The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields.

PubMed

Jochim, Bethany; Siemering, R; Zohrabi, M; Voznyuk, O; Mahowald, J B; Schmitz, D G; Betsch, K J; Berry, Ben; Severt, T; Kling, Nora G; Burwitz, T G; Carnes, K D; Kling, M F; Ben-Itzhak, I; Wells, E; de Vivie-Riedle, R

2017-06-30

Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A combined experimental and theoretical investigation of strong-field ionization followed by hydrogen elimination in the hydrocarbon series C 2 D 2 , C 2 D 4 and C 2 D 6 reveals that the photofragment angular distributions can only be understood when the field-dressed orbitals rather than the field-free orbitals are considered. Our measured angular distributions and intensity dependence show that these field-dressed orbitals can have strong Rydberg character for certain orientations of the molecule relative to the laser polarization and that they may contribute significantly to the hydrogen elimination dissociative ionization yield. These findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields.

Differential electron emission from polycyclic aromatic hydrocarbon molecules under fast ion impact

DOE PAGES

Biswas, Shubhadeep; Champion, Christophe; Weck, P. F.; ...

2017-07-17

Interaction between polycyclic aromatic hydrocarbon (PAH) molecule and energetic ion is a subject of interest in different areas of modern physics. Here, we present measurements of energy and angular distributions of absolute double differential electron emission cross section for coronene (C 24H 12) and fluorene (C 13H 10) molecules under fast bare oxygen ion impact. For coronene, the angular distributions of the low energy electrons are quite different from that of simpler targets like Ne or CH 4, which is not the case for fluorene. The behaviour of the higher electron energy distributions for both the targets are similar tomore » that for simple targets. In case of coronene, a clear signature of plasmon resonance is observed in the analysis of forward-backward angular asymmetry of low energy electron emission. For fluorene, such signature is not identified probably due to lower oscillator strength of plasmon compared to the coronene. The theoretical calculation based on the first-order Born approximation with correct boundary conditions (CB1), in general, reproduced the experimental observations qualitatively, for both the molecules, except in the low energy region for coronene, which again indicates the role of collective excitation. Single differential and total cross sections are also deduced. An overall comparative study is presented.« less

Relativistic properties of a molecule: energy, linear momentum, angular momentum and boost momentum to order 1/c 2

NASA Astrophysics Data System (ADS)

Cameron, Robert P.; Cotter, J. P.

2018-05-01

We give an explicit and general description of the energy, linear momentum, angular momentum and boost momentum of a molecule to order 1/c 2, where it necessary to take account of kinetic contributions made by the electrons and nuclei as well as electromagnetic contributions made by the intramolecular field. A wealth of interesting subtleties are encountered that are not seen at order 1/c 0, including relativistic Hall shifts, anomalous velocities and hidden momenta. Some of these have well known analogues in solid state physics.

Variational Calculations of Ro-Vibrational Energy Levels and Transition Intensities for Tetratomic Molecules

NASA Technical Reports Server (NTRS)

Schwenke, David W.; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

A description is given of an algorithm for computing ro-vibrational energy levels for tetratomic molecules. The expressions required for evaluating transition intensities are also given. The variational principle is used to determine the energy levels and the kinetic energy operator is simple and evaluated exactly. The computational procedure is split up into the determination of one dimensional radial basis functions, the computation of a contracted rotational-bending basis, followed by a final variational step coupling all degrees of freedom. An angular basis is proposed whereby the rotational-bending contraction takes place in three steps. Angular matrix elements of the potential are evaluated by expansion in terms of a suitable basis and the angular integrals are given in a factorized form which simplifies their evaluation. The basis functions in the final variational step have the full permutation symmetries of the identical particles. Sample results are given for HCCH and BH3.

Thermodynamics properties study of diatomic molecules with q-deformed modified Poschl-Teller plus Manning Rosen non-central potential in D dimensions using SUSYQM approach

NASA Astrophysics Data System (ADS)

Suparmi, A.; Cari, C.; Pratiwi, B. N.

2016-04-01

D-dimensional Dirac equation of q-deformed modified Poschl-Teller plus Manning Rosen non-central potential was solved using supersymmetric quantum mechanics (SUSY QM). The relativistic energy spectra were analyzed by using SUSY QM and shape invariant properties from radial part of D dimensional Dirac equation and the angular quantum numbers were obtained from angular part of D dimensional Dirac equation. The SUSY operators was used to generate the D dimensional relativistic wave functions both for radial and angular parts. In the non-relativistic limit, the relativistic energy equation was reduced to the non-relativistic energy. In the classical limit, the partition function of vibrational, the specific heat of vibrational, and the mean energy of vibrational of some diatomic molecules were calculated from the equation of non-relativistic energy with the help of error function and Mat-lab 2011.

Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor.

PubMed

Averbukh, I S; Arvieu, R

2001-10-15

Semiclassical catastrophes in the dynamics of a quantum rotor (molecule) driven by a strong time-varying field are considered. We show that for strong enough fields, a sharp peak in the rotor angular distribution can be achieved via a time-domain focusing phenomenon, followed by the formation of rainbowlike angular structures. A strategy leading to the enhanced angular squeezing is proposed that uses a specially designed sequence of pulses. The predicted effects can be observed in many processes, ranging from molecular alignment (orientation) by laser fields to heavy-ion collisions, and the trapping of cold atoms by a standing light wave.

Angular resolution and range of dipole-dipole correlations in water

NASA Astrophysics Data System (ADS)

Mathias, Gerald; Tavan, Paul

2004-03-01

We investigate the dipolar correlations in liquid water at angular resolution by molecular-dynamics simulations of a large periodic simulation system containing about 40 000 molecules. Because we are particularly interested in the long-range ordering, we use a simple three-point model for these molecules. The electrostatics is treated both by Ewald summation and by minimum image truncation combined with a reaction field approach. To gain insight into the angular dependence of the simulated dipolar ordering we introduce a suitable expansion of the molecular pair distribution function into a set of two-dimensional correlation functions. We show that these functions enable detailed insights into the shell structure of the dipolar ordering around a given water molecule. For these functions we derive analytical expressions in the particular case in which liquid water is conceived as a dielectric continuum. Comparisons of these continuum models with the correlation functions derived from the simulations yield the key result that liquid water behaves like a continuum dielectric beyond distances of about 15 Å from a given water molecule. We argue that this should be a generic property of water independent of our modeling. By comparison of the results of the two different electrostatics treatments with the continuum description we show that the boundary artifacts occurring in both methods are isotropically distributed and are locally small in the respective boundary regions.

Angular distribution measurement of fragment ions from a molecule using a new beamline consisting of a Grasshopper monochromator

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

Saito, N.; Suzuki, I. H.; Onuki, H.

1989-07-01

Optical characteristics of a new beamline consisting of a premirror, a Grasshopper monochromator, and a refocusing mirror have been investigated. The intensity of the monochromatic soft x-ray was estimated to be about 10/sup 8/ photons/(s 100 mA) at 500 eV with the storage electron energy of 600 MeV and the minimum slit width. This slit width provides a resolution of about 500. Angular distributions of fragment ions from an inner-shell excited nitrogen molecule have been measured with a rotatable time-of-flight mass spectrometer by using this beamline.

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

Biswas, Shubhadeep; Champion, Christophe; Weck, P. F.

Interaction between polycyclic aromatic hydrocarbon (PAH) molecule and energetic ion is a subject of interest in different areas of modern physics. Here, we present measurements of energy and angular distributions of absolute double differential electron emission cross section for coronene (C 24H 12) and fluorene (C 13H 10) molecules under fast bare oxygen ion impact. For coronene, the angular distributions of the low energy electrons are quite different from that of simpler targets like Ne or CH 4, which is not the case for fluorene. The behaviour of the higher electron energy distributions for both the targets are similar tomore » that for simple targets. In case of coronene, a clear signature of plasmon resonance is observed in the analysis of forward-backward angular asymmetry of low energy electron emission. For fluorene, such signature is not identified probably due to lower oscillator strength of plasmon compared to the coronene. The theoretical calculation based on the first-order Born approximation with correct boundary conditions (CB1), in general, reproduced the experimental observations qualitatively, for both the molecules, except in the low energy region for coronene, which again indicates the role of collective excitation. Single differential and total cross sections are also deduced. An overall comparative study is presented.« less

Matrix elements of explicitly correlated Gaussian basis functions with arbitrary angular momentum

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

Joyce, Tennesse; Varga, Kálmán

2016-05-14

A new algorithm for calculating the Hamiltonian matrix elements with all-electron explicitly correlated Gaussian functions for quantum-mechanical calculations of atoms with arbitrary angular momentum is presented. The calculations are checked on several excited states of three and four electron systems. The presented formalism can be used as unified framework for high accuracy calculations of properties of small atoms and molecules.

Impulsive Collision Dynamics of CO Super Rotors from an Optical Centrifuge.

PubMed

Murray, Matthew J; Ogden, Hannah M; Toro, Carlos; Liu, Qingnan; Mullin, Amy S

2016-11-18

We report state-resolved collision dynamics for CO molecules prepared in an optical centrifuge and measured with high-resolution transient IR absorption spectroscopy. Time-resolved polarization-sensitive measurements of excited CO molecules in the J=29 rotational state reveal that the oriented angular momentum of CO rotors is relaxed by impulsive collisions. The translational energy gains for molecules in the initial plane of rotation are threefold larger than for randomized angular momentum orientations, indicating the presence of anisotropic kinetic energy. The transient data show enhanced population for CO molecules in the initial plane of rotation immediately following the optical centrifuge pulse. A comparison with previous CO 2 super rotor studies illustrates the behavior of molecular gyroscopes; spatial reorientation of CO 2 J=76 rotors takes substantially longer than that for CO J=29 rotors, despite similarities in classical rotational period and rotational energy gap. High-resolution transient IR absorption measurements of the CO J=29-39 rotational states show that the collisional depopulation rates increase with J quantum number. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Observation of pendular butterfly Rydberg molecules

PubMed Central

Niederprüm, Thomas; Thomas, Oliver; Eichert, Tanita; Lippe, Carsten; Pérez-Ríos, Jesús; Greene, Chris H.; Ott, Herwig

2016-01-01

Engineering molecules with a tunable bond length and defined quantum states lies at the heart of quantum chemistry. The unconventional binding mechanism of Rydberg molecules makes them a promising candidate to implement such tunable molecules. A very peculiar type of Rydberg molecules are the so-called butterfly molecules, which are bound by a shape resonance in the electron–perturber scattering. Here we report the observation of these exotic molecules and employ their exceptional properties to engineer their bond length, vibrational state, angular momentum and orientation in a small electric field. Combining the variable bond length with their giant dipole moment of several hundred Debye, we observe counter-intuitive molecules which locate the average electron position beyond the internuclear distance. PMID:27703143

Reactive Collisions in Crossed Molecular Beams

DOE R&D Accomplishments Database

Herschbach, D. R.

1962-02-01

The distribution of velocity vectors of reaction products is discussed with emphasis on the restrictions imposed by the conservation laws. The recoil velocity that carries the products away from the center of mass shows how the energy of reaction is divided between internal excitation and translation. Similarly, the angular distributions, as viewed from the center of mass, reflect the partitioning of the total angular momentum between angular momenta of individual molecules and orbital angular momentum associated with their relative motion. Crossed-beam studies of several reactions of the type M + RI yields R + MI are described, where M = K, Rb, Cs, and R = CH{sub 3}, C{sub 3}H{sub 5}, etc. The results show that most of the energy of reaction goes into internal excitation of the products and that the angular distribution is quite anisotropic, with most of the MI recoiling backward (and R forward) with respect to the incoming K beam. (auth)

H and H2 NMR properties in amorphous hydrogenated silicon (a-Si:H)

NASA Astrophysics Data System (ADS)

Lee, Sook

1986-07-01

It is shown that the basic NMR properties of ortho-H2 molecules with a rotational angular momentum J and a spin angular momentum I under the influence of a completely asymmetric crystalline field in an amorphous matrix can be described by an effective nuclear spin Hamiltonian which contains only the nuclear spin angular momentum operators (Ii), but is independent of the molecular rotational angular momentum operators (Ji). By directly applying the existing magnetic-resonance theories to this effective nuclear spin Hamiltonian, a simple description is presented for various static and dynamic NMR properties of the ortho-H2 NMR centers in amorphous hydrogenated silicon (a-Si:H), thereby resolving many difficulties and uncertainties encountered in understanding and explaining the H and H2 NMR observations in a-Si:H.

The angular structure of ONC201, a TRAIL pathway-inducing compound, determines its potent anti-cancer activity

PubMed Central

Wagner, Jessica; Kline, Christina Leah; Pottorf, Richard S.; Nallaganchu, Bhaskara Rao; Olson, Gary L.; Dicker, David T.; Allen, Joshua E.; El-Deiry, Wafik S.

2014-01-01

We previously identified TRAIL-inducing compound 10 (TIC10), also known as NSC350625 or ONC201, from a NCI chemical library screen as a small molecule that has potent anti-tumor efficacy and a benign safety profile in preclinical cancer models. The chemical structure that was originally published by Stahle, et. al. in the patent literature was described as an imidazo[1,2-a]pyrido[4,3-d]pyrimidine derivative. The NCI and others generally accepted this as the correct structure, which was consistent with the mass spectrometry analysis outlined in the publication by Allen et. al. that first reported the molecule's anticancer properties. A recent publication demonstrated that the chemical structure of ONC201 material from the NCI is an angular [3,4-e] isomer of the originally disclosed, linear [4,3-d] structure. Here we confirm by NMR and X-ray structural analysis of the dihydrochloride salt form that the ONC201 material produced by Oncoceutics is the angular [3,4-e] structure and not the linear structure originally depicted in the patent literature and by the NCI. Similarly, in accordance with our biological evaluation, the previously disclosed anti-cancer activity is associated with the angular structure and not the linear isomer. Together these studies confirm that ONC201, produced by Oncoceutics or obtained from the NCI, possesses an angular [3,4-e] structure that represents the highly active anti-cancer compound utilized in prior preclinical studies and now entering clinical trials in advanced cancers. PMID:25587031

The angular structure of ONC201, a TRAIL pathway-inducing compound, determines its potent anti-cancer activity.

PubMed

Wagner, Jessica; Kline, Christina Leah; Pottorf, Richard S; Nallaganchu, Bhaskara Rao; Olson, Gary L; Dicker, David T; Allen, Joshua E; El-Deiry, Wafik S

2014-12-30

We previously identified TRAIL-inducing compound 10 (TIC10), also known as NSC350625 or ONC201, from a NCI chemical library screen as a small molecule that has potent anti-tumor efficacy and a benign safety profile in preclinical cancer models. The chemical structure that was originally published by Stahle, et. al. in the patent literature was described as an imidazo[1,2-a]pyrido[4,3-d]pyrimidine derivative. The NCI and others generally accepted this as the correct structure, which was consistent with the mass spectrometry analysis outlined in the publication by Allen et. al. that first reported the molecule's anticancer properties. A recent publication demonstrated that the chemical structure of ONC201 material from the NCI is an angular [3,4-e] isomer of the originally disclosed, linear [4,3-d] structure. Here we confirm by NMR and X-ray structural analysis of the dihydrochloride salt form that the ONC201 material produced by Oncoceutics is the angular [3,4-e] structure and not the linear structure originally depicted in the patent literature and by the NCI. Similarly, in accordance with our biological evaluation, the previously disclosed anti-cancer activity is associated with the angular structure and not the linear isomer. Together these studies confirm that ONC201, produced by Oncoceutics or obtained from the NCI, possesses an angular [3,4-e] structure that represents the highly active anti-cancer compound utilized in prior preclinical studies and now entering clinical trials in advanced cancers.

Infrared Atmospheric Emission. I.

DTIC Science & Technology

1982-03-01

work efitrely in the I-i coupling scheme. Since the electrostatic energies are usually given in a coupling scheme resulting in total orbital angular...For heteronuclear diatomic molecules, the case either molecule or atom. The energy lor sufered IR emission does not necessitate the electronic...apparently to work sufficiently pood in many cases, they are not ccurate enough . .. . . .. . . . . . .... . .1 6 S for the computation of the

On the gas-phase formation of the HCO radical: accurate quantum study of the H+CO radiative association

NASA Astrophysics Data System (ADS)

Stoecklin, Thierry; Halvick, Philippe; Yu, Hua-Gen; Nyman, Gunnar; Ellinger, Yves

2018-04-01

We present the first quantum study of the radiative association of H and CO to form the HCO molecule within a time-independent approach. We use a recently published 3D potential energy surface of spectroscopic accuracy and two 3D dipole moment surfaces, which were calculated for this study. We discuss the variation of the radiative association cross-section as a function of both the rotational angular momentum of CO and the total angular momentum and use the uniform J-shifting approach to obtain the global radiative association rate coefficient. The effect of the saddle point separating the HCO molecule from the H+CO reactants and the main features of the radiative association cross-sections are analysed and discussed. The calculated rate coefficient is below 10-23 cm3 molecule-1 s-1 for temperatures lower than 30 K, and increases up to 5 × 10-20 cm3 molecule-1 s-1 at T = 300 K. These results demonstrate that the gas-phase H+CO radiative association cannot be the process at the origin of the sequence leading to the formation of methanol in a cold interstellar medium.

Spin relaxation in ultracold collisions of molecular radicals with alkali-metal atoms

NASA Astrophysics Data System (ADS)

Tscherbul, Timur; Klos, Jacek; Zukowski, Piotr

2016-05-01

We present accurate quantum scattering calculations of spin relaxation in ultracold collisions of alkali-metal atoms and polar 2 Σ molecules CaH, SrF, and SrOH. The calculations employ state-of-the-art ab initio interaction potentials and a rigorous quantum theory of atom-molecule collisions in a magnetic field based on the total angular momentum representation. We will further discuss the relevance of the results to atom-molecule sympathetic cooling experiments in a magnetic trap.

Quantum rotor model for a Bose-Einstein condensate of dipolar molecules.

PubMed

Armaitis, J; Duine, R A; Stoof, H T C

2013-11-22

We show that a Bose-Einstein condensate of heteronuclear molecules in the regime of small and static electric fields is described by a quantum rotor model for the macroscopic electric dipole moment of the molecular gas cloud. We solve this model exactly and find the symmetric, i.e., rotationally invariant, and dipolar phases expected from the single-molecule problem, but also an axial and planar nematic phase due to many-body effects. Investigation of the wave function of the macroscopic dipole moment also reveals squeezing of the probability distribution for the angular momentum of the molecules.

Angular momentum transport with twisted exciton wave packets

NASA Astrophysics Data System (ADS)

Zang, Xiaoning; Lusk, Mark T.

2017-10-01

A chain of cofacial molecules with CN or CN h symmetry supports excitonic states with a screwlike structure. These can be quantified with the combination of an axial wave number and an azimuthal winding number. Combinations of these states can be used to construct excitonic wave packets that spiral down the chain with well-determined linear and angular momenta. These twisted exciton wave packets can be created and annihilated using laser pulses, and their angular momentum can be optically modified during transit. This allows for the creation of optoexcitonic circuits in which information, encoded in the angular momentum of light, is converted into excitonic wave packets that can be manipulated, transported, and then reemitted. A tight-binding paradigm is used to demonstrate the key ideas. The approach is then extended to quantify the evolution of twisted exciton wave packets in a many-body, multilevel time-domain density functional theory setting. In both settings, numerical methods are developed that allow the site-to-site transfer of angular momentum to be quantified.

Influence of the photon orbital angular momentum on electric dipole transitions: negative experimental evidence.

PubMed

Giammanco, F; Perona, A; Marsili, P; Conti, F; Fidecaro, F; Gozzini, S; Lucchesini, A

2017-01-15

We describe an experiment of atomic spectroscopy devoted to ascertaining whether the orbital angular momentum (OAM) of photons has the same property of interacting with atoms or molecules as occurs for the spin angular momentum (SAM). In our experiment, rubidium vapors are excited by means of laser radiation with different combinations of OAM and SAM, particularly selected to inhibit or enhance the fluorescence according to the selection rules for the electric dipole transitions between the fundamental state and the first excited doublet. Our results clearly show that an electric-dipole-type transition is insensitive to the OAM value, and provide an original validation of a problem long debated in theoretical works.

Quantum angular momentum diffusion of rigid bodies

NASA Astrophysics Data System (ADS)

Papendell, Birthe; Stickler, Benjamin A.; Hornberger, Klaus

2017-12-01

We show how to describe the diffusion of the quantized angular momentum vector of an arbitrarily shaped rigid rotor as induced by its collisional interaction with an environment. We present the general form of the Lindblad-type master equation and relate it to the orientational decoherence of an asymmetric nanoparticle in the limit of small anisotropies. The corresponding diffusion coefficients are derived for gas particles scattering off large molecules and for ambient photons scattering off dielectric particles, using the elastic scattering amplitudes.

A comparative study of methods for describing non-adiabatic coupling: diabatic representation of the 1Sigma +/1Pi HOH and HHO conical intersections

NASA Astrophysics Data System (ADS)

Dobbyn, Abigail J.; Knowles, Peter J.

A number of established techniques for obtaining diabatic electronic states in small molecules are critically compared for the example of the X and B states in the water molecule, which contribute to the two lowest-energy conical intersections. Integration of the coupling matrix elements and analysis of configuration mixing coefficients both produce reliable diabatic states globally. Methods relying on diagonalization of dipole moment and angular momentum operators are shown to fail in large regions of coordinate space. However, the use of transition angular momentum matrix elements involving the A state, which is degenerate with B at the conical intersections, is successful globally, provided that an appropriate choice of coordinates is made. Long range damping of non-adiabatic coupling to give correct asymptotic mixing angles also is investigated.

An exact variational method to calculate rovibrational spectra of polyatomic molecules with large amplitude motion

NASA Astrophysics Data System (ADS)

Yu, Hua-Gen

2016-08-01

We report a new full-dimensional variational algorithm to calculate rovibrational spectra of polyatomic molecules using an exact quantum mechanical Hamiltonian. The rovibrational Hamiltonian of system is derived in a set of orthogonal polyspherical coordinates in the body-fixed frame. It is expressed in an explicitly Hermitian form. The Hamiltonian has a universal formulation regardless of the choice of orthogonal polyspherical coordinates and the number of atoms in molecule, which is suitable for developing a general program to study the spectra of many polyatomic systems. An efficient coupled-state approach is also proposed to solve the eigenvalue problem of the Hamiltonian using a multi-layer Lanczos iterative diagonalization approach via a set of direct product basis set in three coordinate groups: radial coordinates, angular variables, and overall rotational angles. A simple set of symmetric top rotational functions is used for the overall rotation whereas a potential-optimized discrete variable representation method is employed in radial coordinates. A set of contracted vibrationally diabatic basis functions is adopted in internal angular variables. Those diabatic functions are first computed using a neural network iterative diagonalization method based on a reduced-dimension Hamiltonian but only once. The final rovibrational energies are computed using a modified Lanczos method for a given total angular momentum J, which is usually fast. Two numerical applications to CH4 and H2CO are given, together with a comparison with previous results.

