielectric nanospheres to generate near-fields with adjustable structure and study the resulting strong-field dynamics via photoelectron imaging. We demonstrate field propagation-induced tunability of the emission direction of fast recollision electrons up to a regime, where nonlinear charge interaction effects become dominant in the acceleration process. Our analysis supports that the timing of the recollision process remains controllable with attosecond resolution by the carrier-envelope phase, indicating the possibility to expand near-field-mediated control far into the realm of high-field phenomena. PMID:26264422

Field propagation-induced directionality of carrier-envelope phase-controlled photoemission from nanospheres.

PubMed

Süßmann, F; Seiffert, L; Zherebtsov, S; Mondes, V; Stierle, J; Arbeiter, M; Plenge, J; Rupp, P; Peltz, C; Kessel, A; Trushin, S A; Ahn, B; Kim, D; Graf, C; Rühl, E; Kling, M F; Fennel, T

2015-08-12

Near-fields of non-resonantly laser-excited nanostructures enable strong localization of ultrashort light fields and have opened novel routes to fundamentally modify and control electronic strong-field processes. Harnessing spatiotemporally tunable near-fields for the steering of sub-cycle electron dynamics may enable ultrafast optoelectronic devices and unprecedented control in the generation of attosecond electron and photon pulses. Here we utilize unsupported sub-wavelength dielectric nanospheres to generate near-fields with adjustable structure and study the resulting strong-field dynamics via photoelectron imaging. We demonstrate field propagation-induced tunability of the emission direction of fast recollision electrons up to a regime, where nonlinear charge interaction effects become dominant in the acceleration process. Our analysis supports that the timing of the recollision process remains controllable with attosecond resolution by the carrier-envelope phase, indicating the possibility to expand near-field-mediated control far into the realm of high-field phenomena.

Optimal control on hybrid ode systems with application to a tick disease model.

PubMed

Ding, Wandi

2007-10-01

We are considering an optimal control problem for a type of hybrid system involving ordinary differential equations and a discrete time feature. One state variable has dynamics in only one season of the year and has a jump condition to obtain the initial condition for that corresponding season in the next year. The other state variable has continuous dynamics. Given a general objective functional, existence, necessary conditions and uniqueness for an optimal control are established. We apply our approach to a tick-transmitted disease model with age structure in which the tick dynamics changes seasonally while hosts have continuous dynamics. The goal is to maximize disease-free ticks and minimize infected ticks through an optimal control strategy of treatment with acaricide. Numerical examples are given to illustrate the results.

Performance evaluation of the inverse dynamics method for optimal spacecraft reorientation

NASA Astrophysics Data System (ADS)

Ventura, Jacopo; Romano, Marcello; Walter, Ulrich

2015-05-01

This paper investigates the application of the inverse dynamics in the virtual domain method to Euler angles, quaternions, and modified Rodrigues parameters for rapid optimal attitude trajectory generation for spacecraft reorientation maneuvers. The impact of the virtual domain and attitude representation is numerically investigated for both minimum time and minimum energy problems. Owing to the nature of the inverse dynamics method, it yields sub-optimal solutions for minimum time problems. Furthermore, the virtual domain improves the optimality of the solution, but at the cost of more computational time. The attitude representation also affects solution quality and computational speed. For minimum energy problems, the optimal solution can be obtained without the virtual domain with any considered attitude representation.

Auroral and photoelectron fluxes in cometary ionospheres

NASA Astrophysics Data System (ADS)

Bhardwaj, A.; Haider, S. A.; Spinghal, R. P.

1990-05-01

The analytical yield spectrum method has been used to ascertain photoelectron and auroral electron fluxes in cometary ionospheres, with a view to determining the effects of cometocentric distances, solar zenith angle, and solar minimum and maximum conditions. Auroral electron fluxes are thus calculated for monoenergetic and observed primary electron spectra; auroral electrons are found to make a larger contribution to the observed electron spectrum than EUV-generated photoelectrons. Good agreement is established with extant theoretical works.

Ar 3p photoelectron sideband spectra in two-color XUV + NIR laser fields

NASA Astrophysics Data System (ADS)

Minemoto, Shinichirou; Shimada, Hiroyuki; Komatsu, Kazma; Komatsubara, Wataru; Majima, Takuya; Mizuno, Tomoya; Owada, Shigeki; Sakai, Hirofumi; Togashi, Tadashi; Yoshida, Shintaro; Yabashi, Makina; Yagishita, Akira

2018-04-01

We performed photoelectron spectroscopy using femtosecond XUV pulses from a free-electron laser and femtosecond near-infrared pulses from a synchronized laser, and succeeded in measuring Ar 3p photoelectron sideband spectra due to the two-color above-threshold ionization. In our calculations of the first-order time-dependent perturbation theoretical model based on the strong field approximation, the photoelectron sideband spectra and their angular distributions are well reproduced by considering the timing jitter between the XUV and the NIR pulses, showing that the timing jitter in our experiments was distributed over the width of {1.0}+0.4-0.2 ps. The present approach can be used as a method to evaluate the timing jitter inevitable in FEL experiments.

Competition between photodetachment and autodetachment of the 2{sup 1}ππ{sup *} state of the green fluorescent protein chromophore anion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mooney, Ciarán R. S.; Parkes, Michael A.; Zhang, Lijuan

2014-05-28

Using a combination of photoelectron spectroscopy measurements and quantum chemistry calculations, we have identified competing electron emission processes that contribute to the 350–315 nm photoelectron spectra of the deprotonated green fluorescent protein chromophore anion, p-hydroxybenzylidene-2,3-dimethylimidazolinone. As well as direct electron detachment from S{sub 0}, we observe resonant excitation of the 2{sup 1}ππ* state of the anion followed by autodetachment. The experimental photoelectron spectra are found to be significantly broader than photoelectron spectrum calculated using the Franck-Condon method and we attribute this to rapid (∼10 fs) vibrational decoherence, or intramolecular vibrational energy redistribution, within the neutral radical.

Computational and photoelectron spectroscopic study of the dipole-bound anions, indole(H2O)1,2 (.).

PubMed

Buytendyk, A M; Buonaugurio, A M; Xu, S-J; Nilles, J M; Bowen, K H; Kirnosov, N; Adamowicz, L

2016-07-14

We report our joint computational and anion photoelectron spectroscopic study of indole-water cluster anions, indole(H2O)1,2 (-). The photoelectron spectra of both cluster anions show the characteristics of dipole-bound anions, and this is confirmed by our theoretical computations. The experimentally determined vertical electron detachment (VDE) energies for indole(H2O)1 (-) and indole(H2O)2 (-) are 144 meV and 251 meV, respectively. The corresponding theoretically determined VDE values for indole(H2O)1 (-) and indole(H2O)2 (-) are 124 meV and 255 meV, respectively. The vibrational features in the photoelectron spectra of these cluster anions are assigned as the vibrations of the water molecule.

Computational and photoelectron spectroscopic study of the dipole-bound anions, indole(H2O)1,2-

NASA Astrophysics Data System (ADS)

Buytendyk, A. M.; Buonaugurio, A. M.; Xu, S.-J.; Nilles, J. M.; Bowen, K. H.; Kirnosov, N.; Adamowicz, L.

2016-07-01

We report our joint computational and anion photoelectron spectroscopic study of indole-water cluster anions, indole(H2O)1,2-. The photoelectron spectra of both cluster anions show the characteristics of dipole-bound anions, and this is confirmed by our theoretical computations. The experimentally determined vertical electron detachment (VDE) energies for indole(H2O)1- and indole(H2O)2- are 144 meV and 251 meV, respectively. The corresponding theoretically determined VDE values for indole(H2O)1- and indole(H2O)2- are 124 meV and 255 meV, respectively. The vibrational features in the photoelectron spectra of these cluster anions are assigned as the vibrations of the water molecule.

Efficient dynamic optimization of logic programs

NASA Technical Reports Server (NTRS)

Laird, Phil

1992-01-01

A summary is given of the dynamic optimization approach to speed up learning for logic programs. The problem is to restructure a recursive program into an equivalent program whose expected performance is optimal for an unknown but fixed population of problem instances. We define the term 'optimal' relative to the source of input instances and sketch an algorithm that can come within a logarithmic factor of optimal with high probability. Finally, we show that finding high-utility unfolding operations (such as EBG) can be reduced to clause reordering.

Proton transfer mediated by the vibronic coupling in oxygen core ionized states of glyoxalmonoxime studied by infrared-X-ray pump-probe spectroscopy.

PubMed

Felicíssimo, V C; Guimarães, F F; Cesar, A; Gel'mukhanov, F; Agren, H

2006-11-30

The theory of IR-X-ray pump-probe spectroscopy beyond the Born-Oppenheimer approximation is developed and applied to the study of the dynamics of intramolecular proton transfer in glyoxalmonoxime leading to the formation of the tautomer 2-nitrosoethenol. Due to the IR pump pulses the molecule gains sufficient energy to promote a proton to a weakly bound well. A femtosecond X-ray pulse snapshots the wave packet route and, hence, the dynamics of the proton transfer. The glyoxalmonoxime molecule contains two chemically nonequivalent oxygen atoms that possess distinct roles in the hydrogen bond, a hydrogen donor and an acceptor. Core ionizations of these form two intersecting core-ionized states, the vibronic coupling between which along the OH stretching mode partially delocalizes the core hole, resulting in a hopping of the core hole from one site to another. This, in turn, affects the dynamics of the proton transfer in the core-ionized state. The quantum dynamical simulations of X-ray photoelectron spectra of glyoxalmonoxime driven by strong IR pulses demonstrate the general applicability of the technique for studies of intramolecular proton transfer in systems with vibronic coupling.

Decay dynamics of nascent acetonitrile and nitromethane dipole-bound anions produced by intracluster charge-transfer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yandell, Margaret A.; King, Sarah B.; Neumark, Daniel M., E-mail: dneumark@berkeley.edu

2014-05-14

Decay dynamics of nascent dipole bound states of acetonitrile and nitromethane are examined using time-resolved photoelectron imaging of iodide-acetonitrile (I{sup −}·CH{sub 3}CN) and iodide-nitromethane (I{sup −}·CH{sub 3}NO{sub 2}) complexes. Dipole-bound anions are created by UV-initiated electron transfer to the molecule of interest from the associated iodide ion at energies just below the vertical detachment energy of the halide-molecule complex. The acetonitrile anion is observed to decay biexponentially with time constants in the range of 4–900 ps. In contrast, the dipole bound state of nitromethane decays rapidly over 400 fs to form the valence bound anion. The nitromethane valence anion speciesmore » then decays biexponentially with time constants of 2 ps and 1200 ps. The biexponential decay dynamics in acetonitrile are interpreted as iodine atom loss and autodetachment from the excited dipole-bound anion, followed by slower autodetachment of the relaxed metastable ion, while the dynamics of the nitromethane system suggest that a dipole-bound anion to valence anion transition proceeds via intramolecular vibrational energy redistribution to nitro group modes in the vicinity of the iodine atom.« less

Decay dynamics of nascent acetonitrile and nitromethane dipole-bound anions produced by intracluster charge-transfer.

PubMed

Yandell, Margaret A; King, Sarah B; Neumark, Daniel M

2014-05-14

Decay dynamics of nascent dipole bound states of acetonitrile and nitromethane are examined using time-resolved photoelectron imaging of iodide-acetonitrile (I(-)·CH3CN) and iodide-nitromethane (I(-)·CH3NO2) complexes. Dipole-bound anions are created by UV-initiated electron transfer to the molecule of interest from the associated iodide ion at energies just below the vertical detachment energy of the halide-molecule complex. The acetonitrile anion is observed to decay biexponentially with time constants in the range of 4-900 ps. In contrast, the dipole bound state of nitromethane decays rapidly over 400 fs to form the valence bound anion. The nitromethane valence anion species then decays biexponentially with time constants of 2 ps and 1200 ps. The biexponential decay dynamics in acetonitrile are interpreted as iodine atom loss and autodetachment from the excited dipole-bound anion, followed by slower autodetachment of the relaxed metastable ion, while the dynamics of the nitromethane system suggest that a dipole-bound anion to valence anion transition proceeds via intramolecular vibrational energy redistribution to nitro group modes in the vicinity of the iodine atom.

Adsorption of n-butane on graphene/Ru(0001)—A molecular beam scattering study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sivapragasam, Nilushni; Nayakasinghe, Mindika T.; Burghaus, Uwe, E-mail: uwe.burghaus@ndsu.edu

2016-07-15

Adsorption kinetics/dynamics of n-butane on graphene, physical vapor deposited on Ru(0001) (hereafter G/Ru), and bare Ru(0001) (hereafter Ru) are discussed. The chemical activity of the supported-graphene as well as the support was probed by thermal desorption spectroscopy (adsorption kinetics). In addition and to the best of our knowledge, for the first time, molecular beam scattering data of larger molecules were collected for graphene (probing the adsorption dynamics). Furthermore, samples were inspected by x-ray photoelectron spectroscopy and Auger electron spectroscopy. At the measuring conditions used here, n-butane adsorption kinetics/dynamics are molecular and nonactivated. Binding energies of butane on Ru and G/Rumore » are indistinguishable within experimental uncertainty. Thus, G/Ru is “kinetically transparent.” Initial adsorption probabilities, S{sub 0}, of n-butane decrease with increasing impact energy (0.76–1.72 eV) and are adsorption temperature independent for both Ru and G/Ru, again consistent with molecular adsorption. Also, S{sub 0} of Ru and G/Ru are indistinguishable within experimental uncertainty. Thus, G/Ru is “dynamically transparent.” Coverage dependent adsorption probabilities indicate precursor effects for graphene/Ru.« less

Ultrafast dynamics of photogenerated electrons in CdS nanocluster multilayers assembled on solid substrates: effects of assembly and electrode potential.

PubMed

Yagi, Ichizo; Mikami, Kensuke; Okamura, Masayuki; Uosaki, Kohei

2013-07-22

The ultrafast dynamics of photogenerated electrons in multilayer assemblies of CdS nanoparticles prepared on quartz and indium-tin oxide (ITO) substrates were followed by femtosecond (fs) visible-pump/mid-IR probe spectroscopy. Based on the observation of the photoinduced transient absorption spectra in the broad mid-IR range at the multilayer assembly of CdS nanoparticles, the occupation and fast relaxation of higher electronic states (1P(e)) were clarified. As compared with the electron dynamics of isolated (dispersed in solution) nanoparticles, the decay of photoexcited electrons in the multilayer assembly was clearly accelerated probably due to both electron hopping and scattering during interparticle electron tunneling. By using an ITO electrode as a substrate, the effect of the electric field on the photoelectron dynamics in the multilayer assembly was also investigated in situ. Both the amplitude and lifetime of photoexcited electrons gradually reduced as the potential became more positive. This result was explained by considering the reduction of the interparticle tunneling probability and the increase in the electron-transfer rate from the CdS nanoparticle assembly to the ITO electrode. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optimization of a pH-shift control strategy for producing monoclonal antibodies in Chinese hamster ovary cell cultures using a pH-dependent dynamic model.

PubMed

Hogiri, Tomoharu; Tamashima, Hiroshi; Nishizawa, Akitoshi; Okamoto, Masahiro

2018-02-01

To optimize monoclonal antibody (mAb) production in Chinese hamster ovary cell cultures, culture pH should be temporally controlled with high resolution. In this study, we propose a new pH-dependent dynamic model represented by simultaneous differential equations including a minimum of six system component, depending on pH value. All kinetic parameters in the dynamic model were estimated using an evolutionary numerical optimization (real-coded genetic algorithm) method based on experimental time-course data obtained at different pH values ranging from 6.6 to 7.2. We determined an optimal pH-shift schedule theoretically. We validated this optimal pH-shift schedule experimentally and mAb production increased by approximately 40% with this schedule. Throughout this study, it was suggested that the culture pH-shift optimization strategy using a pH-dependent dynamic model is suitable to optimize any pH-shift schedule for CHO cell lines used in mAb production projects. Copyright © 2017 The Society for Biotechnology, Japan. Published by Elsevier B.V. All rights reserved.

A potentiometric non-enzymatic glucose sensor using a molecularly imprinted layer bonded on a conducting polymer.

PubMed

Kim, Dong-Min; Moon, Jong-Min; Lee, Won-Chul; Yoon, Jang-Hee; Choi, Cheol Soo; Shim, Yoon-Bo

2017-05-15

A non-enzymatic potentiometric glucose sensor for the determination of glucose in the micomolar level in saliva was developed based on a molecularly imprinted polymer (MIP) binding on a conducting polymer layer. A MIP containing acrylamide, and aminophenyl boronic acid, as a host molecule to glucose, was immobilized on benzoic acid-functionalized poly(terthiophene) (pTBA) by the amide bond formation onto a gold nanoparticles deposited-screen printed carbon electrode (pTBA/AuNPs/SPCE). Aromatic boronic acid was incorporated into the MIP layer to stably capture glucose and create a potentiometric signal through the changed pKa value of polymer film by the formation of boronate anion-glucose complex with generation of H + ions by the cis-diol reaction. Reversible binding and extraction of glucose on the sensor surface was observed using a quartz crystal microbalance. Each layer of the sensor probe was characterized by cyclic voltammetry, electrochemical impedance spectroscopy, X-ray photoelectron spectroscopy, and atomic force microscopy. The potentiometric response at the optimized conditions exhibited a wide linear dynamic range of 3.2×10 -7 to 1.0×10 -3 M, with a detection limit of 1.9 (±0.15)×10 -7 M. The sensor probe revealed an excellent selectivity and sensitivity for glucose compared to other saccharides. In addition, the reliability of the proposed glucose sensor was evaluated in physiological fluid samples of saliva and finger prick blood. Copyright © 2016 Elsevier B.V. All rights reserved.

Achieving Optimal Self-Adaptivity for Dynamic Tuning of Organic Semiconductors through Resonance Engineering.

PubMed

Tao, Ye; Xu, Lijia; Zhang, Zhen; Chen, Runfeng; Li, Huanhuan; Xu, Hui; Zheng, Chao; Huang, Wei

2016-08-03

Current static-state explorations of organic semiconductors for optimal material properties and device performance are hindered by limited insights into the dynamically changed molecular states and charge transport and energy transfer processes upon device operation. Here, we propose a simple yet successful strategy, resonance variation-based dynamic adaptation (RVDA), to realize optimized self-adaptive properties in donor-resonance-acceptor molecules by engineering the resonance variation for dynamic tuning of organic semiconductors. Organic light-emitting diodes hosted by these RVDA materials exhibit remarkably high performance, with external quantum efficiencies up to 21.7% and favorable device stability. Our approach, which supports simultaneous realization of dynamically adapted and selectively enhanced properties via resonance engineering, illustrates a feasible design map for the preparation of smart organic semiconductors capable of dynamic structure and property modulations, promoting the studies of organic electronics from static to dynamic.

Nonlinear dynamics optimization with particle swarm and genetic algorithms for SPEAR3 emittance upgrade

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huang, Xiaobiao; Safranek, James

2014-09-01

Nonlinear dynamics optimization is carried out for a low emittance upgrade lattice of SPEAR3 in order to improve its dynamic aperture and Touschek lifetime. Two multi-objective optimization algorithms, a genetic algorithm and a particle swarm algorithm, are used for this study. The performance of the two algorithms are compared. The result shows that the particle swarm algorithm converges significantly faster to similar or better solutions than the genetic algorithm and it does not require seeding of good solutions in the initial population. These advantages of the particle swarm algorithm may make it more suitable for many accelerator optimization applications.

Neural dynamic optimization for control systems. I. Background.

PubMed

Seong, C Y; Widrow, B

2001-01-01

The paper presents neural dynamic optimization (NDO) as a method of optimal feedback control for nonlinear multi-input-multi-output (MIMO) systems. The main feature of NDO is that it enables neural networks to approximate the optimal feedback solution whose existence dynamic programming (DP) justifies, thereby reducing the complexities of computation and storage problems of the classical methods such as DP. This paper mainly describes the background and motivations for the development of NDO, while the two other subsequent papers of this topic present the theory of NDO and demonstrate the method with several applications including control of autonomous vehicles and of a robot arm, respectively.

Neural dynamic optimization for control systems.III. Applications.

PubMed

Seong, C Y; Widrow, B

2001-01-01

For pt.II. see ibid., p. 490-501. The paper presents neural dynamic optimization (NDO) as a method of optimal feedback control for nonlinear multi-input-multi-output (MIMO) systems. The main feature of NDO is that it enables neural networks to approximate the optimal feedback solution whose existence dynamic programming (DP) justifies, thereby reducing the complexities of computation and storage problems of the classical methods such as DP. This paper demonstrates NDO with several applications including control of autonomous vehicles and of a robot-arm, while the two other companion papers of this topic describes the background for the development of NDO and present the theory of the method, respectively.

Neural dynamic optimization for control systems.II. Theory.

PubMed

Seong, C Y; Widrow, B

2001-01-01

The paper presents neural dynamic optimization (NDO) as a method of optimal feedback control for nonlinear multi-input-multi-output (MIMO) systems. The main feature of NDO is that it enables neural networks to approximate the optimal feedback solution whose existence dynamic programming (DP) justifies, thereby reducing the complexities of computation and storage problems of the classical methods such as DP. This paper mainly describes the theory of NDO, while the two other companion papers of this topic explain the background for the development of NDO and demonstrate the method with several applications including control of autonomous vehicles and of a robot arm, respectively.

Robust input design for nonlinear dynamic modeling of AUV.

PubMed

Nouri, Nowrouz Mohammad; Valadi, Mehrdad

2017-09-01

Input design has a dominant role in developing the dynamic model of autonomous underwater vehicles (AUVs) through system identification. Optimal input design is the process of generating informative inputs that can be used to generate the good quality dynamic model of AUVs. In a problem with optimal input design, the desired input signal depends on the unknown system which is intended to be identified. In this paper, the input design approach which is robust to uncertainties in model parameters is used. The Bayesian robust design strategy is applied to design input signals for dynamic modeling of AUVs. The employed approach can design multiple inputs and apply constraints on an AUV system's inputs and outputs. Particle swarm optimization (PSO) is employed to solve the constraint robust optimization problem. The presented algorithm is used for designing the input signals for an AUV, and the estimate obtained by robust input design is compared with that of the optimal input design. According to the results, proposed input design can satisfy both robustness of constraints and optimality. Copyright © 2017 ISA. Published by Elsevier Ltd. All rights reserved.

Improving the Dynamic Characteristics of Body-in-White Structure Using Structural Optimization

PubMed Central

Yahaya Rashid, Aizzat S.; Mohamed Haris, Sallehuddin; Alias, Anuar

2014-01-01

The dynamic behavior of a body-in-white (BIW) structure has significant influence on the noise, vibration, and harshness (NVH) and crashworthiness of a car. Therefore, by improving the dynamic characteristics of BIW, problems and failures associated with resonance and fatigue can be prevented. The design objectives attempt to improve the existing torsion and bending modes by using structural optimization subjected to dynamic load without compromising other factors such as mass and stiffness of the structure. The natural frequency of the design was modified by identifying and reinforcing the structure at critical locations. These crucial points are first identified by topology optimization using mass and natural frequencies as the design variables. The individual components obtained from the analysis go through a size optimization step to find their target thickness of the structure. The thickness of affected regions of the components will be modified according to the analysis. The results of both optimization steps suggest several design modifications to achieve the target vibration specifications without compromising the stiffness of the structure. A method of combining both optimization approaches is proposed to improve the design modification process. PMID:25101312

Optimal control of multiphoton ionization dynamics of small alkali aggregates

NASA Astrophysics Data System (ADS)

Lindinger, A.; Bartelt, A.; Lupulescu, C.; Vajda, S.; Woste, Ludger

2003-11-01

We have performed transient multi-photon ionization experiments on small alkali clusters of different size in order to probe their wave packet dynamics, structural reorientations, charge transfers and dissociative events in different vibrationally excited electronic states including their ground state. The observed processes were highly dependent on the irradiated pulse parameters like wavelength range or its phase and amplitude; an emphasis to employ a feedback control system for generating the optimum pulse shapes. Their spectral and temporal behavior reflects interesting properties about the investigated system and the irradiated photo-chemical process. First, we present the vibrational dynamics of bound electronically excited states of alkali dimers and trimers. The scheme for observing the wave packet dynamics in the electronic ground state using stimulated Raman-pumping is shown. Since the employed pulse parameters significantly influence the efficiency of the irradiated dynamic pathways photo-induced ioniziation experiments were carried out. The controllability of 3-photon ionization pathways is investigated on the model-like systems NaK and K2. A closed learning loop for adaptive feedback control is used to find the optimal fs pulse shape. Sinusoidal parameterizations of the spectral phase modulation are investigated in regard to the obtained optimal field. By reducing the number of parameters and thereby the complexity of the phase moduation, optimal pulse shapes can be generated that carry fingerprints of the molecule's dynamical properties. This enables to find "understandable" optimal pulse forms and offers the possiblity to gain insight into the photo-induced control process. Characteristic motions of the involved wave packets are proposed to explain the optimized dynamic dissociation pathways.

Characterizing the effects of regolith surface roughness on photoemission from surfaces in space

NASA Astrophysics Data System (ADS)

Dove, A.; Horanyi, M.; Wang, X.

2017-12-01

Surfaces of airless bodies and spacecraft in space are exposed to a variety of charging environments. A balance of currents due to plasma bombardment, photoemission, electron and ion emission and collection, and secondary electron emission determines the surface's charge. Photoelectron emission is the dominant charging process on sunlit surfaces in the inner solar system due to the intense solar UV radiation. This can result in a net positive surface potential, with a cloud of photoelectrons immediately above the surface, called the photoelectron sheath. Conversely, the unlit side of the body will charge negatively due the collection of the fast-moving solar wind electrons. The interaction of charged dust grains with these positively and negatively charged surfaces, and within the photoelectron and plasma sheaths may explain the occurrence of dust lofting, levitation and transport above the lunar surface. The surface potential of exposed objects is also dependent on the material properties of their surfaces. Composition and particle size primarily affect the quantum efficiency of photoelectron generation; however, surface roughness can also control the charging process. In order to characterize these effects, we have conducted laboratory experiments to examine the role of surface roughness in generating photoelectrons in dedicated laboratory experiments using solid and dusty surfaces of the same composition (CeO2), and initial comparisons with JSC-1 lunar simulant. Using Langmuir probe measurements, we explore the measured potentials above insulating surfaces exposed to UV and an electric field, and we show that the photoemission current from a dusty surface is largely reduced due to its higher surface roughness, which causes a significant fraction of the emitted photoelectrons to be re-absorbed within the surface. We will discuss these results in context of similar situations on planetary surfaces.

Adaptive critics for dynamic optimization.

PubMed

Kulkarni, Raghavendra V; Venayagamoorthy, Ganesh Kumar

2010-06-01

A novel action-dependent adaptive critic design (ACD) is developed for dynamic optimization. The proposed combination of a particle swarm optimization-based actor and a neural network critic is demonstrated through dynamic sleep scheduling of wireless sensor motes for wildlife monitoring. The objective of the sleep scheduler is to dynamically adapt the sleep duration to node's battery capacity and movement pattern of animals in its environment in order to obtain snapshots of the animal on its trajectory uniformly. Simulation results show that the sleep time of the node determined by the actor critic yields superior quality of sensory data acquisition and enhanced node longevity. Copyright 2010 Elsevier Ltd. All rights reserved.

Chemo-physical properties of renal capsules under ultraviolet-c exposure

NASA Astrophysics Data System (ADS)

Baghapour, Sh.; Parvin, P.; Reyhani, A.; Mortazavi, S. Z.; Mokhtari, S.; Amjadi, A.

2014-08-01

The renal capsule tissue of lamb was irradiated with ultraviolet-C light and the treated samples were analyzed by uniaxial tensile test, dynamic mechanical analysis, attenuated total reflectance Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and contact angle measurements. It was shown that the skin cross-linking is dominant in low doses in accordance with the contact angle assessment. Conversely, the strong bulk degradation takes place at high doses. Similarly, the bulk cross-linking affects the mechanical tests as to enhance the stiffness at low doses, whereas strong degradation occurs at high doses that mainly arises from the strong bulk chain scission.

Distilling two-center-interference information during tunneling of aligned molecules with orthogonally polarized two-color laser fields

NASA Astrophysics Data System (ADS)

Gao, F.; Chen, Y. J.; Xin, G. G.; Liu, J.; Fu, L. B.

2017-12-01

When electrons tunnel through a barrier formed by the strong laser field and the two-center potential of a diatomic molecule, a double-slit-like interference can occur. However, this interference effect can not be probed directly right now, as it is strongly coupled with other dynamical processes during tunneling. Here, we show numerically and analytically that orthogonally polarized two-color (OTC) laser fields are capable of resolving the interference effect in tunneling, while leaving clear footprints of this effect in photoelectron momentum distributions. Moreover, this effect can be manipulated by changing the relative field strength of OTC fields.

Double-slit interference in H2^, subjected to ultrashort x-ray radiation

NASA Astrophysics Data System (ADS)

Secor, Ethan; Guan, Xiaoxu; Bartschat, Klaus; Schneider, Barry I.

2012-06-01

Extending our earlier work [1], we consider the double-slit interference effect [2,3] in the H2^, ion irradiated by intense short x-ray laser pulses with central photon energies from 200-500 eV. The time-dependent Schr"odinger equation in prolate spheroidal coordinates is solved to extract the angle-differential cross section of the photo-electron. The spatical coordinates are discretized by means of a finite-element discrete-variable representation. We discuss the confinement effect [3] in the parallel geometry, in which the emission mode of the photoelectron along the laser polarization direction is dynamically forbidden. This confinement appears periodically, with the details depending on both the momentum of the electron and the internuclear separation. On the other hand, the effect disappears in the perpendicular geometry. We compare our results to those obtained from a simple plane-wave model based on time-independent perturbation theory.[4pt] [1] X. Guan, E. Secor, K. Bartschat, and B. I. Schneider, Phys. Rev. A 84 (2011) 032420.[0pt] [2] I. G. Kaplan and A. P. Markin, Sov. Phys. Dokl. 14 (1969) 36.[0pt] [3] J. Fern'andez, F. L. Yip, T. N. Rescigno, C. W. McCurdy, and F. Mart'in, Phys. Rev. A 79 (2009) 043409.

Development of a Portable Single Photon Ionization-Photoelectron Ionization Time-of-Flight Mass Spectrometer

PubMed Central

Huang, Yunguang; Li, Jinxu; Tang, Bin; Zhu, Liping; Hou, Keyong; Li, Haiyang

2015-01-01

A vacuum ultraviolet lamp based single photon ionization- (SPI-) photoelectron ionization (PEI) portable reflecting time-of-flight mass spectrometer (TOFMS) was designed for online monitoring gas samples. It has a dual mode ionization source: SPI for analyte with ionization energy (IE) below 10.6 eV and PEI for IE higher than 10.6 eV. Two kinds of sampling inlets, a capillary inlet and a membrane inlet, are utilized for high concentration and trace volatile organic compounds, respectively. A mass resolution of 1100 at m/z 64 has been obtained with a total size of 40 × 31 × 29 cm, the weight is 27 kg, and the power consumption is only 70 W. A mixture of benzene, toluene, and xylene (BTX), SO2, and discharging products of SF6 were used to test its performance, and the result showed that the limit of quantitation for BTX is as low as 5 ppbv (S/N = 10 : 1) with linear dynamic ranges greater than four orders of magnitude. The portable TOFMS was also evaluated by analyzing volatile organic compounds from wine and decomposition products of SF6 inside of a gas-insulated switchgear. PMID:26587023

Real-time observation of multi-mode vibronic coherence in pentafluoropyridine

NASA Astrophysics Data System (ADS)

Kus, J. A.; Hüter, O.; Temps, F.

2017-07-01

The ultrafast dynamics of pentafluoropyridine in the 1 1B2 (ππ*) electronic state excited at λpump = 255 nm is investigated by femtosecond time-resolved time-of-flight mass spectrometry and photoelectron imaging spectroscopy. A pronounced, long-lived, and complex periodic modulation of the transient ion yield signal with contributions by four distinct frequency components, 72 cm-1, 144 cm-1, 251 cm-1, and 281 cm-1, is observed for up to 9 ps. The recorded photoelectron images display a spectral band from the excited 1 1B2 (ππ*) state only in the oscillation maxima; the signal is strongly reduced in the oscillation minima. Supported by electronic structure calculations at the RI-SCS-CC2 and XMCQDPT2 levels of theory, the oscillating components of the signal are identified as frequencies of b1 symmetry coupling modes in a vibronic coherence of the 1 1B2 (ππ*) and 1 1A2 (πσ*) electronic states. The optical excitation initiates regular and periodic wavepacket motion along those out-of-plane modes. In the distorted molecular structure, the initially excited state acquires substantial πσ* character that modulates the transition dipole moment for ionization and results in the observed oscillations.

Temperature-dependent Raman and ultraviolet photoelectron spectroscopy studies on phase transition behavior of VO{sub 2} films with M1 and M2 phases

DOE Office of Scientific and Technical Information (OSTI.GOV)

Okimura, Kunio, E-mail: okifn@keyaki.cc.u-tokai.ac.jp; Hanis Azhan, Nurul; Hajiri, Tetsuya

Structural and electronic phase transitions behavior of two polycrystalline VO{sub 2} films, one with pure M1 phase and the other with pure M2 phase at room temperature, were investigated by temperature-controlled Raman spectroscopy and ultraviolet photoelectron spectroscopy (UPS). We observed characteristic transient dynamics in which the Raman modes at 195 cm{sup −1} (V-V vibration) and 616 cm{sup −1} (V-O vibration) showed remarkable hardening along the temperature in M1 phase film, indicating the rearrangements of V-V pairs and VO{sub 6} octahedra. It was also shown that the M1 Raman mode frequency approached those of invariant M2 peaks before entering rutile phase. In UPSmore » spectra with high energy resolution of 0.03 eV for the M2 phase film, narrower V{sub 3d} band was observed together with smaller gap compared to those of M1 phase film, supporting the nature of Mott insulator of M2 phase even in the polycrystalline film. Cooperative behavior of lattice rearrangements and electronic phase transition was suggested for M1 phase film.« less

Photoelectron Transfer at ZnTPyP Self-Assembly/TiO2 Interfaces for Enhanced Two-Photon Photodynamic Therapy.

PubMed

Liu, Yanyan; Meng, Xianfu; Wang, Han; Tang, Zhongmin; Zuo, Changjing; He, Mingyuan; Bu, Wenbo

2018-01-17

Two-photon (TP) absorption nanomaterials are highly desirable for deep-tissue clinical diagnostics and orthotopic disease treatment. Here, a well-designed core/shell nanostructure was successfully synthesized with a ZnTPyP self-assembly nanocrystal (ZSN) inner core coated by a homogeneous TiO 2 layer outside (ZSN-TO). The ZSN is a good photosemiconductor, showing both one-photon (OP) and TP absorption properties for red fluorescence emission and electron-hole pair generation; TiO 2 with good biocompatibility acts as the electron acceptor, which can transfer photoelectron from ZSN to TiO 2 for highly effective electron-hole separation, favoring the production of long-life superoxide anion (O 2 •- ) by electrons and oxygen and strong oxidizing hydroxyl radical (•OH) by holes and surrounding H 2 O. Once pretreated with ZSN-TO, the simultaneous OP-405 nm or TP-800 nm laser stimulation and fluorescent imaging of reactive oxygen species (ROS) showed dynamical and continuous generation of ROS in HeLa cells, with cytotoxicity significantly increasing via the type-1-like photodynamic therapy process. The results demonstrated that the combination of organic ZSN with inorganic TiO 2 has great applications as an excellent photosensitizer for deep-tissue fluorescent imaging and noninvasive disease treatment via TP photodynamic therapy.

Optimal dynamic pricing and replenishment policy for perishable items with inventory-level-dependent demand

NASA Astrophysics Data System (ADS)

Lu, Lihao; Zhang, Jianxiong; Tang, Wansheng

2016-04-01

An inventory system for perishable items with limited replenishment capacity is introduced in this paper. The demand rate depends on the stock quantity displayed in the store as well as the sales price. With the goal to realise profit maximisation, an optimisation problem is addressed to seek for the optimal joint dynamic pricing and replenishment policy which is obtained by solving the optimisation problem with Pontryagin's maximum principle. A joint mixed policy, in which the sales price is a static decision variable and the replenishment rate remains to be a dynamic decision variable, is presented to compare with the joint dynamic policy. Numerical results demonstrate the advantages of the joint dynamic one, and further show the effects of different system parameters on the optimal joint dynamic policy and the maximal total profit.

Analytic approach to photoelectron transport.

NASA Technical Reports Server (NTRS)

Stolarski, R. S.

1972-01-01

The equation governing the transport of photoelectrons in the ionosphere is shown to be equivalent to the equation of radiative transfer. In the single-energy approximation this equation is solved in closed form by the method of discrete ordinates for isotropic scattering and for a single-constituent atmosphere. The results include prediction of the angular distribution of photoelectrons at all altitudes and, in particular, the angular distribution of the escape flux. The implications of these solutions in real atmosphere calculations are discussed.

Symmetry adapted cluster-configuration interaction calculation of the photoelectron spectra of famous biological active steroids

NASA Astrophysics Data System (ADS)

Abyar, Fatemeh; Farrokhpour, Hossein

2014-11-01

The photoelectron spectra of some famous steroids, important in biology, were calculated in the gas phase. The selected steroids were 5α-androstane-3,11,17-trione, 4-androstane-3,11,17-trione, cortisol, cortisone, corticosterone, dexamethasone, estradiol and cholesterol. The calculations were performed employing symmetry-adapted cluster/configuration interaction (SAC-CI) method using the 6-311++G(2df,pd) basis set. The population ratios of conformers of each steroid were calculated and used for simulating the photoelectron spectrum of steroid. It was found that more than one conformer contribute to the photoelectron spectra of some steroids. To confirm the calculated photoelectron spectra, they compared with their corresponding experimental spectra. There were no experimental gas phase Hesbnd I photoelectron spectra for some of the steroids of this work in the literature and their calculated spectra can show a part of intrinsic characteristics of this molecules in the gas phase. The canonical molecular orbitals involved in the ionization of each steroid were calculated at the HF/6-311++g(d,p) level of theory. The spectral bands of each steroid were assigned by natural bonding orbital (NBO) calculations. Knowing the electronic structures of steroids helps us to understand their biological activities and find which sites of steroid become active when a modification is performing under a biological pathway.

Photoelectron wave function in photoionization: plane wave or Coulomb wave?

PubMed

Gozem, Samer; Gunina, Anastasia O; Ichino, Takatoshi; Osborn, David L; Stanton, John F; Krylov, Anna I

2015-11-19

The calculation of absolute total cross sections requires accurate wave functions of the photoelectron and of the initial and final states of the system. The essential information contained in the latter two can be condensed into a Dyson orbital. We employ correlated Dyson orbitals and test approximate treatments of the photoelectron wave function, that is, plane and Coulomb waves, by comparing computed and experimental photoionization and photodetachment spectra. We find that in anions, a plane wave treatment of the photoelectron provides a good description of photodetachment spectra. For photoionization of neutral atoms or molecules with one heavy atom, the photoelectron wave function must be treated as a Coulomb wave to account for the interaction of the photoelectron with the +1 charge of the ionized core. For larger molecules, the best agreement with experiment is often achieved by using a Coulomb wave with a partial (effective) charge smaller than unity. This likely derives from the fact that the effective charge at the centroid of the Dyson orbital, which serves as the origin of the spherical wave expansion, is smaller than the total charge of a polyatomic cation. The results suggest that accurate molecular photoionization cross sections can be computed with a modified central potential model that accounts for the nonspherical charge distribution of the core by adjusting the charge in the center of the expansion.

Fast optimization of glide vehicle reentry trajectory based on genetic algorithm

NASA Astrophysics Data System (ADS)

Jia, Jun; Dong, Ruixing; Yuan, Xuejun; Wang, Chuangwei

2018-02-01

An optimization method of reentry trajectory based on genetic algorithm is presented to meet the need of reentry trajectory optimization for glide vehicle. The dynamic model for the glide vehicle during reentry period is established. Considering the constraints of heat flux, dynamic pressure, overload etc., the optimization of reentry trajectory is investigated by utilizing genetic algorithm. The simulation shows that the method presented by this paper is effective for the optimization of reentry trajectory of glide vehicle. The efficiency and speed of this method is comparative with the references. Optimization results meet all constraints, and the on-line fast optimization is potential by pre-processing the offline samples.

Comparative dynamics in a health investment model.

PubMed

Eisenring, C

1999-10-01

The method of comparative dynamics fully exploits the inter-temporal structure of optimal control models. I derive comparative dynamic results in a simplified demand for health model. The effect of a change in the depreciation rate on the optimal paths for health capital and investment in health is studied by use of a phase diagram.

Electronic structure of lanthanide scandates

NASA Astrophysics Data System (ADS)

Mizzi, Christopher A.; Koirala, Pratik; Marks, Laurence D.

2018-02-01

X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and density functional theory calculations were used to study the electronic structure of three lanthanide scandates: GdSc O3,TbSc O3 , and DySc O3 . X-ray photoelectron spectra simulated from first-principles calculations using a combination of on-site hybrid and GGA +U methods were found to be in good agreement with experimental x-ray photoelectron spectra. The hybrid method was used to model the ground state electronic structure and the GGA +U method accounted for the shift of valence state energies due to photoelectron emission via a Slater-Janak transition state approach. From these results, the lanthanide scandate valence bands were determined to be composed of Ln 4 f ,O 2 p , and Sc 3 d states, in agreement with previous work. However, contrary to previous work the minority Ln 4 f states were found to be located closer to, and in some cases at, the valence band maximum. This suggests that minority Ln 4 f electrons may play a larger role in lanthanide scandate properties than previously thought.

Photoelectron angular distributions from rotationally resolved autoionizing states of N 2

DOE PAGES

Chartrand, A. M.; McCormack, E. F.; Jacovella, U.; ...

2017-12-08

The single-photon, photoelectron-photoion coincidence spectrum of N 2 has been recorded at high (~1.5 cm -1) resolution in the region between the N 2 + X 2Σ g +, v + = 0 and 1 ionization thresholds by using a double imaging spectrometer and intense vacuum-ultraviolet light from the Synchrotron SOLEIL. This approach provides the relative photoionization cross section, the photoelectron energy distribution, and the photoelectron angular distribution as a function of photon energy. The region of interest contains autoionizing valence states, vibrationally autoionizing Rydberg states converging to vibrationally excited levels of the N 2 + X 2Σ g +more » ground state, and electronically autoionizing states converging to the N 2 + A 2Π and B 2Σ u + states. The wavelength resolution is sufficient to resolve rotational structure in the autoionizing states, but the electron energy resolution is insufficient to resolve rotational structure in the photoion spectrum. Here, a simplified approach based on multichannel quantum defect theory is used to predict the photoelectron angular distribution parameters, β, and the results are in reasonably good agreement with experiment.« less

Improving photoelectron counting and particle identification in scintillation detectors with Bayesian techniques

NASA Astrophysics Data System (ADS)

Akashi-Ronquest, M.; Amaudruz, P.-A.; Batygov, M.; Beltran, B.; Bodmer, M.; Boulay, M. G.; Broerman, B.; Buck, B.; Butcher, A.; Cai, B.; Caldwell, T.; Chen, M.; Chen, Y.; Cleveland, B.; Coakley, K.; Dering, K.; Duncan, F. A.; Formaggio, J. A.; Gagnon, R.; Gastler, D.; Giuliani, F.; Gold, M.; Golovko, V. V.; Gorel, P.; Graham, K.; Grace, E.; Guerrero, N.; Guiseppe, V.; Hallin, A. L.; Harvey, P.; Hearns, C.; Henning, R.; Hime, A.; Hofgartner, J.; Jaditz, S.; Jillings, C. J.; Kachulis, C.; Kearns, E.; Kelsey, J.; Klein, J. R.; Kuźniak, M.; LaTorre, A.; Lawson, I.; Li, O.; Lidgard, J. J.; Liimatainen, P.; Linden, S.; McFarlane, K.; McKinsey, D. N.; MacMullin, S.; Mastbaum, A.; Mathew, R.; McDonald, A. B.; Mei, D.-M.; Monroe, J.; Muir, A.; Nantais, C.; Nicolics, K.; Nikkel, J. A.; Noble, T.; O'Dwyer, E.; Olsen, K.; Orebi Gann, G. D.; Ouellet, C.; Palladino, K.; Pasuthip, P.; Perumpilly, G.; Pollmann, T.; Rau, P.; Retière, F.; Rielage, K.; Schnee, R.; Seibert, S.; Skensved, P.; Sonley, T.; Vázquez-Jáuregui, E.; Veloce, L.; Walding, J.; Wang, B.; Wang, J.; Ward, M.; Zhang, C.

2015-05-01

Many current and future dark matter and neutrino detectors are designed to measure scintillation light with a large array of photomultiplier tubes (PMTs). The energy resolution and particle identification capabilities of these detectors depend in part on the ability to accurately identify individual photoelectrons in PMT waveforms despite large variability in pulse amplitudes and pulse pileup. We describe a Bayesian technique that can identify the times of individual photoelectrons in a sampled PMT waveform without deconvolution, even when pileup is present. To demonstrate the technique, we apply it to the general problem of particle identification in single-phase liquid argon dark matter detectors. Using the output of the Bayesian photoelectron counting algorithm described in this paper, we construct several test statistics for rejection of backgrounds for dark matter searches in argon. Compared to simpler methods based on either observed charge or peak finding, the photoelectron counting technique improves both energy resolution and particle identification of low energy events in calibration data from the DEAP-1 detector and simulation of the larger MiniCLEAN dark matter detector.

Distinguishability of N Composition Profiles In SiON Films On Si By Angle-Resolved X-ray Photoelectron Spectroscopy

NASA Astrophysics Data System (ADS)

Powell, C. J.; Werner, W. S. M.; Smekal, W.

2007-09-01

We report on the use of the NIST Database for the Simulation of Electron Spectra for Surface Analysis (SESSA) to determine N 1s, O 1s, and Si 2p3/2 photoelectron intensities for a 25 Å SiON film on a Si substrate with different distributions of N in the film. These simulations were made to assess the distinguishability of angle-resolved x-ray photoelectron spectroscopy (ARXPS) signals for each N distribution. Our approach differs from conventional simulations of ARXPS data in that we do not neglect elastic scattering of the photoelectrons and the finite solid angle of the analyzer. Appreciable dispersion of the photoelectron intensities was found only for the N 1s intensities at an emission angle of 75° (with respect to the surface normal). Conventional analyses of ARXPS data that include such large emission angles are unlikely to be valid due to angle-dependent changes of the attenuation length. We demonstrate the magnitude of elastic-scattering and analyzer solid-angle effects on the calculated angular distributions.

Discrete Adjoint-Based Design Optimization of Unsteady Turbulent Flows on Dynamic Unstructured Grids

NASA Technical Reports Server (NTRS)

Nielsen, Eric J.; Diskin, Boris; Yamaleev, Nail K.

2009-01-01

An adjoint-based methodology for design optimization of unsteady turbulent flows on dynamic unstructured grids is described. The implementation relies on an existing unsteady three-dimensional unstructured grid solver capable of dynamic mesh simulations and discrete adjoint capabilities previously developed for steady flows. The discrete equations for the primal and adjoint systems are presented for the backward-difference family of time-integration schemes on both static and dynamic grids. The consistency of sensitivity derivatives is established via comparisons with complex-variable computations. The current work is believed to be the first verified implementation of an adjoint-based optimization methodology for the true time-dependent formulation of the Navier-Stokes equations in a practical computational code. Large-scale shape optimizations are demonstrated for turbulent flows over a tiltrotor geometry and a simulated aeroelastic motion of a fighter jet.

Global dynamic optimization approach to predict activation in metabolic pathways.

PubMed

de Hijas-Liste, Gundián M; Klipp, Edda; Balsa-Canto, Eva; Banga, Julio R

2014-01-06

During the last decade, a number of authors have shown that the genetic regulation of metabolic networks may follow optimality principles. Optimal control theory has been successfully used to compute optimal enzyme profiles considering simple metabolic pathways. However, applying this optimal control framework to more general networks (e.g. branched networks, or networks incorporating enzyme production dynamics) yields problems that are analytically intractable and/or numerically very challenging. Further, these previous studies have only considered a single-objective framework. In this work we consider a more general multi-objective formulation and we present solutions based on recent developments in global dynamic optimization techniques. We illustrate the performance and capabilities of these techniques considering two sets of problems. First, we consider a set of single-objective examples of increasing complexity taken from the recent literature. We analyze the multimodal character of the associated non linear optimization problems, and we also evaluate different global optimization approaches in terms of numerical robustness, efficiency and scalability. Second, we consider generalized multi-objective formulations for several examples, and we show how this framework results in more biologically meaningful results. The proposed strategy was used to solve a set of single-objective case studies related to unbranched and branched metabolic networks of different levels of complexity. All problems were successfully solved in reasonable computation times with our global dynamic optimization approach, reaching solutions which were comparable or better than those reported in previous literature. Further, we considered, for the first time, multi-objective formulations, illustrating how activation in metabolic pathways can be explained in terms of the best trade-offs between conflicting objectives. This new methodology can be applied to metabolic networks with arbitrary topologies, non-linear dynamics and constraints.