An exact variational method to calculate rovibrational spectra of polyatomic molecules with large amplitude motion

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

Yu, Hua-Gen, E-mail: hgy@bnl.gov

We report a new full-dimensional variational algorithm to calculate rovibrational spectra of polyatomic molecules using an exact quantum mechanical Hamiltonian. The rovibrational Hamiltonian of system is derived in a set of orthogonal polyspherical coordinates in the body-fixed frame. It is expressed in an explicitly Hermitian form. The Hamiltonian has a universal formulation regardless of the choice of orthogonal polyspherical coordinates and the number of atoms in molecule, which is suitable for developing a general program to study the spectra of many polyatomic systems. An efficient coupled-state approach is also proposed to solve the eigenvalue problem of the Hamiltonian using amore » multi-layer Lanczos iterative diagonalization approach via a set of direct product basis set in three coordinate groups: radial coordinates, angular variables, and overall rotational angles. A simple set of symmetric top rotational functions is used for the overall rotation whereas a potential-optimized discrete variable representation method is employed in radial coordinates. A set of contracted vibrationally diabatic basis functions is adopted in internal angular variables. Those diabatic functions are first computed using a neural network iterative diagonalization method based on a reduced-dimension Hamiltonian but only once. The final rovibrational energies are computed using a modified Lanczos method for a given total angular momentum J, which is usually fast. Two numerical applications to CH{sub 4} and H{sub 2}CO are given, together with a comparison with previous results.« less

Energy Deposition and Escape Fluxes Induced by Energetic Solar Wind Ions and ENAs Precipitating into Mars Atmosphere: Accurate Consideration of Energy Transfer Collisions

NASA Astrophysics Data System (ADS)

Kharchenko, V. A.; Lewkow, N.; Gacesa, M.

2014-12-01

Formation and evolution of neutral fluxes of atoms and molecules escaping from the Mars atmosphere have been investigated for the sputtering and photo-chemical mechanisms. Energy and momentum transfer in collisions between the atmospheric gas and fast atoms and molecules have been considered using our recently obtained angular and energy dependent cross sections[1]. We have showed that accurate angular dependent collision cross sections are critical for the description of the energy relaxation of precipitating keV energetic ions/ENAs and for computations of altitude profiles of the fast atom and molecule production rates in recoil collisions. Upward and escape fluxes of the secondary energetic He and O atoms and H2, N2, CO and CO2 molecules, induced by precipitating ENAs, have been determined and their non-thermal energy distribution functions have been computed at different altitudes for different solar conditions. Precipitation and energy deposition of the energetic H2O molecules and products of their dissociations into the Mars atmosphere in the Comet C/2013 A1 (Siding Spring) - Mars interaction have been modeled using accurate cross sections. Reflection of precipitating ENAs by the Mars atmosphere has been analyzed in detail. [1] N. Lewkow and V. Kharchenko, "Precipitation of Energetic Neutral Atoms and Escape Fluxes induced from the Mars Atmosphere, ApJ, v.790, p.98 (2014).

Effects on a Landau-type system for a neutral particle with no permanent electric dipole moment subject to the Kratzer potential in a rotating frame.

PubMed

Oliveira, Abinael B; Bakke, Knut

2016-06-01

The behaviour of a neutral particle (atom, molecule) with an induced electric dipole moment in a region with a uniform effective magnetic field under the influence of the Kratzer potential (Kratzer 1920 Z. Phys. 3 , 289-307. (doi:10.1007/BF01327754)), and rotating effects is analysed. It is shown that the degeneracy of the Landau-type levels is broken and the angular frequency of the system acquires a new contribution that stems from the rotation effects. Moreover, in the search for bound state solutions, it is shown that the possible values of this angular frequency of the system are determined by the quantum numbers associated with the radial modes and the angular momentum, the angular velocity of the rotating frame and by the parameters associated with the Kratzer potential.

Tunable orbital angular momentum in high-harmonic generation

PubMed Central

Gauthier, D.; Ribič, P. Rebernik; Adhikary, G.; Camper, A.; Chappuis, C.; Cucini, R.; DiMauro, L. F.; Dovillaire, G.; Frassetto, F.; Géneaux, R.; Miotti, P.; Poletto, L.; Ressel, B.; Spezzani, C.; Stupar, M.; Ruchon, T.; De Ninno, G.

2017-01-01

Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly nonlinear light–matter interactions, and the disentanglement and independent control of the intrinsic and extrinsic components of the photon's angular momentum at short-wavelengths. The methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules and violation of dipolar selection rules in atoms. PMID:28378741

Cd hyperfine interactions in DNA bases and DNA of mouse strains infected with Trypanosoma cruzi investigated by perturbed angular correlation spectroscopy and ab initio calculations.

PubMed

Petersen, Philippe A D; Silva, Andreia S; Gonçalves, Marcos B; Lapolli, André L; Ferreira, Ana Maria C; Carbonari, Artur W; Petrilli, Helena M

2014-06-03

In this work, perturbed angular correlation (PAC) spectroscopy is used to study differences in the nuclear quadrupole interactions of Cd probes in DNA molecules of mice infected with the Y-strain of Trypanosoma cruzi. The possibility of investigating the local genetic alterations in DNA, which occur along generations of mice infected with T. cruzi, using hyperfine interactions obtained from PAC measurements and density functional theory (DFT) calculations in DNA bases is discussed. A comparison of DFT calculations with PAC measurements could determine the type of Cd coordination in the studied molecules. To the best of our knowledge, this is the first attempt to use DFT calculations and PAC measurements to investigate the local environment of Cd ions bound to DNA bases in mice infected with Chagas disease. The obtained results also allowed the detection of local changes occurring in the DNA molecules of different generations of mice infected with T. cruzi, opening the possibility of using this technique as a complementary tool in the characterization of complicated biological systems.

Molecular-beam Studies of Primary Photochemical Processes

DOE R&D Accomplishments Database

Lee, Y. T.

1982-12-01

Application of the method of molecular-beam photofragmentation translational spectroscopy to the investigation of primary photochemical processes of polyatomic molecules is described. Examples will be given to illustrate how information concerning the energetics, dynamics, and mechanism of dissociation processes can be obtained from the precise measurements of angular and velocity distributions of products in an experiment in which a well-defined beam of molecules is crossed with a laser.

Transfer of Orbital and Spin angular momentum from non-paraxial optical vortex to atomic BEC

NASA Astrophysics Data System (ADS)

Bhowmik, Anal; Mondal, Pradip Kumar; Majumder, Sonjoy; Deb, Bimalendu

2017-04-01

Allen and co-workers first brought up the realization that optical vortex can carry well defined orbital angular momentum (OAM) associated with its spatial mode. Spin angular momentum (SAM) of the light, associated with the polarization, interacts with the internal electronic motion of the atom. The exchange of orbital angular momentum (OAM) between optical vortex and the center-of-mass (CM) motion of an atom or molecule is well known in paraxial approximation. We show that, how the total angular momentum (TAM) of non-paraxial optical vortex is shared with atom, in terms of OAM and SAM. Both the angular momenta are now possible to be transferred to the internal electronic and external CM motion of atom. Here we have studied how the Rabi frequencies of the excitations of two-photon Raman transitions with respect to focusing angles. Also, we investigate the properties of the vortex superposed state for a Bose-Einstein condensate condensate by a single non-paraxial vortex beam. The density distribution of the vortex-antivortex superposed state has a petal structure which is determined by the quantum circulations and proportion of the vortex and antivortex.

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.

Unambiguous observation of F-atom core-hole localization in CF 4 through body-frame photoelectron angular distributions

DOE PAGES

McCurdy, C. W.; Rescigno, T. N.; Trevisan, C. S.; ...

2017-01-17

A dramatic symmetry breaking in K-shell photoionization of the CF 4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. In observing the photoejected electron in coincidence with an F + atomic ion after Auger decay we see how selecting the dissociation path where the core hole was localized was almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF 3 + and F + atoms elucidates themore » underlying physics that derives from the Ne-like valence structure of the F(1s -1) core-excited atom.« less

Crossed-beam experiment for the scattering of low- and intermediate-energy electrons from BF{sub 3}: A comparative study with XF{sub 3} (X = C, N, and CH) molecules

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

Hoshino, M., E-mail: masami-h@sophia.ac.jp; Suga, A.; Kato, H.

2015-07-14

Absolute differential cross sections (DCSs) for electron interaction with BF{sub 3} molecules have been measured in the impact energy range of 1.5–200 eV and recorded over a scattering angle range of 15°–150°. These angular distributions have been normalized by reference to the elastic DCSs of the He atom and integrated by employing a modified phase shift analysis procedure to generate integral cross sections (ICSs) and momentum transfer cross sections (MTCSs). The calculations of DCSs and ICSs have been carried out using an independent atom model under the screening corrected additivity rule (IAM-SCAR). The present elastic DCSs have been found tomore » agree well with the results of IAM-SCAR calculation above 20 eV, and also with a recent Schwinger multichannel calculation below 30 eV. Furthermore, in the comparison with the XF{sub 3} (X = B, C, N, and CH) molecules, the elastic DCSs reveal a similar angular distribution which are approximately equal in magnitude from 30 to 200 eV. This feature suggests that the elastic scattering is dominated virtually by the 3-outer fluorine atoms surrounding the XF{sub 3} molecules. The vibrational DCSs have also been obtained in the energy range of 1.5–15 eV and vibrational analysis based on the angular correlation theory has been carried out to explain the nature of the shape resonances. Limited experiments on vibrational inelastic scattering confirmed the existence of a shape resonance with a peak at 3.8 eV, which is also observed in the vibrational ICS. Finally, the estimated elastic ICSs, MTCSs, as well as total cross sections are compared with the previous cross section data available.« less

Visualizing electron dynamics in organic materials: Charge transport through molecules and angular resolved photoemission

NASA Astrophysics Data System (ADS)

Kümmel, Stephan

Being able to visualize the dynamics of electrons in organic materials is a fascinating perspective. Simulations based on time-dependent density functional theory allow to realize this hope, as they visualize the flow of charge through molecular structures in real-space and real-time. We here present results on two fundamental processes: Photoemission from organic semiconductor molecules and charge transport through molecular structures. In the first part we demonstrate that angular resolved photoemission intensities - from both theory and experiment - can often be interpreted as a visualization of molecular orbitals. However, counter-intuitive quantum-mechanical electron dynamics such as emission perpendicular to the direction of the electrical field can substantially alter the picture, adding surprising features to the molecular orbital interpretation. In a second study we calculate the flow of charge through conjugated molecules. The calculations show in real time how breaks in the conjugation can lead to a local buildup of charge and the formation of local electrical dipoles. These can interact with neighboring molecular chains. As a consequence, collections of ''molecular electrical wires'' can show distinctly different characteristics than ''classical electrical wires''. German Science Foundation GRK 1640.

Tunable orbital angular momentum in high-harmonic generation

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

Gauthier, David; Ribič, P. Rebernik; Adhikary, G.

Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly nonlinear light–matter interactions,more » and the disentanglement and independent control of the intrinsic and extrinsic components of the photon’s angular momentum at short-wavelengths. Finally, the methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules and violation of dipolar selection rules in atoms.« less

Capillary-scale direct measurement of hemoglobin concentration of erythrocytes using photothermal angular light scattering.

PubMed

Kim, Uihan; Song, Jaewoo; Lee, Donghak; Ryu, Suho; Kim, Soocheol; Hwang, Jaehyun; Joo, Chulmin

2015-12-15

We present a direct, rapid and chemical-free detection method for hemoglobin concentration ([Hb]), based on photothermal angular light scattering. The iron oxides contained in hemoglobin molecules exhibit high absorption of 532-nm light and generate heat under the illumination of 532-nm light, which subsequently alters the refractive index of blood. We measured this photothermal change in refractive index by employing angular light scattering spectroscopy with the goal of quantifying [Hb] in blood samples. Highly sensitive [Hb] measurement of blood samples was performed by monitoring the shifts in angularly dispersed scattering patterns from the blood-loaded microcapillary tubes. Our system measured [Hb] over the range of 0.35-17.9 g/dL with a detection limit of ~0.12 g/dL. Our sensor was characterized by excellent correlation with a reference hematology analyzer (r>0.96), and yielded a precision of 0.63 g/dL for a blood sample of 9.0 g/dL. Copyright © 2015 Elsevier B.V. All rights reserved.

Tunable orbital angular momentum in high-harmonic generation

DOE PAGES

Gauthier, David; Ribič, P. Rebernik; Adhikary, G.; ...

2017-04-05

Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly nonlinear light–matter interactions,more » and the disentanglement and independent control of the intrinsic and extrinsic components of the photon’s angular momentum at short-wavelengths. Finally, the methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules and violation of dipolar selection rules in atoms.« less

DUO: Spectra of diatomic molecules

NASA Astrophysics Data System (ADS)

Yurchenko, Sergei N.; Lodi, Lorenzo; Tennyson, Jonathan; Stolyarov, Andrey V.

2016-05-01

Duo computes rotational, rovibrational and rovibronic spectra of diatomic molecules. The software, written in Fortran 2003, solves the Schrödinger equation for the motion of the nuclei for the simple case of uncoupled, isolated electronic states and also for the general case of an arbitrary number and type of couplings between electronic states. Possible couplings include spin-orbit, angular momenta, spin-rotational and spin-spin. Introducing the relevant couplings using so-called Born-Oppenheimer breakdown curves can correct non-adiabatic effects.

Precipitation of energetic neutral atoms and induced non-thermal escape fluxes from the Martian atmosphere

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

Lewkow, N. R.; Kharchenko, V.

2014-08-01

The precipitation of energetic neutral atoms, produced through charge exchange collisions between solar wind ions and thermal atmospheric gases, is investigated for the Martian atmosphere. Connections between parameters of precipitating fast ions and resulting escape fluxes, altitude-dependent energy distributions of fast atoms and their coefficients of reflection from the Mars atmosphere, are established using accurate cross sections in Monte Carlo (MC) simulations. Distributions of secondary hot (SH) atoms and molecules, induced by precipitating particles, have been obtained and applied for computations of the non-thermal escape fluxes. A new collisional database on accurate energy-angular-dependent cross sections, required for description of themore » energy-momentum transfer in collisions of precipitating particles and production of non-thermal atmospheric atoms and molecules, is reported with analytic fitting equations. Three-dimensional MC simulations with accurate energy-angular-dependent cross sections have been carried out to track large ensembles of energetic atoms in a time-dependent manner as they propagate into the Martian atmosphere and transfer their energy to the ambient atoms and molecules. Results of the MC simulations on the energy-deposition altitude profiles, reflection coefficients, and time-dependent atmospheric heating, obtained for the isotropic hard sphere and anisotropic quantum cross sections, are compared. Atmospheric heating rates, thermalization depths, altitude profiles of production rates, energy distributions of SH atoms and molecules, and induced escape fluxes have been determined.« less

Fragilidad y su asociación con mortalidad, hospitalizaciones y dependencia funcional en mexicanos de 60 años o más

PubMed Central

de León González, Enrique Díaz; Pérez, Héctor Eloy Tamez; Hermosillo, Hugo Gutiérrez; Rodríguez, Javier Armando Cedillo; Torres, Gabriela

2016-01-01

Fundamento y objetivo Determinar la asociación entre fragilidad y mortalidad, dependencia funcional, caídas y hospitalizaciones en el Estudio Nacional de Salud y Envejecimiento en México (ENASEM). Sujetos y métodos Estudio prospectivo poblacional en México en el que se seleccionaron sujetos de 60 años o más, que fueron evaluados en las variables de fragilidad durante la primera vuelta del estudio en el año 2001 y que incluyó: dificultad para levantarse de una silla después de haber estado sentado(a) durante largo tiempo, pérdida de peso de 5 kilogramos o más en los últimos dos años y falta de energía. Los sujetos fueron catalogados como robustos, prefrágiles y frágiles cuando tenían cero, una o dos de las características anteriores, respectivamente. La mortalidad, hospitalizaciones, caídas y dependencia funcional fueron evaluadas en la segunda vuelta del estudio en el año 2003. Se calculó el riesgo relativo para cada una de las complicaciones, así como análisis multivariado con regresión de Cox para el caso de mortalidad y regresión logística para el resto. Resultados Los estados de prefragilidad y fragilidad se asociaron independientemente con mortalidad, con índices de riesgo ajustados de 1,61 (intervalo de confianza del 95% [IC 95%] 1,01-2,55) y 1,94 (IC 95% 1,20-3,13), respectivamente. Sólo el estado de fragilidad se asoció independientemente con hospitalización y dependencia funcional, con una razón de momios ajustada de 1,53 (IC 95% 1,13-2,07) y 3,07 (IC 95% 1,76-5,34), respectivamente. No hubo asociación entre los estados de prefragilidad y fragilidad con caídas. Conclusión El estado de fragilidad se asocia independientemente con mortalidad, hospitalizaciones y disfuncionalidad en actividades básicas de la vida diaria en los siguientes dos años en población mexicana. PMID:21612803

Electron Spectroscopy: Ultraviolet and X-Ray Excitation.

ERIC Educational Resources Information Center

Baker, A. D.; And Others

1980-01-01

Reviews recent growth in electron spectroscopy (54 papers cited). Emphasizes advances in instrumentation and interpretation (52); photoionization, cross-sections and angular distributions (22); studies of atoms and small molecules (35); transition, lanthanide and actinide metal complexes (50); organometallic (12) and inorganic compounds (2);…

Linear- and angular-shaped naphthodithiophenes: selective synthesis, properties, and application to organic field-effect transistors.

PubMed

Shinamura, Shoji; Osaka, Itaru; Miyazaki, Eigo; Nakao, Akiko; Yamagishi, Masakazu; Takeya, Jun; Takimiya, Kazuo

2011-04-06

A straightforward synthetic approach that exploits linear- and angular-shaped naphthodithiophenes (NDTs) being potential as new core structures for organic semiconductors is described. The newly established synthetic procedure involves two important steps; one is the chemoselective Sonogashira coupling reaction on the trifluoromethanesulfonyloxy site over the bromine site enabling selective formation of o-bromoethynylbenzene substructures on the naphthalene core, and the other is a facile ring closing reaction of fused-thiophene rings from the o-bromoethynylbenzene substructures. As a result, three isomeric NDTs, naphtho[2,3-b:6,7-b']dithiophene, naphtho[2,3-b:7,6-b']dithiophenes, and naphtho[2,1-b:6,5-b']dithiophene, are selectively synthesized. Electrochemical and optical measurements of the parent NDTs indicated that the shape of the molecules plays an important role in determining the electronic structure of the compounds; the linear-shaped NDTs formally isoelectronic with naphthacene have lower oxidation potentials and more red-shifted absorption bands than those of the angular-shaped NDTs isoelectronic with chrysene. On the contrary, the performance of the thin-film-based field-effect transistors (FETs) using the dioctyl or diphenyl derivatives were much influenced by the symmetry of the molecules; centrosymmetric derivatives tend to give higher mobility (up to 1.5 cm(2) V(-1) s(-1)) than axisymmetric ones (∼0.06 cm(2) V(-1) s(-1)), implying that the intermolecular orbital overlap in the solid state is influenced by the symmetry of the molecules. These results indicate that the present NDT cores, in particular the linear-shaped, centrosymmetric naphtho[2,3-b:6,7-b']dithiophene, are promising building blocks for the development of organic semiconducting materials. © 2011 American Chemical Society

Electronic structure differences between H(2)-, Fe-, Co-, and Cu-phthalocyanine highly oriented thin films observed using NEXAFS spectroscopy.

PubMed

Willey, T M; Bagge-Hansen, M; Lee, J R I; Call, R; Landt, L; van Buuren, T; Colesniuc, C; Monton, C; Valmianski, I; Schuller, Ivan K

2013-07-21

Phthalocyanines, a class of macrocyclic, square planar molecules, are extensively studied as semiconductor materials for chemical sensors, dye-sensitized solar cells, and other applications. In this study, we use angular dependent near-edge x-ray absorption fine structure (NEXAFS) spectroscopy as a quantitative probe of the orientation and electronic structure of H2-, Fe-, Co-, and Cu-phthalocyanine molecular thin films. NEXAFS measurements at both the carbon and nitrogen K-edges reveal that phthalocyanine films deposited on sapphire have upright molecular orientations, while films up to 50 nm thick deposited on gold substrates contain prostrate molecules. Although great similarity is observed in the carbon and nitrogen K-edge NEXAFS spectra recorded for the films composed of prostrate molecules, the H2-phthalocyanine exhibits the cleanest angular dependence due to its purely out-of-plane π* resonances at the absorption onset. In contrast, organometallic-phthalocyanine nitrogen K-edges have a small in-plane resonance superimposed on this π* region that is due to a transition into molecular orbitals interacting with the 3dx(2)-y(2) empty state. NEXAFS spectra recorded at the metal L-edges for the prostrate films reveal dramatic variations in the angular dependence of specific resonances for the Cu-phthalocyanines compared with the Fe-, and Co-phthalocyanines. The Cu L3,2 edge exhibits a strong in-plane resonance, attributed to its b1g empty state with dx(2)-y(2) character at the Cu center. Conversely, the Fe- and Co- phthalocyanine L3,2 edges have strong out-of-plane resonances; these are attributed to transitions into not only b1g (dz(2)) but also eg states with dxz and dyz character at the metal center.

Direct Imaging of Transient Fano Resonances in N_{2} Using Time-, Energy-, and Angular-Resolved Photoelectron Spectroscopy.

PubMed

Eckstein, Martin; Yang, Chung-Hsin; Frassetto, Fabio; Poletto, Luca; Sansone, Giuseppe; Vrakking, Marc J J; Kornilov, Oleg

2016-04-22

Autoionizing Rydberg states of molecular N_{2} are studied using time-, energy-, and angular-resolved photoelectron spectroscopy. A femtosecond extreme ultraviolet pulse with a photon energy of 17.5 eV excites the resonance and a subsequent IR pulse ionizes the molecule before the autoionization takes place. The angular-resolved photoelectron spectra depend on pump-probe time delay and allow for the distinguishing of two electronic states contributing to the resonance. The lifetime of one of the contributions is determined to be 14±1  fs, while the lifetime of the other appears to be significantly shorter than the time resolution of the experiment. These observations suggest that the Rydberg states in this energy region are influenced by the effect of interference stabilization and merge into a complex resonance.