Design optimization of dual-axis driving mechanism for satellite antenna with two planar revolute clearance joints

NASA Astrophysics Data System (ADS)

Bai, Zheng Feng; Zhao, Ji Jun; Chen, Jun; Zhao, Yang

2018-03-01

In the dynamic analysis of satellite antenna dual-axis driving mechanism, it is usually assumed that the joints are ideal or perfect without clearances. However, in reality, clearances in joints are unavoidable due to assemblage, manufacturing errors and wear. When clearance is introduced to the mechanism, it will lead to poor dynamic performances and undesirable vibrations due to impact forces in clearance joint. In this paper, a design optimization method is presented to reduce the undesirable vibrations of satellite antenna considering clearance joints in dual-axis driving mechanism. The contact force model in clearance joint is established using a nonlinear spring-damper model and the friction effect is considered using a modified Coulomb friction model. Firstly, the effects of clearances on dynamic responses of satellite antenna are investigated. Then the optimization method for dynamic design of the dual-axis driving mechanism with clearance is presented. The objective of the optimization is to minimize the maximum absolute vibration peak of antenna acceleration by reducing the impact forces in clearance joint. The main consideration here is to optimize the contact parameters of the joint elements. The contact stiffness coefficient, damping coefficient and the dynamic friction coefficient for clearance joint elements are taken as the optimization variables. A Generalized Reduced Gradient (GRG) algorithm is used to solve this highly nonlinear optimization problem for dual-axis driving mechanism with clearance joints. The results show that the acceleration peaks of satellite antenna and contact forces in clearance joints are reduced obviously after design optimization, which contributes to a better performance of the satellite antenna. Also, the application and limitation of the proposed optimization method are discussed.

Multiobjective optimization of temporal processes.

PubMed

Song, Zhe; Kusiak, Andrew

2010-06-01

This paper presents a dynamic predictive-optimization framework of a nonlinear temporal process. Data-mining (DM) and evolutionary strategy algorithms are integrated in the framework for solving the optimization model. DM algorithms learn dynamic equations from the process data. An evolutionary strategy algorithm is then applied to solve the optimization problem guided by the knowledge extracted by the DM algorithm. The concept presented in this paper is illustrated with the data from a power plant, where the goal is to maximize the boiler efficiency and minimize the limestone consumption. This multiobjective optimization problem can be either transformed into a single-objective optimization problem through preference aggregation approaches or into a Pareto-optimal optimization problem. The computational results have shown the effectiveness of the proposed optimization framework.

Optimal Guaranteed Cost Sliding Mode Control for Constrained-Input Nonlinear Systems With Matched and Unmatched Disturbances.

PubMed

Zhang, Huaguang; Qu, Qiuxia; Xiao, Geyang; Cui, Yang

2018-06-01

Based on integral sliding mode and approximate dynamic programming (ADP) theory, a novel optimal guaranteed cost sliding mode control is designed for constrained-input nonlinear systems with matched and unmatched disturbances. When the system moves on the sliding surface, the optimal guaranteed cost control problem of sliding mode dynamics is transformed into the optimal control problem of a reformulated auxiliary system with a modified cost function. The ADP algorithm based on single critic neural network (NN) is applied to obtain the approximate optimal control law for the auxiliary system. Lyapunov techniques are used to demonstrate the convergence of the NN weight errors. In addition, the derived approximate optimal control is verified to guarantee the sliding mode dynamics system to be stable in the sense of uniform ultimate boundedness. Some simulation results are presented to verify the feasibility of the proposed control scheme.

A weak Hamiltonian finite element method for optimal control problems

NASA Technical Reports Server (NTRS)

Hodges, Dewey H.; Bless, Robert R.

1989-01-01

A temporal finite element method based on a mixed form of the Hamiltonian weak principle is developed for dynamics and optimal control problems. The mixed form of Hamilton's weak principle contains both displacements and momenta as primary variables that are expanded in terms of nodal values and simple polynomial shape functions. Unlike other forms of Hamilton's principle, however, time derivatives of the momenta and displacements do not appear therein; instead, only the virtual momenta and virtual displacements are differentiated with respect to time. Based on the duality that is observed to exist between the mixed form of Hamilton's weak principle and variational principles governing classical optimal control problems, a temporal finite element formulation of the latter can be developed in a rather straightforward manner. Several well-known problems in dynamics and optimal control are illustrated. The example dynamics problem involves a time-marching problem. As optimal control examples, elementary trajectory optimization problems are treated.

A weak Hamiltonian finite element method for optimal control problems

NASA Technical Reports Server (NTRS)

Hodges, Dewey H.; Bless, Robert R.

1990-01-01

A temporal finite element method based on a mixed form of the Hamiltonian weak principle is developed for dynamics and optimal control problems. The mixed form of Hamilton's weak principle contains both displacements and momenta as primary variables that are expanded in terms of nodal values and simple polynomial shape functions. Unlike other forms of Hamilton's principle, however, time derivatives of the momenta and displacements do not appear therein; instead, only the virtual momenta and virtual displacements are differentiated with respect to time. Based on the duality that is observed to exist between the mixed form of Hamilton's weak principle and variational principles governing classical optimal control problems, a temporal finite element formulation of the latter can be developed in a rather straightforward manner. Several well-known problems in dynamics and optimal control are illustrated. The example dynamics problem involves a time-marching problem. As optimal control examples, elementary trajectory optimization problems are treated.

Weak Hamiltonian finite element method for optimal control problems

NASA Technical Reports Server (NTRS)

Hodges, Dewey H.; Bless, Robert R.

1991-01-01

A temporal finite element method based on a mixed form of the Hamiltonian weak principle is developed for dynamics and optimal control problems. The mixed form of Hamilton's weak principle contains both displacements and momenta as primary variables that are expanded in terms of nodal values and simple polynomial shape functions. Unlike other forms of Hamilton's principle, however, time derivatives of the momenta and displacements do not appear therein; instead, only the virtual momenta and virtual displacements are differentiated with respect to time. Based on the duality that is observed to exist between the mixed form of Hamilton's weak principle and variational principles governing classical optimal control problems, a temporal finite element formulation of the latter can be developed in a rather straightforward manner. Several well-known problems in dynamics and optimal control are illustrated. The example dynamics problem involves a time-marching problem. As optimal control examples, elementary trajectory optimization problems are treated.

Feshbach resonances in the exit channel of the F + CH3OH → HF + CH3O reaction observed using transition-state spectroscopy

NASA Astrophysics Data System (ADS)

Weichman, Marissa L.; Devine, Jessalyn A.; Babin, Mark C.; Li, Jun; Guo, Lifen; Ma, Jianyi; Guo, Hua; Neumark, Daniel M.

2017-10-01

The transition state governs how chemical bonds form and cleave during a chemical reaction and its direct characterization is a long-standing challenge in physical chemistry. Transition state spectroscopy experiments based on negative-ion photodetachment provide a direct probe of the vibrational structure and metastable resonances that are characteristic of the reactive surface. Dynamical resonances are extremely sensitive to the topography of the reactive surface and provide an exceptional point of comparison with theory. Here we study the seven-atom F + CH3OH → HF + CH3O reaction using slow photoelectron velocity-map imaging spectroscopy of cryocooled CH3OHF- anions. These measurements reveal spectral features associated with a manifold of vibrational Feshbach resonances and bound states supported by the post-transition state potential well. Quantum dynamical calculations yield excellent agreement with the experimental results, allow the assignment of spectral structure and demonstrate that the key dynamics of complex bimolecular reactions can be captured with a relatively simple theoretical framework.

Feshbach resonances in the exit channel of the F + CH3OH → HF + CH3O reaction observed using transition-state spectroscopy.

PubMed

Weichman, Marissa L; DeVine, Jessalyn A; Babin, Mark C; Li, Jun; Guo, Lifen; Ma, Jianyi; Guo, Hua; Neumark, Daniel M

2017-10-01

The transition state governs how chemical bonds form and cleave during a chemical reaction and its direct characterization is a long-standing challenge in physical chemistry. Transition state spectroscopy experiments based on negative-ion photodetachment provide a direct probe of the vibrational structure and metastable resonances that are characteristic of the reactive surface. Dynamical resonances are extremely sensitive to the topography of the reactive surface and provide an exceptional point of comparison with theory. Here we study the seven-atom F + CH 3 OH → HF + CH 3 O reaction using slow photoelectron velocity-map imaging spectroscopy of cryocooled CH 3 OHF - anions. These measurements reveal spectral features associated with a manifold of vibrational Feshbach resonances and bound states supported by the post-transition state potential well. Quantum dynamical calculations yield excellent agreement with the experimental results, allow the assignment of spectral structure and demonstrate that the key dynamics of complex bimolecular reactions can be captured with a relatively simple theoretical framework.

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

DOE PAGES

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.; ...

2017-03-17

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

DOE Office of Scientific and Technical Information (OSTI.GOV)

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

A dynamic model of functioning of a bank

NASA Astrophysics Data System (ADS)

Malafeyev, Oleg; Awasthi, Achal; Zaitseva, Irina; Rezenkov, Denis; Bogdanova, Svetlana

2018-04-01

In this paper, we analyze dynamic programming as a novel approach to solve the problem of maximizing the profits of a bank. The mathematical model of the problem and the description of bank's work is described in this paper. The problem is then approached using the method of dynamic programming. Dynamic programming makes sure that the solutions obtained are globally optimal and numerically stable. The optimization process is set up as a discrete multi-stage decision process and solved with the help of dynamic programming.

KMC-1: a high resolution and high flux soft x-ray beamline at BESSY.

PubMed

Schaefers, F; Mertin, M; Gorgoi, M

2007-12-01

The crystal monochromator beamline KMC-1 at a BESSY II bending magnet covers the energy range from soft (1.7 keV) to hard x-rays (12 keV) employing the (n,-n) double crystal arrangement with constant beam offset. The monochromator is equipped with three sets of crystals, InSb, Si (111), and Si (422) which are exchangeable in situ within a few minutes. Beamline and monochromator have been optimized for high flux and high resolution. This could be achieved by (1) a windowless setup under ultrahigh-vacuum conditions up to the experiment, (2) by the use of only three optical elements to minimize reflection losses, (3) by collecting an unusually large horizontal radiation fan (6 mrad) with the toroidal premirror, and (4) the optimization of the crystal optics to the soft x-ray range necessitating quasibackscattering crystal geometry (theta(Bragg,max)=82 degrees) delivering crystal limited resolution. The multipurpose beamline is in use for a variety of user facilities such as extended x-ray absorption fine structure, ((Bio-)EXAFS) near-edge x-ray absorption fine structure (NEXAFS), absorption and fluorescence spectroscopy. Due to the windowless UHV setup the k edges of the technologically and biologically important elements such as Si, P, and S are accessible. In addition to these experiments this beamline is now extensively used for photoelectron spectroscopy at high kinetic energies. Photon flux in the 10(11)-10(12) photons/s range and beamline resolving powers of more than E/DeltaE approximately 100.000 have been measured at selected energies employing Si (nnn) high order radiation in quasibackscattering geometry, thus photoelectron spectroscopy with a total instrumental resolution of about 150 meV is possible. This article describes the design features of the beamline and reports some experimental results in the above mentioned fields.

KMC-1: A high resolution and high flux soft x-ray beamline at BESSY

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schaefers, F.; Mertin, M.; Gorgoi, M.

2007-12-15

The crystal monochromator beamline KMC-1 at a BESSY II bending magnet covers the energy range from soft (1.7 keV) to hard x-rays (12 keV) employing the (n,-n) double crystal arrangement with constant beam offset. The monochromator is equipped with three sets of crystals, InSb, Si (111), and Si (422) which are exchangeable in situ within a few minutes. Beamline and monochromator have been optimized for high flux and high resolution. This could be achieved by (1) a windowless setup under ultrahigh-vacuum conditions up to the experiment, (2) by the use of only three optical elements to minimize reflection losses, (3)more » by collecting an unusually large horizontal radiation fan (6 mrad) with the toroidal premirror, and (4) the optimization of the crystal optics to the soft x-ray range necessitating quasibackscattering crystal geometry ({theta}{sub Bragg,max}=82 deg.) delivering crystal limited resolution. The multipurpose beamline is in use for a variety of user facilities such as extended x-ray absorption fine structure, ((Bio-)EXAFS) near-edge x-ray absorption fine structure (NEXAFS), absorption and fluorescence spectroscopy. Due to the windowless UHV setup the k edges of the technologically and biologically important elements such as Si, P, and S are accessible. In addition to these experiments this beamline is now extensively used for photoelectron spectroscopy at high kinetic energies. Photon flux in the 10{sup 11}-10{sup 12} photons/s range and beamline resolving powers of more than E/{delta}E{approx_equal}100.000 have been measured at selected energies employing Si (nnn) high order radiation in quasibackscattering geometry, thus photoelectron spectroscopy with a total instrumental resolution of about 150 meV is possible. This article describes the design features of the beamline and reports some experimental results in the above mentioned fields.« less

Photoelectron spectroscopic and microspectroscopic probes of ferroelectrics

NASA Astrophysics Data System (ADS)

Tǎnase, Liviu C.; Abramiuc, Laura E.; Teodorescu, Cristian M.

2017-12-01

This contribution is a review of recent aspects connected with photoelectron spectroscopy of free ferroelectric surfaces, metals interfaced with these surfaces, graphene-like layers together with some exemplifications concerning molecular adsorption, dissociations and desorptions occurring from ferroelectrics. Standard photoelectron spectroscopy is used nowadays in correlation with other characterization techniques, such as piezoresponse force microscopy, high resolution transmission electron spectroscopy, and ferroelectric hysteresis cycles. In this work we will concentrate mainly on photoelectron spectroscopy and spectro-microscopy characterization of ferroelectric thin films, starting from atomically clean ferroelectric surfaces of lead zirco-titanate, then going towards heterostructures using this material in combination with graphene-like carbon layers or with metals. Concepts involving charge accumulation and depolarization near surface will be revisited by taking into account the newest findings in this area.

Coherent control of photoelectron wavepacket angular interferograms

NASA Astrophysics Data System (ADS)

Hockett, P.; Wollenhaupt, M.; Baumert, T.

2015-11-01

Coherent control over photoelectron wavepackets, via the use of polarization-shaped laser pulses, can be understood as a time and polarization-multiplexed process, where the final (time-integrated) observable coherently samples all instantaneous states of the light-matter interaction. In this work, we investigate this multiplexing via computation of the observable photoelectron angular interferograms resulting from multi-photon atomic ionization with polarization-shaped laser pulses. We consider the polarization sensitivity of both the instantaneous and cumulative continuum wavefunction; the nature of the coherent control over the resultant photoelectron interferogram is thus explored in detail. Based on this understanding, the use of coherent control with polarization-shaped pulses as a methodology for a highly multiplexed coherent quantum metrology is also investigated, and defined in terms of the information content of the observable.

Analysis of penumbral eclipse data

NASA Technical Reports Server (NTRS)

Garrett, H. B.

1977-01-01

Two days of data from the ATS-6 1976 eclipse season were analyzed to determine the effects of varying photoelectron flux on spacecraft potential. Particular emphasis was placed on the variation in potential as the satellite entered the earth's penumbra. Measurements from the AE-C satellite of the solar UV radiation were used to construct a model of atmospheric attenuation. This model was found to be consistent with direct measurements of the variations in photoelectron flux as Injun 5 passed into eclipse. Applying the model to the ATS-6 data gave the time dependency of the solar illumination/photoelectron flux as the satellite was eclipsed. This relationship, when combined with the ATS-6 measurements of satellite potential, revealed a nearly linear relation between the solar illumination/photoelectron flux and the logarithm of the satellite potential.

STIC3 - Silicon Photomultiplier Timing Chip with picosecond resolution

NASA Astrophysics Data System (ADS)

Stankova, Vera; Shen, Wei; Briggl, Konrad; Chen, Huangshan; Fischer, Peter; Gil, Alejandro; Harion, Tobias; Kiworra, Volker; Munwes, Yonathan; Ritzert, Michael; Schultz-Coulon, Hans-Christian

2015-07-01

The diagnostic of pancreas and prostate cancer is a challenging task due to the background noise coming from the closer organs. The EndoToFPET-US project aims to combine the synergy between metabolic and anatomical (ultrasound) image in order to improve the precision in the tumor localization. The goal of the project is to develop a Positron Emission Tomography (PET) system that provides a time-of-flight resolution of 200 ps FWHM for improving the signal to noise ratio and further to improve the medical image quality. In order to achieve this purpose an ASIC has been designed for very high timing resolution in time-of-flight (ToF) applications. In this paper we present the ASIC performance and the first characterization measurements with the 64-channels prototype version (STiC3). Measurements are performed with LYSO scintillator crystal and a Multi Pixel Photon Counter (MPPC). Measurements with the chip show an analog-front-end stage jitter of 35 ps for the first photo-electron equivalent charge and reach 18 ps for the third photo-electron. Coincidence time resolution (CTR) of 240 ps FWHM is measured with 3.1×3.1×15 mm3 LYSO crystal and 50 μm pixel pitch MPPC. Further optimization including the Time-to-Digital Converter (TDC) non-linearity corrections and setup fine tuning are ongoing for achieving the desired CTR of 200 ps FWHM.

X-ray photoelectron spectrum and electronic properties of a noncentrosymmetric chalcopyrite compound HgGa(2)S(4): LDA, GGA, and EV-GGA.

PubMed

Reshak, Ali Hussain; Khenata, R; Kityk, I V; Plucinski, K J; Auluck, S

2009-04-30

An all electron full potential linearized augmented plane wave method has been applied for a theoretical study of the band structure, density of states, and electron charge density of a noncentrosymmetric chalcopyrite compound HgGa(2)S(4) using three different approximations for the exchange correlation potential. Our calculations show that the valence band maximum (VBM) and conduction band minimum (CBM) are located at Gamma resulting in a direct energy gap of about 2.0, 2.2, and 2.8 eV for local density approximation (LDA), generalized gradient approximation (GGA), and Engel-Vosko (EVGGA) compared to the experimental value of 2.84 eV. We notice that EVGGA shows excellent agreement with the experimental data. This agreement is attributed to the fact that the Engel-Vosko GGA formalism optimizes the corresponding potential for band structure calculations. We make a detailed comparison of the density of states deduced from the X-ray photoelectron spectra with our calculations. We find that there is a strong covalent bond between the Hg and S atoms and Ga and S atoms. The Hg-Hg, Ga-Ga, and S-S bonds are found to be weaker than the Hg-S and Ga-S bonds showing that a covalent bond exists between Hg and S atoms and Ga and S atoms.

Solving mixed integer nonlinear programming problems using spiral dynamics optimization algorithm

NASA Astrophysics Data System (ADS)

Kania, Adhe; Sidarto, Kuntjoro Adji

2016-02-01

Many engineering and practical problem can be modeled by mixed integer nonlinear programming. This paper proposes to solve the problem with modified spiral dynamics inspired optimization method of Tamura and Yasuda. Four test cases have been examined, including problem in engineering and sport. This method succeeds in obtaining the optimal result in all test cases.

Conceptual Design Optimization of an Augmented Stability Aircraft Incorporating Dynamic Response Performance Constraints

NASA Technical Reports Server (NTRS)

Welstead, Jason

2014-01-01

This research focused on incorporating stability and control into a multidisciplinary de- sign optimization on a Boeing 737-class advanced concept called the D8.2b. A new method of evaluating the aircraft handling performance using quantitative evaluation of the sys- tem to disturbances, including perturbations, continuous turbulence, and discrete gusts, is presented. A multidisciplinary design optimization was performed using the D8.2b transport air- craft concept. The con guration was optimized for minimum fuel burn using a design range of 3,000 nautical miles. Optimization cases were run using xed tail volume coecients, static trim constraints, and static trim and dynamic response constraints. A Cessna 182T model was used to test the various dynamic analysis components, ensuring the analysis was behaving as expected. Results of the optimizations show that including stability and con- trol in the design process drastically alters the optimal design, indicating that stability and control should be included in conceptual design to avoid system level penalties later in the design process.

Control Parameters Optimization Based on Co-Simulation of a Mechatronic System for an UA-Based Two-Axis Inertially Stabilized Platform.

PubMed

Zhou, Xiangyang; Zhao, Beilei; Gong, Guohao

2015-08-14

This paper presents a method based on co-simulation of a mechatronic system to optimize the control parameters of a two-axis inertially stabilized platform system (ISP) applied in an unmanned airship (UA), by which high control performance and reliability of the ISP system are achieved. First, a three-dimensional structural model of the ISP is built by using the three-dimensional parametric CAD software SOLIDWORKS(®); then, to analyze the system's kinematic and dynamic characteristics under operating conditions, dynamics modeling is conducted by using the multi-body dynamics software ADAMS™, thus the main dynamic parameters such as displacement, velocity, acceleration and reaction curve are obtained, respectively, through simulation analysis. Then, those dynamic parameters were input into the established MATLAB(®) SIMULINK(®) controller to simulate and test the performance of the control system. By these means, the ISP control parameters are optimized. To verify the methods, experiments were carried out by applying the optimized parameters to the control system of a two-axis ISP. The results show that the co-simulation by using virtual prototyping (VP) is effective to obtain optimized ISP control parameters, eventually leading to high ISP control performance.

Control Parameters Optimization Based on Co-Simulation of a Mechatronic System for an UA-Based Two-Axis Inertially Stabilized Platform

PubMed Central

Zhou, Xiangyang; Zhao, Beilei; Gong, Guohao

2015-01-01

This paper presents a method based on co-simulation of a mechatronic system to optimize the control parameters of a two-axis inertially stabilized platform system (ISP) applied in an unmanned airship (UA), by which high control performance and reliability of the ISP system are achieved. First, a three-dimensional structural model of the ISP is built by using the three-dimensional parametric CAD software SOLIDWORKS®; then, to analyze the system’s kinematic and dynamic characteristics under operating conditions, dynamics modeling is conducted by using the multi-body dynamics software ADAMS™, thus the main dynamic parameters such as displacement, velocity, acceleration and reaction curve are obtained, respectively, through simulation analysis. Then, those dynamic parameters were input into the established MATLAB® SIMULINK® controller to simulate and test the performance of the control system. By these means, the ISP control parameters are optimized. To verify the methods, experiments were carried out by applying the optimized parameters to the control system of a two-axis ISP. The results show that the co-simulation by using virtual prototyping (VP) is effective to obtain optimized ISP control parameters, eventually leading to high ISP control performance. PMID:26287210

Lithium cluster anions: photoelectron spectroscopy and ab initio calculations.

PubMed

Alexandrova, Anastassia N; Boldyrev, Alexander I; Li, Xiang; Sarkas, Harry W; Hendricks, Jay H; Arnold, Susan T; Bowen, Kit H

2011-01-28

Structural and energetic properties of small, deceptively simple anionic clusters of lithium, Li(n)(-), n = 3-7, were determined using a combination of anion photoelectron spectroscopy and ab initio calculations. The most stable isomers of each of these anions, the ones most likely to contribute to the photoelectron spectra, were found using the gradient embedded genetic algorithm program. Subsequently, state-of-the-art ab initio techniques, including time-dependent density functional theory, coupled cluster, and multireference configurational interactions methods, were employed to interpret the experimental spectra.

Photoelectron Imaging Spectroscopy as a Window to Unexpected Molecules

NASA Astrophysics Data System (ADS)

Blackstone, Christopher C.

2017-06-01

Targeting an anion with the formula CH_{3}O_{3} for exploration with photoelectron imaging spectroscopy, we determine its identity to be dihydroxymethanolate, an anion largely absent in the literature, and the conjugate base of the hypothetical species orthoformic acid. Comparing the observed photoelectron spectrum to CCSD-EOM-IP and CCSD-EOM-SF calculations completed in QChem and Franck-Condon overlap simulations in PESCAL, we are able to determine with confidence the connectivity of the atoms in this molecule.

Interatomic scattering in energy dependent photoelectron spectra of Ar clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patanen, M.; Benkoula, S.; Nicolas, C.

2015-09-28

Soft X-ray photoelectron spectra of Ar 2p levels of atomic argon and argon clusters are recorded over an extended range of photon energies. The Ar 2p intensity ratios between atomic argon and clusters’ surface and bulk components reveal oscillations similar to photoelectron extended X-ray absorption fine structure signal (PEXAFS). We demonstrate here that this technique allows us to analyze separately the PEXAFS signals from surface and bulk sites of free-standing, neutral clusters, revealing a bond contraction at the surface.

Photoelectron spectroscopy of nitromethane anion clusters

NASA Astrophysics Data System (ADS)

Pruitt, Carrie Jo M.; Albury, Rachael M.; Goebbert, Daniel J.

2016-08-01

Nitromethane anion and nitromethane dimer, trimer, and hydrated cluster anions were studied by photoelectron spectroscopy. Vertical detachment energies, estimated electron affinities, and solvation energies were obtained from the photoelectron spectra. Cluster structures were investigated using theoretical calculations. Predicted detachment energies agreed with experiment. Calculations show water binds to nitromethane anion through two hydrogen bonds. The dimer has a non-linear structure with a single ionic Csbnd H⋯O hydrogen bond. The trimer has two different solvent interactions, but both involve the weak Csbnd H⋯O hydrogen bond.

Three-dimensional data-tracking dynamic optimization simulations of human locomotion generated by direct collocation.

PubMed

Lin, Yi-Chung; Pandy, Marcus G

2017-07-05

The aim of this study was to perform full-body three-dimensional (3D) dynamic optimization simulations of human locomotion by driving a neuromusculoskeletal model toward in vivo measurements of body-segmental kinematics and ground reaction forces. Gait data were recorded from 5 healthy participants who walked at their preferred speeds and ran at 2m/s. Participant-specific data-tracking dynamic optimization solutions were generated for one stride cycle using direct collocation in tandem with an OpenSim-MATLAB interface. The body was represented as a 12-segment, 21-degree-of-freedom skeleton actuated by 66 muscle-tendon units. Foot-ground interaction was simulated using six contact spheres under each foot. The dynamic optimization problem was to find the set of muscle excitations needed to reproduce 3D measurements of body-segmental motions and ground reaction forces while minimizing the time integral of muscle activations squared. Direct collocation took on average 2.7±1.0h and 2.2±1.6h of CPU time, respectively, to solve the optimization problems for walking and running. Model-computed kinematics and foot-ground forces were in good agreement with corresponding experimental data while the calculated muscle excitation patterns were consistent with measured EMG activity. The results demonstrate the feasibility of implementing direct collocation on a detailed neuromusculoskeletal model with foot-ground contact to accurately and efficiently generate 3D data-tracking dynamic optimization simulations of human locomotion. The proposed method offers a viable tool for creating feasible initial guesses needed to perform predictive simulations of movement using dynamic optimization theory. The source code for implementing the model and computational algorithm may be downloaded at http://simtk.org/home/datatracking. Copyright © 2017 Elsevier Ltd. All rights reserved.

Optimal Control Strategy Design Based on Dynamic Programming for a Dual-Motor Coupling-Propulsion System

PubMed Central

Zhang, Shuo; Zhang, Chengning; Han, Guangwei; Wang, Qinghui

2014-01-01

A dual-motor coupling-propulsion electric bus (DMCPEB) is modeled, and its optimal control strategy is studied in this paper. The necessary dynamic features of energy loss for subsystems is modeled. Dynamic programming (DP) technique is applied to find the optimal control strategy including upshift threshold, downshift threshold, and power split ratio between the main motor and auxiliary motor. Improved control rules are extracted from the DP-based control solution, forming near-optimal control strategies. Simulation results demonstrate that a significant improvement in reducing energy loss due to the dual-motor coupling-propulsion system (DMCPS) running is realized without increasing the frequency of the mode switch. PMID:25540814

Optimal control strategy design based on dynamic programming for a dual-motor coupling-propulsion system.

PubMed

Zhang, Shuo; Zhang, Chengning; Han, Guangwei; Wang, Qinghui

2014-01-01

A dual-motor coupling-propulsion electric bus (DMCPEB) is modeled, and its optimal control strategy is studied in this paper. The necessary dynamic features of energy loss for subsystems is modeled. Dynamic programming (DP) technique is applied to find the optimal control strategy including upshift threshold, downshift threshold, and power split ratio between the main motor and auxiliary motor. Improved control rules are extracted from the DP-based control solution, forming near-optimal control strategies. Simulation results demonstrate that a significant improvement in reducing energy loss due to the dual-motor coupling-propulsion system (DMCPS) running is realized without increasing the frequency of the mode switch.

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection.

PubMed

Lehmann, C Stefan; Ram, N Bhargava; Powis, Ivan; Janssen, Maurice H M

2013-12-21

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flight mass spectra. The coincident photoelectron spectra of the parent camphor ion and the various fragment ions are the same, so it can be concluded that fragmentation of camphor happens after ionization. We discuss the forward-backward asymmetry in the photoelectron angular distribution which is expressed in Legendre polynomials with moments up to order six. Furthermore, we present a method, similar to one-photon electron circular dichroism, to quantify the strength of the chiral electron asymmetry in a single parameter. The circular dichroism in the photoelectron angular distribution of camphor is measured to be 8% at 400 nm. The electron circular dichroism using femtosecond multiphoton excitation is of opposite sign and about 60% larger than the electron dichroism observed before in near-threshold one-photon ionization with synchrotron excitation. We interpret our multiphoton ionization as being resonant at the two-photon level with the 3s and 3p Rydberg states of camphor. Theoretical calculations are presented that model the photoelectron angular distribution from a prealigned camphor molecule using density functional theory and continuum multiple scattering X alpha photoelectron scattering calculations. Qualitative agreement is observed between the experimental results and the theoretical calculations of the Legendre moments representing the angular distribution for the two enantiomers. The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.

Imaging photoelectron circular dichroism of chiral molecules by femtosecond multiphoton coincidence detection

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lehmann, C. Stefan; Ram, N. Bhargava; Janssen, Maurice H. M., E-mail: m.h.m.janssen@vu.nl

2013-12-21

Here, we provide a detailed account of novel experiments employing electron-ion coincidence imaging to discriminate chiral molecules. The full three-dimensional angular scattering distribution of electrons is measured after photoexcitation with either left or right circular polarized light. The experiment is performed using a simplified photoelectron-photoion coincidence imaging setup employing only a single particle imaging detector. Results are reported applying this technique to enantiomers of the chiral molecule camphor after three-photon ionization by circularly polarized femtosecond laser pulses at 400 nm and 380 nm. The electron-ion coincidence imaging provides the photoelectron spectrum of mass-selected ions that are observed in the time-of-flightmore » mass spectra. The coincident photoelectron spectra of the parent camphor ion and the various fragment ions are the same, so it can be concluded that fragmentation of camphor happens after ionization. We discuss the forward-backward asymmetry in the photoelectron angular distribution which is expressed in Legendre polynomials with moments up to order six. Furthermore, we present a method, similar to one-photon electron circular dichroism, to quantify the strength of the chiral electron asymmetry in a single parameter. The circular dichroism in the photoelectron angular distribution of camphor is measured to be 8% at 400 nm. The electron circular dichroism using femtosecond multiphoton excitation is of opposite sign and about 60% larger than the electron dichroism observed before in near-threshold one-photon ionization with synchrotron excitation. We interpret our multiphoton ionization as being resonant at the two-photon level with the 3s and 3p Rydberg states of camphor. Theoretical calculations are presented that model the photoelectron angular distribution from a prealigned camphor molecule using density functional theory and continuum multiple scattering X alpha photoelectron scattering calculations. Qualitative agreement is observed between the experimental results and the theoretical calculations of the Legendre moments representing the angular distribution for the two enantiomers. The electron-ion coincidence technique using multiphoton ionization opens new directions in table-top analytical mass-spectrometric applications of mixtures of chiral molecules.« less

Recursive multibody dynamics and discrete-time optimal control

NASA Technical Reports Server (NTRS)

Deleuterio, G. M. T.; Damaren, C. J.

1989-01-01

A recursive algorithm is developed for the solution of the simulation dynamics problem for a chain of rigid bodies. Arbitrary joint constraints are permitted, that is, joints may allow translational and/or rotational degrees of freedom. The recursive procedure is shown to be identical to that encountered in a discrete-time optimal control problem. For each relevant quantity in the multibody dynamics problem, there exists an analog in the context of optimal control. The performance index that is minimized in the control problem is identified as Gibbs' function for the chain of bodies.

Comparison of kinematic and dynamic leg trajectory optimization techniques for biped robot locomotion

NASA Astrophysics Data System (ADS)

Khusainov, R.; Klimchik, A.; Magid, E.

2017-01-01

The paper presents comparison analysis of two approaches in defining leg trajectories for biped locomotion. The first one operates only with kinematic limitations of leg joints and finds the maximum possible locomotion speed for given limits. The second approach defines leg trajectories from the dynamic stability point of view and utilizes ZMP criteria. We show that two methods give different trajectories and demonstrate that trajectories based on pure dynamic optimization cannot be realized due to joint limits. Kinematic optimization provides unstable solution which can be balanced by upper body movement.

Optimal Least-Squares Unidimensional Scaling: Improved Branch-and-Bound Procedures and Comparison to Dynamic Programming

ERIC Educational Resources Information Center

Brusco, Michael J.; Stahl, Stephanie

2005-01-01

There are two well-known methods for obtaining a guaranteed globally optimal solution to the problem of least-squares unidimensional scaling of a symmetric dissimilarity matrix: (a) dynamic programming, and (b) branch-and-bound. Dynamic programming is generally more efficient than branch-and-bound, but the former is limited to matrices with…

Dynamic regime marginal structural mean models for estimation of optimal dynamic treatment regimes, Part I: main content.

PubMed

Orellana, Liliana; Rotnitzky, Andrea; Robins, James M

2010-01-01

Dynamic treatment regimes are set rules for sequential decision making based on patient covariate history. Observational studies are well suited for the investigation of the effects of dynamic treatment regimes because of the variability in treatment decisions found in them. This variability exists because different physicians make different decisions in the face of similar patient histories. In this article we describe an approach to estimate the optimal dynamic treatment regime among a set of enforceable regimes. This set is comprised by regimes defined by simple rules based on a subset of past information. The regimes in the set are indexed by a Euclidean vector. The optimal regime is the one that maximizes the expected counterfactual utility over all regimes in the set. We discuss assumptions under which it is possible to identify the optimal regime from observational longitudinal data. Murphy et al. (2001) developed efficient augmented inverse probability weighted estimators of the expected utility of one fixed regime. Our methods are based on an extension of the marginal structural mean model of Robins (1998, 1999) which incorporate the estimation ideas of Murphy et al. (2001). Our models, which we call dynamic regime marginal structural mean models, are specially suitable for estimating the optimal treatment regime in a moderately small class of enforceable regimes of interest. We consider both parametric and semiparametric dynamic regime marginal structural models. We discuss locally efficient, double-robust estimation of the model parameters and of the index of the optimal treatment regime in the set. In a companion paper in this issue of the journal we provide proofs of the main results.

Review of dynamic optimization methods in renewable natural resource management

USGS Publications Warehouse

Williams, B.K.

1989-01-01

In recent years, the applications of dynamic optimization procedures in natural resource management have proliferated. A systematic review of these applications is given in terms of a number of optimization methodologies and natural resource systems. The applicability of the methods to renewable natural resource systems are compared in terms of system complexity, system size, and precision of the optimal solutions. Recommendations are made concerning the appropriate methods for certain kinds of biological resource problems.

Stochastic dynamics and combinatorial optimization

NASA Astrophysics Data System (ADS)

Ovchinnikov, Igor V.; Wang, Kang L.

2017-11-01

Natural dynamics is often dominated by sudden nonlinear processes such as neuroavalanches, gamma-ray bursts, solar flares, etc., that exhibit scale-free statistics much in the spirit of the logarithmic Ritcher scale for earthquake magnitudes. On phase diagrams, stochastic dynamical systems (DSs) exhibiting this type of dynamics belong to the finite-width phase (N-phase for brevity) that precedes ordinary chaotic behavior and that is known under such names as noise-induced chaos, self-organized criticality, dynamical complexity, etc. Within the recently proposed supersymmetric theory of stochastic dynamics, the N-phase can be roughly interpreted as the noise-induced “overlap” between integrable and chaotic deterministic dynamics. As a result, the N-phase dynamics inherits the properties of the both. Here, we analyze this unique set of properties and conclude that the N-phase DSs must naturally be the most efficient optimizers: on one hand, N-phase DSs have integrable flows with well-defined attractors that can be associated with candidate solutions and, on the other hand, the noise-induced attractor-to-attractor dynamics in the N-phase is effectively chaotic or aperiodic so that a DS must avoid revisiting solutions/attractors thus accelerating the search for the best solution. Based on this understanding, we propose a method for stochastic dynamical optimization using the N-phase DSs. This method can be viewed as a hybrid of the simulated and chaotic annealing methods. Our proposition can result in a new generation of hardware devices for efficient solution of various search and/or combinatorial optimization problems.

Titan's plasma interaction: photoelectrons and negative ions

NASA Astrophysics Data System (ADS)

Coates, Coates; Welbrock, Anne; Desai, Ravi; Waite, Hunter

2016-06-01

We present a review of some of the most important results from the CAPS electron spectrometer.These include the role of photoelectrons and polar wind escape processes, and remarkable negative ion observations.

Classifying EEG for Brain-Computer Interface: Learning Optimal Filters for Dynamical System Features

PubMed Central

Song, Le; Epps, Julien

2007-01-01

Classification of multichannel EEG recordings during motor imagination has been exploited successfully for brain-computer interfaces (BCI). In this paper, we consider EEG signals as the outputs of a networked dynamical system (the cortex), and exploit synchronization features from the dynamical system for classification. Herein, we also propose a new framework for learning optimal filters automatically from the data, by employing a Fisher ratio criterion. Experimental evaluations comparing the proposed dynamical system features with the CSP and the AR features reveal their competitive performance during classification. Results also show the benefits of employing the spatial and the temporal filters optimized using the proposed learning approach. PMID:18364986

An engineering optimization method with application to STOL-aircraft approach and landing trajectories

NASA Technical Reports Server (NTRS)

Jacob, H. G.

1972-01-01

An optimization method has been developed that computes the optimal open loop inputs for a dynamical system by observing only its output. The method reduces to static optimization by expressing the inputs as series of functions with parameters to be optimized. Since the method is not concerned with the details of the dynamical system to be optimized, it works for both linear and nonlinear systems. The method and the application to optimizing longitudinal landing paths for a STOL aircraft with an augmented wing are discussed. Noise, fuel, time, and path deviation minimizations are considered with and without angle of attack, acceleration excursion, flight path, endpoint, and other constraints.

Dynamic programming for optimization of timber production and grazing in ponderosa pine

Treesearch

Kurt H. Riitters; J. Douglas Brodie; David W. Hann

1982-01-01

Dynamic programming procedures are presented for optimizing thinning and rotation of even-aged ponderosa pine by using the four descriptors: age, basal area, number of trees, and time since thinning. Because both timber yield and grazing yield are functions of stand density, the two outputs-forage and timber-can both be optimized. The soil expectation values for single...

A photoelectron spectroscopic investigation of vinyl fluoride (C2H3F): the HeI, threshold and CIS photoelectron spectroscopy

NASA Astrophysics Data System (ADS)

Locht, R.; Leyh, B.; Dehareng, D.; Hottmann, K.; Baumgärtel, H.

2010-01-01

The threshold photoelectron spectrum (TPES) and the constant ion state (CIS) spectra of the individual ionic states of C2H3F have been recorded using synchrotron radiation. For comparison a well-resolved HeI photoelectron spectrum (HeI-PES) has also been measured and analysed in detail. The TPES has been measured between 9.5 eV and 35 eV photon energy. Numerous vibrational structures, reported for the first time, observed in the ground state and the six excited states of the cation are analysed. Quantum chemical calculations have been performed and provide strong support to the assignments. State-selected CIS spectra highlighted the major importance of autoionization for the production of almost all ionized states of C2H3F observed in this work.

Study of Nb2O(y) (y = 2-5) anion and neutral clusters using anion photoelectron spectroscopy and density functional theory calculations.

PubMed

Mann, Jennifer E; Waller, Sarah E; Rothgeb, David W; Jarrold, Caroline Chick

2011-09-14

A study combining anion photoelectron spectroscopy and density functional theory calculations on the transition metal suboxide series, Nb(2)O(y)(-) (y = 2-5), is described. Photoelectron spectra of the clusters are obtained, and Franck-Condon simulations using calculated anion and neutral structures and frequencies are used to evaluate the calculations and assign transitions observed in the spectra. The spectra, several of which exhibit partially resolved vibrational structure, show an increase in electron affinity with increasing cluster oxidation state. Hole-burning experiments suggest that the photoelectron spectra of both Nb(2)O(2)(-) and Nb(2)O(3)(-) have contributions from more than one structural isomer. Reasonable agreement between experiment and computational results is found among all oxides. © 2011 American Institute of Physics

Rocket measurements of conjugate photoelectrons during the total solar eclipse of 7 March 1970 over Wallops Island.

NASA Technical Reports Server (NTRS)

Maier, E. J.; Narasinga Rao, B. C.

1972-01-01

Results of measurements made with a retarding potential analyzer on a Nike-Tomahawk rocket during the totality of the solar eclipse, showing definite evidence for the existence of photoelectrons from the conjugate hemisphere. Photoelectrons are observed in the altitude range from 120 to 260 km. The observed flux in the energy range from 2 to 30 eV is relatively constant above about 200 km, but decreased below that altitude. The flux of 5-eV energy electrons above 200 km altitude is about 10 to the 7th power electrons/cm/sec/eV. Higher-energy electrons were also observed, and it is possible that the energy content of these observed fluxes of conjugate-point photoelectrons is sufficient to maintain the observed electron densities and temperatures during the total eclipse.

Photoelectric dust levitation around airless bodies revised using realistic photoelectron velocity distributions

NASA Astrophysics Data System (ADS)

Senshu, H.; Kimura, H.; Yamamoto, T.; Wada, K.; Kobayashi, M.; Namiki, N.; Matsui, T.

2015-10-01

The velocity distribution function of photoelectrons from a surface exposed to solar UV radiation is fundamental to the electrostatic status of the surface. There is one and only one laboratory measurement of photoelectron emission from astronomically relevant material, but the energy distribution function was measured only in the emission angle from the normal to the surface of 0 to about π / 4. Therefore, the measured distribution is not directly usable to estimate the vertical structure of a photoelectric sheath above the surface. In this study, we develop a new analytical method to calculate an angle-resolved velocity distribution function of photoelectrons from the laboratory measurement data. We find that the photoelectric current and yield for lunar surface fines measured in a laboratory have been underestimated by a factor of two. We apply our new energy distribution function of photoelectrons to model the formation of photoelectric sheath above the surface of asteroid 433 Eros. Our model shows that a 0.1 μm-radius dust grain can librate above the surface of asteroid 433 Eros regardless of its launching velocity. In addition, a 0.5 μm grain can hover over the surface if the grain was launched at a velocity slower than 0.4 m/s, which is a more stringent condition for levitation than previous studies. However, a lack of high-energy data on the photoelectron energy distribution above 6 eV prevents us from firmly placing a constraint on the levitation condition.

Dynamic Aberration Correction for Conformal Window of High-Speed Aircraft Using Optimized Model-Based Wavefront Sensorless Adaptive Optics.

PubMed

Dong, Bing; Li, Yan; Han, Xin-Li; Hu, Bin

2016-09-02

For high-speed aircraft, a conformal window is used to optimize the aerodynamic performance. However, the local shape of the conformal window leads to large amounts of dynamic aberrations varying with look angle. In this paper, deformable mirror (DM) and model-based wavefront sensorless adaptive optics (WSLAO) are used for dynamic aberration correction of an infrared remote sensor equipped with a conformal window and scanning mirror. In model-based WSLAO, aberration is captured using Lukosz mode, and we use the low spatial frequency content of the image spectral density as the metric function. Simulations show that aberrations induced by the conformal window are dominated by some low-order Lukosz modes. To optimize the dynamic correction, we can only correct dominant Lukosz modes and the image size can be minimized to reduce the time required to compute the metric function. In our experiment, a 37-channel DM is used to mimic the dynamic aberration of conformal window with scanning rate of 10 degrees per second. A 52-channel DM is used for correction. For a 128 × 128 image, the mean value of image sharpness during dynamic correction is 1.436 × 10(-5) in optimized correction and is 1.427 × 10(-5) in un-optimized correction. We also demonstrated that model-based WSLAO can achieve convergence two times faster than traditional stochastic parallel gradient descent (SPGD) method.

Dynamic positioning configuration and its first-order optimization

NASA Astrophysics Data System (ADS)

Xue, Shuqiang; Yang, Yuanxi; Dang, Yamin; Chen, Wu

2014-02-01

Traditional geodetic network optimization deals with static and discrete control points. The modern space geodetic network is, on the other hand, composed of moving control points in space (satellites) and on the Earth (ground stations). The network configuration composed of these facilities is essentially dynamic and continuous. Moreover, besides the position parameter which needs to be estimated, other geophysical information or signals can also be extracted from the continuous observations. The dynamic (continuous) configuration of the space network determines whether a particular frequency of signals can be identified by this system. In this paper, we employ the functional analysis and graph theory to study the dynamic configuration of space geodetic networks, and mainly focus on the optimal estimation of the position and clock-offset parameters. The principle of the D-optimization is introduced in the Hilbert space after the concept of the traditional discrete configuration is generalized from the finite space to the infinite space. It shows that the D-optimization developed in the discrete optimization is still valid in the dynamic configuration optimization, and this is attributed to the natural generalization of least squares from the Euclidean space to the Hilbert space. Then, we introduce the principle of D-optimality invariance under the combination operation and rotation operation, and propose some D-optimal simplex dynamic configurations: (1) (Semi) circular configuration in 2-dimensional space; (2) the D-optimal cone configuration and D-optimal helical configuration which is close to the GPS constellation in 3-dimensional space. The initial design of GPS constellation can be approximately treated as a combination of 24 D-optimal helixes by properly adjusting the ascending node of different satellites to realize a so-called Walker constellation. In the case of estimating the receiver clock-offset parameter, we show that the circular configuration, the symmetrical cone configuration and helical curve configuration are still D-optimal. It shows that the given total observation time determines the optimal frequency (repeatability) of moving known points and vice versa, and one way to improve the repeatability is to increase the rotational speed. Under the Newton's law of motion, the frequency of satellite motion determines the orbital altitude. Furthermore, we study three kinds of complex dynamic configurations, one of which is the combination of D-optimal cone configurations and a so-called Walker constellation composed of D-optimal helical configuration, the other is the nested cone configuration composed of n cones, and the last is the nested helical configuration composed of n orbital planes. It shows that an effective way to achieve high coverage is to employ the configuration composed of a certain number of moving known points instead of the simplex configuration (such as D-optimal helical configuration), and one can use the D-optimal simplex solutions or D-optimal complex configurations in any combination to achieve powerful configurations with flexile coverage and flexile repeatability. Alternately, how to optimally generate and assess the discrete configurations sampled from the continuous one is discussed. The proposed configuration optimization framework has taken the well-known regular polygons (such as equilateral triangle and quadrangular) in two-dimensional space and regular polyhedrons (regular tetrahedron, cube, regular octahedron, regular icosahedron, or regular dodecahedron) into account. It shows that the conclusions made by the proposed technique are more general and no longer limited by different sampling schemes. By the conditional equation of D-optimal nested helical configuration, the relevance issues of GNSS constellation optimization are solved and some examples are performed by GPS constellation to verify the validation of the newly proposed optimization technique. The proposed technique is potentially helpful in maintenance and quadratic optimization of single GNSS of which the orbital inclination and the orbital altitude change under the precession, as well as in optimally nesting GNSSs to perform global homogeneous coverage of the Earth.

Energy Optimal Path Planning: Integrating Coastal Ocean Modelling with Optimal Control

NASA Astrophysics Data System (ADS)

Subramani, D. N.; Haley, P. J., Jr.; Lermusiaux, P. F. J.