Theory of liquid crystal orientation under action of light wave field and aligning surfaces

NASA Astrophysics Data System (ADS)

Dadivanyan, A. K.; Chausov, D. N.; Belyaev, V. V.; Barabanova, N. N.; Chausova, O. V.; Kuleshova, Yu D.

2018-03-01

Theoretical models developed in the MRSU group under leadership of Professor Artem Dadivanyan in area of the LC orientation and photo-induced effects are presented. Angular distribution functions of the dye and liquid crystal molecules under action of intensive light beam have been derived. The number of molecules in cluster is estimated. A model of dimers formation in the photoalignment dye is suggested that explains influence of the dye molecular structure on both polar and azimuthal anchoring energy.

The vibrational excitation of hot molecules by low energy electron impact

NASA Astrophysics Data System (ADS)

Kato, H.; Ohkawa, M.; Hoshino, M.; Campbell, L.; Brunger, M. J.; Tanaka, H.

2010-01-01

We report vibrational excitation functions and angular distributions for electron scattering from the ground vibrational quantum (000), the bending vibrational quantum (010) and the unresolved first bending overtone (020) and symmetric stretch (100) modes of the ground-electronic state in hot (750 K) carbon dioxide (CO2) molecules. The excitation function measurements were carried out at incident electron energies in the range of 1-9 eV, and at the electron scattering angles of 30°, 60°, 90° and 120°.

Molecular Beam Chemistry: Reactions of Oxygen Atoms with Halogen Molecules.

DTIC Science & Technology

1982-10-15

nonlinear one has s = 3, r = 1, and n = 3/2. In the "loose" complex the bending modes go over to free rotation of the product diatomit molecule; thus s...contains no adjustable parameters. All observable properties *l of the reaction may be predicted including product velocity and angular dis- tributions...example, P. R. Bevington, Data Reduction and Error Analysis for the Physical Sciences (McGraw-Hill Book Co., New York, 1969). 65. Equation (3) is strictly

Theoretical study of asymmetric super-rotors: Alignment and orientation

NASA Astrophysics Data System (ADS)

Omiste, Juan J.

2018-02-01

We report a theoretical study of the optical centrifuge acceleration of an asymmetric top molecule interacting with an electric static field by solving the time-dependent Schrödinger equation in the rigid rotor approximation. A detailed analysis of the mixing of the angular momentum in both the molecular and the laboratory fixed frames allows us to deepen the understanding of the main features of the acceleration process, for instance, the effective angular frequency of the molecule at the end of the pulse. For the case of the SO2 molecular super-rotor, we show numerically that it rotates around one internal axis and that its dynamics is confined to the plane defined by the polarization axis of the laser, in agreement with experimental findings. Furthermore, we consider the orientation patterns induced by the dc field, showing the characteristics of their structure as a function of the strength of the static field and the initial configuration of the fields.

Line Mixing in Parallel and Perpendicular Bands of CO2: A Further Test of the Refined Robert-Bonamy Formalism

NASA Technical Reports Server (NTRS)

Boulet, C.; Ma, Qiancheng; Tipping, R. H.

2015-01-01

Starting from the refined Robert-Bonamy formalism [Q. Ma, C. Boulet, and R. H. Tipping, J. Chem. Phys. 139, 034305 (2013)], we propose here an extension of line mixing studies to infrared absorptions of linear polyatomic molecules having stretching and bending modes. The present formalism does not neglect the internal degrees of freedom of the perturbing molecules, contrary to the energy corrected sudden (ECS) modeling, and enables one to calculate the whole relaxation matrix starting from the potential energy surface. Meanwhile, similar to the ECS modeling, the present formalism properly accounts for roles played by all the internal angular momenta in the coupling process, including the vibrational angular momentum. The formalism has been applied to the important case of CO2 broadened by N2. Applications to two kinds of vibrational bands (sigma yields sigma and sigma yields pi) have shown that the present results are in good agreement with both experimental data and results derived from the ECS model.

The Rydberg electronic transitions of the hydrogen molecule

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

Babb, J.F.; Chang, E.S.

1992-01-01

Transition energies and relative line strengths, without Boltzmann weighting, for the electric dipole transitions between Rydberg states n{prime}L{prime} and nL of the hydrogen molecule (one electron in a near-hydrogenic state of high n and L, with n the principal quantum number and L the orbital angular momentum quantum number of the electron) are calculated. Since the H{sup +}{sub 2} core is loosely coupled to the Rydberg electron, numerous lines occur, depending on the vector sum of L and the core rotational angular momentum. For the core vibrational quantum numbers v = 0 to 5 the strongest lines among the P,more » Q, and R branches for the lowest 12 core rotational levels are given for the particular transition arrays 6h-5g, 8i-6h, 7i-6h, 8k-7i, and 9l-8k, for which transitions occur in the wave number range 350 to 1,400 cm {sup {minus}1}.« less

Tables of the coefficients A

NASA Technical Reports Server (NTRS)

Chandra, N.

1974-01-01

Numerical coefficients required to express the angular distribution for the rotationally elastic or inelastic scattering of electrons from a diatomic molecule were tabulated for the case of nitrogen and in the energy range from 0.20 eV to 10.0 eV. Five different rotational states are considered.

Quantifying entanglement of rotor chains using basis truncation: Application to dipolar endofullerene peapods.

PubMed

Halverson, Tom; Iouchtchenko, Dmitri; Roy, Pierre-Nicholas

2018-02-21

We propose a variational approach for the calculation of the quantum entanglement entropy of assemblies of rotating dipolar molecules. A basis truncation scheme based on the total angular momentum quantum number is proposed. The method is tested on hydrogen fluoride (HF) molecules confined in C 60 fullerene cages themselves trapped in a nanotube to form a carbon peapod. The rotational degrees of freedom of the HF molecules and dipolar interactions between neighboring molecules are considered in our model Hamiltonian. Both screened and unscreened dipoles are simulated and results are obtained for the ground state and one excited state that is expected to be accessible via a far-infrared collective excitation. The effect of basis truncation on energetic and entanglement properties is examined and discussed in terms of size extensivity. It is empirically found that for unscreened dipoles, a total angular momentum cutoff that increases linearly with the number of rotors is required in order to obtain proper system size scaling of the chemical potential and entanglement entropy. Recent experiments [A. Krachmalnicoff et al., Nat. Chem. 8, 953 (2016)] suggest substantial screening of the HF dipole moment, so much smaller basis sets are required to obtain converged results in this realistic case. Static correlation functions are also computed and are shown to decay much quicker in the case of screened dipoles. Our variational results are also used to test the accuracy of perturbative and pairwise ansatz treatments.

Exploring Molecular Complexity with Alma (EMoCA): High-Angular Observations of SAGITTARIUS~B2(N) at 3~mm

NASA Astrophysics Data System (ADS)

Müller, Holger S. P.; Belloche, Arnaud; Menten, Karl M.; Garrod, Robin T.

2015-06-01

Sagittarius (Sgr for short) B2 is the most massive and luminous star-forming region in our Galaxy, located close to the Galactic Center. We have carried out a molecular line survey with the IRAM~30~m telescope toward its two major sites of star-formation, Sgr~B2(M) and (N). Toward the latter source, which is particularly rich in Complex Organic Molecules (COMs), we detected three molecules for the first time in space, aminoacetonitrile, ethyl formate, and n}-propyl cyanide. We have recently obtained ALMA data of Sgr~B2(N) between ˜84 and ˜111~GHz within Cycle~0 and one additional setup up to 114.4~GHz within Cycle~1. At angular resolutions of 1.8'' and 1.4'', respectively, the two main hot cores, the prolific Sgr~B2(N-LMH) (or Sgr~B2(N)-SMA1) and the likely less evolved Sgr~B2(N)-SMA2 are well separated, and line confusion is reduced greatly for the latter. As a consequence, we have been able to identify the first branched alkyl molecule in space, iso-propyl cyanide, toward Sgr~B2(N)-SMA2. Our ongoing analyses include investigations of cyanides and isocyanides, alkanols and thioalkanols, and deuterated molecules among others. We will present some of our results. A. Belloche et al., A&A 559 (2013) Art. No. A47. A. Belloche et al., Science 345 (2014) 1584.

Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure

DOE PAGES

Mendez, Derek; Watkins, Herschel; Qiao, Shenglan; ...

2016-09-26

During X-ray exposure of a molecular solution, photons scattered from the same molecule are correlated. If molecular motion is insignificant during exposure, then differences in momentum transfer between correlated photons are direct measurements of the molecular structure. In conventional small- and wide-angle solution scattering, photon correlations are ignored. This report presents advances in a new biomolecular structural analysis technique, correlated X-ray scattering (CXS), which uses angular intensity correlations to recover hidden structural details from molecules in solution. Due to its intense rapid pulses, an X-ray free electron laser (XFEL) is an excellent tool for CXS experiments. A protocol is outlinedmore » for analysis of a CXS data set comprising a total of half a million X-ray exposures of solutions of small gold nanoparticles recorded at the Spring-8 Ångström Compact XFEL facility (SACLA). From the scattered intensities and their correlations, two populations of nanoparticle domains within the solution are distinguished: small twinned, and large probably non-twinned domains. Finally, it is shown analytically how, in a solution measurement, twinning information is only accessible via intensity correlations, demonstrating how CXS reveals atomic-level information from a disordered solution of like molecules.« less

Angular-momentum-assisted dissociation of CO in strong optical fields

NASA Astrophysics Data System (ADS)

Mullin, Amy; Ogden, Hannah; Murray, Matthew; Liu, Qingnan; Toro, Carlos

2017-04-01

Filaments are produced in CO gas by intense, chirped laser pulses. Visible emission from C2 is observed as a result of chemical reactions of highly excited CO. At laser intensities greater than 1014 W cm-2, the C2 emission shows a strong dependence on laser polarization. Oppositely chirped pulses of light with ω0 = 800 nm are recombined spatially and temporally to generate angularly accelerating electric fields (up to 30 THz) that either have an instantaneous linear polarization or act as a dynamic polarization grating that oscillates among linear and circular polarizations. The angularly accelerating linear polarization corresponds to an optical centrifuge that concurrently drives molecules into high rotational states (with J 50) and induces strong-field dissociation. Higher order excitation is observed for the time-varying laser polarization configuration that does not induce rotational excitation. The results indicate that the presence of rotational angular momentum lowers the threshold for CO dissociation in strong optical fields by coupling nuclear and electronic degrees of freedom. Support from NSF CHE-1058721 and the University of Maryland.

A new potential energy surface for vibration-vibration coupling in HF-HF collisions. Formulation and quantal scattering calculations

NASA Astrophysics Data System (ADS)

Schwenke, David W.; Truhlar, Donald G.

1988-04-01

We present new ab initio calculations of the HF-HF interaction potential for the case where both molecules are simultaneously displaced from their equilibrium internuclear distance. These and previous ab initio calculations are then fit to a new analytic representation which is designed to be efficient to evaluate and to provide an especially faithful account of the forces along the vibrational coordinates. We use the new potential for two sets of quantal scattering calculations for collisions in three dimensions with total angular momentum zero. First we test that the angular harmonic representation of the anisotropy is adequate by comparing quantal rigid rotator calculations to those carried out for potentials involving higher angular harmonics and for which the expansion in angular harmonics is systematically increased to convergence. Then we carry out large-scale quantal calculations of vibration-vibration energy transfer including the coupling of both sets of vibrational and rotational coordinates. These calculations indicate that significant rotational energy transfer accompanies the vibration-to-vibration energy transfer process.

Analisis de mecanismos alternos de coordinacion de la operacion en los puertos fronterizos entre Mexico y Estados Unidos.

DOT National Transportation Integrated Search

2001-12-01

Identificar los problemas de coordinacin Intersectoriales entre dependencias pblicas de Mxico, los problemas originados por la falta de Coordinacin Binacional en los Puertos Fronterizos y los costos que se derivan de estos problemas. Desarrol...

Optical control of recovery speed of photoinduced third-harmonic generation in azo-copolymer thin films

NASA Astrophysics Data System (ADS)

Lin, Jian Hung; Lai, Ngoc Diep; Hsu, Chia Chen

2006-03-01

Recovery speed of photoinduced third-harmonic (TH) generation in azo-copolymer thin films can be controlled by a nanosecond laser excitation. When the excitation is tuned on, the TH signal decreases because of angular hole burning and angular redistribution effects. After turning off the excitation, the TH signal can recover to its original level either within 1min (high intensity excitation) or longer than several days (low intensity excitation). The fast recovery of the TH signal is attributed to the increase of temperature in the sample that causes molecules to more easily reorient and return to the original trans form.

Adsorption of naphthalene and ozone on atmospheric air/ice interfaces coated with surfactants: a molecular simulation study.

PubMed

Liyana-Arachchi, Thilanga P; Valsaraj, Kalliat T; Hung, Francisco R

2012-03-15

The adsorption of gas-phase naphthalene and ozone molecules onto air/ice interfaces coated with different surfactant species (1-octanol, 1-hexadecanol, or 1-octanal) was investigated using classical molecular dynamics (MD) simulations. Naphthalene and ozone exhibit a strong preference to be adsorbed at the surfactant-coated air/ice interfaces, as opposed to either being dissolved into the bulk of the quasi-liquid layer (QLL) or being incorporated into the ice crystals. The QLL becomes thinner when the air/ice interface is coated with surfactant molecules. The adsorption of both naphthalene and ozone onto surfactant-coated air/ice interfaces is enhanced when compared to bare air/ice interface. Both naphthalene and ozone tend to stay dissolved in the surfactant layer and close to the QLL, rather than adsorbing on top of the surfactant molecules and close to the air region of our systems. Surfactants prefer to orient at a tilted angle with respect to the air/ice interface; the angular distribution and the most preferred angle vary depending on the hydrophilic end group, the length of the hydrophobic tail, and the surfactant concentration at the air/ice interface. Naphthalene prefers to have a flat orientation on the surfactant coated air/ice interface, except at high concentrations of 1-hexadecanol at the air/ice interface; the angular distribution of naphthalene depends on the specific surfactant and its concentration at the air/ice interface. The dynamics of naphthalene molecules at the surfactant-coated air/ice interface slow down as compared to those observed at bare air/ice interfaces. The presence of surfactants does not seem to affect the self-association of naphthalene molecules at the air/ice interface, at least for the specific surfactants and the range of concentrations considered in this study.

End-to-end distance and contour length distribution functions of DNA helices

NASA Astrophysics Data System (ADS)

Zoli, Marco

2018-06-01

I present a computational method to evaluate the end-to-end and the contour length distribution functions of short DNA molecules described by a mesoscopic Hamiltonian. The method generates a large statistical ensemble of possible configurations for each dimer in the sequence, selects the global equilibrium twist conformation for the molecule, and determines the average base pair distances along the molecule backbone. Integrating over the base pair radial and angular fluctuations, I derive the room temperature distribution functions as a function of the sequence length. The obtained values for the most probable end-to-end distance and contour length distance, providing a measure of the global molecule size, are used to examine the DNA flexibility at short length scales. It is found that, also in molecules with less than ˜60 base pairs, coiled configurations maintain a large statistical weight and, consistently, the persistence lengths may be much smaller than in kilo-base DNA.

Microsecond Resolution of Single-Molecule Rotation Catalyzed by Molecular Motors

PubMed Central

Hornung, Tassilo; Martin, James; Spetzler, David; Ishmukhametov, Robert; Frasch, Wayne D.

2017-01-01

Single-molecule measurements of rotation catalyzed by the F1-ATPase or the FoF1 ATP synthase have provided new insights into the molecular mechanisms of the F1 and Fo molecular motors. We recently developed a method to record ATPase-driven rotation of F1 or FoF1 in a manner that solves several technical limitations of earlier approaches that were significantly hampered by time and angular resolution, and restricted the duration of data collection. With our approach it is possible to collect data for hours and obtain statistically significant quantities of data on each molecule examined with a time resolution of up to 5 μs at unprecedented signal-to-noise. PMID:21809213

Hyperfine-Structure-Induced Depolarization of Impulsively Aligned I2 Molecules

NASA Astrophysics Data System (ADS)

Thomas, Esben F.; Søndergaard, Anders A.; Shepperson, Benjamin; Henriksen, Niels E.; Stapelfeldt, Henrik

2018-04-01

A moderately intense 450 fs laser pulse is used to create rotational wave packets in gas phase I2 molecules. The ensuing time-dependent alignment, measured by Coulomb explosion imaging with a delayed probe pulse, exhibits the characteristic revival structures expected for rotational wave packets but also a complex nonperiodic substructure and decreasing mean alignment not observed before. A quantum mechanical model attributes the phenomena to coupling between the rotational angular momenta and the nuclear spins through the electric quadrupole interaction. The calculated alignment trace agrees very well with the experimental results.

Orientation and Rotational Motions of Single Molecules by Polarized Total Internal Reflection Fluorescence Microscopy (polTIRFM)

PubMed Central

Beausang, John F.; Sun, Yujie; Quinlan, Margot E.; Forkey, Joseph N.; Goldman, Yale E.

2013-01-01

In this article, we describe methods to detect the spatial orientation and rotational dynamics of single molecules using polarized total internal reflection fluorescence microscopy (polTIRFM). polTIRFM determines the three-dimensional angular orientation and the extent of wobble of a fluorescent probe bound to the macromolecule of interest. We discuss single-molecule versus ensemble measurements, as well as single-molecule techniques for orientation and rotation, and fluorescent probes for orientation studies. Using calmodulin (CaM) as an example of a target protein, we describe a method for labeling CaM with bifunctional rhodamine (BR). We also describe the physical principles and experimental setup of polTIRFM. We conclude with a brief introduction to assays using polTIRFM to assess the interaction of actin and myosin. PMID:22550303

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.

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

McCurdy, C. W.; Rescigno, T. N.; Trevisan, C. S.

A dramatic symmetry breaking in K-shell photoionization of the CF 4 molecule in which a core-hole vacancy is created in one of four equivalent fluorine atoms is displayed in the molecular frame angular distribution of the photoelectrons. In observing the photoejected electron in coincidence with an F + atomic ion after Auger decay we see how selecting the dissociation path where the core hole was localized was almost exclusively on that atom. A combination of measurements and ab initio calculations of the photoelectron angular distribution in the frame of the recoiling CF 3 + and F + atoms elucidates themore » underlying physics that derives from the Ne-like valence structure of the F(1s -1) core-excited atom.« less

Energy and angular distributions of electron emission from diatomic molecules by bare ion impact

NASA Astrophysics Data System (ADS)

Mondal, A.; Mandal, C. R.; Purkait, M.

2015-06-01

The three-Coulomb wave model has been used extensively to study the energy and angular distributions of double-differential cross sections (DDCS) of electron emissions from hydrogen and nitrogen molecules by bare ion impact at intermediate and high energies. In the present model, we have expressed the molecular triple differential cross section in terms of the corresponding atomic triple differential cross section multiplied by the occupation number and the average Rayleigh interference factor, which accounts for the two-center interference effect. Here we have used an active electron approximation of the molecule as a whole in the initial channel. To account for the effect of passive electrons, we have constructed a model potential that satisfies the initial conditions and the corresponding wavefunction has been calculated from the model Hamiltonian of the active electron in the target. In the final channel, we have used a hydrogenic model with an effective nuclear charge that is calculated from its binding energy. In this model, the correlated motion of the particles in the exit channel of the reaction is considered by an adequate product of three-Coulomb functions. The emitted electron, the incident projectile ion and the residual ion are considered to be in same plane. The obtained results are compared with other recent theoretical and experimental findings. There is an overall agreement of the calculations with the experimental data for electron emission cross sections.

Absolute cross section measurements for the scattering of low- and intermediate-energy electrons from PF3. I. Elastic scattering

NASA Astrophysics Data System (ADS)

Hishiyama, N.; Hoshino, M.; Blanco, F.; García, G.; Tanaka, H.

2017-12-01

We report absolute elastic differential cross sections (DCSs) for electron collisions with phosphorus trifluoride, PF3, molecules (e- + PF3) in the impact energy range of 2.0-200 eV and over a scattering angle range of 10°-150°. Measured angular distributions of scattered electron intensities were normalized by reference to the elastic DCSs of He. Corresponding integral and momentum-transfer cross sections were derived by extrapolating the angular range from 0° to 180° with the help of a modified phase-shift analysis. In addition, due to the large dipole moment of the considered molecule, the dipole-Born correction for the forward scattering angles has also been applied. As a part of this study, independent atom model calculations in combination with screening corrected additivity rule were also performed for elastic and inelastic (electronic excitation plus ionization) scattering using a complex optical potential method. Rotational excitation cross sections have been estimated with a dipole-Born approximation procedure. Vibrational excitations are not considered in this calculation. Theoretical data, at the differential and integral levels, were found to reasonably agree with the present experimental results. Furthermore, we explore the systematics of the elastic DCSs for the four-atomic trifluoride molecules of XF3 (X = B, N, and P) and central P-atom in PF3, showing that, owing to the comparatively small effect of the F-atoms, the present angular distributions of elastic DCSs are essentially dominated by the characteristic of the central P-atom at lower impact energies. Finally, these quantitative results for e- - PF3 collisions were compiled together with the previous data available in the literature in order to obtain a cross section dataset for modeling purposes. To comprehensively describe such a considerable amount of data, we proceed by first discussing, in this paper, the vibrationally elastic scattering processes whereas vibrational and electronic excitation shall be the subject of our following paper devoted to inelastic collisions.

Molecular threading: mechanical extraction, stretching and placement of DNA molecules from a liquid-air interface.

PubMed

Payne, Andrew C; Andregg, Michael; Kemmish, Kent; Hamalainen, Mark; Bowell, Charlotte; Bleloch, Andrew; Klejwa, Nathan; Lehrach, Wolfgang; Schatz, Ken; Stark, Heather; Marblestone, Adam; Church, George; Own, Christopher S; Andregg, William

2013-01-01

We present "molecular threading", a surface independent tip-based method for stretching and depositing single and double-stranded DNA molecules. DNA is stretched into air at a liquid-air interface, and can be subsequently deposited onto a dry substrate isolated from solution. The design of an apparatus used for molecular threading is presented, and fluorescence and electron microscopies are used to characterize the angular distribution, straightness, and reproducibility of stretched DNA deposited in arrays onto elastomeric surfaces and thin membranes. Molecular threading demonstrates high straightness and uniformity over length scales from nanometers to micrometers, and represents an alternative to existing DNA deposition and linearization methods. These results point towards scalable and high-throughput precision manipulation of single-molecule polymers.

Observation of an angular change in the structure of an RNA complex using Fluorescence Resonance Energy Transfer

NASA Astrophysics Data System (ADS)

Rahmanseresht, Sheema; Milas, Peker; Parrot, Louis; Goldner, Lori S.

Single-molecular-pair FRET is often used to study distance fluctuations of single molecules. It is harder to capture angular changes using FRET, because rotational motion of the dyes tends to wash out the angular sensitivity. Using a dye labeling scheme that minimizes the rotational motion of the dyes with respect to the RNA, we use spFRET to measure an angular change in structure of an RNA kissing complex upon protein binding. The model system studied here, R1inv-R2inv, is derived from the RNAI-RNAII complex in E.coli. RNA II is a primer for replication of the ColE1 plasmid; its function is modulated by interaction with RNA I, Rop protein is known to stabilize the bent R1inv-R2inv kissing complex against dissociation. The effect, if any, of Rop protein on the conformation of the kissing complex is not known. The eight minimized-energy NMR structures reported for R1inv-R2inv show a small difference in end-to-end distances and much larger differences in twist and bend angles. We compare a first-principles model with spFRET data to determine if the observed change in FRET is consistent with an angular change in structure, as suggested by the model. Grant Number: NSF DBI-1152386.

Anatomy of F1-ATPase powered rotation.

PubMed

Martin, James L; Ishmukhametov, Robert; Hornung, Tassilo; Ahmad, Zulfiqar; Frasch, Wayne D

2014-03-11

F1-ATPase, the catalytic complex of the ATP synthase, is a molecular motor that can consume ATP to drive rotation of the γ-subunit inside the ring of three αβ-subunit heterodimers in 120° power strokes. To elucidate the mechanism of ATPase-powered rotation, we determined the angular velocity as a function of rotational position from single-molecule data collected at 200,000 frames per second with unprecedented signal-to-noise. Power stroke rotation is more complex than previously understood. This paper reports the unexpected discovery that a series of angular accelerations and decelerations occur during the power stroke. The decreases in angular velocity that occurred with the lower-affinity substrate ITP, which could not be explained by an increase in substrate-binding dwells, provides direct evidence that rotation depends on substrate binding affinity. The presence of elevated ADP concentrations not only increased dwells at 35° from the catalytic dwell consistent with competitive product inhibition but also decreased the angular velocity from 85° to 120°, indicating that ADP can remain bound to the catalytic site where product release occurs for the duration of the power stroke. The angular velocity profile also supports a model in which rotation is powered by Van der Waals repulsive forces during the final 85° of rotation, consistent with a transition from F1 structures 2HLD1 and 1H8E (Protein Data Bank).

Anatomy of F1-ATPase powered rotation

PubMed Central

Martin, James L.; Ishmukhametov, Robert; Hornung, Tassilo; Ahmad, Zulfiqar; Frasch, Wayne D.

2014-01-01

F1-ATPase, the catalytic complex of the ATP synthase, is a molecular motor that can consume ATP to drive rotation of the γ-subunit inside the ring of three αβ-subunit heterodimers in 120° power strokes. To elucidate the mechanism of ATPase-powered rotation, we determined the angular velocity as a function of rotational position from single-molecule data collected at 200,000 frames per second with unprecedented signal-to-noise. Power stroke rotation is more complex than previously understood. This paper reports the unexpected discovery that a series of angular accelerations and decelerations occur during the power stroke. The decreases in angular velocity that occurred with the lower-affinity substrate ITP, which could not be explained by an increase in substrate-binding dwells, provides direct evidence that rotation depends on substrate binding affinity. The presence of elevated ADP concentrations not only increased dwells at 35° from the catalytic dwell consistent with competitive product inhibition but also decreased the angular velocity from 85° to 120°, indicating that ADP can remain bound to the catalytic site where product release occurs for the duration of the power stroke. The angular velocity profile also supports a model in which rotation is powered by Van der Waals repulsive forces during the final 85° of rotation, consistent with a transition from F1 structures 2HLD1 and 1H8E (Protein Data Bank). PMID:24567403

HO2 rovibrational eigenvalue studies for nonzero angular momentum

NASA Astrophysics Data System (ADS)

Wu, Xudong T.; Hayes, Edward F.

1997-08-01

An efficient parallel algorithm is reported for determining all bound rovibrational energy levels for the HO2 molecule for nonzero angular momentum values, J=1, 2, and 3. Performance tests on the CRAY T3D indicate that the algorithm scales almost linearly when up to 128 processors are used. Sustained performance levels of up to 3.8 Gflops have been achieved using 128 processors for J=3. The algorithm uses a direct product discrete variable representation (DVR) basis and the implicitly restarted Lanczos method (IRLM) of Sorensen to compute the eigenvalues of the polyatomic Hamiltonian. Since the IRLM is an iterative method, it does not require storage of the full Hamiltonian matrix—it only requires the multiplication of the Hamiltonian matrix by a vector. When the IRLM is combined with a formulation such as DVR, which produces a very sparse matrix, both memory and computation times can be reduced dramatically. This algorithm has the potential to achieve even higher performance levels for larger values of the total angular momentum.

Crossed Molecular Beam Studies and Dynamics of Decomposition of Chemically Activated Radicals

DOE R&D Accomplishments Database

Lee, Y. T.

1973-09-01

The power of the crossed molecular beams method in the investigation of the dynamics of chemical reactions lies mainly in the direct observation of the consequences of single collisions of well controlled reactant molecules. The primary experimental observations which provide information on reaction dynamics are the measurements of angular and velocity distributions of reaction products.

An advanced molecule-surface scattering instrument for study of vibrational energy transfer in gas-solid collisions.

PubMed

Ran, Qin; Matsiev, Daniel; Wodtke, Alec M; Auerbach, Daniel J

2007-10-01

We describe an advanced and highly sensitive instrument for quantum state-resolved molecule-surface energy transfer studies under ultrahigh vacuum (UHV) conditions. The apparatus includes a beam source chamber, two differential pumping chambers, and a UHV chamber for surface preparation, surface characterization, and molecular beam scattering. Pulsed and collimated supersonic molecular beams are generated by expanding target molecule mixtures through a home-built pulsed nozzle, and excited quantum state-selected molecules were prepared via tunable, narrow-band laser overtone pumping. Detection systems have been designed to measure specific vibrational-rotational state, time-of-flight, angular and velocity distributions of molecular beams coming to and scattered off the surface. Facilities are provided to clean and characterize the surface under UHV conditions. Initial experiments on the scattering of HCl(v = 0) from Au(111) show many advantages of this new instrument for fundamental studies of the energy transfer at the gas-surface interface.

Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses

DOE PAGES

Yang, Jie; Guehr, Markus; Vecchione, Theodore; ...

2016-04-05

Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angström spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 Å) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule.more » In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Lastly, our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.« less

Dissipation dynamics of field-free molecular alignment for symmetric-top molecules: Ethane (C2H6)

NASA Astrophysics Data System (ADS)

Zhang, H.; Billard, F.; Yu, X.; Faucher, O.; Lavorel, B.

2018-03-01

The field-free molecular alignment of symmetric-top molecules, ethane, induced by intense non-resonant linearly polarized femtosecond laser pulses is investigated experimentally in the presence of collisional relaxation. The dissipation dynamics of field-free molecular alignment are measured by the balanced detection of ultrafast molecular birefringence of ethane gas samples at high pressures. By separating the molecular alignment into the permanent alignment and the transient alignment, the decay time-constants of both components are quantified at the same pressure. It is observed that the permanent alignment always decays slower compared to the transient alignment within the measured pressure range. This demonstrates that the propensity of molecules to conserve the orientation of angular momentum during collisions, previously observed for linear species, is also applicable to symmetric-top molecules. The results of this work provide valuable information for further theoretical understanding of collisional relaxation within nonlinear polyatomic molecules, which are expected to present interesting and nontrivial features due to an extra rotational degree of freedom.

Observation of correlated excitations in bimolecular collisions

NASA Astrophysics Data System (ADS)

Gao, Zhi; Karman, Tijs; Vogels, Sjoerd N.; Besemer, Matthieu; van der Avoird, Ad; Groenenboom, Gerrit C.; van de Meerakker, Sebastiaan Y. T.

2018-02-01

Although collisions between atoms and molecules are largely understood, collisions between two molecules have proven much harder to study. In both experiment and theory, our ability to determine quantum-state-resolved bimolecular cross-sections lags behind their atom-molecule counterparts by decades. For many bimolecular systems, even rules of thumb—much less intuitive understanding—of scattering cross sections are lacking. Here, we report the measurement of state-to-state differential cross sections on the collision of state-selected and velocity-controlled nitric oxide (NO) radicals and oxygen (O2) molecules. Using velocity map imaging of the scattered NO radicals, the full product-pair correlations of rotational excitation that occurs in both collision partners from individual encounters are revealed. The correlated cross sections show surprisingly good agreement with quantum scattering calculations using ab initio NO-O2 potential energy surfaces. The observations show that the well-known energy-gap law that governs atom-molecule collisions does not generally apply to bimolecular excitation processes, and reveal a propensity rule for the vector correlation of product angular momenta.

[In Process Citation].

PubMed

Cuerda, Cristina; Álvarez, Julia; Ramos, Primitivo; Abánades, Juan Carlos; García-de-Lorenzo, Abelardo; Gil, Pedro; De-la-Cruz, Juan José

2016-03-25

Introducción: la desnutrición relacionada con la enfermedad (DRE) es un problema sociosanitario frecuente que afecta preferentemente a los mayores de 65 años, que aumenta la morbimortalidad y disminuye la calidad de vida.  Objetivo: estudiar la prevalencia de DRE en mayores de 65 años en diferentes centros sociosanitarios del Servicio Regional de Bienestar Social de la Comunidad de Madrid. Métodos: estudio transversal en 33 centros sociosanitarios de Madrid (6 centros de atención primaria [AP], 9 centros de mayores [CM], 9 hospitales [H] y 9 residencias [R]) seleccionados mediante muestreo polietápico. Las variables estudiadas fueron edad, sexo, nivel de dependencia según la escala de incapacidad de la Cruz Roja, motivo de ingreso y enfermedad de base, hábitat (urbano-periurbano-rural) y distribución geográfica (norte centro-sur). Como herramienta de cribado nutricional se utilizó el Mini Nutritional Assessment (MNA-cribaje) en todos los centros. En los pacientes con cribado positivo (en riesgo-desnutrición) se realizó el MNA-evaluación. El estudio estadístico se realizó con el paquete SSS 21.0 e incluyó estadística descriptiva, test de Chi-cuadrado y prueba exacta de Fisher, ANOVA de un factor, Kruskal-Wallis y análisis de regresión logística (RL) binaria univariante y multivariante. Se consideró significación estadística p < 0,05. Resultados: se reclutaron 1.103 sujetos (275 AP, 278 CM, 281 H, 269 R), edad media de 79,5 ± 8,4 años (41,2% varones, 58,8% mujeres). Los sujetos procedentes de H y R tuvieron un mayor grado de incapacidad (p < 0,001). La prevalencia global de DRE fue del 10%, encontrándose un 23,3% en riesgo de desnutrición, con diferencias entre los cuatro tipos de centros sociosanitarios (p < 0,001). El análisis univariante de RL mostró diferencia significativas en la prevalencia de desnutrición según la edad, sexo, grado de dependencia, tipo de centro sociosanitario, hábitat y zona geográfica. Sin embargo, en el análisis multivariante solo el grado de dependencia, el tipo de centro y el hábitat tuvieron significación estadística. Conclusiones: la prevalencia de DRE en mayores de 65 años en la Comunidad de Madrid es del 10%, encontrándose además un 23,3% en riesgo de desnutrición. Las únicas variables que se relacionaron de forma independiente con la desnutrición en el análisis multivariante fueron el nivel de dependencia de los pacientes y el tipo y hábitat de centro sociosanitario.

Torsional mechanics of DNA are regulated by small-molecule intercalation.

PubMed

Celedon, Alfredo; Wirtz, Denis; Sun, Sean

2010-12-23

Whether the bend and twist mechanics of DNA molecules are coupled is unclear. Here, we report the direct measurement of the resistive torque of single DNA molecules to study the effect of ethidium bromide (EtBr) intercalation and pulling force on DNA twist mechanics. DNA molecules were overwound and unwound using recently developed magnetic tweezers where the molecular resistive torque was obtained from Brownian angular fluctuations. The effect of EtBr intercalation on the twist stiffness was found to be significantly different from the effect on the bend persistence length. The twist stiffness of DNA was dramatically reduced at low intercalator concentration (<10 nM); however, it did not decrease further when the intercalator concentration was increased by 3 orders of magnitude. We also determined the dependence of EtBr intercalation on the torque applied to DNA. We propose a model for the elasticity of DNA base pairs with intercalated EtBr molecules to explain the abrupt decrease of twist stiffness at low EtBr concentration. These results indicate that the bend and twist stiffnesses of DNA are independent and can be differently affected by small-molecule binding.

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

Manipulating spins of magnetic molecules: Hysteretic behavior with respect to bias voltage

NASA Astrophysics Data System (ADS)

Płomińska, Anna; Misiorny, Maciej; Weymann, Ireneusz

2018-02-01

Formation of a magnetic hysteresis loop with respect to a bias voltage is investigated theoretically in a spin-valve device based on a single magnetic molecule. We consider a device consisting of two ferromagnetic electrodes bridged by a carbon nanotube, acting as a quantum dot, to which a spin-anisotropic molecule is exchange-coupled. Such a coupling allows for transfer of angular momentum between the molecule and a spin current flowing through the dot, and thus, for switching orientation of the molecular spin. We demonstrate that this current-induced switching process exhibits a hysteretic behavior with respect to a bias voltage applied to the device. The analysis is carried out with the use of the real-time diagrammatic technique in the lowest-order expansion of the tunnel coupling of the dot to electrodes. The influence of both the intrinsic properties of the spin-valve device (the spin polarization of electrodes and the coupling strength of the molecule to the dot) and those of the molecule itself (magnetic anisotropy and spin relaxation) on the size of the magnetic hysteresis loop is discussed.

Effects of the finite size of the ion (dd{mu}){sup +} on the energy levels of the molecules (dd{mu})e and (dd{mu})dee

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

Harston, M.R.; Hara, S.; Kino, Y.

1997-10-01

The energy shift due to the finite size of the pseudonucleus (dd{mu}){sub 11}{sup +} in the molecules (dd{mu}){sub 11}e and (dd{mu}){sub 11}dee, the subscripts indicating the first excited state with total angular momentum of one unit, is of importance in the theoretical estimation of the rate of d-d fusion catalyzed by negative muons. The energy shift in the molecule (dd{mu}){sub 11}e is calculated using perturbation theory up to second order. The finite-size shift is found to be 1.46 meV. This is significantly larger than the value of 0.7 meV for this energy shift calculated by Bakalov [Muon Catalyzed Fusion {boldmore » 3}, 321 (1988)] by a method similar to the present method; recently found excellent agreement of theory with experimental results for the formation rate of the molecule (dd{mu}){sub 11}dee was based on Bakalov{close_quote}s value with some modifications. The results of a direct calculation of the finite-size energy shifts in (dd{mu}){sub 11}dee using first-order perturbation theory are presented. The contribution from the quadrupole component of the (dd{mu}){sub 11} charge distribution, which is not taken into account in the conventional scaling procedure based on the finite-size energy shifts of (dd{mu}){sub 11}e, is found to be of the order of 1 meV and to depend on the angular-momentum states of (dd{mu}){sub 11}dee. Sources of uncertainty in the current theoretical estimates are also discussed. {copyright} {ital 1997} {ital The American Physical Society}« less

Hidden-charm pentaquarks as a meson-baryon molecule with coupled channels for D¯ (*)Λc and D¯ (*)Σc(*)

NASA Astrophysics Data System (ADS)

Yamaguchi, Yasuhiro; Santopinto, Elena

2017-07-01

The recent observation of two hidden-charm pentaquark states by LHCb collaborations prompted us to investigate the exotic states close to the D ¯Λc, D¯ *Λc , D ¯ Σc , D ¯ Σc* , D¯ *Σc and D¯ *Σc* thresholds. We therefore studied the hadronic molecules that form the coupled-channel system of D¯ (*)Λc and D¯(*)Σc(*). As the heavy quark spin symmetry manifests the mass degenerations of D ¯ and D¯* mesons, and of Σc and Σc* baryons, the coupled channels of D¯(*)Σc(*) are important in these molecules. In addition, we consider the coupling to the D¯(*)Λc channel whose thresholds are near the D¯(*)Σc(*) thresholds, and the coupling to the state with nonzero orbital angular momentum mixed by the tensor force. This full coupled-channel analysis of D¯(*)Λc-D¯(*)Σc(*) with larger orbital angular momentum has never been performed before. By solving the coupled-channel Schrödinger equations with the one meson exchange potentials with respect to the heavy quark spin and chiral symmetries, we studied the hidden-charm hadronic molecules with I (JP)=1 /2 (3 /2±) and 1 /2 (5 /2±) . We conclude that the JP assignment of the observed pentaquarks is 3 /2+ for Pc+(4380 ) and 5 /2- for Pc+(4450 ), which is in agreement with the results of the LHCb analysis. In addition, we give predictions for other JP=3 /2± states at 4136.0, 4307.9 and 4348.7 MeV in JP=3 /2-, and 4206.7 MeV in JP=3 /2+, which can be further investigated by means of experiment.

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

Waitz, M.; Metz, D.; Lower, J.

Here, wWe investigate the photodouble ionization of H 2 molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. Conversely, the quasiparticle consisting of both electrons (i.e., the "dielectron") does. The work highlights the fact that nonlocal effects are embedded everywhere in nature where many-particle processes are involved.

Reversible geminate recombination of hydrogen-bonded water molecule pair

NASA Astrophysics Data System (ADS)

Markovitch, Omer; Agmon, Noam

2008-08-01

The (history independent) autocorrelation function for a hydrogen-bonded water molecule pair, calculated from classical molecular dynamics trajectories of liquid water, exhibits a t-3/2 asymptotic tail. Its whole time dependence agrees quantitatively with the solution for reversible diffusion-influenced geminate recombination derived by Agmon and Weiss [J. Chem. Phys. 91, 6937 (1989)]. Agreement with diffusion theory is independent of the precise definition of the bound state. Given the water self-diffusion constant, this theory enables us to determine the dissociation and bimolecular recombination rate parameters for a water dimer. (The theory is indispensable for obtaining the bimolecular rate coefficient.) Interestingly, the activation energies obtained from the temperature dependence of these rate coefficients are similar, rather than differing by the hydrogen-bond (HB) strength. This suggests that recombination requires displacing another water molecule, which meanwhile occupied the binding site. Because these activation energies are about twice the HB strength, cleavage of two HBs may be required to allow pair separation. The autocorrelation function without the HB angular restriction yields a recombination rate coefficient that is larger than that for rebinding to all four tetrahedral water sites (with angular restrictions), suggesting the additional participation of interstitial sites. Following dissociation, the probability of the pair to be unbound but within the reaction sphere rises more slowly than expected, possibly because binding to the interstitial sites delays pair separation. An extended diffusion model, which includes an additional binding site, can account for this behavior.

One-electron densities of freely rotating Wigner molecules

NASA Astrophysics Data System (ADS)

Cioslowski, Jerzy

2017-12-01

A formalism enabling computation of the one-particle density of a freely rotating assembly of identical particles that vibrate about their equilibrium positions with amplitudes much smaller than their average distances is presented. It produces densities as finite sums of products of angular and radial functions, the length of the expansion being determined by the interplay between the point-group and permutational symmetries of the system in question. Obtaining from a convolution of the rotational and bosonic components of the parent wavefunction, the angular functions are state-dependent. On the other hand, the radial functions are Gaussians with maxima located at the equilibrium lengths of the position vectors of individual particles and exponents depending on the scalar products of these vectors and the eigenvectors of the corresponding Hessian as well as the respective eigenvalues. Although the new formalism is particularly useful for studies of the Wigner molecules formed by electrons subject to weak confining potentials, it is readily adaptable to species (such as ´balliums’ and Coulomb crystals) composed of identical particles with arbitrary spin statistics and permutational symmetry. Several examples of applications of the present approach to the harmonium atoms within the strong-correlation regime are given.

Control of Ultracold Photodissociation with Magnetic Fields

NASA Astrophysics Data System (ADS)

McDonald, M.; Majewska, I.; Lee, C.-H.; Kondov, S. S.; McGuyer, B. H.; Moszynski, R.; Zelevinsky, T.

2018-01-01

Photodissociation of a molecule produces a spatial distribution of photofragments determined by the molecular structure and the characteristics of the dissociating light. Performing this basic reaction at ultracold temperatures allows its quantum mechanical features to dominate. In this regime, weak applied fields can be used to control the reaction. Here, we photodissociate ultracold diatomic strontium in magnetic fields below 10 G and observe striking changes in photofragment angular distributions. The observations are in excellent agreement with a multichannel quantum chemistry model that includes nonadiabatic effects and predicts strong mixing of partial waves in the photofragment energy continuum. The experiment is enabled by precise quantum-state control of the molecules.

Quantum effects in the capture of charged particles by dipolar polarizable symmetric top molecules. I. General axially nonadiabatic channel treatment.

PubMed

Auzinsh, M; Dashevskaya, E I; Litvin, I; Nikitin, E E; Troe, J

2013-08-28

The rate coefficients for capture of charged particles by dipolar polarizable symmetric top molecules in the quantum collision regime are calculated within an axially nonadiabatic channel approach. It uses the adiabatic approximation with respect to rotational transitions of the target within first-order charge-dipole interaction and takes into account the gyroscopic effect that decouples the intrinsic angular momentum from the collision axis. The results are valid for a wide range of collision energies (from single-wave capture to the classical limit) and dipole moments (from the Vogt-Wannier and fly-wheel to the adiabatic channel limit).

Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT

NASA Astrophysics Data System (ADS)

Wopperer, Philipp; De Giovannini, Umberto; Rubio, Angel

2017-03-01

We derive and extend the time-dependent surface-flux method introduced in [L. Tao, A. Scrinzi, New J. Phys. 14, 013021 (2012)] within a time-dependent density-functional theory (TDDFT) formalism and use it to calculate photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses. We present other, existing computational TDDFT methods that are suitable for the calculation of electron emission in compact spatial regions, and compare their results. We illustrate the performance of the new method by simulating strong-field ionization of C60 fullerene and discuss final state effects in the orbital reconstruction of planar organic molecules.