2016-02-01

A stochastic optimization methodology is formulated for computing energy-optimal paths from among time-optimal paths of autonomous vehicles navigating in a dynamic flow field. To set up the energy optimization, the relative vehicle speed and headings are considered to be stochastic, and new stochastic Dynamically Orthogonal (DO) level-set equations that govern their stochastic time-optimal reachability fronts are derived. Their solution provides the distribution of time-optimal reachability fronts and corresponding distribution of time-optimal paths. An optimization is then performed on the vehicle's energy-time joint distribution to select the energy-optimal paths for each arrival time, among all stochastic time-optimal paths for that arrival time. The accuracy and efficiency of the DO level-set equations for solving the governing stochastic level-set reachability fronts are quantitatively assessed, including comparisons with independent semi-analytical solutions. Energy-optimal missions are studied in wind-driven barotropic quasi-geostrophic double-gyre circulations, and in realistic data-assimilative re-analyses of multiscale coastal ocean flows. The latter re-analyses are obtained from multi-resolution 2-way nested primitive-equation simulations of tidal-to-mesoscale dynamics in the Middle Atlantic Bight and Shelbreak Front region. The effects of tidal currents, strong wind events, coastal jets, and shelfbreak fronts on the energy-optimal paths are illustrated and quantified. Results showcase the opportunities for longer-duration missions that intelligently utilize the ocean environment to save energy, rigorously integrating ocean forecasting with optimal control of autonomous vehicles.

Dynamic optimization of distributed biological systems using robust and efficient numerical techniques.

PubMed

Vilas, Carlos; Balsa-Canto, Eva; García, Maria-Sonia G; Banga, Julio R; Alonso, Antonio A

2012-07-02

Systems biology allows the analysis of biological systems behavior under different conditions through in silico experimentation. The possibility of perturbing biological systems in different manners calls for the design of perturbations to achieve particular goals. Examples would include, the design of a chemical stimulation to maximize the amplitude of a given cellular signal or to achieve a desired pattern in pattern formation systems, etc. Such design problems can be mathematically formulated as dynamic optimization problems which are particularly challenging when the system is described by partial differential equations.This work addresses the numerical solution of such dynamic optimization problems for spatially distributed biological systems. The usual nonlinear and large scale nature of the mathematical models related to this class of systems and the presence of constraints on the optimization problems, impose a number of difficulties, such as the presence of suboptimal solutions, which call for robust and efficient numerical techniques. Here, the use of a control vector parameterization approach combined with efficient and robust hybrid global optimization methods and a reduced order model methodology is proposed. The capabilities of this strategy are illustrated considering the solution of a two challenging problems: bacterial chemotaxis and the FitzHugh-Nagumo model. In the process of chemotaxis the objective was to efficiently compute the time-varying optimal concentration of chemotractant in one of the spatial boundaries in order to achieve predefined cell distribution profiles. Results are in agreement with those previously published in the literature. The FitzHugh-Nagumo problem is also efficiently solved and it illustrates very well how dynamic optimization may be used to force a system to evolve from an undesired to a desired pattern with a reduced number of actuators. The presented methodology can be used for the efficient dynamic optimization of generic distributed biological systems.

Band Alignment for Rectification and Tunneling Effects in Al2O3 Atomic-Layer-Deposited on Back Contact for CdTe Solar Cell.

PubMed

Su, Yantao; Xin, Chao; Feng, Yancong; Lin, Qinxian; Wang, Xinwei; Liang, Jun; Zheng, Jiaxin; Lin, Yuan; Pan, Feng

2016-10-11

The present work intends to explain why ultrathin Al 2 O 3 atomic-layer-deposited (ALD) on the back contact with rectification and tunneling effects can significantly improve the performance of CdTe solar cells in our previous work [ Liang , J. ; et al. Appl. Phys. Lett. 2015 , 107 , 013907 ]. Herein, we further study the mechanism through establishing the interfacial energy band diagram configuration of the ALD Al 2 O 3 /Cu x Te by experiment of X-ray photoelectron spectroscopy and first-principles calculations and conclude to find the band alignment with optimized layer thickness (about 1 nm ALD Al 2 O 3 ) as the key factor for rectification and tunneling effects.

Depth elemental characterization of 1D self-aligned TiO2 nanotubes using calibrated radio frequency glow discharge optical emission spectroscopy (GDOES)

NASA Astrophysics Data System (ADS)

Mohajernia, Shiva; Mazare, Anca; Hwang, Imgon; Gaiaschi, Sofia; Chapon, Patrick; Hildebrand, Helga; Schmuki, Patrik

2018-06-01

In this work we study the depth composition of anodic TiO2 nanotube layers. We use elemental depth profiling with Glow Discharge Optical Emission Spectroscopy and calibrate the results of this technique with X-ray photoelectron spectroscopy (XPS) and energy dispersive spectroscopy (EDS). We establish optimized sputtering conditions for nanotubular structures using the pulsed RF mode, which causes minimized structural damage during the depth profiling of the nanotubular structures. This allows to obtain calibrated sputter rates that account for the nanotubular "porous" morphology. Most importantly, sputter-artifact free compositional profiles of these high aspect ratio 3D structures are obtained, as well as, in combination with SEM, elegant depth sectional imaging.

Synthesis and Characterization of the Nano-TiO2 Visible Light Photocatalysts: Vanadium Surface Doping Modification

NASA Astrophysics Data System (ADS)

Wang, Xia; Li, Zongbao; Jia, Lichao; Xing, Xiaobo

2018-05-01

A simple strategy to greatly increase the photocatalytic ability of nanocrystalline anatase has been put forward to fabricate efficient TiO2-based photocatalysts under visible irradiation. By surface modification with V ion, samples with different ratios were synthesized by using an incipient wetness impregnation method. The as-prepared specimens were characterized using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and UV-vis diffuse reflectance spectroscopy. The photocatalytic activities were evaluated by using methylene blue degradations. Meanwhile, the optimized loading structure and electronic structures were calculated by using the density function theory (DFT). This work should provide a practical route to reasonably design and synthesize high-performance TiO2-based nanostructured photocatalysts.

Temperature- and Intensity-Dependent Photovoltaic Measurements to Identify Dominant Recombination Pathways

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brandt, Riley E.; Mangan, Niall M.; Li, Jian V.

2016-11-21

In novel photovoltaic absorbers, it is often difficult to assess the root causes of low open-circuit voltages, which may be due to bulk recombination or sub-optimal contacts. In the present work, we discuss the role of temperature- and illumination-dependent device electrical measurements in quantifying and distinguishing these performance losses - in particular, for determining bounds on interface recombination velocities, band alignment, and minority carrier lifetime. We assess the accuracy of this approach by direct comparison to photoelectron spectroscopy. Then, we demonstrate how more computationally intensive model parameter fitting approaches can draw more insights from this broad measurement space. We applymore » this measurement and modeling approach to high-performance III-V and thin-film chalcogenide devices.« less

Comparison of trimethylgallium and triethylgallium as “Ga” source materials for the growth of ultrathin GaN films on Si (100) substrates via hollow-cathode plasma-assisted atomic layer deposition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alevli, Mustafa, E-mail: mustafaalevli@marmara.edu.tr; Haider, Ali; Kizir, Seda

2016-01-15

GaN films grown by hollow cathode plasma-assisted atomic layer deposition using trimethylgallium (TMG) and triethylgallium (TEG) as gallium precursors are compared. Optimized and saturated TMG/TEG pulse widths were used in order to study the effect of group-III precursors. The films were characterized by grazing incidence x-ray diffraction, atomic force microscopy, x-ray photoelectron spectroscopy, and spectroscopic ellipsometry. Refractive index follows the same trend of crystalline quality, mean grain, and crystallite sizes. GaN layers grown using TMG precursor exhibited improved structural and optical properties when compared to GaN films grown with TEG precursor.

Estimating the arrival times of photon-limited laser pulses in the presence of shot and speckle noise

NASA Technical Reports Server (NTRS)

Abshire, James B.; Mcgarry, Jan F.

1987-01-01

Maximum-likelihood (ML) receivers are frequently used to optimize the timing performance of laser-ranging and laser-altimetry systems in the presence of shot and speckle noise. Monte Carlo method was used to examine ML-receiver performance with return signals in the 10-5000-photoelectron (pe) range. The simulations were performed for shot noise only and for shot and speckle noise. The results agree with previous theory for signal strengths greater than about 100 pe's but show that the theory can significantly underestimate timing errors for weaker received signals. Sharp high-bandwidth features in the detected signals are shown to improve timing performance only if their signal levels are greater than 4-5 pe's.

Focusing light through dynamical samples using fast continuous wavefront optimization.

PubMed

Blochet, B; Bourdieu, L; Gigan, S

2017-12-01

We describe a fast continuous optimization wavefront shaping system able to focus light through dynamic scattering media. A micro-electro-mechanical system-based spatial light modulator, a fast photodetector, and field programmable gate array electronics are combined to implement a continuous optimization of a wavefront with a single-mode optimization rate of 4.1 kHz. The system performances are demonstrated by focusing light through colloidal solutions of TiO 2 particles in glycerol with tunable temporal stability.

An inverse dynamics approach to trajectory optimization for an aerospace plane

NASA Technical Reports Server (NTRS)

Lu, Ping

1992-01-01

An inverse dynamics approach for trajectory optimization is proposed. This technique can be useful in many difficult trajectory optimization and control problems. The application of the approach is exemplified by ascent trajectory optimization for an aerospace plane. Both minimum-fuel and minimax types of performance indices are considered. When rocket augmentation is available for ascent, it is shown that accurate orbital insertion can be achieved through the inverse control of the rocket in the presence of disturbances.

Integrated Network Decompositions and Dynamic Programming for Graph Optimization (INDDGO)

DOE Office of Scientific and Technical Information (OSTI.GOV)

The INDDGO software package offers a set of tools for finding exact solutions to graph optimization problems via tree decompositions and dynamic programming algorithms. Currently the framework offers serial and parallel (distributed memory) algorithms for finding tree decompositions and solving the maximum weighted independent set problem. The parallel dynamic programming algorithm is implemented on top of the MADNESS task-based runtime.

Do homologous thermophilic-mesophilic proteins exhibit similar structures and dynamics at optimal growth temperatures? A molecular dynamics simulation study.

PubMed

Basu, Sohini; Sen, Srikanta

2013-02-25

Structure and dynamics both are known to be important for the activity of a protein. A fundamental question is whether a thermophilic protein and its mesophilic homologue exhibit similar dynamics at their respective optimal growth temperatures. We have addressed this question by performing molecular dynamics (MD) simulations of a natural mesophilic-thermophilic homologue pair at their respective optimal growth temperatures to compare their structural, dynamical, and solvent properties. The MD simulations were done in explicit aqueous solvent under periodic boundary and constant pressure and temperature (CPT) conditions and continued for 10.0 ns using the same protocol for the two proteins, excepting the temperatures. The trajectories were analyzed to compare the properties of the two proteins. Results indicated that the dynamical behaviors of the two proteins at the respective optimal growth temperatures were remarkably similar. For the common residues in the thermophilic protein, the rms fluctuations have a general trend to be slightly higher compared to that in the mesophilic counterpart. Lindemann parameter values indicated that only a few residues exhibited solid-like dynamics while the protein as a whole appeared as a molten globule in each case. Interestingly, the water-water interaction was found to be strikingly similar in spite of the difference in temperatures while, the protein-water interaction was significantly different in the two simulations.

An analytical investigation: Effect of solar wind on lunar photoelectron sheath

NASA Astrophysics Data System (ADS)

Mishra, S. K.; Misra, Shikha

2018-02-01

The formation of a photoelectron sheath over the lunar surface and subsequent dust levitation, under the influence of solar wind plasma and continuous solar radiation, has been analytically investigated. The photoelectron sheath characteristics have been evaluated using the Poisson equation configured with population density contributions from half Fermi-Dirac distribution of the photoemitted electrons and simplified Maxwellian statistics of solar wind plasma; as a consequence, altitude profiles for electric potential, electric field, and population density within the photoelectron sheath have been derived. The expression for the accretion rate of sheath electrons over the levitated spherical particles using anisotropic photoelectron flux has been derived, which has been further utilized to characterize the charging of levitating fine particles in the lunar sheath along with other constituent photoemission and solar wind fluxes. This estimate of particle charge has been further manifested with lunar sheath characteristics to evaluate the altitude profile of the particle size exhibiting levitation. The inclusion of solar wind flux into analysis is noticed to reduce the sheath span and altitude of the particle levitation; the dependence of the sheath structure and particle levitation on the solar wind plasma parameters has been discussed and graphically presented.

X-ray Photoelectron Spectroscopy of High-κ Dielectrics

NASA Astrophysics Data System (ADS)

Mathew, A.; Demirkan, K.; Wang, C.-G.; Wilk, G. D.; Watson, D. G.; Opila, R. L.

2005-09-01

Photoelectron spectroscopy is a powerful technique for the analysis of gate dielectrics because it can determine the elemental composition, the chemical states, and the compositional depth profiles non-destructively. The sampling depth, determined by the escape depth of the photoelectrons, is comparable to the thickness of current gate oxides. A maximum entropy algorithm was used to convert photoelectron collection angle dependence of the spectra to compositional depth profiles. A nitrided hafnium silicate film is used to demonstrate the utility of the technique. The algorithm balances deviations from a simple assumed depth profile against a calculated depth profile that best fits the angular dependence of the photoelectron spectra. A flow chart of the program is included in this paper. The development of the profile is also shown as the program is iterated. Limitations of the technique include the electron escape depths and elemental sensitivity factors used to calculate the profile. The technique is also limited to profiles that extend to the depth of approximately twice the escape depth. These limitations restrict conclusions to comparison among a family of similar samples. Absolute conclusions about depths and concentrations must be used cautiously. Current work to improve the algorithm is also described.

Photoelectron Spectroscopy Study of Quinonimides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hossain, Ekram; Deng, Shihu M.; Gozem, Samer

Structures and energetics of o-, m- and p-quinonimide anions (OC6H4N) and quinoniminyl radicals have been investigated by using negative ion photoelectron spectroscopy. Modeling of the photoelectron spectrum of the ortho isomer shows that the ground state of the anion is a triplet, while the quinoniminyl radical has a doublet ground state with a doublet-quartet splitting of 35.5 kcal/mol. The para radical has doublet ground state, but a band for a quartet state is missing from the photoelectron spectrum indicating that the anion has a singlet ground state, in contrast to previously reported calculations. The theoretical modeling is revisited here, andmore » it is shown that accurate predictions for the electronic structure of the para quinonimide anion require both an accurate account of electron correlation and a sufficiently diffuse basis set. Electron affinities of o- and p-quinoniminyl radicals are measured to be 1.715 ± 0.010 and 1.675 ± 0.010 eV, respectively. The photoelectron spectrum of the m-quinonimide anion shows that the ion undergoes several different rearrangements, including a rearrangement to the energetically favorable para isomer. Such rearrangements preclude a meaningful analysis of the experimental spectrum.« less

Energy-optimal path planning by stochastic dynamically orthogonal level-set optimization

NASA Astrophysics Data System (ADS)

Subramani, Deepak N.; Lermusiaux, Pierre F. J.

2016-04-01

A stochastic optimization methodology is formulated for computing energy-optimal paths from among time-optimal paths of autonomous vehicles navigating in a dynamic flow field. Based on partial differential equations, the methodology rigorously leverages the level-set equation that governs time-optimal reachability fronts for a given relative vehicle-speed function. To set up the energy optimization, the relative vehicle-speed and headings are considered to be stochastic and new stochastic Dynamically Orthogonal (DO) level-set equations are derived. Their solution provides the distribution of time-optimal reachability fronts and corresponding distribution of time-optimal paths. An optimization is then performed on the vehicle's energy-time joint distribution to select the energy-optimal paths for each arrival time, among all stochastic time-optimal paths for that arrival time. Numerical schemes to solve the reduced stochastic DO level-set equations are obtained, and accuracy and efficiency considerations are discussed. These reduced equations are first shown to be efficient at solving the governing stochastic level-sets, in part by comparisons with direct Monte Carlo simulations. To validate the methodology and illustrate its accuracy, comparisons with semi-analytical energy-optimal path solutions are then completed. In particular, we consider the energy-optimal crossing of a canonical steady front and set up its semi-analytical solution using a energy-time nested nonlinear double-optimization scheme. We then showcase the inner workings and nuances of the energy-optimal path planning, considering different mission scenarios. Finally, we study and discuss results of energy-optimal missions in a wind-driven barotropic quasi-geostrophic double-gyre ocean circulation.

Global Optimal Trajectory in Chaos and NP-Hardness

NASA Astrophysics Data System (ADS)

Latorre, Vittorio; Gao, David Yang

This paper presents an unconventional theory and method for solving general nonlinear dynamical systems. Instead of the direct iterative methods, the discretized nonlinear system is first formulated as a global optimization problem via the least squares method. A newly developed canonical duality theory shows that this nonconvex minimization problem can be solved deterministically in polynomial time if a global optimality condition is satisfied. The so-called pseudo-chaos produced by linear iterative methods are mainly due to the intrinsic numerical error accumulations. Otherwise, the global optimization problem could be NP-hard and the nonlinear system can be really chaotic. A conjecture is proposed, which reveals the connection between chaos in nonlinear dynamics and NP-hardness in computer science. The methodology and the conjecture are verified by applications to the well-known logistic equation, a forced memristive circuit and the Lorenz system. Computational results show that the canonical duality theory can be used to identify chaotic systems and to obtain realistic global optimal solutions in nonlinear dynamical systems. The method and results presented in this paper should bring some new insights into nonlinear dynamical systems and NP-hardness in computational complexity theory.

Online adaptive optimal control for continuous-time nonlinear systems with completely unknown dynamics

NASA Astrophysics Data System (ADS)

Lv, Yongfeng; Na, Jing; Yang, Qinmin; Wu, Xing; Guo, Yu

2016-01-01

An online adaptive optimal control is proposed for continuous-time nonlinear systems with completely unknown dynamics, which is achieved by developing a novel identifier-critic-based approximate dynamic programming algorithm with a dual neural network (NN) approximation structure. First, an adaptive NN identifier is designed to obviate the requirement of complete knowledge of system dynamics, and a critic NN is employed to approximate the optimal value function. Then, the optimal control law is computed based on the information from the identifier NN and the critic NN, so that the actor NN is not needed. In particular, a novel adaptive law design method with the parameter estimation error is proposed to online update the weights of both identifier NN and critic NN simultaneously, which converge to small neighbourhoods around their ideal values. The closed-loop system stability and the convergence to small vicinity around the optimal solution are all proved by means of the Lyapunov theory. The proposed adaptation algorithm is also improved to achieve finite-time convergence of the NN weights. Finally, simulation results are provided to exemplify the efficacy of the proposed methods.

Can Structural Optimization Explain Slow Dynamics of Rocks?

NASA Astrophysics Data System (ADS)

Kim, H.; Vistisen, O.; Tencate, J. A.

2009-12-01

Slow dynamics is a recovery process that describes the return to an equilibrium state after some external energy input is applied and then removed. Experimental studies on many rocks have shown that a modest acoustic energy input results in slow dynamics. The recovery process of the stiffness has consistently been found to be linear to log(time) for a wide range of geomaterials and the time constants appear to be unique to the material [TenCate JA, Shankland TJ (1996), Geophys Res Lett 23, 3019-3022]. Measurements of this nonequilibrium effect in rocks (e.g. sandstones and limestones) have been linked directly to the cement holding the individual grains together [Darling TW, TenCate JA, Brown DW, Clausen B, Vogel SC (2004), Geophys Res Lett 31, L16604], also suggesting a potential link to porosity and permeability. Noting that slow dynamics consistently returns the overall stiffness of rocks to its maximum (original) state, it is hypothesized that the original state represents the global minimum strain energy state. Consequently the slow dynamics process represents the global minimization or optimization process. Structural optimization, which has been developed for engineering design, minimises the total strain energy by rearranging the material distribution [Kim H, Querin OM, Steven GP, Xie YM (2002), Struct Multidiscip Optim 24, 441-448]. The optimization process effectively rearranges the way the material is cemented. One of the established global optimization methods is simulated annealing (SA). Derived from cooling of metal to a thermal equilibrium, SA finds an optimum solution by iteratively moving the system towards the minimum energy state with a probability of 'uphill' moves. It has been established that the global optimum can be guaranteed by applying a log(time) linear cooling schedule [Hajek B (1988, Math Ops Res, 15, 311-329]. This work presents the original study of applying SA to the maximum stiffness optimization problem. Preliminary results indicate that the maximum stiffness solutions are achieved when using log(time) linear cooling schedule. The optimization history reveals that the overall stiffness of the structure is increased linearly to log(time). The results closely resemble the slow dynamics stiffness recovery of geomaterials and support the hypothesis that the slow dynamics is an optimization process for strain energy. [Work supported by the Department of Energy through the LANL/LDRD Program].

Structural Model Tuning Capability in an Object-Oriented Multidisciplinary Design, Analysis, and Optimization Tool

NASA Technical Reports Server (NTRS)

Lung, Shun-fat; Pak, Chan-gi

2008-01-01

Updating the finite element model using measured data is a challenging problem in the area of structural dynamics. The model updating process requires not only satisfactory correlations between analytical and experimental results, but also the retention of dynamic properties of structures. Accurate rigid body dynamics are important for flight control system design and aeroelastic trim analysis. Minimizing the difference between analytical and experimental results is a type of optimization problem. In this research, a multidisciplinary design, analysis, and optimization (MDAO) tool is introduced to optimize the objective function and constraints such that the mass properties, the natural frequencies, and the mode shapes are matched to the target data as well as the mass matrix being orthogonalized.

Structural Model Tuning Capability in an Object-Oriented Multidisciplinary Design, Analysis, and Optimization Tool

NASA Technical Reports Server (NTRS)

Lung, Shun-fat; Pak, Chan-gi

2008-01-01

Updating the finite element model using measured data is a challenging problem in the area of structural dynamics. The model updating process requires not only satisfactory correlations between analytical and experimental results, but also the retention of dynamic properties of structures. Accurate rigid body dynamics are important for flight control system design and aeroelastic trim analysis. Minimizing the difference between analytical and experimental results is a type of optimization problem. In this research, a multidisciplinary design, analysis, and optimization [MDAO] tool is introduced to optimize the objective function and constraints such that the mass properties, the natural frequencies, and the mode shapes are matched to the target data as well as the mass matrix being orthogonalized.

Low-Thrust Many-Revolution Trajectory Optimization via Differential Dynamic Programming and a Sundman Transformation

NASA Technical Reports Server (NTRS)

Aziz, Jonathan D.; Parker, Jeffrey S.; Scheeres, Daniel J.; Englander, Jacob A.

2017-01-01

Low-thrust trajectories about planetary bodies characteristically span a high count of orbital revolutions. Directing the thrust vector over many revolutions presents a challenging optimization problem for any conventional strategy. This paper demonstrates the tractability of low-thrust trajectory optimization about planetary bodies by applying a Sundman transformation to change the independent variable of the spacecraft equations of motion to the eccentric anomaly and performing the optimization with differential dynamic programming. Fuel-optimal geocentric transfers are shown in excess of 1000 revolutions while subject to Earths J2 perturbation and lunar gravity.

X-Ray Photoelectron Spectroscopy of Stabilized Zirconia Films with Embedded Au Nanoparticles Formed under Irradiation with Gold Ions

NASA Astrophysics Data System (ADS)

Zubkov, S. Yu.; Antonov, I. N.; Gorshkov, O. N.; Kasatkin, A. P.; Kryukov, R. N.; Nikolichev, D. E.; Pavlov, D. A.; Shenina, M. E.

2018-03-01

Nanosized films of stabilized zirconia with Au nanoparticles formed by implanting Au ions are studied by X-ray photoelectron spectroscopy and transmission electron microscopy. The effect of irradiation of films with Au ions and postimplantation annealing on the distribution of chemical elements and zirconium- containing ZrO x compounds over the depth of the films is studied. Based on the data on the dimensional shift of the Au 4 f photoelectron line, the average value of the nanoparticle size is determined.

p-Type dopant incorporation and surface charge properties of catalyst-free GaN nanowires revealed by micro-Raman scattering and X-ray photoelectron spectroscopy.

PubMed

Wang, Q; Liu, X; Kibria, M G; Zhao, S; Nguyen, H P T; Li, K H; Mi, Z; Gonzalez, T; Andrews, M P

2014-09-07

Micro-Raman scattering and X-ray photoelectron spectroscopy were employed to investigate Mg-doped GaN nanowires. With the increase of Mg doping level, pronounced Mg-induced local vibrational modes were observed. The evolution of longitudinal optical phonon-plasmon coupled mode, together with detailed X-ray photoelectron spectroscopy studies, show that the near-surface region of nanowires can be transformed from weakly n-type to p-type with the increase of Mg doping.

Effects of anisotropic electron-ion interactions in atomic photoelectron angular distributions

NASA Technical Reports Server (NTRS)

Dill, D.; Starace, A. F.; Manson, S. T.

1975-01-01

A summary of the angular momentum transfer formulation of the differential photoionization cross section is presented and photoionization amplitudes in LS coupling are considered. The application of the theoretical concepts and relations developed is illustrated with the aid of an example involving the calculation of the angular distribution of photoelectrons ionized from atomic sulfur according to a certain reaction. The investigation shows that anisotropic electron-ion interactions in atomic sulfur lead to measurable differences between photoelectron angular distribution asymmetry parameters corresponding to alternative ionic term levels.

Observation of circular dichroism in photoelectron angular distributions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Appling, J.R.; White, M.G.; Orlando, T.M.

1986-12-01

The first observations of dichroic effects in photoelectron angular distributions are reported for photoionization of aligned molecular excited states with circularly polarized light. Photoelectron angular distributions resulting from the two-color, (2+1) REMPI of NO via the A /sup 2/summation/sup +/, v = 0, J = 3/2,5/2 excited states exhibit significant left--right asymmetry. The experimental CD angular distributions are found to be well described by the general theoretical framework recently developed by Dubs, Dixit, and McKoy and are in good qualitative agreement with their calculated REMPI--CD distributions.

Observation of circular dichroism in photoelectron angular distributions

NASA Astrophysics Data System (ADS)

Appling, Jeffrey R.; White, Michael G.; Orlando, Thomas M.; Anderson, Scott L.

1986-12-01

The first observations of dichroic effects in photoelectron angular distributions are reported for photoionization of aligned molecular excited states with circularly polarized light. Photoelectron angular distributions resulting from the two-color, (2+1) REMPI of NO via the A 2∑+, v=0, J=3/2,5/2 excited states exhibit significant left-right asymmetry. The experimental CD angular distributions are found to be well described by the general theoretical framework recently developed by Dubs, Dixit, and McKoy and are in good qualitative agreement with their calculated REMPI-CD distributions.

High-Resolution Photoionization, Photoelectron and Photodissociation Studies. Determination of Accurate Energetic and Spectroscopic Database for Combustion Radicals and Molecules

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ng, Cheuk-Yiu

2016-04-25

The main goal of this research program was to obtain accurate thermochemical and spectroscopic data, such as ionization energies (IEs), 0 K bond dissociation energies, 0 K heats of formation, and spectroscopic constants for radicals and molecules and their ions of relevance to combustion chemistry. Two unique, generally applicable vacuum ultraviolet (VUV) laser photoion-photoelectron apparatuses have been developed in our group, which have used for high-resolution photoionization, photoelectron, and photodissociation studies for many small molecules of combustion relevance.

The production and photoelectron spectrum of thiazyl iodide. NSI

NASA Astrophysics Data System (ADS)

Allaf, A. W.; Matti, G. Y.; Suffolk, R. J.; Watts, J. D.

1989-02-01

The previously unknown molecule thiazyl iodide, NSI, has been prepared and studied by HeI photoelectron and low-resolution infrared spectroscopy. It has been produced by an on-line process using thiazyl chloride, NSCl, as precursor. The observed photoelectron spectrum has been rationalised using ab initio molecular-orbital calculations. The first ionisation energy is 10.06±0.05 eV, assigned to a largely non-bonding orbital with major components on nitrogen and iodine. Gas-phase infrared spectra yield a value for ν 1 of 1295 cm -1.

Modeling forest stand dynamics from optimal balances of carbon and nitrogen

Treesearch

Harry T. Valentine; Annikki Makela

2012-01-01

We formulate a dynamic evolutionary optimization problem to predict the optimal pattern by which carbon (C) and nitrogen (N) are co-allocated to fine-root, leaf, and wood production, with the objective of maximizing height growth rate, year by year, in an even-aged stand. Height growth is maximized with respect to two adaptive traits, leaf N concentration and the ratio...

How to formulate and solve "optimal stand density over time" problems for even-aged stands using dynamic programming.

Treesearch

Chung M. Chen; Dietmar W. Rose; Rolfe A. Leary

1980-01-01

Describes how dynamic programming can be used to solve optimal stand density problems when yields are given by prior simulation or by a new stand growth equation that is a function of the decision variable. Formulations of the latter type allow use of a calculus-based search procedure; they determine exact optimal residual density at each stage.

Free-time and fixed end-point optimal control theory in dissipative media: application to entanglement generation and maintenance.

PubMed

Mishima, K; Yamashita, K

2009-07-07

We develop monotonically convergent free-time and fixed end-point optimal control theory (OCT) in the density-matrix representation to deal with quantum systems showing dissipation. Our theory is more general and flexible for tailoring optimal laser pulses in order to control quantum dynamics with dissipation than the conventional fixed-time and fixed end-point OCT in that the optimal temporal duration of laser pulses can also be optimized exactly. To show the usefulness of our theory, it is applied to the generation and maintenance of the vibrational entanglement of carbon monoxide adsorbed on the copper (100) surface, CO/Cu(100). We demonstrate the numerical results and clarify how to combat vibrational decoherence as much as possible by the tailored shapes of the optimal laser pulses. It is expected that our theory will be general enough to be applied to a variety of dissipative quantum dynamics systems because the decoherence is one of the quantum phenomena sensitive to the temporal duration of the quantum dynamics.

Can market-based policies accomplish the optimal floodplain management? A gap between static and dynamic models.

PubMed

Mori, Koichiro

2009-02-01

The purpose of this short article is to set static and dynamic models for optimal floodplain management and to compare policy implications from the models. River floodplains are important multiple resources in that they provide various ecosystem services. It is fundamentally significant to consider environmental externalities that accrue from ecosystem services of natural floodplains. There is an interesting gap between static and dynamic models about policy implications for floodplain management, although they are based on the same assumptions. Essentially, we can derive the same optimal conditions, which imply that the marginal benefits must equal the sum of the marginal costs and the social external costs related to ecosystem services. Thus, we have to internalise the external costs by market-based policies. In this respect, market-based policies seem to be effective in a static model. However, they are not sufficient in the context of a dynamic model because the optimal steady state turns out to be unstable. Based on a dynamic model, we need more coercive regulation policies.

Optimizing legacy molecular dynamics software with directive-based offload

NASA Astrophysics Data System (ADS)

Michael Brown, W.; Carrillo, Jan-Michael Y.; Gavhane, Nitin; Thakkar, Foram M.; Plimpton, Steven J.

2015-10-01

Directive-based programming models are one solution for exploiting many-core coprocessors to increase simulation rates in molecular dynamics. They offer the potential to reduce code complexity with offload models that can selectively target computations to run on the CPU, the coprocessor, or both. In this paper, we describe modifications to the LAMMPS molecular dynamics code to enable concurrent calculations on a CPU and coprocessor. We demonstrate that standard molecular dynamics algorithms can run efficiently on both the CPU and an x86-based coprocessor using the same subroutines. As a consequence, we demonstrate that code optimizations for the coprocessor also result in speedups on the CPU; in extreme cases up to 4.7X. We provide results for LAMMPS benchmarks and for production molecular dynamics simulations using the Stampede hybrid supercomputer with both Intel® Xeon Phi™ coprocessors and NVIDIA GPUs. The optimizations presented have increased simulation rates by over 2X for organic molecules and over 7X for liquid crystals on Stampede. The optimizations are available as part of the "Intel package" supplied with LAMMPS.

Optimal blood glucose control in diabetes mellitus treatment using dynamic programming based on Ackerman’s linear model

NASA Astrophysics Data System (ADS)

Pradanti, Paskalia; Hartono

2018-03-01

Determination of insulin injection dose in diabetes mellitus treatment can be considered as an optimal control problem. This article is aimed to simulate optimal blood glucose control for patient with diabetes mellitus. The blood glucose regulation of diabetic patient is represented by Ackerman’s Linear Model. This problem is then solved using dynamic programming method. The desired blood glucose level is obtained by minimizing the performance index in Lagrange form. The results show that dynamic programming based on Ackerman’s Linear Model is quite good to solve the problem.

Surrogate Based Uni/Multi-Objective Optimization and Distribution Estimation Methods

NASA Astrophysics Data System (ADS)

Gong, W.; Duan, Q.; Huo, X.

2017-12-01

Parameter calibration has been demonstrated as an effective way to improve the performance of dynamic models, such as hydrological models, land surface models, weather and climate models etc. Traditional optimization algorithms usually cost a huge number of model evaluations, making dynamic model calibration very difficult, or even computationally prohibitive. With the help of a serious of recently developed adaptive surrogate-modelling based optimization methods: uni-objective optimization method ASMO, multi-objective optimization method MO-ASMO, and probability distribution estimation method ASMO-PODE, the number of model evaluations can be significantly reduced to several hundreds, making it possible to calibrate very expensive dynamic models, such as regional high resolution land surface models, weather forecast models such as WRF, and intermediate complexity earth system models such as LOVECLIM. This presentation provides a brief introduction to the common framework of adaptive surrogate-based optimization algorithms of ASMO, MO-ASMO and ASMO-PODE, a case study of Common Land Model (CoLM) calibration in Heihe river basin in Northwest China, and an outlook of the potential applications of the surrogate-based optimization methods.

Investigation on the use of optimization techniques for helicopter airframe vibrations design studies

NASA Technical Reports Server (NTRS)

Sreekanta Murthy, T.

1992-01-01

Results of the investigation of formal nonlinear programming-based numerical optimization techniques of helicopter airframe vibration reduction are summarized. The objective and constraint function and the sensitivity expressions used in the formulation of airframe vibration optimization problems are presented and discussed. Implementation of a new computational procedure based on MSC/NASTRAN and CONMIN in a computer program system called DYNOPT for optimizing airframes subject to strength, frequency, dynamic response, and dynamic stress constraints is described. An optimization methodology is proposed which is thought to provide a new way of applying formal optimization techniques during the various phases of the airframe design process. Numerical results obtained from the application of the DYNOPT optimization code to a helicopter airframe are discussed.

Dynamic regime of coherent population trapping and optimization of frequency modulation parameters in atomic clocks.

PubMed

Yudin, V I; Taichenachev, A V; Basalaev, M Yu; Kovalenko, D V

2017-02-06

We theoretically investigate the dynamic regime of coherent population trapping (CPT) in the presence of frequency modulation (FM). We have formulated the criteria for quasi-stationary (adiabatic) and dynamic (non-adiabatic) responses of atomic system driven by this FM. Using the density matrix formalism for Λ system, the error signal is exactly calculated and optimized. It is shown that the optimal FM parameters correspond to the dynamic regime of atomic-field interaction, which significantly differs from conventional description of CPT resonances in the frame of quasi-stationary approach (under small modulation frequency). Obtained theoretical results are in good qualitative agreement with different experiments. Also we have found CPT-analogue of Pound-Driver-Hall regime of frequency stabilization.

Implicit methods for efficient musculoskeletal simulation and optimal control

PubMed Central

van den Bogert, Antonie J.; Blana, Dimitra; Heinrich, Dieter

2011-01-01

The ordinary differential equations for musculoskeletal dynamics are often numerically stiff and highly nonlinear. Consequently, simulations require small time steps, and optimal control problems are slow to solve and have poor convergence. In this paper, we present an implicit formulation of musculoskeletal dynamics, which leads to new numerical methods for simulation and optimal control, with the expectation that we can mitigate some of these problems. A first order Rosenbrock method was developed for solving forward dynamic problems using the implicit formulation. It was used to perform real-time dynamic simulation of a complex shoulder arm system with extreme dynamic stiffness. Simulations had an RMS error of only 0.11 degrees in joint angles when running at real-time speed. For optimal control of musculoskeletal systems, a direct collocation method was developed for implicitly formulated models. The method was applied to predict gait with a prosthetic foot and ankle. Solutions were obtained in well under one hour of computation time and demonstrated how patients may adapt their gait to compensate for limitations of a specific prosthetic limb design. The optimal control method was also applied to a state estimation problem in sports biomechanics, where forces during skiing were estimated from noisy and incomplete kinematic data. Using a full musculoskeletal dynamics model for state estimation had the additional advantage that forward dynamic simulations, could be done with the same implicitly formulated model to simulate injuries and perturbation responses. While these methods are powerful and allow solution of previously intractable problems, there are still considerable numerical challenges, especially related to the convergence of gradient-based solvers. PMID:22102983

Anion photoelectron spectroscopy of radicals and clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Travis, Taylor R.

1999-12-01

Anion photoelectron spectroscopy is used to study free radicals and clusters. The low-lying 2Σ and 2π states of C 2nH (n = 1--4) have been studied. The anion photoelectron spectra yielded electron affinities, term values, and vibrational frequencies for these combustion and astrophysically relevant species. Photoelectron angular distributions allowed the author to correctly assign the electronic symmetry of the ground and first excited states and to assess the degree of vibronic coupling in C 2H and C 4H. Other radicals studied include NCN and I 3. The author was able to observe the low-lying singlet and triplet states of NCNmore » for the first time. Measurement of the electron affinity of I 3 revealed that it has a bound ground state and attachment of an argon atom to this moiety enabled him to resolve the symmetric stretching progression.« less

X-Ray photoelectron diffraction and photoelectron holography as methods for investigating the local atomic structure of the surface of solids

NASA Astrophysics Data System (ADS)

Kuznetsov, M. V.; Ogorodnikov, I. I.; Vorokh, A. S.

2014-01-01

The state-of-the-art theory and experimental applications of X-ray photoelectron diffraction (XPD) and photoelectron holography (PH) are discussed. These methods are rapidly progressing and serve to examine the surface atomic structure of solids, including nanostructures formed on surfaces during adsorption of gases, epitaxial film growth, etc. The depth of analysis by these methods is several nanometres, which makes it possible to characterize the positions of atoms localized both on and beneath the surface. A remarkable feature of the XPD and PH methods is their sensitivity to the type of examined atoms and, in the case of high energy resolution, to the particular chemical form of the element under study. The data on experimental applications of XPD and PH to studies of various surface structures are analyzed and generalized. The bibliography includes 121 references.

X-ray photoelectron study of Si+ ion implanted polymers

NASA Astrophysics Data System (ADS)

Tsvetkova, T.; Balabanov, S.; Bischoff, L.; Krastev, V.; Stefanov, P.; Avramova, I.

2010-11-01

X-ray photoelectron spectroscopy was used to characterize different polymer materials implanted with low energy Si+ ions (E=30 keV, D= 1.1017 cm-2). Two kinds of polymers were studied - ultra-high-molecular-weight poly-ethylene (UHMWPE), and poly-methyl-methacrylate (PMMA). The non-implanted polymer materials show the expected variety of chemical bonds: carbon-carbon, carbon being three- and fourfold coordinated, and carbon-oxygen in the case of PMMA samples. The X-ray photoelectron and Raman spectra show that Si+ ion implantation leads to the introduction of additional disorder in the polymer material. The X-ray photoelectron spectra of the implanted polymers show that, in addition to already mentioned bonds, silicon creates new bonds with the host elements - Si-C and Si-O, together with additional Si dangling bonds as revealed by the valence band study of the implanted polymer materials.

Determination of the absolute carrier-envelope phase by angle-resolved photoelectron spectra of Ar by intense circularly polarized few-cycle pulses

NASA Astrophysics Data System (ADS)

Fukahori, Shinichi; Ando, Toshiaki; Miura, Shun; Kanya, Reika; Yamanouchi, Kaoru; Rathje, Tim; Paulus, Gerhard G.

2017-05-01

The angle-resolved photoelectron spectra of Ar are recorded using intense circularly polarized near-infrared few-cycle laser pulses, and the effect of the depletion of Ar atoms by the ionization and the effect of the Coulombic potential are examined by the classical trajectory Monte Carlo simulations. On the basis of the comparison between the experimental and theoretical photoelectron spectra, a procedure for estimating the absolute carrier-envelope phase (CEP) of the few-cycle laser pulses interacting with atoms and molecules is proposed. It is confirmed that the absolute CEP can securely be estimated without any numerical calculations once the angular distribution of the yield of photoelectrons having the kinetic energy larger than 30 eV is measured with the peak laser intensity in the range between 1 ×1014 and 5 ×1014W /c m2 .

Dark field photoelectron emission microscopy of micron scale few layer graphene

NASA Astrophysics Data System (ADS)

Barrett, N.; Conrad, E.; Winkler, K.; Krömker, B.

2012-08-01

We demonstrate dark field imaging in photoelectron emission microscopy (PEEM) of heterogeneous few layer graphene (FLG) furnace grown on SiC(000-1). Energy-filtered, threshold PEEM is used to locate distinct zones of FLG graphene. In each region, selected by a field aperture, the k-space information is imaged using appropriate transfer optics. By selecting the photoelectron intensity at a given wave vector and using the inverse transfer optics, dark field PEEM gives a spatial distribution of the angular photoelectron emission. In the results presented here, the wave vector coordinates of the Dirac cones characteristic of commensurate rotations of FLG on SiC(000-1) are selected providing a map of the commensurate rotations across the surface. This special type of contrast is therefore a method to map the spatial distribution of the local band structure and offers a new laboratory tool for the characterisation of technically relevant, microscopically structured matter.

Measurement configuration optimization for dynamic metrology using Stokes polarimetry

NASA Astrophysics Data System (ADS)

Liu, Jiamin; Zhang, Chuanwei; Zhong, Zhicheng; Gu, Honggang; Chen, Xiuguo; Jiang, Hao; Liu, Shiyuan

2018-05-01

As dynamic loading experiments such as a shock compression test are usually characterized by short duration, unrepeatability and high costs, high temporal resolution and precise accuracy of the measurements is required. Due to high temporal resolution up to a ten-nanosecond-scale, a Stokes polarimeter with six parallel channels has been developed to capture such instantaneous changes in optical properties in this paper. Since the measurement accuracy heavily depends on the configuration of the probing beam incident angle and the polarizer azimuth angle, it is important to select an optimal combination from the numerous options. In this paper, a systematic error propagation-based measurement configuration optimization method corresponding to the Stokes polarimeter was proposed. The maximal Frobenius norm of the combinatorial matrix of the configuration error propagating matrix and the intrinsic error propagating matrix is introduced to assess the measurement accuracy. The optimal configuration for thickness measurement of a SiO2 thin film deposited on a Si substrate has been achieved by minimizing the merit function. Simulation and experimental results show a good agreement between the optimal measurement configuration achieved experimentally using the polarimeter and the theoretical prediction. In particular, the experimental result shows that the relative error in the thickness measurement can be reduced from 6% to 1% by using the optimal polarizer azimuth angle when the incident angle is 45°. Furthermore, the optimal configuration for the dynamic metrology of a nickel foil under quasi-dynamic loading is investigated using the proposed optimization method.

Numerical integration and optimization of motions for multibody dynamic systems

NASA Astrophysics Data System (ADS)

Aguilar Mayans, Joan

This thesis considers the optimization and simulation of motions involving rigid body systems. It does so in three distinct parts, with the following topics: optimization and analysis of human high-diving motions, efficient numerical integration of rigid body dynamics with contacts, and motion optimization of a two-link robot arm using Finite-Time Lyapunov Analysis. The first part introduces the concept of eigenpostures, which we use to simulate and analyze human high-diving motions. Eigenpostures are used in two different ways: first, to reduce the complexity of the optimal control problem that we solve to obtain such motions, and second, to generate an eigenposture space to which we map existing real world motions to better analyze them. The benefits of using eigenpostures are showcased through different examples. The second part reviews an extensive list of integration algorithms used for the integration of rigid body dynamics. We analyze the accuracy and stability of the different integrators in the three-dimensional space and the rotation space SO(3). Integrators with an accuracy higher than first order perform more efficiently than integrators with first order accuracy, even in the presence of contacts. The third part uses Finite-time Lyapunov Analysis to optimize motions for a two-link robot arm. Finite-Time Lyapunov Analysis diagnoses the presence of time-scale separation in the dynamics of the optimized motion and provides the information and methodology for obtaining an accurate approximation to the optimal solution, avoiding the complications that timescale separation causes for alternative solution methods.

Optimizing Dynamical Network Structure for Pinning Control

NASA Astrophysics Data System (ADS)

Orouskhani, Yasin; Jalili, Mahdi; Yu, Xinghuo

2016-04-01

Controlling dynamics of a network from any initial state to a final desired state has many applications in different disciplines from engineering to biology and social sciences. In this work, we optimize the network structure for pinning control. The problem is formulated as four optimization tasks: i) optimizing the locations of driver nodes, ii) optimizing the feedback gains, iii) optimizing simultaneously the locations of driver nodes and feedback gains, and iv) optimizing the connection weights. A newly developed population-based optimization technique (cat swarm optimization) is used as the optimization method. In order to verify the methods, we use both real-world networks, and model scale-free and small-world networks. Extensive simulation results show that the optimal placement of driver nodes significantly outperforms heuristic methods including placing drivers based on various centrality measures (degree, betweenness, closeness and clustering coefficient). The pinning controllability is further improved by optimizing the feedback gains. We also show that one can significantly improve the controllability by optimizing the connection weights.

Optimal interdependence enhances the dynamical robustness of complex systems.

PubMed

Singh, Rishu Kumar; Sinha, Sitabhra

2017-08-01

Although interdependent systems have usually been associated with increased fragility, we show that strengthening the interdependence between dynamical processes on different networks can make them more likely to survive over long times. By coupling the dynamics of networks that in isolation exhibit catastrophic collapse with extinction of nodal activity, we demonstrate system-wide persistence of activity for an optimal range of interdependence between the networks. This is related to the appearance of attractors of the global dynamics comprising disjoint sets ("islands") of stable activity.

Optimal interdependence enhances the dynamical robustness of complex systems

NASA Astrophysics Data System (ADS)

Singh, Rishu Kumar; Sinha, Sitabhra

2017-08-01

Although interdependent systems have usually been associated with increased fragility, we show that strengthening the interdependence between dynamical processes on different networks can make them more likely to survive over long times. By coupling the dynamics of networks that in isolation exhibit catastrophic collapse with extinction of nodal activity, we demonstrate system-wide persistence of activity for an optimal range of interdependence between the networks. This is related to the appearance of attractors of the global dynamics comprising disjoint sets ("islands") of stable activity.

Improvement of band gap profile in Cu(InGa)Se{sub 2} solar cells through rapid thermal annealing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, D.S.; College of Mathematics and Physics, Shanghai University of Electric Power, Shanghai, 200090; Yang, J.

Highlights: • Proper RTA treatment can effectively optimize band gap profile to more expected level. • Inter-diffusion of atoms account for the improvement of the graded band gap profile. • The variation of the band gap profile created an absolute gain in the efficiency by 1.22%. - Abstract: In the paper, the effect of rapid thermal annealing on non-optimal double-graded band gap profiles was investigated by using X-ray photoelectron spectroscopy and capacitance–voltage measurement techniques. Experimental results revealed that proper rapid thermal annealing treatment can effectively improve band gap profile to more optimal level. The annealing treatment could not only reducemore » the values of front band gap and minimum band gap, but also shift the position of the minimum band gap toward front electrode and enter into space charge region. In addition, the thickness of Cu(InGa)Se{sub 2} thin film decreased by 25 nm after rapid thermal annealing treatment. All of these modifications were attributed to the inter-diffusion of atoms during thermal treatment process. Simultaneously, the variation of the band gap profile created an absolute gain in the efficiency by 1.22%, short-circuit current density by 2.16 mA/cm{sup 2} and filled factor by 3.57%.« less

Thickness effects of yttria-doped ceria interlayers on solid oxide fuel cells

NASA Astrophysics Data System (ADS)

Fan, Zeng; An, Jihwan; Iancu, Andrei; Prinz, Fritz B.

2012-11-01

Determining the optimal thickness range of the interlayed yttria-doped ceria (YDC) films promises to further enhance the performance of solid oxide fuel cells (SOFCs) at low operating temperatures. The YDC interlayers are fabricated by the atomic layer deposition (ALD) method with one super cycle of the YDC deposition consisting of 6 ceria deposition cycles and one yttria deposition cycle. YDC films of various numbers of ALD super cycles, ranging from 2 to 35, are interlayered into bulk fuel cells with a 200 um thick yttria-stabilized zirconia (YSZ) electrolyte. Measurements and analysis of the linear sweep voltammetry of these fuel cells reveal that the performance of the given cells is maximized at 10 super cycles. Auger elemental mapping and X-ray photoelectron spectroscopy (XPS) techniques are employed to determine the film completeness, and they verify 10 super cycles of YDC to be the critical thickness point. This optimal YDC interlayer condition (6Ce1Y × 10 super cycles) is applied to the case of micro fuel cells as well, and the average performance enhancement factor is 1.4 at operating temperatures of 400 and 450 °C. A power density of 1.04 W cm-2 at 500 °C is also achieved with the optimal YDC recipe.