Third-order-harmonic generation in coherently spinning molecules

NASA Astrophysics Data System (ADS)

Prost, E.; Zhang, H.; Hertz, E.; Billard, F.; Lavorel, B.; Bejot, P.; Zyss, Joseph; Averbukh, Ilya Sh.; Faucher, O.

2017-10-01

The rotational Doppler effect occurs when circularly polarized light interacts with a rotating anisotropic material. It is manifested by the appearance of a spectral shift ensuing from the transfer of angular momentum and energy between radiation and matter. Recently, we reported terahertz-range rotational Doppler shifts produced in third-order nonlinear optical conversion [O. Faucher et al., Phys. Rev. A 94, 051402(R) (2016), 10.1103/PhysRevA.94.051402]. The experiment was performed in an ensemble of coherently spinning molecules prepared by a short laser pulse exhibiting a twisted linear polarization. The present work provides an extensive analysis of the rotational Doppler effect in third-order-harmonic generation from spinning linear molecules. The underlying physics is investigated both experimentally and theoretically. The implication of the rotational Doppler effect in higher-order processes like high-order-harmonic generation is discussed.

Engineering a light-emitting planar defect within three-dimensional photonic crystals

PubMed Central

Liu, Guiqiang; Chen, Yan; Ye, Zhiqing

2009-01-01

Sandwich structures, constructed from a planar defect of rhodamine-B (RhB)-doped titania (TiO2) and two photonic crystals, were synthesized via the self-assembly method combined with spin-coating. The modification of the spontaneous emission of RhB molecules in such structures was investigated experimentally. The spontaneous emission of RhB-doped TiO2 film with photonic crystals was reduced by a factor of 5.5 over a large bandwidth of 13% of the first-order Bragg diffraction frequency when compared with that of RhB-doped TiO2 film without photonic crystals. The angular dependence of the modification and the photoluminescence lifetime of RhB molecules demonstrate that the strong and wide suppression of the spontaneous emission of the RhB molecules is due to the presence of the photonic band gap. PMID:27877309

USSR Report, International Affairs, The Working Class and the Contemporary World, Number 4, July-August 1985

DTIC Science & Technology

1986-01-02

34 [The Church’s Social Role in Liberated Countries], Moscow, 1978. 13. See: G. Guttierrez, " Teologia de la liberacion" [The Theology of Liberation...details see: N.A. Kovalskiy, "Sostialnoye rol’ tserkvi...", op. cit., p 21 ff. 20. See: Gera Buentig y Catena, " Teologia , pastoral y dependencia

The engagement of optical angular momentum in nanoscale chirality

NASA Astrophysics Data System (ADS)

Andrews, David L.

2017-09-01

Wide-ranging developments in optical angular momentum have recently led to refocused attention on issues of material chirality. The connection between optical spin and circular polarization, linking to well-known and utilized probes of chirality such as circular dichroism, has prompted studies aiming to achieve enhanced means of differentiating enantiomers - molecules or particles of opposite handedness. A number of newly devised schemes for physically separating mirror-image components by optical methods have also been gaining traction, together with a developing appreciation of how the scale of physical dimensions ultimately determines any capacity to differentially select for material chirality. The scope of such enquiries has substantially widened on recognition that suitably structured, topologically charged beams of light - often known as `twisted light' or `optical vortices' can additionally convey orbital angular momentum. A case can be made that understanding the full scope and constraints upon chiroptical interactions in the nanoscale regime involves the resolution of CPT symmetry conditions governing the fundamental interactions between matter and photons. The principles provide a sound theoretical test-bed for new methodologies.

Experimental Observation of Dynamical Localization in Laser-Kicked Molecular Rotors

NASA Astrophysics Data System (ADS)

Bitter, M.; Milner, V.

2016-09-01

The periodically kicked rotor is a paradigm system for studying quantum effects on classically chaotic dynamics. The wave function of the quantum rotor localizes in angular momentum space, similarly to Anderson localization of the electronic wave function in disordered solids. Here, we observe dynamical localization in a system of true quantum rotors by subjecting nitrogen molecules to periodic sequences of femtosecond pulses. Exponential distribution of the molecular angular momentum—the hallmark of dynamical localization—is measured directly by means of coherent Raman scattering. We demonstrate the suppressed rotational energy growth with the number of laser kicks and study the dependence of the localization length on the kick strength. Because of its quantum coherent nature, both timing and amplitude noise are shown to destroy the localization and revive the diffusive growth of energy.

Experimental Observation of Dynamical Localization in Laser-Kicked Molecular Rotors.

PubMed

Bitter, M; Milner, V

2016-09-30

The periodically kicked rotor is a paradigm system for studying quantum effects on classically chaotic dynamics. The wave function of the quantum rotor localizes in angular momentum space, similarly to Anderson localization of the electronic wave function in disordered solids. Here, we observe dynamical localization in a system of true quantum rotors by subjecting nitrogen molecules to periodic sequences of femtosecond pulses. Exponential distribution of the molecular angular momentum-the hallmark of dynamical localization-is measured directly by means of coherent Raman scattering. We demonstrate the suppressed rotational energy growth with the number of laser kicks and study the dependence of the localization length on the kick strength. Because of its quantum coherent nature, both timing and amplitude noise are shown to destroy the localization and revive the diffusive growth of energy.

The role of angular momentum in the superrotor theory for rovibrational motion of extremely flexible molecules

NASA Astrophysics Data System (ADS)

Schmiedt, Hanno; Jensen, Per; Schlemmer, Stephan

2017-12-01

Recently, we proposed a novel approach to the description of the rotation-vibration motion for extremely flexible molecules (Schmiedt et al., 2016, 2017). Such molecules have multiple very "soft" vibrational modes and so, they lack a well-defined equilibrium structure. We have applied the new superrotor model to the prototype example of an extremely flexible molecule, CH5+, for which we combine two, essentially free vibrational modes (describing internal rotation) with the over-all rotation of the molecule and consider the resulting motion as a free rotation in five-dimensional space, with a Hamiltonian whose symmetry is described by SO(5), the five-dimensional rotation group. In the present work we discuss the correlation between the superrotor energies and those obtained in the more usual situation of the internal and over-all rotations being separable, and we give an initial discussion of the selection rules for electric dipole transitions obtained in the superrotor approach. Such selection rules are required for a detailed comparison between the superrotor predictions and the available, experimentally derived energy spacings (Asvany et al., 2015; Brackertz, 2016).

High precision optical spectroscopy and quantum state selected photodissociation of ultracold 88Sr2 molecules in an optical lattice

NASA Astrophysics Data System (ADS)

McDonald, Mickey

2017-04-01

Over the past several decades, rapid progress has been made toward the accurate characterization and control of atoms, epitomized by the ever-increasing accuracy and precision of optical atomic lattice clocks. Extending this progress to molecules will have exciting implications for chemistry, condensed matter physics, and precision tests of physics beyond the Standard Model. My thesis describes work performed over the past six years to establish the state of the art in manipulation and quantum control of ultracold molecules. We describe a thorough set of measurements characterizing the rovibrational structure of weakly bound 88Sr2 molecules from several different perspectives, including determinations of binding energies; linear, quadratic, and higher order Zeeman shifts; transition strengths between bound states; and lifetimes of narrow subradiant states. Finally, we discuss measurements of photofragment angular distributions produced by photodissociation of molecules in single quantum states, leading to an exploration of quantum-state-resolved ultracold chemistry. The images of exploding photofragments produced in these studies exhibit dramatic interference effects and strongly violate semiclassical predictions, instead requiring a fully quantum mechanical description.

N(2)O in small para-hydrogen clusters: Structures and energetics.

PubMed

Zhu, Hua; Xie, Daiqian

2009-04-30

We present the minimum-energy structures and energetics of clusters of the linear N(2)O molecule with small numbers of para-hydrogen molecules with pairwise additive potentials. Interaction energies of (p-H(2))-N(2)O and (p-H(2))-(p-H(2)) complexes were calculated by averaging the corresponding full-dimensional potentials over the H(2) angular coordinates. The averaged (p-H(2))-N(2)O potential has three minima corresponding to the T-shaped and the linear (p-H(2))-ONN and (p-H(2))-NNO structures. Optimization of the minimum-energy structures was performed using a Genetic Algorithm. It was found that p-H(2) molecules fill three solvation rings around the N(2)O axis, each of them containing up to five p-H(2) molecules, followed by accumulation of two p-H(2) molecules at the oxygen and nitrogen ends. The first solvation shell is completed at N = 17. The calculated chemical potential oscillates with cluster size up to the completed first solvation shell. These results are consistent with the available experimental measurements. (c) 2009 Wiley Periodicals, Inc.

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

Electromagnetic torque tweezers: a versatile approach for measurement of single-molecule twist and torque.

PubMed

Janssen, Xander J A; Lipfert, Jan; Jager, Tessa; Daudey, Renier; Beekman, Jaap; Dekker, Nynke H

2012-07-11

The well-established single-molecule force-spectroscopy techniques have recently been complemented by methods that can measure torque and twist directly, notably magnetic torque tweezers and the optical torque wrench. A limitation of the current torque measurement schemes is the intrinsic coupling between the force and torque degrees of freedom. Here we present electromagnetic torque tweezers (eMTT) that combine permanent and electromagnets to enable independent control of the force and torsional trap stiffness for sensitive measurements of single molecule torque and twist. Using the eMTT, we demonstrate sensitive torque measurements on tethered DNA molecules from simple tracking of the beads' (x,y)-position, obviating the need for any angular tracking algorithms or markers. Employing the eMTT for high-resolution torque measurements, we experimentally confirm the theoretically predicted torque overshoot at the DNA buckling transition in high salt conditions. We envision that the flexibility and control afforded by the eMTT will enable a range of new torque and twist measurement schemes from single-molecules to living cells.

Spectroscopic and structural study of novel interaction product of pyrrolidine-2-thione with molecular iodine. Presumable mechanisms of oxidation

NASA Astrophysics Data System (ADS)

Chernov'yants, Margarita S.; Burykin, Igor V.; Starikova, Zoya A.; Tereznikov, Alexander Yu.; Kolesnikova, Tatiana S.

2013-09-01

Synthesis, spectroscopic and structural characterization of novel interaction product of pyrrolidine-2-thione with molecular iodine is reported. The ability of pyrrolidine-2-thione to form the outer-sphere charge-transfer complex C4H7NS·I2 with iodine molecule in dilute chloroform solution has been studied by UV/vis spectroscopy. Oxidative desulfurization promotes ring fusion of two pyrrolidine-2-thione molecules. The product of iodine induced oxidative desulfurization has been studied by X-ray diffraction method. The crystal structure of the reaction product is formed by 5-(2-thioxopyrrolidine-1-yl)-3,4-dihydro-2H-pyrrolium (C8H13N2S+) cations and pentaiodide anions I5-, which are linked by the intermolecular I⋯Hsbnd C and I⋯C close contacts. The angular pentaiodide anions can be considered as structures formed by coordination of two iodine molecules to the iodide ion (type 1) or by the coordination of iodine molecule to the triiodide ion (type 2).

Electron scattering on molecules: search for semi-empirical indications

NASA Astrophysics Data System (ADS)

Fedus, Kamil; Karwasz, Grzegorz P.

2017-06-01

Reliable cross-sections for electron-molecule collisions are urgently needed for numerical modeling of various processes important from technological point of view. Unfortunately, a significant progress in theory and experiment over the last decade is not usually accompanied by the convergence of cross-sections measured at different laboratories and calculated with different methods. Moreover the most advanced contemporary theories involve such large basis sets and complicated equations that they are not easily applied to each specific molecule for which data are needed. For these reasons the search for semi-empirical indications in angular and energy dependencies of scattering cross-section becomes important. In this paper we make a brief review of the applicability of the Born-dipole approximation for elastic, rotational, vibrational and ionization processes that can occur during electron-molecule collisions. We take into account the most recent experimental findings as the reference points. Contribution to the Topical Issue "Atomic and Molecular Data and Their Applications", edited by Gordon W.F. Drake, Jung-Sik Yoon, Daiji Kato, and Grzegorz Karwasz.

Asymmetric molecular-orbital tomography by manipulating electron trajectories

NASA Astrophysics Data System (ADS)

Wang, Bincheng; Zhang, Qingbin; Zhu, Xiaosong; Lan, Pengfei; Rezvani, Seyed Ali; Lu, Peixiang

2017-11-01

We present a scheme for tomographic imaging of asymmetric molecular orbital based on high-order harmonic generation with a two-color orthogonally polarized multicycle laser field. With the two-dimensional manipulation of the electron trajectories, the electrons can recollide with the target molecule from two noncollinear directions, and then the dipole moment generated from the single direction can be obtained to reconstructed the asymmetric molecular orbital. The recollision is independent from the molecular structure and the angular dependence of the ionization rate in the external field. For this reason, this scheme can avoid the negative effects arising from the modification of the angle-dependent ionization rate induced by Stark shift and be applied to various molecules.

Spectral Analysis of Two Coupled Diatomic Rotor Molecules

PubMed Central

Crogman, Horace T.; Harter, William G.

2014-01-01

In a previous article the theory of frame transformation relation between Body Oriented Angular (BOA) states and Lab Weakly Coupled states (LWC) was developed to investigate simple rotor–rotor interactions. By analyzing the quantum spectrum for two coupled diatomic molecules and comparing it with spectrum and probability distribution of simple models, evidence was found that, as we move from a LWC state to a strongly coupled state, a single rotor emerges in the strong limit. In the low coupling, the spectrum was quadratic which indicates the degree of floppiness in the rotor–rotor system. However in the high coupling behavior it was found that the spectrum was linear which corresponds to a rotor deep in a well. PMID:25353181

Analyzing Global Interdependence. Volume I. Analytical Perspectives and Policy Implications,

DTIC Science & Technology

1974-11-01

clearly explored in the school of social psychology called Role Theory. The language of dependency is transmuted into "matrices of possible interactions...imperialism or from sexual differences. The colonial oppression (dependencia) literature is polemical in style and normative in substance. b The orientation... sexual inequality, 7 one can glean several propositions about the dynamic characteristics of the dominant and subordinate members in the dependent

Spin-symmetry conversion and internal rotation in high J molecular systems

NASA Astrophysics Data System (ADS)

Mitchell, Justin; Harter, William

2006-05-01

Dynamics and spectra of molecules with internal rotation or rovibrational coupling is approximately modeled by rigid or semi-rigid rotors with attached gyroscopes. Using Rotational Energy (RE)^1 surfaces, high resolution molecular spectra for high angular momentum show two distinct but related phenomena; spin-symmetry conversion and internal rotation. For both cases the high total angular momentum allows for transitions that would otherwise be forbidden. Molecular body-frame J-localization effects associated with tight energy level-clusters dominate the rovibronic spectra of high symmetry molecules, particularly spherical tops at J>10. ^2 The effects include large and widespread spin-symmetry mixing contrary to conventional wisdom^3 about weak nuclear moments. Such effects are discussed showing how RE surface plots may predict them even at low J. Classical dynamics of axially constrained rotors are approximated by intersecting rotational-energy-surfaces (RES) that have (J-S).B.(J-S) forms in the limit of constraints that do no work. Semi-classical eigensolutions are compared to those found by direct diagonalization. ^1 W.G Hater, in Handbook of Atomic, Molecular and Optical Physics, edited by G.W.F Drake (Springer, Germany 2006) ^2 W. G. Harter, Phys. Rev. A24,192-262(1981). ^3 G. Herzberg, Infrared and Raman Spectra (VanNostrand 1945) pp. 458,463.

Velocity-tunable slow beams of cold O2 in a single spin-rovibronic state with full angular-momentum orientation by multistage Zeeman deceleration

NASA Astrophysics Data System (ADS)

Wiederkehr, A. W.; Schmutz, H.; Motsch, M.; Merkt, F.

2012-08-01

Cold samples of oxygen molecules in supersonic beams have been decelerated from initial velocities of 390 and 450 m s-1 to final velocities in the range between 150 and 280 m s-1 using a 90-stage Zeeman decelerator. (2 + 1) resonance-enhanced-multiphoton-ionization (REMPI) spectra of the 3sσ g 3Π g (C) ? two-photon transition of O2 have been recorded to characterize the state selectivity of the deceleration process. The decelerated molecular sample was found to consist exclusively of molecules in the J ‧‧ = 2 spin-rotational component of the X ? ground state of O2. Measurements of the REMPI spectra using linearly polarized laser radiation with polarization vector parallel to the decelerator axis, and thus to the magnetic-field vector of the deceleration solenoids, further showed that only the ? magnetic sublevel of the N‧‧ = 1, J ‧‧ = 2 spin-rotational level is populated in the decelerated sample, which therefore is characterized by a fully oriented total-angular-momentum vector. By maintaining a weak quantization magnetic field beyond the decelerator, the polarization of the sample could be maintained over the 5 cm distance separating the last deceleration solenoid and the detection region.

Quantum Chemistry on Quantum Computers: A Polynomial-Time Quantum Algorithm for Constructing the Wave Functions of Open-Shell Molecules.

PubMed

Sugisaki, Kenji; Yamamoto, Satoru; Nakazawa, Shigeaki; Toyota, Kazuo; Sato, Kazunobu; Shiomi, Daisuke; Takui, Takeji

2016-08-18

Quantum computers are capable to efficiently perform full configuration interaction (FCI) calculations of atoms and molecules by using the quantum phase estimation (QPE) algorithm. Because the success probability of the QPE depends on the overlap between approximate and exact wave functions, efficient methods to prepare accurate initial guess wave functions enough to have sufficiently large overlap with the exact ones are highly desired. Here, we propose a quantum algorithm to construct the wave function consisting of one configuration state function, which is suitable for the initial guess wave function in QPE-based FCI calculations of open-shell molecules, based on the addition theorem of angular momentum. The proposed quantum algorithm enables us to prepare the wave function consisting of an exponential number of Slater determinants only by a polynomial number of quantum operations.

Wigner molecules: the strong-correlation limit of the three-electron harmonium.

PubMed

Cioslowski, Jerzy; Pernal, Katarzyna

2006-08-14

At the strong-correlation limit, electronic states of the three-electron harmonium atom are described by asymptotically exact wave functions given by products of distinct Slater determinants and a common Gaussian factor that involves interelectron distances and the center-of-mass position. The Slater determinants specify the angular dependence and the permutational symmetry of the wave functions. As the confinement strength becomes infinitesimally small, the states of different spin multiplicities become degenerate, their limiting energy reflecting harmonic vibrations of the electrons about their equilibrium positions. The corresponding electron densities are given by products of angular factors and a Gaussian function centered at the radius proportional to the interelectron distance at equilibrium. Thanks to the availability of both the energy and the electron density, the strong-correlation limit of the three-electron harmonium is well suited for testing of density functionals.

Sub- and super-Maxwellian evaporation of simple gases from liquid water

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

Kann, Z. R.; Skinner, J. L., E-mail: skinner@chem.wisc.edu

2016-04-21

Non-Maxwellian evaporation of light atoms and molecules (particles) such as He and H{sub 2} from liquids has been observed experimentally. In this work, we use simulations to study systematically the evaporation of Lennard-Jones particles from liquid water. We find instances of sub- and super-Maxwellian evaporation, depending on the mass of the particle and the particle-water interaction strength. The observed trends are in qualitative agreement with experiment. We interpret these trends in terms of the potential of mean force and the effectiveness and frequency of collisions during the evaporation process. The angular distribution of evaporating particles is also analyzed, and itmore » is shown that trends in the energy from velocity components tangential and normal to the liquid surface must be understood separately in order to interpret properly the angular distributions.« less

Acetone in Orion BN/KL. High-resolution maps of a special oxygen-bearing molecule

NASA Astrophysics Data System (ADS)

Peng, T.-C.; Despois, D.; Brouillet, N.; Baudry, A.; Favre, C.; Remijan, A.; Wootten, A.; Wilson, T. L.; Combes, F.; Wlodarczak, G.

2013-06-01

Aims: As one of the prime targets of interstellar chemistry study, Orion BN/KL clearly shows different molecular distributions between large nitrogen- (e.g., C2H5CN) and oxygen-bearing (e.g., HCOOCH3) molecules. However, acetone (CH3)2CO, a special complex O-bearing molecule, has been shown to have a very different distribution from other typical O-bearing molecules in the BN/KL region. Therefore, it is worth investigating acetone in detail at high angular resolutions, which will help us understand the formation of this molecule and its chemical role in the complex BN/KL region. Methods: We searched for acetone within our IRAM Plateau de Bure Interferometer 3 mm and 1.3 mm data sets. Twenty-two acetone lines were searched within these data sets. The angular resolution ranged from 1farcs8×0farcs8 to 6farcs0×2farcs3, and the spectral resolution ranged from 0.4 to 1.9 km s-1. Results: Nine of the acetone lines appear free of contamination. Three main acetone peaks (Ace-1, 2, and 3) are identified in Orion BN/KL. The new acetone source Ace-3 and the extended emission in the north of the hot core region have been found for the first time. An excitation temperature of about 150 K is determined toward Ace-1 and Ace-2, and the acetone column density is estimated to be 2-4 × 1016 cm-2 with a relative abundance of 1-6 × 10-8 toward these two peaks. Acetone is a few times less abundant toward the hot core and Ace-3 compared with Ace-1 and Ace-2. Conclusions: We find that the overall distribution of acetone in BN/KL is similar to that of N-bearing molecules, e.g., NH3 and C2H5CN, and very different from those of large O-bearing molecules, e.g., HCOOCH3 and (CH3)2O. Our findings show the acetone distribution is more extended than in previous studies and does not originate only in those areas where both N-bearing and O-bearing species are present. Moreover, because the N-bearing molecules may be associated with shocked gas in Orion BN/KL, this suggests that the formation and/or destruction of acetone may involve ammonia or large N-bearing molecules in a shocked-gas environment. Based on observations carried out with the IRAM Plateau de Bure Interferometer. IRAM is supported by INSU/CNRS (France), MPG (Germany), and IGN (Spain).Appendices and movie are available in electronic form at http://www.aanda.org

Joint and Combined Military Force: A Possible Solution to African Economic Problems.

DTIC Science & Technology

1992-06-01

New York Monthly Review Press, N.Y.: 1966). 4. Enzo Falloto and Frenando Henrique Cardoso, Dependencia (Mexico Siglo XX1: 1969). 5. David Apter and...the most volatile and explosive political destabilizers in Africa today is religion . However, religious differences serving as catalysts to political...crises is not peculiar to African. From the beginning of civilization, religion has caused major political crises within and between nations. Nearly

Angular distributions for the inelastic scattering of NO(X2Π ) with O2(X3Σg-)

NASA Astrophysics Data System (ADS)

Brouard, M.; Gordon, S. D. S.; Nichols, B.; Squires, E.; Walpole, V.; Aoiz, F. J.; Stolte, S.

2017-05-01

The inelastic scattering of NO(X2Π ) by O2(X3Σg-) was studied at a mean collision energy of 550 cm-1 using velocity-map ion imaging. The initial quantum state of the NO(X2Π , v = 0, j = 0.5, Ω =0.5 , 𝜖 = -1 , f) molecule was selected using a hexapole electric field, and specific Λ-doublet levels of scattered NO were probed using (1 +1' ) resonantly enhanced multiphoton ionization. A modified "onion-peeling" algorithm was employed to extract angular scattering information from the series of "pancaked," nested Newton spheres arising as a consequence of the rotational excitation of the molecular oxygen collision partner. The extracted differential cross sections for NO(X) f →f and f →e Λ-doublet resolved, spin-orbit conserving transitions, partially resolved in the oxygen co-product rotational quantum state, are reported, along with O2 fragment pair-correlated rotational state population. The inelastic scattering of NO with O2 is shown to share many similarities with the scattering of NO(X) with the rare gases. However, subtle differences in the angular distributions between the two collision partners are observed.

Two-Particle Interference of Electron Pairs on a Molecular Level

DOE PAGES

Waitz, M.; Metz, D.; Lower, J.; ...

2016-08-15

Here, wWe investigate the photodouble ionization of H 2 molecules with 400 eV photons. We find that the emitted electrons do not show any sign of two-center interference fringes in their angular emission distributions if considered separately. Conversely, the quasiparticle consisting of both electrons (i.e., the "dielectron") does. The work highlights the fact that nonlocal effects are embedded everywhere in nature where many-particle processes are involved.

Momentum-imaging apparatus for the study of dissociative electron attachment dynamics

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

Moradmand, A.; Williams, J. B.; Landers, A. L.

An ion-momentum spectrometer is used to study the dissociative dynamics of electron attachment to molecules. A skimmed, supersonic gas jet is crossed with a pulsed beam of low-energy electrons, and the resulting negative ions are extracted toward a time- and position-sensitive detector. Calculations of the momentum in three dimensions may be used to determine the angular dependence of dissociative attachment as well as the energetics of the reaction.

Symmetry lowering of pentacene molecular states interacting with a Cu surface

NASA Astrophysics Data System (ADS)

Baldacchini, Chiara; Mariani, Carlo; Betti, Maria Grazia; Vobornik, Ivana; Fujii, Jun; Annese, Emilia; Rossi, Giorgio; Ferretti, Andrea; Calzolari, Arrigo; di Felice, Rosa; Ruini, Alice; Molinari, Elisa

2007-12-01

Pentacene adsorbed on the Cu(119) vicinal surface forms long-range ordered chain structures. Photoemission spectroscopy measurements and ab initio density functional theory simulations provide consistent evidences that pentacene molecular orbitals mix with the copper bands, giving rise to interaction states localized at the interface. Angular-resolved and polarization dependent photoemission spectroscopy shows that most of the pentacene derived intensity is strongly dichroic. The symmetry of the molecular states of the free pentacene molecules is reduced upon adsorption on Cu(119), as a consequence of the molecule-metal interaction. Theoretical results show a redistribution of the charge density in π molecular states close to the Fermi level, consistent with the photoemission intensities (density of states) and polarization dependence (orbital symmetry).

Control of π-Electron Rotations in Chiral Aromatic Molecules Using Intense Laser Pulses

NASA Astrophysics Data System (ADS)

Kanno, Manabu; Kono, Hirohiko; Fujimura, Yuichi

Our recent theoretical studies on laser-induced π-electron rotations in chiral aromatic molecules are reviewed. π electrons of a chiral aromatic molecule can be rotated along its aromatic ring by a nonhelical, linearly polarized laser pulse. An ansa aromatic molecule with a six-membered ring, 2,5-dichloro[n](3,6) pyrazinophane, which belongs to a planar-chiral molecule group, and its simplified molecule 2,5-dichloropyrazine are taken as model molecules. Electron wavepacket simulations in the frozen-molecular-vibration approximation show that the initial direction of π-electron rotation depends on the polarization direction of a linearly polarized laser pulse applied. Consecutive unidirectional rotation can be achieved by applying a sequence of linearly polarized pump and dump pulses to prevent reverse rotation. Optimal control simulations of π-electron rotation show that another controlling factor for unidirectional rotation is the relative optical phase between the different frequency components of an incident pulse in addition to photon polarization direction. Effects of nonadiabatic coupling between π-electron rotation and molecular vibrations are also presented, where the constraints of the frozen approximation are removed. The angular momentum gradually decays mainly owing to nonadiabatic coupling, while the vibrational amplitudes greatly depend on their rotation direction. This suggests that the direction of π-electron rotation on an attosecond timescale can be identified by detecting femtosecond molecular vibrations.

Adsorbing H₂S onto a single graphene sheet: A possible gas sensor

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

Reshak, A. H., E-mail: maalidph@yahoo.co.uk; Center of Excellence Geopolymer and Green Technology, School of Material Engineering, University Malaysia Perlis, 01007 Kangar, Perlis; Auluck, S.

2014-09-14

The electronic structure of pristine graphene sheet and the resulting structure of adsorbing a single molecule of H₂S on pristine graphene in three different sites (bridge, top, and hollow) are studied using the full potential linearized augmented plane wave method. Our calculations show that the adsorption of H₂S molecule on the bridge site opens up a small direct energy gap of about 0.1 eV at symmetry point M, while adsorption of H₂S on top site opens a gap of 0.3 eV around the symmetry point K. We find that adsorbed H₂S onto the hollow site of pristine graphene sheet causesmore » to push the conduction band minimum and the valence band maximum towards Fermi level resulting in a metallic behavior. Comparing the angular momentum decomposition of the atoms projected electronic density of states of pristine graphene sheet with that of H₂S–graphene for three different cases, we find a significant influence of the location of the H₂S molecule on the electronic properties especially the strong hybridization between H₂S molecule and graphene sheet.« less

Low-temperature matrix effects on orientational motion of Methyl radical trapped in gas solids: Angular tunneling vs. libration

NASA Astrophysics Data System (ADS)

Dmitriev, Yurij A.; Zelenetckii, Ilia A.; Benetis, Nikolas P.

2018-05-01

EPR investigation of the lineshape of matrix -isolated methyl radical, CH3, spectra recorded in solid N2O and CO2 was carried out. Reversible temperature-dependent line width anisotropy was observed in both matrices. This effect is a fingerprint of the extra-slow radical rotation about the in-plane C2 axes. The rotation was found to be anisotropic and closely correlated to the orientational dynamics of the matrix molecules. It was suggested that a recently discovered "hoping precession" effect of matrix molecules in solid CO2 is a common feature of matrices of the linear molecules CO, N2O, and CO2. A new low-temperature matrix effect, referred to as "libration trap", was proposed which accounts for the changing CH3 reorientational motion about the radical C3-axis from rotation to libration. Temperature dependence of the intensity of the EPR satellites produced by these nonrotating-but librating methyls was presented. This allowed for a rough estimation of the rotation hindering potential due to correlation mismatch between the radical and the nearest matrix molecules' librations.

Some fundamental questions concerning the kinetic theory of electrons in molecular gases and the e H2 vibrational cross section controversy

NASA Astrophysics Data System (ADS)

Robson, R. E.; White, R. D.; Morrison, Michael A.

2003-10-01

We commence a fundamental re-examination of the kinetic theory of charged particle swarms in molecular gases, focusing on collisional excitation of molecular rotational and ro-vibrational states by electrons. Modern day analysis of electron swarms has been based upon the kinetic equation of Wang-Chang et al, which simply treats all processes as scalar energy excitations, and ignores angular momentum conservation and the vector dynamics associated with rotational excitation. It is pointed out that there is no alternative, more exact kinetic equation readily available for electrons which enables one to directly ascertain the degree of error introduced by this approximation. Thus in this preliminary study, we approach the problem indirectly, from the standpoint of the neutral molecules, using the Waldmann-Snider quantum kinetic equation, and insist that an electron-molecule collision must look the same from the perspective of both electron and molecule. We give a formula for quantitatively assessing the importance of scalar versus vectorial treatments of rotational excitation by looking at the post-collisional 'echo' produced by an electron swarm as it passes through the gas. It is then pointed out that in order to remedy any deficiency, it will be necessary to introduce a kinetic collisional operator non-local in space to properly account for angular momentum conservation, as has long been established in the literature. This is a major exercise and given the preliminary nature of this study, we consider the inclusion of such effects from a formal point of view only. In particular we show how non-local effects lead to a spatially dependent 'source' term in the equation of continuity, and hence to corrections for both drift velocity and diffusion coefficients. The magnitude of these corrections has yet to be established.

The origin of transverse anisotropy in axially symmetric single molecule magnets.

PubMed

Barra, Anne-Laure; Caneschi, Andrea; Cornia, Andrea; Gatteschi, Dante; Gorini, Lapo; Heiniger, Leo-Philipp; Sessoli, Roberta; Sorace, Lorenzo

2007-09-05

Single-crystal high-frequency electron paramagnetic resonance spectroscopy has been employed on a truly axial single molecule magnet of formula [Mn(12)O(12)(tBu-CH(2)CO(2))16(CH(3)OH)4].CH(3)OH to investigate the origin of the transverse magnetic anisotropy, a crucial parameter that rules the quantum tunneling of the magnetization. The crystal structure, including the absolute structure of the crystal used for EPR experiments, has been fully determined and found to belong to I4 tetragonal space group. The angular dependence of the resonance fields in the crystallographic ab plane shows the presence of high-order tetragonal anisotropy and strong dependence on the MS sublevels with the second-highest-field transition being angular independent. This was rationalized including competing fourth- and sixth-order transverse parameters in a giant spin Hamiltonian which describes the magnetic anisotropy in the ground S = 10 spin state of the cluster. To establish the origin of these anisotropy terms, the experimental results have been further analyzed using a simplified multispin Hamiltonian which takes into account the exchange interactions and the single ion magnetic anisotropy of the Mn(III) centers. It has been possible to establish magnetostructural correlations with spin Hamiltonian parameters up to the sixth order. Transverse anisotropy in axial single molecule magnets was found to originate from the multispin nature of the system and from the breakdown of the strong exchange approximation. The tilting of the single-ion easy axes of magnetization with respect to the 4-fold molecular axis of the cluster plays the major role in determining the transverse anisotropy. Counterintuitively, the projections of the single ion easy axes on the ab plane correspond to hard axes of magnetization.

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

Petrik, Nikolay G.; Kimmel, Gregory A.

Weakly bound (physisorbed) atoms and molecules such as Ar, Kr, Xe, CO, CH4, CH3OH, CO2 and N2 are used to probe the photochemical interactions of O2 on rutile TiO2(110). UV irradiation of chemisorbed O2 along with the physisorbed probe species leads to photon-stimulated desorption (PSD) of Ar, Kr, CO, CH4 and N2. Without co-adsorbed O2, the PSD yields of the probe species are very low or not observed. No PSD was observed for CO2, N2O, CH3OH and the PSD yield for Xe is very low compared to the other probe atoms or molecules. The angular distribution of the photo-desorbing Kr,more » which is broad and cosine, is quite different from the O2 PSD angular distribution, which is sharply peaked along the surface normal. The Kr PSD yields increase with increasing coverage of Kr and of chemisorbed O2. We propose a mechanism for the observed phenomena where the chemisorbed O2 serves as photoactive center, excited via electronic excitations (electrons and/or holes) created in the TiO2 substrate by UV photon irradiation. The photo-excited O2 may transfer its energy to neighboring co-adsorbed atom or molecule resulting in desorption of the latter. Simple momentum transfer considerations suggest that heavier adsorbates (like Xe) and adsorbates with higher binding energy (like CO2) should desorb less efficiently according to the proposed mechanism. Various forms of chemisorbed O2 appeared photoactive in such stimulated desorption of Kr atoms: molecular anions (O22-, O2-), adatoms (Oa), and others. The observed phenomenon provides a new tool for study of photocatalysis.« less

Balloon-borne three-meter telescope for far-infrared and submillimeter astronomy

NASA Technical Reports Server (NTRS)

Fazio, G. G.

1985-01-01

Presented are scientific objectives, engineering analysis and design, and results of technology development for a Three-Meter Balloon-Borne Far-Infrared and Submillimeter Telescope. The scientific rationale is based on two crucial instrumental capabilities: high angular resolution which approaches eight arcseconds at one hundred micron wavelength, and high resolving power spectroscopy with good sensitivity throughout the telescope's 30-micron to 1-mm wavelength range. The high angular resolution will allow us to resolve and study in detail such objects as collapsing protostellar condensations in our own galaxy, clusters of protostars in the Magellanic clouds, giant molecular clouds in nearby galaxies, and spiral arms in distant galaxies. The large aperture of the telescope will permit sensitive spectral line measurements of molecules, atoms, and ions, which can be used to probe the physical, chemical, and dynamical conditions in a wide variety of objects.

Angularly resolved X-ray photoelectron spectroscopy investigation of PTFE after prolonged space exposure

NASA Technical Reports Server (NTRS)

Dalins, I.; Karimi, M.

1992-01-01

Monochromatized angularly resolved X-ray photoelectron spectroscopy (ARXPS) was used to study PTFE (Teflon) that had been exposed to an earth orbital environment for approximately six years. The primary interest of the research is on a very reactive component of this environment (atomic oxygen) which, because of the typical orbital velocities of a spacecraft, impinge on exposed surfaces with 5 eV energy. This presentation deals with the method of analysis, the findings as they pertain to a rather complex carbon, oxygen, and fluorine XPS peak analysis, and the character of the valence bands. An improved bias referencing method, based on ARXPS, is also demonstrated for evaluating specimen charging effects. It was found that the polymer molecule tends to resist the atomic oxygen attack by reorienting itself, so that the most electronegative CF3 groups are facing the incoming hyperthermal oxygen atoms. The implications of these findings to ground-based laboratory studies are discussed.

Perpetual Motion with Maxwell's Demon

NASA Astrophysics Data System (ADS)

Gordon, Lyndsay G. M.

2002-11-01

A method for producing a temperature gradient by Brownian motion in an equilibrated isolated system composed of two fluid compartments and a separating adiabatic membrane is discussed. This method requires globular protein molecules, partially embedded in the membrane, to alternate between two conformations which lie on opposite sides of the membrane. The greater part of each conformer is bathed by one of the fluids and rotates in Brownian motion around its axis, perpendicular to the membrane. Rotational energy is transferred through the membrane during conformational changes. Angular momentum is conserved during the transitions. The energy flow becomes asymmetrical when the conformational changes of the protein are sterically hindered by two of its side-chains, the positions of which are affected by the angular velocity of the rotor. The heat flow increases the temperature gradient in contravention of the Second Law. A second hypothetical model which illustrates solute transfer at variance with the Second Law is also discussed.

Effect of the third π ∗ resonance on the angular distributions for electron-pyrimidine scattering

NASA Astrophysics Data System (ADS)

Mašín, Zdeněk; Gorfinkiel, Jimena D.

2016-07-01

We present a detailed analysis of the effect of the well known third π∗ resonance on the angular behaviour of the elastic cross section in electron scattering from pyrimidine. This resonance, occurring approximately at 4.7 eV, is of mixed shape and core-excited character. Experimental and theoretical results show the presence of a peak/dip behaviour in this energy range, that is absent for other resonances. Our investigations show that the cause of the peak/dip is an interference of background p-wave to p-wave scattering amplitudes with the amplitudes for resonant scattering. The equivalent resonance in pyrazine shows the same behaviour and the effect is therefore likely to appear in other benzene-like molecules. Contribution to the Topical Issue "Advances in Positron and Electron Scattering", edited by Paulo Limao-Vieira, Gustavo Garcia, E. Krishnakumar, James Sullivan, Hajime Tanuma and Zoran Petrovic.

The role of nanopore shape in surface-induced crystallization

NASA Astrophysics Data System (ADS)

Diao, Ying; Harada, Takuya; Myerson, Allan S.; Alan Hatton, T.; Trout, Bernhardt L.

2011-11-01

Crystallization of a molecular liquid from solution often initiates at solid-liquid interfaces, and nucleation rates are generally believed to be enhanced by surface roughness. Here we show that, on a rough surface, the shape of surface nanopores can also alter nucleation kinetics. Using lithographic methods, we patterned polymer films with nanopores of various shapes and found that spherical nanopores 15-120 nm in diameter hindered nucleation of aspirin crystals, whereas angular nanopores of the same size promoted it. We also show that favourable surface-solute interactions are required for angular nanopores to promote nucleation, and propose that pore shape affects nucleation kinetics through the alteration of the orientational order of the crystallizing molecule near the angles of the pores. Our findings have clear technological implications, for instance in the control of pharmaceutical polymorphism and in the design of ‘seed’ particles for the regulation of crystallization of fine chemicals.

Dissection of molecular assembly dynamics by tracking orientation and position of single molecules in live cells

PubMed Central

McQuilken, Molly; La Riviere, Patrick J.; Occhipinti, Patricia; Verma, Amitabh; Oldenbourg, Rudolf; Gladfelter, Amy S.; Tani, Tomomi

2016-01-01

Regulation of order, such as orientation and conformation, drives the function of most molecular assemblies in living cells but remains difficult to measure accurately through space and time. We built an instantaneous fluorescence polarization microscope, which simultaneously images position and orientation of fluorophores in living cells with single-molecule sensitivity and a time resolution of 100 ms. We developed image acquisition and analysis methods to track single particles that interact with higher-order assemblies of molecules. We tracked the fluctuations in position and orientation of molecules from the level of an ensemble of fluorophores down to single fluorophores. We tested our system in vitro using fluorescently labeled DNA and F-actin, in which the ensemble orientation of polarized fluorescence is known. We then tracked the orientation of sparsely labeled F-actin network at the leading edge of migrating human keratinocytes, revealing the anisotropic distribution of actin filaments relative to the local retrograde flow of the F-actin network. Additionally, we analyzed the position and orientation of septin-GFP molecules incorporated in septin bundles in growing hyphae of a filamentous fungus. Our data indicate that septin-GFP molecules undergo positional fluctuations within ∼350 nm of the binding site and angular fluctuations within ∼30° of the central orientation of the bundle. By reporting position and orientation of molecules while they form dynamic higher-order structures, our approach can provide insights into how micrometer-scale ordered assemblies emerge from nanoscale molecules in living cells. PMID:27679846

Angular motion of a PAH molecule in interstellar environment

NASA Technical Reports Server (NTRS)

Rouan, D.; Leger, Alain; Omont, A.; Giard, Martin

1989-01-01

Polycyclic aromatic hydrocarbon (PAH) molecules have recently been proposed as an important and hitherto undetected component of the Interstellar Medium (ISM). The theory was based on an explanation of the Unidentified IR Emission Bands by Leger et al. It has already led to a verified prediction on extended galactic and extragalactic emissions measured by IRAS, or by a recent balloon borne experiment. The physics that rules the motion of such molecules in the ISM was studied, taking into account their coupling with the ambient gas, the radiation field (absorption and emission) and the static magnetic field. This is important for many implications of the PAH theory such as the radio emission by these molecules or the expected polarization of their IR emission. A reflection nebulae is considered where the situation is rather well known. Every day life of a mean PAH molecule in such a region is as follows: every 3 hrs a UV photon is absorbed heating the molecule to a thousand degs; the temperature decay due to cooling by IR emission follows then within a few seconds. A collision with a molecule of gas occurs typically once a week, while an H atom is ejected or captured at the same rate. A typical cooling cycle after a heat impulse is given. The PAH molecules studied as representative of the family has typically 50 atoms, a radius of 4.5 A, is circular and has a molecular mass of M = 300; its permanent dipole moment is 3 Debye.

Nucleation and growth of vortices in a rotating Bose-Einstein condensate.

PubMed

Vorov, O K; Isacker, P Van; Hussein, M S; Bartschat, K

2005-12-02

An analytic solution of the Gross-Pitaevskii equation for a rotating Bose-Einstein condensate of trapped atoms describes the onset of vorticity when the rotational speed is increased, starting with the entry of the first vortex and followed by the formation of growing symmetric Wigner molecules. It explains the staircase of angular momentum jumps and the behavior of the bosonic occupancies observed in numerical studies. The similarity of this behavior and mesoscopic superconductors is discussed.

The parity-adapted basis set in the formulation of the photofragment angular momentum polarization problem: The role of the Coriolis interaction

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

Shternin, Peter S.; Vasyutinskii, Oleg S.

We present a theoretical framework for calculating the recoil-angle dependence of the photofragment angular momentum polarization taking into account both radial and Coriolis nonadiabatic interactions in the diatomic/linear photodissociating molecules. The parity-adapted representation of the total molecular wave function has been used throughout the paper. The obtained full quantum-mechanical expressions for the photofragment state multipoles have been simplified by using the semiclassical approximation in the high-J limit and then analyzed for the cases of direct photodissociation and slow predissociation in terms of the anisotropy parameters. In both cases, each anisotropy parameter can be presented as a linear combination of themore » generalized dynamical functions f{sub K}(q,q{sup '},q-tilde,q-tilde{sup '}) of the rank K representing contribution from different dissociation mechanisms including possible radial and Coriolis nonadiabatic transitions, coherent effects, and the rotation of the recoil axis. In the absence of the Coriolis interactions, the obtained results are equivalent to the earlier published ones. The angle-recoil dependence of the photofragment state multipoles for an arbitrary photolysis reaction is derived. As shown, the polarization of the photofragments in the photolysis of a diatomic or a polyatomic molecule can be described in terms of the anisotropy parameters irrespective of the photodissociation mechanism.« less

Time-dependent polar distribution of outgassing from a spacecraft

NASA Technical Reports Server (NTRS)

Scialdone, J. J.

1974-01-01

A technique has been developed to obtain a characterization of the self-generated environment of a spacecraft and its variation with time, angular position, and distance. The density, pressure, outgassing flux, total weight loss, and other important parameters were obtained from data provided by two mass measuring crystal microbalances, mounted back to back, at distance of 1 m from the spacecraft equivalent surface. A major outgassing source existed at an angular position of 300 deg to 340 deg, near the rocket motor, while the weakest source was at the antennas. The strongest source appeared to be caused by a material diffusion process which produced a directional density at 1 m distance of about 1.6 x 10 to the 11th power molecules/cu cm after 1 hr in vacuum and decayed to 1.6 x 10 to the 9th power molecules/cu cm after 200 hr. The total average outgassing flux at the same distance and during the same time span changed from 1.2 x 10 to the minus 7th power to 1.4 x to the minus 10th power g/sq cm/s. These values are three times as large at the spacecraft surface. Total weight loss was 537 g after 10 hr and about 833 g after 200 hr. Self-contamination of the spacecraft was equivalent to that in orbit at about 300-km altitude.