Advanced launch system trajectory optimization using suboptimal control

NASA Technical Reports Server (NTRS)

Shaver, Douglas A.; Hull, David G.

1993-01-01

The maximum-final mass trajectory of a proposed configuration of the Advanced Launch System is presented. A model for the two-stage rocket is given; the optimal control problem is formulated as a parameter optimization problem; and the optimal trajectory is computed using a nonlinear programming code called VF02AD. Numerical results are presented for the controls (angle of attack and velocity roll angle) and the states. After the initial rotation, the angle of attack goes to a positive value to keep the trajectory as high as possible, returns to near zero to pass through the transonic regime and satisfy the dynamic pressure constraint, returns to a positive value to keep the trajectory high and to take advantage of minimum drag at positive angle of attack due to aerodynamic shading of the booster, and then rolls off to negative values to satisfy the constraints. Because the engines cannot be throttled, the maximum dynamic pressure occurs at a single point; there is no maximum dynamic pressure subarc. To test approximations for obtaining analytical solutions for guidance, two additional optimal trajectories are computed: one using untrimmed aerodynamics and one using no atmospheric effects except for the dynamic pressure constraint. It is concluded that untrimmed aerodynamics has a negligible effect on the optimal trajectory and that approximate optimal controls should be able to be obtained by treating atmospheric effects as perturbations.

Computer aided analysis and optimization of mechanical system dynamics

NASA Technical Reports Server (NTRS)

Haug, E. J.

1984-01-01

The purpose is to outline a computational approach to spatial dynamics of mechanical systems that substantially enlarges the scope of consideration to include flexible bodies, feedback control, hydraulics, and related interdisciplinary effects. Design sensitivity analysis and optimization is the ultimate goal. The approach to computer generation and solution of the system dynamic equations and graphical methods for creating animations as output is outlined.

Rethinking Traffic Management: Design of Optimizable Networks

DTIC Science & Technology

2008-06-01

Though this paper used optimization theory to design and analyze DaVinci , op- timization theory is one of many possible tools to enable a grounded...dynamically allocate bandwidth shares. The distributed protocols can be implemented using DaVinci : Dynamically Adaptive VIrtual Networks for a Customized...Internet. In DaVinci , each virtual network runs traffic-management protocols optimized for a traffic class, and link bandwidth is dynamically allocated

Dynamic malware containment under an epidemic model with alert

NASA Astrophysics Data System (ADS)

Zhang, Tianrui; Yang, Lu-Xing; Yang, Xiaofan; Wu, Yingbo; Tang, Yuan Yan

2017-03-01

Alerting at the early stage of malware invasion turns out to be an important complement to malware detection and elimination. This paper addresses the issue of how to dynamically contain the prevalence of malware at a lower cost, provided alerting is feasible. A controlled epidemic model with alert is established, and an optimal control problem based on the epidemic model is formulated. The optimality system for the optimal control problem is derived. The structure of an optimal control for the proposed optimal control problem is characterized under some conditions. Numerical examples show that the cost-efficiency of an optimal control strategy can be enhanced by adjusting the upper and lower bounds on admissible controls.

Trajectory optimization for the National Aerospace Plane

NASA Technical Reports Server (NTRS)

Lu, Ping

1993-01-01

The objective of this second phase research is to investigate the optimal ascent trajectory for the National Aerospace Plane (NASP) from runway take-off to orbital insertion and address the unique problems associated with the hypersonic flight trajectory optimization. The trajectory optimization problem for an aerospace plane is a highly challenging problem because of the complexity involved. Previous work has been successful in obtaining sub-optimal trajectories by using energy-state approximation and time-scale decomposition techniques. But it is known that the energy-state approximation is not valid in certain portions of the trajectory. This research aims at employing full dynamics of the aerospace plane and emphasizing direct trajectory optimization methods. The major accomplishments of this research include the first-time development of an inverse dynamics approach in trajectory optimization which enables us to generate optimal trajectories for the aerospace plane efficiently and reliably, and general analytical solutions to constrained hypersonic trajectories that has wide application in trajectory optimization as well as in guidance and flight dynamics. Optimal trajectories in abort landing and ascent augmented with rocket propulsion and thrust vectoring control were also investigated. Motivated by this study, a new global trajectory optimization tool using continuous simulated annealing and a nonlinear predictive feedback guidance law have been under investigation and some promising results have been obtained, which may well lead to more significant development and application in the near future.

Long range personalized cancer treatment strategies incorporating evolutionary dynamics.

PubMed

Yeang, Chen-Hsiang; Beckman, Robert A

2016-10-22

Current cancer precision medicine strategies match therapies to static consensus molecular properties of an individual's cancer, thus determining the next therapeutic maneuver. These strategies typically maintain a constant treatment while the cancer is not worsening. However, cancers feature complicated sub-clonal structure and dynamic evolution. We have recently shown, in a comprehensive simulation of two non-cross resistant therapies across a broad parameter space representing realistic tumors, that substantial improvement in cure rates and median survival can be obtained utilizing dynamic precision medicine strategies. These dynamic strategies explicitly consider intratumoral heterogeneity and evolutionary dynamics, including predicted future drug resistance states, and reevaluate optimal therapy every 45 days. However, the optimization is performed in single 45 day steps ("single-step optimization"). Herein we evaluate analogous strategies that think multiple therapeutic maneuvers ahead, considering potential outcomes at 5 steps ahead ("multi-step optimization") or 40 steps ahead ("adaptive long term optimization (ALTO)") when recommending the optimal therapy in each 45 day block, in simulations involving both 2 and 3 non-cross resistant therapies. We also evaluate an ALTO approach for situations where simultaneous combination therapy is not feasible ("Adaptive long term optimization: serial monotherapy only (ALTO-SMO)"). Simulations utilize populations of 764,000 and 1,700,000 virtual patients for 2 and 3 drug cases, respectively. Each virtual patient represents a unique clinical presentation including sizes of major and minor tumor subclones, growth rates, evolution rates, and drug sensitivities. While multi-step optimization and ALTO provide no significant average survival benefit, cure rates are significantly increased by ALTO. Furthermore, in the subset of individual virtual patients demonstrating clinically significant difference in outcome between approaches, by far the majority show an advantage of multi-step or ALTO over single-step optimization. ALTO-SMO delivers cure rates superior or equal to those of single- or multi-step optimization, in 2 and 3 drug cases respectively. In selected virtual patients incurable by dynamic precision medicine using single-step optimization, analogous strategies that "think ahead" can deliver long-term survival and cure without any disadvantage for non-responders. When therapies require dose reduction in combination (due to toxicity), optimal strategies feature complex patterns involving rapidly interleaved pulses of combinations and high dose monotherapy. This article was reviewed by Wendy Cornell, Marek Kimmel, and Andrzej Swierniak. Wendy Cornell and Andrzej Swierniak are external reviewers (not members of the Biology Direct editorial board). Andrzej Swierniak was nominated by Marek Kimmel.

Nanoparticle formation of deposited Agn-clusters on free-standing graphene

NASA Astrophysics Data System (ADS)

Al-Hada, M.; Peters, S.; Gregoratti, L.; Amati, M.; Sezen, H.; Parisse, P.; Selve, S.; Niermann, T.; Berger, D.; Neeb, M.; Eberhardt, W.

2017-11-01

Size-selected Agn-clusters on unsupported graphene of a commercial Quantifoil sample have been investigated by surface and element-specific techniques such as transmission electron microscopy (TEM), spatially-resolved inner-shell X-ray photoelectron spectroscopy (XPS) and Auger electron spectroscopy (AES). An agglomeration of the highly mobile clusters into nm-sized Ag-nanodots of 2-3 nm is observed. Moreover, crystalline as well as non-periodic fivefold symmetric structures of the Ag-nanoparticles are evident by high-resolution TEM. Using a lognormal size-distribution as revealed by TEM, the measured positive binding energy shift of the air-exposed Ag-nanodots can be explained by the size-dependent dynamical liquid-drop model.

Low temperature synthesis and characterization of carbonated hydroxyapatite nanocrystals

NASA Astrophysics Data System (ADS)

Anwar, Aneela; Asghar, Muhammad Nadeem; Kanwal, Qudsia; Kazmi, Mohsin; Sadiqa, Ayesha

2016-08-01

Carbonate substituted hydroxyapatite (CHA) nanorods were synthesized via coprecipitation method from aqueous solution of calcium nitrate tetrahydrate and diammonium hydrogen phosphate (with urea as carbonate ion source) in the presence of ammonium hydroxide solution at 70 °C at the conditions of pH 11. The obtained powders were physically characterized using transmission electron microscopy (TEM), X-ray powder diffraction analysis (XRD), and FTIR and Raman spectroscopy. The particle size was evaluated by Dynamic light scattering (DLS). The chemical structural analysis of as prepared sample was performed using X-ray photoelectron spectroscopy (XPS). After ageing for 12 h, and heat treatment at 1000 °C for 1 h, the product was obtained as highly crystalline nanorods of CHA.

Imaging ultrafast dynamics of molecules with laser-induced electron diffraction.

PubMed

Lin, C D; Xu, Junliang

2012-10-14

We introduce a laser-induced electron diffraction method (LIED) for imaging ultrafast dynamics of small molecules with femtosecond mid-infrared lasers. When molecules are placed in an intense laser field, both low- and high-energy photoelectrons are generated. According to quantitative rescattering (QRS) theory, high-energy electrons are produced by a rescattering process where electrons born at the early phase of the laser pulse are driven back to rescatter with the parent ion. From the high-energy electron momentum spectra, field-free elastic electron-ion scattering differential cross sections (DCS), or diffraction images, can be extracted. With mid-infrared lasers as the driving pulses, it is further shown that the DCS can be used to extract atomic positions in a molecule with sub-angstrom spatial resolution, in close analogy to the standard electron diffraction method. Since infrared lasers with pulse duration of a few to several tens of femtoseconds are already available, LIED can be used for imaging dynamics of molecules with sub-angstrom spatial and a few-femtosecond temporal resolution. The first experiment with LIED has shown that the bond length of oxygen molecules shortens by 0.1 Å in five femtoseconds after single ionization. The principle behind LIED and its future outlook as a tool for dynamic imaging of molecules are presented.

ODECS -- A computer code for the optimal design of S.I. engine control strategies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arsie, I.; Pianese, C.; Rizzo, G.

1996-09-01

The computer code ODECS (Optimal Design of Engine Control Strategies) for the design of Spark Ignition engine control strategies is presented. This code has been developed starting from the author`s activity in this field, availing of some original contributions about engine stochastic optimization and dynamical models. This code has a modular structure and is composed of a user interface for the definition, the execution and the analysis of different computations performed with 4 independent modules. These modules allow the following calculations: (1) definition of the engine mathematical model from steady-state experimental data; (2) engine cycle test trajectory corresponding to amore » vehicle transient simulation test such as ECE15 or FTP drive test schedule; (3) evaluation of the optimal engine control maps with a steady-state approach; (4) engine dynamic cycle simulation and optimization of static control maps and/or dynamic compensation strategies, taking into account dynamical effects due to the unsteady fluxes of air and fuel and the influences of combustion chamber wall thermal inertia on fuel consumption and emissions. Moreover, in the last two modules it is possible to account for errors generated by a non-deterministic behavior of sensors and actuators and the related influences on global engine performances, and compute robust strategies, less sensitive to stochastic effects. In the paper the four models are described together with significant results corresponding to the simulation and the calculation of optimal control strategies for dynamic transient tests.« less

Technical report on prototype intelligent network flow optimization (INFLO) dynamic speed harmonization and queue warning.

DOT National Transportation Integrated Search

2015-06-01

This Technical Report on Prototype Intelligent Network Flow Optimization (INFLO) Dynamic Speed Harmonization and Queue Warning is the final report for the project. It describes the prototyping, acceptance testing and small-scale demonstration of the ...

Low Energy Electrons in the Mars Plasma Environment

NASA Technical Reports Server (NTRS)

Link, Richard

2001-01-01

The ionosphere of Mars is rather poorly understood. The only direct measurements were performed by the Viking 1 and 2 landers in 1976, both of which carried a Retarding Potential Analyzer. The RPA was designed to measure ion properties during the descent, although electron fluxes were estimated from changes in the ion currents. Using these derived low-energy electron fluxes, Mantas and Hanson studied the photoelectron and the solar wind electron interactions with the atmosphere and ionosphere of Mars. Unanswered questions remain regarding the origin of the low-energy electron fluxes in the vicinity of the Mars plasma boundary. Crider, in an analysis of Mars Global Surveyor Magnetometer/Electron Reflectometer measurements, has attributed the formation of the magnetic pile-up boundary to electron impact ionization of exospheric neutral species by solar wind electrons. However, the role of photoelectrons escaping from the lower ionosphere was not determined. In the proposed work, we will examine the role of solar wind and ionospheric photoelectrons in producing ionization in the upper ionosphere of Mars. Low-energy (< 4 keV) electrons will be modeled using the two-stream electron transport code of Link. The code models both external (solar wind) and internal (photoelectron) sources of ionization, and accounts for Auger electron production. The code will be used to analyze Mars Global Surveyor measurements of solar wind and photoelectrons down to altitudes below 200 km in the Mars ionosphere, in order to determine the relative roles of solar wind and escaping photoelectrons in maintaining plasma densities in the region of the Mars plasma boundary.

Production, Thermalization and Transport of Photoelectrons in the Mars Environment

NASA Astrophysics Data System (ADS)

Mitchell, D. L.; Xu, S.; Mazelle, C. X.; Steckiewicz, M.; Luhmann, J. G.; Connerney, J. E. P.; Andersson, L.

2016-12-01

The Solar Wind Electron Analyzer (SWEA) on the MAVEN spacecraft provides a detailed look at the production, thermalization, and transport of photoelectrons in the Mars environment. The MAVEN orbit routinely samples altitudes down to 150 km over wide ranges of solar zenith angle, local time, longitude, latitude and altitude. The altitude range extends into the region of photochemical equilibrium. SWEA's nominal energy resolution of 17% (ΔE/E, FWHM) is insufficient to resolve the photoelectron peaks at 23 and 27 eV, which result from photoionization of CO2 and O by the intense He II line in the solar EUV spectrum. However, during some orbits the spacecraft charged to -18 V near periapsis, which shifted the He II photoelectron features to lower energies, thus allowing them to be resolved. During several week-long deep dip campaigns, the periapsis altitude was lowered to 120 km. Thermalization of primary photoelectrons is very rapid at this altitude, resulting in a residual population at 7 eV, where the cross section to interaction with CO2 has a minimum. At altitudes above the 200 km, collisions become negligible (mean free path > 100 km), and the motion of suprathermal electrons is controlled by the magnetic field. Electron energy-pitch angle distributions reveal transport of photoelectrons from the day to the night hemisphere on both closed crustal magnetic loops and on open lines that extend into the tail. Mapping of such open field lines reveals the regions of the tail with access to the day-side ionosphere, which provide a conduit for ion outflow and loss.

Optimizing read-out of the NECTAr front-end electronics

NASA Astrophysics Data System (ADS)

Vorobiov, S.; Feinstein, F.; Bolmont, J.; Corona, P.; Delagnes, E.; Falvard, A.; Gascón, D.; Glicenstein, J.-F.; Naumann, C. L.; Nayman, P.; Ribo, M.; Sanuy, A.; Tavernet, J.-P.; Toussenel, F.; Vincent, P.

2012-12-01

We describe the optimization of the read-out specifications of the NECTAr front-end electronics for the Cherenkov Telescope Array (CTA). The NECTAr project aims at building and testing a demonstrator module of a new front-end electronics design, which takes an advantage of the know-how acquired while building the cameras of the CAT, H.E.S.S.-I and H.E.S.S.-II experiments. The goal of the optimization work is to define the specifications of the digitizing electronics of a CTA camera, in particular integration time window, sampling rate, analog bandwidth using physics simulations. We employed for this work real photomultiplier pulses, sampled at 100 ps with a 600 MHz bandwidth oscilloscope. The individual pulses are drawn randomly at the times at which the photo-electrons, originating from atmospheric showers, arrive at the focal planes of imaging atmospheric Cherenkov telescopes. The timing information is extracted from the existing CTA simulations on the GRID and organized in a local database, together with all the relevant physical parameters (energy, primary particle type, zenith angle, distance from the shower axis, pixel offset from the optical axis, night-sky background level, etc.), and detector configurations (telescope types, camera/mirror configurations, etc.). While investigating the parameter space, an optimal pixel charge integration time window, which minimizes relative error in the measured charge, has been determined. This will allow to gain in sensitivity and to lower the energy threshold of CTA telescopes. We present results of our optimizations and first measurements obtained using the NECTAr demonstrator module.

Dynamic Aberration Correction for Conformal Window of High-Speed Aircraft Using Optimized Model-Based Wavefront Sensorless Adaptive Optics

PubMed Central

Dong, Bing; Li, Yan; Han, Xin-li; Hu, Bin

2016-01-01

For high-speed aircraft, a conformal window is used to optimize the aerodynamic performance. However, the local shape of the conformal window leads to large amounts of dynamic aberrations varying with look angle. In this paper, deformable mirror (DM) and model-based wavefront sensorless adaptive optics (WSLAO) are used for dynamic aberration correction of an infrared remote sensor equipped with a conformal window and scanning mirror. In model-based WSLAO, aberration is captured using Lukosz mode, and we use the low spatial frequency content of the image spectral density as the metric function. Simulations show that aberrations induced by the conformal window are dominated by some low-order Lukosz modes. To optimize the dynamic correction, we can only correct dominant Lukosz modes and the image size can be minimized to reduce the time required to compute the metric function. In our experiment, a 37-channel DM is used to mimic the dynamic aberration of conformal window with scanning rate of 10 degrees per second. A 52-channel DM is used for correction. For a 128 × 128 image, the mean value of image sharpness during dynamic correction is 1.436 × 10−5 in optimized correction and is 1.427 × 10−5 in un-optimized correction. We also demonstrated that model-based WSLAO can achieve convergence two times faster than traditional stochastic parallel gradient descent (SPGD) method. PMID:27598161

Control of water distribution networks with dynamic DMA topology using strictly feasible sequential convex programming

NASA Astrophysics Data System (ADS)

Wright, Robert; Abraham, Edo; Parpas, Panos; Stoianov, Ivan

2015-12-01

The operation of water distribution networks (WDN) with a dynamic topology is a recently pioneered approach for the advanced management of District Metered Areas (DMAs) that integrates novel developments in hydraulic modeling, monitoring, optimization, and control. A common practice for leakage management is the sectorization of WDNs into small zones, called DMAs, by permanently closing isolation valves. This facilitates water companies to identify bursts and estimate leakage levels by measuring the inlet flow for each DMA. However, by permanently closing valves, a number of problems have been created including reduced resilience to failure and suboptimal pressure management. By introducing a dynamic topology to these zones, these disadvantages can be eliminated while still retaining the DMA structure for leakage monitoring. In this paper, a novel optimization method based on sequential convex programming (SCP) is outlined for the control of a dynamic topology with the objective of reducing average zone pressure (AZP). A key attribute for control optimization is reliable convergence. To achieve this, the SCP method we propose guarantees that each optimization step is strictly feasible, resulting in improved convergence properties. By using a null space algorithm for hydraulic analyses, the computations required are also significantly reduced. The optimized control is actuated on a real WDN operated with a dynamic topology. This unique experimental program incorporates a number of technologies set up with the objective of investigating pioneering developments in WDN management. Preliminary results indicate AZP reductions for a dynamic topology of up to 6.5% over optimally controlled fixed topology DMAs. This article was corrected on 12 JAN 2016. See the end of the full text for details.

Distributed Optimal Consensus Over Resource Allocation Network and Its Application to Dynamical Economic Dispatch.

PubMed

Li, Chaojie; Yu, Xinghuo; Huang, Tingwen; He, Xing; Chaojie Li; Xinghuo Yu; Tingwen Huang; Xing He; Li, Chaojie; Huang, Tingwen; He, Xing; Yu, Xinghuo

2018-06-01

The resource allocation problem is studied and reformulated by a distributed interior point method via a -logarithmic barrier. By the facilitation of the graph Laplacian, a fully distributed continuous-time multiagent system is developed for solving the problem. Specifically, to avoid high singularity of the -logarithmic barrier at boundary, an adaptive parameter switching strategy is introduced into this dynamical multiagent system. The convergence rate of the distributed algorithm is obtained. Moreover, a novel distributed primal-dual dynamical multiagent system is designed in a smart grid scenario to seek the saddle point of dynamical economic dispatch, which coincides with the optimal solution. The dual decomposition technique is applied to transform the optimization problem into easily solvable resource allocation subproblems with local inequality constraints. The good performance of the new dynamical systems is, respectively, verified by a numerical example and the IEEE six-bus test system-based simulations.

Promotion of redox and stability features of doped Ce-W-Ti for NH3-SCR reaction over a wide temperature range

NASA Astrophysics Data System (ADS)

Zhao, Kun; Han, Weiliang; Lu, Gongxuan; Lu, Jiangyin; Tang, Zhicheng; Zhen, Xinping

2016-08-01

In this study, transition metals Co, Mn, and Cu were introduced into a Ce-W-Ti catalyst to promote low-temperature catalytic activity. Among these metal-modified M/Ce-W-Ti catalysts (M represents Co, Mn, or Cu), the Cu/Ce-W-Ti catalyst with an optimized Cu content of 5 wt.% exhibited more than 90% conversion of nitrogen oxide (NOx) in the selective catalytic reduction by NH3 over a wide temperature range (260-400 °C). This catalyst likewise exhibited higher resistance to SO2 gas and water vapor under severe test conditions. On the basis of the characterization results by powder X-ray diffraction and X-ray photoelectron spectroscopy, we concluded that the superior catalytic properties of the Cu/Ce-W-Ti catalyst could be attributed to the highly dispersed Cu species, which increased the contents of Ce3+ species and adsorbed oxygen species in the catalysts. In addition, the NH3 temperature-programmed desorption results demonstrated that the Cu species doped into the Ce-W-Ti catalysts optimized surface acid content.

Optimization of ion-atomic beam source for deposition of GaN ultrathin films.

PubMed

Mach, Jindřich; Šamořil, Tomáš; Kolíbal, Miroslav; Zlámal, Jakub; Voborny, Stanislav; Bartošík, Miroslav; Šikola, Tomáš

2014-08-01

We describe the optimization and application of an ion-atomic beam source for ion-beam-assisted deposition of ultrathin films in ultrahigh vacuum. The device combines an effusion cell and electron-impact ion beam source to produce ultra-low energy (20-200 eV) ion beams and thermal atomic beams simultaneously. The source was equipped with a focusing system of electrostatic electrodes increasing the maximum nitrogen ion current density in the beam of a diameter of ≈15 mm by one order of magnitude (j ≈ 1000 nA/cm(2)). Hence, a successful growth of GaN ultrathin films on Si(111) 7 × 7 substrate surfaces at reasonable times and temperatures significantly lower (RT, 300 °C) than in conventional metalorganic chemical vapor deposition technologies (≈1000 °C) was achieved. The chemical composition of these films was characterized in situ by X-ray Photoelectron Spectroscopy and morphology ex situ using Scanning Electron Microscopy. It has been shown that the morphology of GaN layers strongly depends on the relative Ga-N bond concentration in the layers.

Silver-dendrimer nanocomposites as oligonucleotide labels for electrochemical stripping detection of DNA hybridization.

PubMed

Jin, Xin; Zhou, Ling; Zhu, Bo; Jiang, Xue; Zhu, Ningning

2018-06-01

Silver-dendrimer nanocomposites were synthesized and used as oligonucleotide labels for electrochemical stripping detection of DNA hybridization. The synthesized silver-dendrimer nanocomposites were characterized by UV-vis spectrophotometry, X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). Ratios of silver/dendrimer were optimized in order to obtain stable nanocomposites with maximal silver loading in the interior of a polymeric shell. The silver-dendrimer nanocomposites were attached to sequence-known DNA probes specific to colitoxin, and used to detect probe hybridization by dissolution of the silver nanoparticles in the interior of dendrimer in a diluted nitric acid, followed by measurement of Ag + ions by anodic stripping voltammetry (ASV). Use of differential pulse voltammetry for the stripping step, along with optimization of the ASV conditions, enabled a detection limit of 0.78 pM. The present strategy, in combination with dendrimer-encapsulated copper labeled oligonucleotides probe reported previously, could potentially be used to detect single or multiple DNA targets in one sample. Copyright © 2018 Elsevier B.V. All rights reserved.