The Hilsch Tube, Rossby Vortices, and a Carnot Engine: Angular Momentum Transport in Astrophysics

NASA Astrophysics Data System (ADS)

Beckley, Howard F.; Klein, B.; Milburn, M.; Schindel, P.; Westpfahl, D. J.; Teare, S.; Li, H.; Colgate, S. A.

2008-05-01

We are attempting to demonstrate that the common laboratory vortex or Hilsch tube is a paradigm for the angular momentum transport by Rossby vortices in Keplerian accretion disks, either in super massive black hole formation or in star formation. Near supersonic rotating flow is induced in a cylinder by gas pressure injected through a tangential nozzle in a typical Ranque vortex or Hilsch tube. The gas exits through both an on-axis hole and a peripheral radially-aligned hole. The surprising result, demonstrated in hundreds of class rooms, is that one of the exit gas streams is hot and the other is cold. Depressing is that the typical explanation is given in terms of a "Maxwell daemon” that separates hot molecules from cold molecules, just as is the basis of any perpetual motion machine that violates the second law of thermodynamics. Instead we believe that the rotational flow is unstable to the formation of Rossby vortices that co-rotate with the azimuthal flow and act like semi-ridged turbine vanes. These quasi-vanes act like a Carnot turbine engine to the flow that escapes on axis and is therefore cooled by doing work. With the resulting free-energy, the vortices accelerate the peripheral flow which in turn becomes hot by friction with the cylinder wall. As a first step we expect to demonstrate that a free-running turbine, where metal vanes form the Carnot engine, will demonstrate the temperature effect. Such a suggestive result may lead to funding of time-dependent Schlerian photography of a vortex tube that can demonstrate the formation and pressure distribution of the Rossby vortices and coherent transport of angular momentum. This work is supported by a cooperative agreement between the New Mexico Institute of Mining and Technology, the University of California, Los Alamos National Laboratory, and the U.S. Dept. of Energy.

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging-ion mass spectrometry

NASA Astrophysics Data System (ADS)

Fanood, Mohammad M. Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan; Powis, Ivan; Janssen, Maurice H. M.

2015-06-01

Simultaneous, enantiomer-specific identification of chiral molecules in multi-component mixtures is extremely challenging. Many established techniques for single-component analysis fail to provide selectivity in multi-component mixtures and lack sensitivity for dilute samples. Here we show how enantiomers may be differentiated by mass-selected photoelectron circular dichroism using an electron-ion coincidence imaging spectrometer. As proof of concept, vapours containing ~1% of two chiral monoterpene molecules, limonene and camphor, are irradiated by a circularly polarized femtosecond laser, resulting in multiphoton near-threshold ionization with little molecular fragmentation. Large chiral asymmetries (2-4%) are observed in the mass-tagged photoelectron angular distributions. These asymmetries switch sign according to the handedness (R- or S-) of the enantiomer in the mixture and scale with enantiomeric excess of a component. The results demonstrate that mass spectrometric identification of mixtures of chiral molecules and quantitative determination of enantiomeric excess can be achieved in a table-top instrument.

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.

Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging–ion mass spectrometry

PubMed Central

Fanood, Mohammad M Rafiee; Ram, N. Bhargava; Lehmann, C. Stefan; Powis, Ivan; Janssen, Maurice H. M.

2015-01-01

Simultaneous, enantiomer-specific identification of chiral molecules in multi-component mixtures is extremely challenging. Many established techniques for single-component analysis fail to provide selectivity in multi-component mixtures and lack sensitivity for dilute samples. Here we show how enantiomers may be differentiated by mass-selected photoelectron circular dichroism using an electron–ion coincidence imaging spectrometer. As proof of concept, vapours containing ∼1% of two chiral monoterpene molecules, limonene and camphor, are irradiated by a circularly polarized femtosecond laser, resulting in multiphoton near-threshold ionization with little molecular fragmentation. Large chiral asymmetries (2–4%) are observed in the mass-tagged photoelectron angular distributions. These asymmetries switch sign according to the handedness (R- or S-) of the enantiomer in the mixture and scale with enantiomeric excess of a component. The results demonstrate that mass spectrometric identification of mixtures of chiral molecules and quantitative determination of enantiomeric excess can be achieved in a table-top instrument. PMID:26104140

Kinetics and dynamics of near-resonant vibrational energy transfer in gas ensembles of atmospheric interest

NASA Astrophysics Data System (ADS)

McCaffery, Anthony J.

2018-03-01

This study of near-resonant, vibration-vibration (V-V) gas-phase energy transfer in diatomic molecules uses the theoretical/computational method, of Marsh & McCaffery (Marsh & McCaffery 2002 J. Chem. Phys. 117, 503 (doi:10.1063/1.1489998)) The method uses the angular momentum (AM) theoretical formalism to compute quantum-state populations within the component molecules of large, non-equilibrium, gas mixtures as the component species proceed to equilibration. Computed quantum-state populations are displayed in a number of formats that reveal the detailed mechanism of the near-resonant V-V process. Further, the evolution of quantum-state populations, for each species present, may be followed as the number of collision cycles increases, displaying the kinetics of evolution for each quantum state of the ensemble's molecules. These features are illustrated for ensembles containing vibrationally excited N2 in H2, O2 and N2 initially in their ground states. This article is part of the theme issue `Modern theoretical chemistry'.

Determination of collagen fibril structure and orientation in connective tissues by X-ray diffraction

NASA Astrophysics Data System (ADS)

Wilkinson, S. J.; Hukins, D. W. L.

1999-08-01

Elastic scattering of X-rays can provide the following information on the fibrous protein collagen: its molecular structure, the axial arrangement of rod-like collagen molecules in a fibril, the lateral arrangement of molecules within a fibril, and the orientation of fibrils within a biological tissue. The first part of the paper reviews the principles involved in deducing this information. The second part describes a new computer program for measuring the equatorial intensity distribution, that provides information on the lateral arrangement of molecules within a fibril, and the angular distribution of the equatorial peaks that provides information on the orientation of fibrils. Orientation of fibrils within a tissue is quantified by the orientation distribution function, g( φ), which represents the probability of finding a fibril oriented between φ and φ+ δφ. The application of the program is illustrated by measurement of g( φ) for the collagen fibrils in demineralised cortical bone from cow tibia.

High translational energy release in H2 (D2) associative desorption from H (D) chemisorbed on C(0001).

PubMed

Baouche, S; Gamborg, G; Petrunin, V V; Luntz, A C; Baurichter, A; Hornekaer, L

2006-08-28

Highly energetic translational energy distributions are reported for hydrogen and deuterium molecules desorbing associatively from the atomic chemisorption states on highly oriented pyrolytic graphite (HOPG). Laser assisted associative desorption is used to measure the time of flight of molecules desorbing from a hydrogen (deuterium) saturated HOPG surface produced by atomic exposure from a thermal atom source at around 2100 K. The translational energy distributions normal to the surface are very broad, from approximately 0.5 to approximately 3 eV, with a peak at approximately 1.3 eV. The highest translational energy measured is close to the theoretically predicted barrier height. The angular distribution of the desorbing molecules is sharply peaked along the surface normal and is consistent with thermal broadening contributing to energy release parallel to the surface. All results are in qualitative agreement with recent density functional theory calculations suggesting a lowest energy para-type dimer recombination path.

Retrieving transient conformational molecular structure information from inner-shell photoionization of laser-aligned molecules

PubMed Central

Wang, Xu; Le, Anh-Thu; Yu, Chao; Lucchese, R. R.; Lin, C. D.

2016-01-01

We discuss a scheme to retrieve transient conformational molecular structure information using photoelectron angular distributions (PADs) that have averaged over partial alignments of isolated molecules. The photoelectron is pulled out from a localized inner-shell molecular orbital by an X-ray photon. We show that a transient change in the atomic positions from their equilibrium will lead to a sensitive change in the alignment-averaged PADs, which can be measured and used to retrieve the former. Exploiting the experimental convenience of changing the photon polarization direction, we show that it is advantageous to use PADs obtained from multiple photon polarization directions. A simple single-scattering model is proposed and benchmarked to describe the photoionization process and to do the retrieval using a multiple-parameter fitting method. PMID:27025410

Highly efficient volume hologram multiplexing in thick dye-doped jelly-like gelatin.

PubMed

Katarkevich, Vasili M; Rubinov, Anatoli N; Efendiev, Terlan Sh

2014-08-01

Dye-doped jelly-like gelatin is a thick-layer self-developing photosensitive medium that allows single and multiplexed volume phase holograms to be successfully recorded using pulsed laser radiation. In this Letter, we present a method for multiplexed recording of volume holograms in a dye-doped jelly-like gelatin, which provides significant increase in their diffraction efficiency. The method is based on the recovery of the photobleached dye molecule concentration in the hologram recording zone of gel, thanks to molecule diffusion from other unexposed gel areas. As an example, an optical recording of a multiplexed hologram consisting of three superimposed Bragg gratings with mean values of the diffraction efficiency and angular selectivity of ∼75% and ∼21^', respectively, is demonstrated by using the proposed method.

Computational Methods for Biomolecular Electrostatics

PubMed Central

Dong, Feng; Olsen, Brett; Baker, Nathan A.

2008-01-01

An understanding of intermolecular interactions is essential for insight into how cells develop, operate, communicate and control their activities. Such interactions include several components: contributions from linear, angular, and torsional forces in covalent bonds, van der Waals forces, as well as electrostatics. Among the various components of molecular interactions, electrostatics are of special importance because of their long range and their influence on polar or charged molecules, including water, aqueous ions, and amino or nucleic acids, which are some of the primary components of living systems. Electrostatics, therefore, play important roles in determining the structure, motion and function of a wide range of biological molecules. This chapter presents a brief overview of electrostatic interactions in cellular systems with a particular focus on how computational tools can be used to investigate these types of interactions. PMID:17964951

Laboratory Rotational Spectroscopy in the Era of ALMA: Applications to Disks and Circumstellar Outflows

NASA Astrophysics Data System (ADS)

Ziurys, Lucy M.; McCarthy, Michael C.; Stancil, Phillip C.; Halfen, DeWayne; Burton, Mark; Gottlieb, Carl A.; Lee, Kelvin

2018-06-01

The enormous leap in sensitivity and angular resolution offered by the Atacama Large Millimeter Array (ALMA) has revealed the presence of ever greater chemical complexity in astronomical sources, with an increasing number of unidentified lines. The need for supporting laboratory spectroscopy has become more urgent to fully exploit the scientific impact of ALMA. Rotational transition measurements are particularly important in this regard, as are the evaluation of line strengths, collisional cross sections, and dipole moments. Here we present new spectroscopic data concerning a wide range of potential interstellar and circumstellar molecules, including silicon and metal-bearing species, lines arising from vibrationally-excited molecules, and supporting theoretical calculations. Recent work concerning AlC2, KO, and vibrationally-excited AlO will be presented.

Vibration-rotation transfer in molecular super rotors

NASA Astrophysics Data System (ADS)

McCaffery, Anthony J.

2000-12-01

The collisional behavior of (X)6Li2 molecules in very high rotational levels of v=0 is considered. Highly efficient vibration-rotation transfer is predicted in these "super rotors" particularly when the conditions for quasiresonant transfer are fulfilled. This requires simultaneous near-resonance in energy and in angular momentum. Values of Δj for which quasiresonant vibration-rotation transfer (QRT) occurs become smaller as initial rotor state increases and transfer is likely to become particularly fast for Δj=2, predicted to occur when ji=130. This behavior is contrasted with the inefficiency of pure rotational transfer within the v=0 level for fast-rotating molecules. QRT will take place for quite cold collisions and thus will provide competition for the spinning-up process used to create the super rotors.

Retrieving transient conformational molecular structure information from inner-shell photoionization of laser-aligned molecules

NASA Astrophysics Data System (ADS)

Wang, Xu; Le, Anh-Thu; Yu, Chao; Lucchese, R. R.; Lin, C. D.

2016-03-01

We discuss a scheme to retrieve transient conformational molecular structure information using photoelectron angular distributions (PADs) that have averaged over partial alignments of isolated molecules. The photoelectron is pulled out from a localized inner-shell molecular orbital by an X-ray photon. We show that a transient change in the atomic positions from their equilibrium will lead to a sensitive change in the alignment-averaged PADs, which can be measured and used to retrieve the former. Exploiting the experimental convenience of changing the photon polarization direction, we show that it is advantageous to use PADs obtained from multiple photon polarization directions. A simple single-scattering model is proposed and benchmarked to describe the photoionization process and to do the retrieval using a multiple-parameter fitting method.

Vibration-translation energy transfer in vibrationally excited diatomic molecules. Ph.D. Thesis - York Univ., Toronto

NASA Technical Reports Server (NTRS)

Mckenzie, R. L.

1976-01-01

A semiclassical collision model is applied to the study of energy transfer rates between a vibrationally excited diatomic molecule and a structureless atom. The molecule is modeled as an anharmonic oscillator with a multitude of dynamically coupled vibrational states. Three main aspects in the prediction of vibrational energy transfer rates are considered. The applicability of the semiclassical model to an anharmonic oscillator is first evaluated for collinear encounters. Second, the collinear semiclassical model is applied to obtain numerical predictions of the vibrational energy transfer rate dependence on the initial vibrational state quantum number. Thermally averaged vibration-translation rate coefficients are predicted and compared with CO-He experimental values for both ground and excited initial states. The numerical model is also used as a basis for evaluating several less complete but analytic models. Third, the role of rational motion in the dynamics of vibrational energy transfer is examined. A three-dimensional semiclassical collision model is constructed with coupled rotational motion included. Energy transfer within the molecule is shown to be dominated by vibration-rotation transitions with small changes in angular momentum. The rates of vibrational energy transfer in molecules with rational frequencies that are very small in comparison to their vibrational frequency are shown to be adequately treated by the preceding collinear models.

Conserved quantities in non-Abelian monopole fields

NASA Astrophysics Data System (ADS)

Horváthy, P. A.; Ngome, J.-P.

2009-06-01

Van Holten’s covariant Hamiltonian framework is used to find conserved quantities for an isospin-carrying particle in a non-Abelian monopolelike field. For a Wu-Yang monopole we find the most general scalar potential such that the combined system admits a conserved Runge-Lenz vector. In the effective non-Abelian field for nuclear motion in a diatomic molecule due to Moody, Shapere, and Wilczek, a conserved angular momentum is constructed, despite the nonconservation of the electric charge. No Runge-Lenz vector has been found.

The role of spinning electrons in paramagnetic phenomena

NASA Technical Reports Server (NTRS)

Bose, D. M.

1986-01-01

An attempt is made to explain paramagnetic phenomena without assuming the orientation of a molecule or ion in a magnetic field. Only the spin angular momentum is assumed to be responsible. A derivative of the Gurie-Langevin law and the magnetic moments of ions are given as a function of the number of electrons in an inner, incomplete shell. An explanation of Gerlach's experiments with iron and nickel vapors is attempted. An explanation of magnetomechanical experiments with ferromagne elements is given.

Communication: Strong laser alignment of solvent-solute aggregates in the gas-phase

NASA Astrophysics Data System (ADS)

Trippel, Sebastian; Wiese, Joss; Mullins, Terry; Küpper, Jochen

2018-03-01

Strong quasi-adiabatic laser alignment of the indole-water-dimer clusters, an amino-acid chromophore bound to a single water molecule through a hydrogen bond, was experimentally realized. The alignment was visualized through ion and electron imaging following strong-field ionization. Molecular-frame photoelectron angular distributions showed a clear suppression of the electron yield in the plane of the ionizing laser's polarization, which was analyzed as strong alignment of the molecular cluster with ⟨cos2 θ2D⟩ ≥ 0.9.

Studies of torsional properties of DNA and nucleosomes using angular optical trapping

NASA Astrophysics Data System (ADS)

Sheinin, Maxim Y.

DNA in vivo is subjected to torsional stress due to the action of molecular motors and other DNA-binding proteins. Several decades of research have uncovered the fascinating diversity of DNA transformations under torsion and the important role they play in the regulation of vital cellular processes such as transcription and replication. Recent studies have also suggested that torsion can influence the structure and stability of nucleosomes---basic building blocks of the eukaryotic genome. However, our understanding of the impact of torsion is far from being complete due to significant experimental challenges. In this work we have used a powerful single-molecule experimental technique, angular optical trapping, to address several long-standing issues in the field of DNA and nucleosome mechanics. First, we utilized the high resolution and direct torque measuring capability of the angular optical trapping to precisely measure DNA twist-stretch coupling. Second, we characterized DNA melting under tension and torsion. We found that torsionally underwound DNA forms a left-handed structure, significantly more flexible compared to the regular B-DNA. Finally, we performed the first comprehensive investigation of the single nucleosome behavior under torque and force. Importantly, we discovered that positive torque causes significant dimer loss, which can have implications for transcription through chromatin.

Non-polymeric asymmetric binary glass-formers. II. Secondary relaxation studied by dielectric, 2H NMR, and 31P NMR spectroscopy

NASA Astrophysics Data System (ADS)

Pötzschner, B.; Mohamed, F.; Bächer, C.; Wagner, E.; Lichtinger, A.; Bock, D.; Kreger, K.; Schmidt, H.-W.; Rössler, E. A.

2017-04-01

We investigate the secondary (β-) relaxations of an asymmetric binary glass former consisting of a spirobichroman derivative (SBC; Tg = 356 K) as the high-Tg component and the low-Tg component tripropyl phosphate (TPP; Tg = 134 K). The main relaxations are studied in Paper I [B. Pötzschner et al., J. Chem. Phys. 146, 164503 (2017)]. A high Tg contrast of ΔTg = 222 K is put into effect in a non-polymeric system. Component-selective studies are carried out by combining results from dielectric spectroscopy (DS) for mass concentrations cTPP ≥ 60% and those from different methods of 2H and 31P NMR spectroscopy. In the case of NMR, the full concentration range (10% ≤ cTPP ≤ 100%) is covered. The neat components exhibit a β-relaxation (β1 (SBC) and β2 (TPP)). The latter is rediscovered by DS in the mixtures for all concentrations with unchanged time constants. NMR spectroscopy identifies the β-relaxations as being alike to those in neat glasses. A spatially highly restricted motion with angular displacement below ±10° encompassing all molecules is involved. In the low temperature range, where TPP shows the typical 31P NMR echo spectra of the β2-process, very similar spectral features are observed for the (deuterated) SBC component by 2H NMR, in addition to its "own" β1-process observed at high temperatures. Apparently, the small TPP molecules enslave the large SBC molecules to perform a common hindered reorientation. The temperature dependence of the spin-lattice relaxation time of both components is the same and reveals an angular displacement of the SBC molecules somewhat smaller than that of TPP, though the time constants τβ2 are the same. Furthermore, T1(T) of TPP in the temperature region of the β2-process is absolutely the same as in the mixture TPP/polystyrene investigated previously. It appears that the manifestations of the β-process introduced by one component are essentially independent of the second component. Finally, at cTPP ≤ 20% one finds indications that the β2-process starts to disintegrate. More and more TPP molecules get immobilized upon decreasing cTPP. We conclude that the β-process is a cooperative process.

Complex organics in IRAS 4A revisited with ALMA and PdBI: Striking contrast between two neighbouring protostellar cores

NASA Astrophysics Data System (ADS)

López-Sepulcre, A.; Sakai, N.; Neri, R.; Imai, M.; Oya, Y.; Ceccarelli, C.; Higuchi, A. E.; Aikawa, Y.; Bottinelli, S.; Caux, E.; Hirota, T.; Kahane, C.; Lefloch, B.; Vastel, C.; Watanabe, Y.; Yamamoto, S.

2017-10-01

Context. Hot corinos are extremely rich in complex organic molecules (COMs). Accurate abundance measurements of COMs in such objects are crucial to constrain astrochemical models. In the particular case of close binary systems this can only be achieved through high angular resolution imaging. Aims: We aim to perform an interferometric study of multiple COMs in NGC 1333 IRAS 4A, which is a protostellar binary hosting hot corino activity, at an angular resolution that is sufficient to distinguish easily the emission from the two cores separated by 1.8''. Methods: We used the Atacama Large (sub-)Millimeter Array (ALMA) in its 1.2 mm band and the IRAM Plateau de Bure Interferometer (PdBI) at 2.7 mm to image, with an angular resolution of 0.5'' (120 au) and 1'' (235 au), respectively, the emission from 11 different organic molecules in IRAS 4A. This allowed us to clearly disentangle A1 and A2, the two protostellar cores. For the first time, we were able to derive the column densities and fractional abundances simultaneously for the two objects, allowing us to analyse the chemical differences between them. Results: Molecular emission from organic molecules is concentrated exclusively in A2, while A1 appears completely devoid of COMs or even simpler organic molecules, such as HNCO, even though A1 is the strongest continuum emitter. The protostellar core A2 displays typical hot corino abundances and its deconvolved size is 70 au. In contrast, the upper limits we placed on COM abundances for A1 are extremely low, lying about one order of magnitude below prestellar values. The difference in the amount of COMs present in A1 and A2 ranges between one and two orders of magnitude. Our results suggest that the optical depth of dust emission at these wavelengths is unlikely to be sufficiently high to completely hide a hot corino in A1 similar in size to that in A2. Thus, the significant contrast in molecular richness found between the two sources is most probably real. We estimate that the size of a hypothetical hot corino in A1 should be less than 12 au. Conclusions: Our results favour a scenario in which the protostar in A2 is either more massive and/or subject to a higher accretion rate than A1, as a result of inhomogeneous fragmentation of the parental molecular clump. This naturally explains the smaller current envelope mass in A2 with respect to A1 along with its molecular richness. The extremely low abundances of organic molecules in A1 with respect to those in A2 demonstrate that the dense inner regions of a young protostellar core lacking hot corino activity may be poorer in COMs than the outer protostellar envelope. The reduced datacube is only available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (http://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/606/A121

Chirality of weakly bound complexes: The potential energy surfaces for the hydrogen-peroxide−noble-gas interactions

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

Roncaratti, L. F., E-mail: lz@fis.unb.br; Leal, L. A.; Silva, G. M. de

2014-10-07

We consider the analytical representation of the potential energy surfaces of relevance for the intermolecular dynamics of weakly bound complexes of chiral molecules. In this paper we study the H{sub 2}O{sub 2}−Ng (Ng=He, Ne, Ar, Kr, and Xe) systems providing the radial and the angular dependence of the potential energy surface on the relative position of the Ng atom. We accomplish this by introducing an analytical representation which is able to fit the ab initio energies of these complexes in a wide range of geometries. Our analysis sheds light on the role that the enantiomeric forms and the symmetry ofmore » the H{sub 2}O{sub 2} molecule play on the resulting barriers and equilibrium geometries. The proposed theoretical framework is useful to study the dynamics of the H{sub 2}O{sub 2} molecule, or other systems involving O–O and S–S bonds, interacting by non-covalent forces with atoms or molecules and to understand how the relative orientation of the O–H bonds changes along collisional events that may lead to a hydrogen bond formation or even to selectivity in chemical reactions.« less

Model of biological quantum logic in DNA.