High-quality single-crystal thulium iron garnet films with perpendicular magnetic anisotropy by off-axis sputtering

NASA Astrophysics Data System (ADS)

Wu, C. N.; Tseng, C. C.; Lin, K. Y.; Cheng, C. K.; Yeh, S. L.; Fanchiang, Y. T.; Hong, M.; Kwo, J.

2018-05-01

High-quality single-crystal thulium iron garnet (TmIG) films of 10-30 nm thick were grown by off-axis sputtering at room temperature (RT) followed by post-annealing. X-ray photoelectron spectroscopy (XPS) was employed to determine the TmIG film composition to optimize the growth conditions, along with the aid of x-ray diffraction (XRD) structural analysis and atomic force microscope (AFM) for surface morphology. The optimized films exhibited perpendicular magnetic anisotropy (PMA) and the saturation magnetization at RT was ˜99 emu/cm3, close to the RT bulk value ˜110 emu/cm3 with a very low coercive field of ˜2.4 Oe. We extracted the H⊥ of 1734 Oe and the peak-to-peak linewidth ΔH of ferromagnetic resonance are only about 99 Oe, significantly lower than that of PLD grown TmIG film and bulk single crystals. The high-quality sputtered single-crystal TmIG films show great potential to be integrated with topological insulators or heavy metals with strong spin-orbit coupling for spintronic applications.

Roll-To-Roll Printing of Meter-Scale Composite Transparent Electrodes with Optimized Mechanical and Optical Properties for Photoelectronics.

PubMed

Meng, Xiangchuan; Hu, Xiaotian; Yang, Xia; Yin, Jingping; Wang, Qingxia; Huang, Liqiang; Yu, Zoukangning; Hu, Ting; Tan, Licheng; Zhou, Weihua; Chen, Yiwang

2018-03-14

Flexible transparent electrodes are an indispensable component for flexible optoelectronic devices. In this work, the meter-scale composite transparent electrodes (CTEs) composed of poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) and Ag grid/polyethylene terephthalate (PET) with optimized mechanical and optical properties are demonstrated by slot-die roll-to-roll technique with solution printing method under a low cost ($15-20 per square meter), via control of the viscosity and surface energy of PEDOT:PSS ink as well as the printing parameters. The CTEs show excellent flexibility remaining 98% of the pristine value after bending 2000 times under various bending situations, and the square resistance ( R s ) of CTEs can be reduced to 4.5-5.0 Ω/sq with an appropriate transmittance. Moreover, the optical performances, such as haze, extinction coefficient, and refractive index, are investigated, as compared with indium tin oxide/PET, which are potential for the inexpensive optoelectronic flexible devices. The CTEs could be successfully employed in polymer solar cells with different areas, showing a maximal power conversion efficiency of 8.08%.

Microfluidic Synthesis of Composite Cross-Gradient Materials for Investigating Cell–Biomaterial Interactions

PubMed Central

He, Jiankang; Du, Yanan; Guo, Yuqi; Hancock, Matthew J.; Wang, Ben; Shin, Hyeongho; Wu, Jinhui; Li, Dichen; Khademhosseini, Ali

2010-01-01

Combinatorial material synthesis is a powerful approach for creating composite material libraries for the high-throughput screening of cell–material interactions. Although current combinatorial screening platforms have been tremendously successful in identifying target (termed “hit”) materials from composite material libraries, new material synthesis approaches are needed to further optimize the concentrations and blending ratios of the component materials. Here we employed a microfluidic platform to rapidly synthesize composite materials containing cross-gradients of gelatin and chitosan for investigating cell–biomaterial interactions. The microfluidic synthesis of the cross-gradient was optimized experimentally and theoretically to produce quantitatively controllable variations in the concentrations and blending ratios of the two components. The anisotropic chemical compositions of the gelatin/chitosan cross-gradients were characterized by Fourier transform infrared spectrometry and X-ray photoelectron spectrometry. The three-dimensional (3D) porous gelatin/chitosan cross-gradient materials were shown to regulate the cellular morphology and proliferation of smooth muscle cells (SMCs) in a gradient-dependent manner. We envision that our microfluidic cross-gradient platform may accelerate the material development processes involved in a wide range of biomedical applications. PMID:20721897

Electronic neural networks for global optimization

NASA Technical Reports Server (NTRS)

Thakoor, A. P.; Moopenn, A. W.; Eberhardt, S.

1990-01-01

An electronic neural network with feedback architecture, implemented in analog custom VLSI is described. Its application to problems of global optimization for dynamic assignment is discussed. The convergence properties of the neural network hardware are compared with computer simulation results. The neural network's ability to provide optimal or near optimal solutions within only a few neuron time constants, a speed enhancement of several orders of magnitude over conventional search methods, is demonstrated. The effect of noise on the circuit dynamics and the convergence behavior of the neural network hardware is also examined.

Voronoi Diagram Based Optimization of Dynamic Reactive Power Sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huang, Weihong; Sun, Kai; Qi, Junjian

2015-01-01

Dynamic var sources can effectively mitigate fault-induced delayed voltage recovery (FIDVR) issues or even voltage collapse. This paper proposes a new approach to optimization of the sizes of dynamic var sources at candidate locations by a Voronoi diagram based algorithm. It first disperses sample points of potential solutions in a searching space, evaluates a cost function at each point by barycentric interpolation for the subspaces around the point, and then constructs a Voronoi diagram about cost function values over the entire space. Accordingly, the final optimal solution can be obtained. Case studies on the WSCC 9-bus system and NPCC 140-busmore » system have validated that the new approach can quickly identify the boundary of feasible solutions in searching space and converge to the global optimal solution.« less

An Energy-Aware Trajectory Optimization Layer for sUAS

NASA Astrophysics Data System (ADS)

Silva, William A.

The focus of this work is the implementation of an energy-aware trajectory optimization algorithm that enables small unmanned aircraft systems (sUAS) to operate in unknown, dynamic severe weather environments. The software is designed as a component of an Energy-Aware Dynamic Data Driven Application System (EA-DDDAS) for sUAS. This work addresses the challenges of integrating and executing an online trajectory optimization algorithm during mission operations in the field. Using simplified aircraft kinematics, the energy-aware algorithm enables extraction of kinetic energy from measured winds to optimize thrust use and endurance during flight. The optimization layer, based upon a nonlinear program formulation, extracts energy by exploiting strong wind velocity gradients in the wind field, a process known as dynamic soaring. The trajectory optimization layer extends the energy-aware path planner developed by Wenceslao Shaw-Cortez te{Shaw-cortez2013} to include additional mission configurations, simulations with a 6-DOF model, and validation of the system with flight testing in June 2015 in Lubbock, Texas. The trajectory optimization layer interfaces with several components within the EA-DDDAS to provide an sUAS with optimal flight trajectories in real-time during severe weather. As a result, execution timing, data transfer, and scalability are considered in the design of the software. Severe weather also poses a measure of unpredictability to the system with respect to communication between systems and available data resources during mission operations. A heuristic mission tree with different cost functions and constraints is implemented to provide a level of adaptability to the optimization layer. Simulations and flight experiments are performed to assess the efficacy of the trajectory optimization layer. The results are used to assess the feasibility of flying dynamic soaring trajectories with existing controllers as well as to verify the interconnections between EA-DDDAS components. Results also demonstrate the usage of the trajectory optimization layer in conjunction with a lattice-based path planner as a method of guiding the optimization layer and stitching together subsequent trajectories.

Fuzzy Mixed Assembly Line Sequencing and Scheduling Optimization Model Using Multiobjective Dynamic Fuzzy GA

PubMed Central

Tahriri, Farzad; Dawal, Siti Zawiah Md; Taha, Zahari

2014-01-01

A new multiobjective dynamic fuzzy genetic algorithm is applied to solve a fuzzy mixed-model assembly line sequencing problem in which the primary goals are to minimize the total make-span and minimize the setup number simultaneously. Trapezoidal fuzzy numbers are implemented for variables such as operation and travelling time in order to generate results with higher accuracy and representative of real-case data. An improved genetic algorithm called fuzzy adaptive genetic algorithm (FAGA) is proposed in order to solve this optimization model. In establishing the FAGA, five dynamic fuzzy parameter controllers are devised in which fuzzy expert experience controller (FEEC) is integrated with automatic learning dynamic fuzzy controller (ALDFC) technique. The enhanced algorithm dynamically adjusts the population size, number of generations, tournament candidate, crossover rate, and mutation rate compared with using fixed control parameters. The main idea is to improve the performance and effectiveness of existing GAs by dynamic adjustment and control of the five parameters. Verification and validation of the dynamic fuzzy GA are carried out by developing test-beds and testing using a multiobjective fuzzy mixed production assembly line sequencing optimization problem. The simulation results highlight that the performance and efficacy of the proposed novel optimization algorithm are more efficient than the performance of the standard genetic algorithm in mixed assembly line sequencing model. PMID:24982962

Optimal control of dissipative nonlinear dynamical systems with triggers of coupled singularities

NASA Astrophysics Data System (ADS)

Stevanović Hedrih, K.

2008-02-01

This paper analyses the controllability of motion of nonconservative nonlinear dynamical systems in which triggers of coupled singularities exist or appear. It is shown that the phase plane method is useful for the analysis of nonlinear dynamics of nonconservative systems with one degree of freedom of control strategies and also shows the way it can be used for controlling the relative motion in rheonomic systems having equivalent scleronomic conservative or nonconservative system For the system with one generalized coordinate described by nonlinear differential equation of nonlinear dynamics with trigger of coupled singularities, the functions of system potential energy and conservative force must satisfy some conditions defined by a Theorem on the existence of a trigger of coupled singularities and the separatrix in the form of "an open a spiral form" of number eight. Task of the defined dynamical nonconservative system optimal control is: by using controlling force acting to the system, transfer initial state of the nonlinear dynamics of the system into the final state of the nonlinear dynamics in the minimal time for that optimal control task

Real-time observation of cascaded electronic relaxation processes in p-Fluorotoluene

NASA Astrophysics Data System (ADS)

Hao, Qiaoli; Deng, Xulan; Long, Jinyou; Wang, Yanmei; Abulimiti, Bumaliya; Zhang, Bing

2017-08-01

Ultrafast electronic relaxation processes following two photoexcitation of 400 nm in p-Fluorotoluene (pFT) have been investigated utilizing time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Cascaded electronic relaxation processes started from the electronically excited S2 state are directly imaged in real time and well characterized by two distinct time constants of 85 ± 10 fs and 2.4 ± 0.3 ps. The rapid component corresponds to the lifetime of the initially excited S2 state, including the structure relaxation from the Franck-Condon region to the conical intersection of S2/S1 and the subsequent internal conversion to the highly excited S1 state. While, the slower relaxation constant is attributed to the further internal conversion to the high levels of S0 from the secondarily populated S1 locating in the channel three region. Moreover, dynamical differences with benzene and toluene of analogous structures, including, specifically, the slightly slower relaxation rate of S2 and the evidently faster decay of S1, are also presented and tentatively interpreted as the substituent effects. In addition, photoelectron kinetic energy and angular distributions reveal the feature of accidental resonances with low-lying Rydberg states (the 3p, 4s and 4p states) during the multi-photon ionization process, providing totally unexpected but very interesting information for pFT.

Effect of charge and composition on the structural fluxionality and stability of nine atom tin-bismuth Zintl analogues.

PubMed

Gupta, Ujjwal; Reber, Arthur C; Clayborne, Penee A; Melko, Joshua J; Khanna, Shiv N; Castleman, A W

2008-12-01

Synergistic studies of bismuth doped tin clusters combining photoelectron spectra with first principles theoretical investigations establish that highly charged Zintl ions, observed in the condensed phase, can be stabilized as isolated gas phase clusters through atomic substitution that preserves the overall electron count but reduces the net charge and thereby avoids instability because of coulomb repulsion. Mass spectrometry studies reveal that Sn(8)Bi(-), Sn(7)Bi(2)(-), and Sn(6)Bi(3)(-) exhibit higher abundances than neighboring species, and photoelectron spectroscopy show that all of these heteroatomic gas phase Zintl analogues (GPZAs) have high adiabatic electron detachment energies. Sn(6)Bi(3)(-) is found to be a particularly stable cluster, having a large highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gap. Theoretical calculations demonstrate that the Sn(6)Bi(3)(-) cluster is isoelectronic with the well know Sn(9)(-4) Zintl ion; however, the fluxionality reported for Sn(9)(-4) is suppressed by substituting Sn atoms with Bi atoms. Thus, while the electronic stability of the clusters is dominated by electron count, the size and position of the atoms affects the dynamics of the cluster as well. Substitution with Bi enlarges the cage compared with Sn(9)(-4) making it favorable for endohedral doping, findings which suggest that these cages may find use for building blocks of cluster assembled materials.

In-operando hard X-ray photoelectron spectroscopy study on the impact of current compliance and switching cycles on oxygen and carbon defects in resistive switching Ti/HfO{sub 2}/TiN cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sowinska, Malgorzata, E-mail: sowinska@ihp-microelectronics.com; Bertaud, Thomas; Walczyk, Damian

2014-05-28

In this study, direct experimental materials science evidence of the important theoretical prediction for resistive random access memory (RRAM) technologies that a critical amount of oxygen vacancies is needed to establish stable resistive switching in metal-oxide-metal samples is presented. In detail, a novel in-operando hard X-ray photoelectron spectroscopy technique is applied to non-destructively investigates the influence of the current compliance and direct current voltage sweep cycles on the Ti/HfO{sub 2} interface chemistry and physics of resistive switching Ti/HfO{sub 2}/TiN cells. These studies indeed confirm that current compliance is a critical parameter to control the amount of oxygen vacancies in themore » conducting filaments in the oxide layer during the RRAM cell operation to achieve stable switching. Furthermore, clear carbon segregation towards the Ti/HfO{sub 2} interface under electrical stress is visible. Since carbon impurities impact the oxygen vacancy defect population under resistive switching, this dynamic carbon segregation to the Ti/HfO{sub 2} interface is suspected to negatively influence RRAM device endurance. Therefore, these results indicate that the RRAM materials engineering needs to include all impurities in the dielectric layer in order to achieve reliable device performance.« less

Spectromicroscope for the PHotoelectron Imaging of Nanostructures with X-rays (SPHINX): performance in biology, medicine and geology.

PubMed

Frazer, Bradley H; Girasole, Marco; Wiese, Lisa M; Franz, Torsten; De Stasio, Gelsomina

2004-05-01

Several X-ray PhotoElectron Emission spectroMicroscopes (X-PEEMs) exist around the world at this time. We present recent performance and resolution tests of one of them, the Spectromicroscope for PHotoelectron Imaging of Nanostructures with X-rays (SPHINX) X-PEEM, installed at the University of Wisconsin Synchrotron Radiation Center. With this state-of-the-art instrument we demonstrate chemical analysis capabilities on conducting and insulating specimens of diverse interests, and an unprecedented lateral resolution of 10 nm with monochromatic X-rays and 7.2 nm with ultraviolet illumination.

Photoelectron interference fringes by super intense x-ray laser pulses

NASA Astrophysics Data System (ADS)

Toyota, Koudai; Tolstikhin, Oleg I.; Morishita, Toru; Watanabe, Shinichi

2009-09-01

The photoelectron spectra of H- produced by circularly polarized strong high-frequency laser pulses are theoretically studied. An oscillating substructure in the above-threshold ionization (ATI) peaks is observed, which extends the validity of the earlier findings in the 1D calculations [K. Toyota et al., Phys. Rev. A 76, 043418 (2007)] and 3D calculations for linear polarization [O. I. Tolstikhin, Phys. Rev. A 77, 032712 (2008)]. Its origin is due to an interference between a pair of photoelectron wave packets created in the rising and falling part of the pulse, which appears clearly in the stabilization regime.

Anion photoelectron imaging spectroscopy of glyoxal

NASA Astrophysics Data System (ADS)

Xue, Tian; Dixon, Andrew R.; Sanov, Andrei

2016-09-01

We report a photoelectron imaging study of the radical-anion of glyoxal. The 532 nm photoelectron spectrum provides the first direct spectroscopic determination of the adiabatic electron affinity of glyoxal, EA = 1.10 ± 0.02 eV. This assignment is supported by a Franck-Condon simulation of the experimental spectrum that successfully reproduces the observed spectral features. The vertical detachment energy of the radical-anion is determined as VDE = 1.30 ± 0.04 eV. The reported EA and VDE values are attributed to the most stable (C2h symmetry) isomers of the neutral and the anion.

Angular distribution of photoelectrons from atomic oxygen, nitrogen and carbon. [in upper atmosphere

NASA Technical Reports Server (NTRS)

Manson, S. J.; Kennedy, D. J.; Starace, A. F.; Dill, D.

1974-01-01

The angular distributions of photoelectrons from atomic oxygen, nitrogen, and carbon are calculated. Both Hartree-Fock and Hartree-Slater (Herman-Skillman) wave functions are used for oxygen, and the agreement is excellent; thus only Hartree-Slater functions are used for carbon and nitrogen. The pitch-angle distribution of photoelectrons is discussed, and it is shown that previous approximations of energy-independent isotropic or sin squared theta distributions are at odds with the authors' results, which vary with energy. This variation with energy is discussed, as is the reliability of these calculations.

Photoelectron photoion molecular beam spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Trevor, D.J.

1980-12-01

The use of supersonic molecular beams in photoionization mass spectroscopy and photoelectron spectroscopy to assist in the understanding of photoexcitation in the vacuum ultraviolet is described. Rotational relaxation and condensation due to supersonic expansion were shown to offer new possibilities for molecular photoionization studies. Molecular beam photoionization mass spectroscopy has been extended above 21 eV photon energy by the use of Stanford Synchrotron Radiation Laboratory (SSRL) facilities. Design considerations are discussed that have advanced the state-of-the-art in high resolution vuv photoelectron spectroscopy. To extend gas-phase studies to 160 eV photon energy, a windowless vuv-xuv beam line design is proposed.

Dynamic PET of human liver inflammation: impact of kinetic modeling with optimization-derived dual-blood input function.

PubMed

Wang, Guobao; Corwin, Michael T; Olson, Kristin A; Badawi, Ramsey D; Sarkar, Souvik

2018-05-30

The hallmark of nonalcoholic steatohepatitis is hepatocellular inflammation and injury in the setting of hepatic steatosis. Recent work has indicated that dynamic 18F-FDG PET with kinetic modeling has the potential to assess hepatic inflammation noninvasively, while static FDG-PET did not show a promise. Because the liver has dual blood supplies, kinetic modeling of dynamic liver PET data is challenging in human studies. The objective of this study is to evaluate and identify a dual-input kinetic modeling approach for dynamic FDG-PET of human liver inflammation. Fourteen human patients with nonalcoholic fatty liver disease were included in the study. Each patient underwent one-hour dynamic FDG-PET/CT scan and had liver biopsy within six weeks. Three models were tested for kinetic analysis: traditional two-tissue compartmental model with an image-derived single-blood input function (SBIF), model with population-based dual-blood input function (DBIF), and modified model with optimization-derived DBIF through a joint estimation framework. The three models were compared using Akaike information criterion (AIC), F test and histopathologic inflammation reference. The results showed that the optimization-derived DBIF model improved the fitting of liver time activity curves and achieved lower AIC values and higher F values than the SBIF and population-based DBIF models in all patients. The optimization-derived model significantly increased FDG K1 estimates by 101% and 27% as compared with traditional SBIF and population-based DBIF. K1 by the optimization-derived model was significantly associated with histopathologic grades of liver inflammation while the other two models did not provide a statistical significance. In conclusion, modeling of DBIF is critical for kinetic analysis of dynamic liver FDG-PET data in human studies. The optimization-derived DBIF model is more appropriate than SBIF and population-based DBIF for dynamic FDG-PET of liver inflammation. © 2018 Institute of Physics and Engineering in Medicine.

Optimization of rotor blades for combined structural, dynamic, and aerodynamic properties

NASA Technical Reports Server (NTRS)

He, Cheng-Jian; Peters, David A.

1990-01-01

Optimal helicopter blade design with computer-based mathematical programming has received more and more attention in recent years. Most of the research has focused on optimum dynamic characteristics of rotor blades to reduce vehicle vibration. There is also work on optimization of aerodynamic performance and on composite structural design. This research has greatly increased our understanding of helicopter optimum design in each of these aspects. Helicopter design is an inherently multidisciplinary process involving strong interactions among various disciplines which can appropriately include aerodynamics; dynamics, both flight dynamics and structural dynamics; aeroelasticity: vibrations and stability; and even acoustics. Therefore, the helicopter design process must satisfy manifold requirements related to the aforementioned diverse disciplines. In our present work, we attempt to combine several of these important effects in a unified manner. First, we design a blade with optimum aerodynamic performance by proper layout of blade planform and spanwise twist. Second, the blade is designed to have natural frequencies that are placed away from integer multiples of the rotor speed for a good dynamic characteristics. Third, the structure is made as light as possible with sufficient rotational inertia to allow for autorotational landing, with safe stress margins and flight fatigue life at each cross-section, and with aeroelastical stability and low vibrations. Finally, a unified optimization refines the solution.

Effects of ultrashort laser pulses on angular distributions of photoionization spectra.

PubMed

Ooi, C H Raymond; Ho, W L; Bandrauk, A D

2017-07-27

We study the photoelectron spectra by intense laser pulses with arbitrary time dependence and phase within the Keldysh framework. An efficient semianalytical approach using analytical transition matrix elements for hydrogenic atoms in any initial state enables efficient and accurate computation of the photoionization probability at any observation point without saddle point approximation, providing comprehensive three dimensional photoelectron angular distribution for linear and elliptical polarizations, that reveal the intricate features and provide insights on the photoionization characteristics such as angular dispersions, shift and splitting of photoelectron peaks from the tunneling or above threshold ionization(ATI) regime to non-adiabatic(intermediate) and multiphoton ionization(MPI) regimes. This facilitates the study of the effects of various laser pulse parameters on the photoelectron spectra and their angular distributions. The photoelectron peaks occur at multiples of 2ħω for linear polarization while  odd-ordered peaks are suppressed in the direction perpendicular to the electric field. Short pulses create splitting and angular dispersion where the peaks are strongly correlated to the angles. For MPI and elliptical polarization with shorter pulses the peaks split into doublets and the first peak vanishes. The carrier envelope phase(CEP) significantly affects the ATI spectra while the Stark effect shifts the spectra of intermediate regime to higher energies due to interference.

Field propagation-induced directionality of carrier-envelope phase-controlled photoemission from nanospheres

DOE PAGES

SuBmann, F.; Seiffert, L.; Zherebtsov, S.; ...

2015-08-12

Near-fields of non-resonantly laser-excited nanostructures enable strong localization of ultrashort light fields and have opened novel routes to fundamentally modify and control electronic strong-field processes. Harnessing spatiotemporally tunable near-fields for the steering of sub-cycle electron dynamics may enable ultrafast optoelectronic devices and unprecedented control in the generation of attosecond electron and photon pulses. Here we utilize unsupported sub-wavelength dielectric nanospheres to generate near-fields with adjustable structure and study the resulting strong-field dynamics via photoelectron imaging. We demonstrate field propagation-induced tunability of the emission direction of fast recollision electrons up to a regime, where nonlinear charge interaction effects become dominant inmore » the acceleration process. In conclusion, our analysis supports that the timing of the recollision process remains controllable with attosecond resolution by the carrier-envelope phase, indicating the possibility to expand near-field-mediated control far into the realm of high-field phenomena.« less

Terahertz control of nanotip photoemission

NASA Astrophysics Data System (ADS)

Wimmer, L.; Herink, G.; Solli, D. R.; Yalunin, S. V.; Echternkamp, K. E.; Ropers, C.

2014-06-01

The active control of matter by strong electromagnetic fields is of growing importance, with applications all across the optical spectrum from the extreme-ultraviolet to the far-infrared. In recent years, phase-stable terahertz fields have shown tremendous potential for observing and manipulating elementary excitations in solids. In the gas phase, on the other hand, driving free charges with terahertz transients provides insight into ultrafast ionization dynamics. Developing such approaches for locally enhanced terahertz fields in nanostructures will create new means to govern electron currents on the nanoscale. Here, we use single-cycle terahertz transients to demonstrate extensive control over nanotip photoelectron emission. The terahertz near-field is shown to either enhance or suppress photocurrents, with the tip acting as an ultrafast rectifying diode. We record phase-resolved sub-cycle dynamics and find spectral compression and expansion arising from electron propagation within the terahertz near-field. These interactions produce rich spectro-temporal features and offer unprecedented control over ultrashort free electron pulses for imaging and diffraction.