PubMed

Mihelic, F Matthew

2013-08-02

The DNA molecule has properties that allow it to act as a quantum logic processor. It has been demonstrated that there is coherent conduction of electrons longitudinally along the DNA molecule through pi stacking interactions of the aromatic nucleotide bases, and it has also been demonstrated that electrons moving longitudinally along the DNA molecule are subject to a very efficient electron spin filtering effect as the helicity of the DNA molecule interacts with the spin of the electron. This means that, in DNA, electrons are coherently conducted along a very efficient spin filter. Coherent electron spin is held in a logically and thermodynamically reversible chiral symmetry between the C2-endo and C3-endo enantiomers of the deoxyribose moiety in each nucleotide, which enables each nucleotide to function as a quantum gate. The symmetry break that provides for quantum decision in the system is determined by the spin direction of an electron that has an orbital angular momentum that is sufficient to overcome the energy barrier of the double well potential separating the C2-endo and C3-endo enantiomers, and that enantiomeric energy barrier is appropriate to the Landauer limit of the energy necessary to randomize one bit of information.

Representing and selecting vibrational angular momentum states for quasiclassical trajectory chemical dynamics simulations.

PubMed

Lourderaj, Upakarasamy; Martínez-Núñez, Emilio; Hase, William L

2007-10-18

Linear molecules with degenerate bending modes have states, which may be represented by the quantum numbers N and L. The former gives the total energy for these modes and the latter identifies their vibrational angular momentum jz. In this work, the classical mechanical analog of the N,L-quantum states is reviewed, and an algorithm is presented for selecting initial conditions for these states in quasiclassical trajectory chemical dynamics simulations. The algorithm is illustrated by choosing initial conditions for the N = 3 and L = 3 and 1 states of CO2. Applications of this algorithm are considered for initial conditions without and with zero-point energy (zpe) included in the vibrational angular momentum states and the C-O stretching modes. The O-atom motions in the x,y-plane are determined for these states from classical trajectories in Cartesian coordinates and are compared with the motion predicted by the normal-mode model. They are only in agreement for the N = L = 3 state without vibrational angular momentum zpe. For the remaining states, the Cartesian O-atom motions are considerably different from the elliptical motion predicted by the normal-mode model. This arises from bend-stretch coupling, including centrifugal distortion, in the Cartesian trajectories, which results in tubular instead of elliptical motion. Including zpe in the C-O stretch modes introduces considerable complexity into the O-atom motions for the vibrational angular momentum states. The short-time O-atom motions for these trajectories are highly irregular and do not appear to have any identifiable characteristics. However, the O-atom motions for trajectories integrated for substantially longer period of times acquire unique properties. With C-O stretch zpe included, the long-time O-atom motion becomes tubular for trajectories integrated to approximately 14 ps for the L = 3 states and to approximately 44 ps for the L = 1 states.

Rotating full- and reduced-dimensional quantum chemical models of molecules

NASA Astrophysics Data System (ADS)

Fábri, Csaba; Mátyus, Edit; Császár, Attila G.

2011-02-01

A flexible protocol, applicable to semirigid as well as floppy polyatomic systems, is developed for the variational solution of the rotational-vibrational Schrödinger equation. The kinetic energy operator is expressed in terms of curvilinear coordinates, describing the internal motion, and rotational coordinates, characterizing the orientation of the frame fixed to the nonrigid body. Although the analytic form of the kinetic energy operator might be very complex, it does not need to be known a priori within this scheme as it is constructed automatically and numerically whenever needed. The internal coordinates can be chosen to best represent the system of interest and the body-fixed frame is not restricted to an embedding defined with respect to a single reference geometry. The features of the technique mentioned make it especially well suited to treat large-amplitude nuclear motions. Reduced-dimensional rovibrational models can be defined straightforwardly by introducing constraints on the generalized coordinates. In order to demonstrate the flexibility of the protocol and the associated computer code, the inversion-tunneling of the ammonia (14NH3) molecule is studied using one, two, three, four, and six active vibrational degrees of freedom, within both vibrational and rovibrational variational computations. For example, the one-dimensional inversion-tunneling model of ammonia is considered also for nonzero rotational angular momenta. It turns out to be difficult to significantly improve upon this simple model. Rotational-vibrational energy levels are presented for rotational angular momentum quantum numbers J = 0, 1, 2, 3, and 4.

Accurate evaporation rates of pure and doped water clusters in vacuum: A statistico-dynamical approach

NASA Astrophysics Data System (ADS)

Calvo, F.; Douady, J.; Spiegelman, F.

2010-01-01

Unimolecular evaporation of selected pure (H2O)n and heterogeneous (H2O)n-1X+ water clusters containing a single hydronium or ammonium impurity is investigated in the framework of phase space theory (PST) in its orbiting transition state version. Using the many-body polarizable Kozack-Jordan potential and its extensions for X+=H3O+ and NH4+, the thermal evaporation of clusters containing 21 and 50 molecules is simulated at several total energies. Numerous molecular dynamics (MD) trajectories at high internal energies provide estimates of the decay rate constant, as well as the kinetic energy and angular momentum released upon dissociation. Additional Monte Carlo simulations are carried out to determine the anharmonic densities of vibrational states, which combined with suitable forms for the rotational densities of states provide expressions for the energy-resolved differential rates. Successful comparison between the MD results and the independent predictions of PST for the distributions of kinetic energy and angular momentum released shows that the latter statistical approach is quantitative. Using MD data as a reference, the absolute evaporation rates are calculated from PST over broad energy and temperature ranges. Based on these results, the presence of an ionic impurity is generally found to decrease the rate, however the effect is much more significant in the 21-molecule clusters. Our calculations also suggest that due to backbendings in the microcanonical densities of states the variations of the evaporation rates may not be strictly increasing with energy or temperature.

Observation of quantum interferences via light-induced conical intersections in diatomic molecules

DOE PAGES

Natan, Adi; Ware, Matthew R.; Prabhudesai, Vaibhav S.; ...

2016-04-07

We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H + 2. The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed 2-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a strong laser field. The interference magnitude and angular period depend strongly on the energy difference between the initial state and the LICI, consistent with coherent diffraction around a cone-shaped potential barrier whose width and thickness depend on the relative energy of the initial state andmore » the cone apex. As a result, these findings are supported by numerical solutions of the time-dependent Schrodinger equation for similar experimental conditions.« less

The fluorescence resonance energy transfer (FRET) gate: a time-resolved study.

PubMed

Xu, Qing-Hua; Wang, Shu; Korystov, Dmitry; Mikhailovsky, Alexander; Bazan, Guillermo C; Moses, Daniel; Heeger, Alan J

2005-01-18

The two-step energy-transfer process in a self-assembled complex comprising a cationic conjugated polymer (CCP) and a dsDNA is investigated by using pump-dump-emission spectroscopy and time-correlated single-photon counting; energy is transferred from the CCP to an ethidium bromide (EB) molecule intercalated into the dsDNA through a fluorescein molecule linked to one terminus of the DNA. Time-dependent anisotropy measurements indicate that the inefficient direct energy transfer from the CCP to the intercalated EB results from the near orthogonality of their transition moments. These measurements also show that the transition moment of the fluorescein spans a range of angular distributions and lies between that of the CCP and EB. Consequently, the fluorescein acts as a fluorescence resonance energy-transfer gate to relay the excitation energy from the CCP to the EB.

The fluorescence resonance energy transfer (FRET) gate: A time-resolved study

PubMed Central

Xu, Qing-Hua; Wang, Shu; Korystov, Dmitry; Mikhailovsky, Alexander; Bazan, Guillermo C.; Moses, Daniel; Heeger, Alan J.

2005-01-01

The two-step energy-transfer process in a self-assembled complex comprising a cationic conjugated polymer (CCP) and a dsDNA is investigated by using pump-dump-emission spectroscopy and time-correlated single-photon counting; energy is transferred from the CCP to an ethidium bromide (EB) molecule intercalated into the dsDNA through a fluorescein molecule linked to one terminus of the DNA. Time-dependent anisotropy measurements indicate that the inefficient direct energy transfer from the CCP to the intercalated EB results from the near orthogonality of their transition moments. These measurements also show that the transition moment of the fluorescein spans a range of angular distributions and lies between that of the CCP and EB. Consequently, the fluorescein acts as a fluorescence resonance energy-transfer gate to relay the excitation energy from the CCP to the EB. PMID:15642946

Observation of quantum interferences via light-induced conical intersections in diatomic molecules

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

Natan, Adi; Ware, Matthew R.; Prabhudesai, Vaibhav S.

We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H + 2. The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed 2-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a strong laser field. The interference magnitude and angular period depend strongly on the energy difference between the initial state and the LICI, consistent with coherent diffraction around a cone-shaped potential barrier whose width and thickness depend on the relative energy of the initial state andmore » the cone apex. As a result, these findings are supported by numerical solutions of the time-dependent Schrodinger equation for similar experimental conditions.« less

Retrieving transient conformational molecular structure information from inner-shell photoionization of laser-aligned molecules

DOE PAGES

Wang, Xu; Le, Anh -Thu; Yu, Chao; ...

2016-03-30

We discuss a scheme to retrieve transient conformational molecular structure information using photoelectron angular distributions (PADs) that have averaged over partial alignments of isolated molecules. The photoelectron is pulled out from a localized inner-shell molecular orbital by an X-ray photon. We show that a transient change in the atomic positions from their equilibrium will lead to a sensitive change in the alignment-averaged PADs, which can be measured and used to retrieve the former. Exploiting the experimental convenience of changing the photon polarization direction, we show that it is advantageous to use PADs obtained from multiple photon polarization directions. Lastly, amore » simple single-scattering model is proposed and benchmarked to describe the photoionization process and to do the retrieval using a multiple-parameter fitting method.« less

Lambertian white top-emitting organic light emitting device with carbon nanotube cathode

NASA Astrophysics Data System (ADS)

Freitag, P.; Zakhidov, Al. A.; Luessem, B.; Zakhidov, A. A.; Leo, K.

2012-12-01

We demonstrate that white organic light emitting devices (OLEDs) with top carbon nanotube (CNT) electrodes show almost no microcavity effect and exhibit essentially Lambertian emission. CNT top electrodes were applied by direct lamination of multiwall CNT sheets onto white small molecule OLED stack. The devices show an external quantum efficiency of 1.5% and high color rendering index of 70. Due to elimination of the cavity effect, the devices show good color stability for different viewing angles. Thus, CNT electrodes are a viable alternative to thin semitransparent metallic films, where the strong cavity effect causes spectral shift and non-Lambertian angular dependence. Our method of the device fabrication is simple yet effective and compatible with virtually any small molecule organic semiconductor stack. It is also compatible with flexible substrates and roll-to-roll fabrication.

Centrifugal distortion coefficients of asymmetric-top molecules: Reduction of the octic terms of the rotational Hamiltonian

NASA Astrophysics Data System (ADS)

Ramachandra Rao, Ch. V. S.

1983-11-01

The rotational Hamiltonian of an asymmetric-top molecule in its standard form, containing terms up to eighth degree in the components of the total angular momentum, is transformed by a unitary transformation with parameters Spqr to a reduced Hamiltonian so as to avoid the indeterminacies inherent in fitting the complete Hamiltonian to observed energy levels. Expressions are given for the nine determinable combinations of octic constants Θ' i ( i = 1 to 9) which are invariant under the unitary transformation. A method of reduction suitable for energy calculations by matrix diagonalization is considered. The relations between the coefficients of the transformed Hamiltonian, for suitable choice of the parameters Spqr, and those of the reduced Hamiltonian are given. This enables the determination of the nine octic constants Θ' i in terms of the experimental constants.

Sensitive and Specific Guest Recognition through Pyridinium-Modification in Spindle-Like Coordination Containers.

PubMed

Bhuvaneswari, Nagarajan; Dai, Feng-Rong; Chen, Zhong-Ning

2018-05-02

An elaborately designed pyridinium-functionalized octanuclear zinc(II) coordination container 1-Zn was prepared through the self-assembly of Zn 2+ , p-tert-butylsulfonylcalix[4]arene, and pyridinium-functionalized angular flexible dicarboxylate linker (H 2 BrL1). The structure was determined by a single-crystal X-ray diffractometer. 1-Zn displays highly sensitive and specific recognition to 2-picolylamine as revealed by drastic blueshifts of the absorption and emission spectra, ascribed to the decrease of intramolecular charge transfer (ICT) character of the container and the occurrence of intermolecular charge transfer between the host and guest molecules. The intramolecular charge transfer plays a key role in the modulation of the electronic properties and is tunable through endo-encapsulation of specific guest molecules. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Low-energy electron scattering from water molecules: A study of angular distributions

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

Gianturco, F.A.; Scialla, S.

1987-12-01

We report quantal calculations of elastic differential and momentum transfercross sections for the scattering of electrons by H/sub 2/O at low and intermediatecollision energies, i.e., from 2 to 20 eV. The fixed-nuclei approximation (FNA) was employed and a single-center expanded (SCE) wave function was used to represent the molecular target. The well-known divergence in the forward direction was corrected via Born closure formulas (see the text) and a parameter-free model, previously tested for methane targets, was used to describe exchange and polarization effects. The present results can be used to adequately describe angular distributions even at very small angles andmore » can be extended beyond the largest angles that have been experimentally measured. The behavior of momentum-transfer cross sections as a function of energy, and the comparison of our results with other static-exchange (SE) calculations, which use an entirely different approach, are presented and discussed.« less

Quantum mechanical treatment of the F+H2 --> HF+H reaction

NASA Astrophysics Data System (ADS)

Baer, Michael; Jellinek, Julius; Kouri, D. J.

1983-03-01

In this paper is presented a quantum dynamical study of the F+H2 reaction within the infinite order sudden approximation for the energy range Etot=0.28-0.50 eV. Results at various stages of the calculation are given ranging from the most detailed phases and S matrices to the total integral cross sections. The accuracy of the IOS is assessed by comparisons of the average l-labeled quantal IOS results with exact classical, initial-l labeled classical IOS, and l-initial labeled quantum IOS results. Comparison with experiment indicates that the qualitative state-to-state angular distributions are reproduced within this method. On the other hand, vibrational branching ratios for the product HF molecule are only partially reproduced. The main part of the discussion in the paper is devoted to the recent hypothesis concerning the existence of a superposition of resonances which strongly influence the angular distributions as a function of final vibrational state of the HF product.

Second rank direction cosine spherical tensor operators and the nuclear electric quadrupole hyperfine structure Hamiltonian of rotating molecules

NASA Astrophysics Data System (ADS)

di Lauro, C.

2018-03-01

Transformations of vector or tensor properties from a space-fixed to a molecule-fixed axis system are often required in the study of rotating molecules. Spherical components λμ,ν of a first rank irreducible tensor can be obtained from the direction cosines between the two axis systems, and a second rank tensor with spherical components λμ,ν(2) can be built from the direct product λ × λ. It is shown that the treatment of the interaction between molecular rotation and the electric quadrupole of a nucleus is greatly simplified, if the coefficients in the axis-system transformation of the gradient of the electric field of the outer charges at the coupled nucleus are arranged as spherical components λμ,ν(2). Then the reduced matrix elements of the field gradient operators in a symmetric top eigenfunction basis, including their dependence on the molecule-fixed z-angular momentum component k, can be determined from the knowledge of those of λ(2) . The hyperfine structure Hamiltonian Hq is expressed as the sum of terms characterized each by a value of the molecule-fixed index ν, whose matrix elements obey the rule Δk = ν. Some of these terms may vanish because of molecular symmetry, and the specific cases of linear and symmetric top molecules, orthorhombic molecules, and molecules with symmetry lower than orthorhombic are considered. Each ν-term consists of a contraction of the rotational tensor λ(2) and the nuclear quadrupole tensor in the space-fixed frame, and its matrix elements in the rotation-nuclear spin coupled representation can be determined by the standard spherical tensor methods.

Twisting short dsDNA with applied tension

NASA Astrophysics Data System (ADS)

Zoli, Marco

2018-02-01

The twisting deformation of mechanically stretched DNA molecules is studied by a coarse grained Hamiltonian model incorporating the fundamental interactions that stabilize the double helix and accounting for the radial and angular base pair fluctuations. The latter are all the more important at short length scales in which DNA fragments maintain an intrinsic flexibility. The presented computational method simulates a broad ensemble of possible molecule conformations characterized by a specific average twist and determines the energetically most convenient helical twist by free energy minimization. As this is done for any external load, the method yields the characteristic twist-stretch profile of the molecule and also computes the changes in the macroscopic helix parameters i.e. average diameter and rise distance. It is predicted that short molecules under stretching should first over-twist and then untwist by increasing the external load. Moreover, applying a constant load and simulating a torsional strain which over-twists the helix, it is found that the average helix diameter shrinks while the molecule elongates, in agreement with the experimental trend observed in kilo-base long sequences. The quantitative relation between percent relative elongation and superhelical density at fixed load is derived. The proposed theoretical model and computational method offer a general approach to characterize specific DNA fragments and predict their macroscopic elastic response as a function of the effective potential parameters of the mesoscopic Hamiltonian.

Molecular hydrogen solvated in water – A computational study

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

Śmiechowski, Maciej, E-mail: Maciej.Smiechowski@pg.gda.pl

2015-12-28

The aqueous hydrogen molecule is studied with molecular dynamics simulations at ambient temperature and pressure conditions, using a newly developed flexible and polarizable H{sub 2} molecule model. The design and implementation of this model, compatible with an existing flexible and polarizable force field for water, is presented in detail. The structure of the hydration layer suggests that first-shell water molecules accommodate the H{sub 2} molecule without major structural distortions and two-dimensional, radial-angular distribution functions indicate that as opposed to strictly tangential, the orientation of these water molecules is such that the solute is solvated with one of the free electronmore » pairs of H{sub 2}O. The calculated self-diffusion coefficient of H{sub 2}(aq) agrees very well with experimental results and the time dependence of mean square displacement suggests the presence of caging on a time scale corresponding to hydrogen bond network vibrations in liquid water. Orientational correlation function of H{sub 2} experiences an extremely short-scale decay, making the H{sub 2}–H{sub 2}O interaction potential essentially isotropic by virtue of rotational averaging. The inclusion of explicit polarizability in the model allows for the calculation of Raman spectra that agree very well with available experimental data on H{sub 2}(aq) under differing pressure conditions, including accurate reproduction of the experimentally noted trends with solute pressure or concentration.« less

Microwave Spectroscopy and Proton Transfer Dynamics in the Formic Acid-Acetic Acid Dimer

NASA Astrophysics Data System (ADS)

Howard, B. J.; Steer, E.; Page, F.; Tayler, M.; Ouyang, B.; Leung, H. O.; Marshall, M. D.; Muenter, J. S.

2012-06-01

The rotational spectrum of the doubly hydrogen-bonded {hetero} dimer formed between formic acid and acetic acid has been recorded between 4 and 18 GHz using a pulsed-nozzle Fourier transform microwave spectrometer. Each rigid-molecule rotational transition is split into four as a result of two concurrent tunnelling motions, one being proton transfer between the two acid molecules, and the other the torsion/rotation of the methyl group within the acetic acid. We present a full assignment of the spectrum for {J} = 1 to {J} = 7 for these four torsion/tunnelling states. Spectra have been observed for the main isotopic species, with deuterium substitution at the C of the formic acid and all 13C species in natural abundance, The observed transitions are fitted to within a few kilohertz using a molecule-fixed effective rotational Hamiltonian for the separate {A} and {E} vibrational species of the G12 permutation-inversion group which is applicable to this complex. To reduce the effects of internal angular momentum, a non-principal axis system is used throughout. Interpretation of the internal motion uses an internal-vibration and overall rotation scheme, and full sets of rotational and centrifugal distortion constants are determined. The proton tunnelling rates and the internal angular momentum of the methyl group in the {E} states is interpreted in terms of a dynamical model which involves coupled proton transfer and internal rotation. The resulting potential energy surface not only describes these internal motions, but can also explain the observed shifts in rotational constants between {A} and {E} species, and the deviations of the tunnelling frequencies from the expected 2:1 ratio. It also permits the determination of spectral constants free from the contamination effects of the internal dynamics. M.C.D. Tayler, B. Ouyang and B.J. Howard, J. Chem. Phys., {134}, 054316 (2011).

The hydrogen molecule under the reaction microscope: single photon double ionization at maximum cross section and threshold (doubly differential cross sections)

DOE PAGES

Weber, Thorsten; Foucar, Lutz; Jahnke, Till; ...

2017-07-07

In this paper, we studied the photo double ionization of hydrogen molecules in the threshold region (50 eV) and the complete photo fragmentation of deuterium molecules at maximum cross section (75 eV) with single photons (linearly polarized) from the Advanced Light Source, using the reaction microscope imaging technique. The 3D-momentum vectors of two recoiling ions and up to two electrons were measured in coincidence. We present the kinetic energy sharing between the electrons and ions, the relative electron momenta, the azimuthal and polar angular distributions of the electrons in the body-fixed frame. We also present the dependency of the kineticmore » energy release in the Coulomb explosion of the two nuclei on the electron emission patterns. We find that the electronic emission in the body-fixed frame is strongly influenced by the orientation of the molecular axis to the polarization vector and the internuclear distance as well as the electronic energy sharing. Finally, traces of a possible breakdown of the Born–Oppenheimer approximation are observed near threshold.« less

Photodissociation of quantum state-selected diatomic molecules yields new insight into ultracold chemistry

NASA Astrophysics Data System (ADS)

McDonald, Mickey; McGuyer, Bart H.; Lee, Chih-Hsi; Apfelbeck, Florian; Zelevinsky, Tanya

2016-05-01

When a molecule is subjected to a sufficiently energetic photon it can break apart into fragments through a process called ``photodissociation''. For over 70 years this simple chemical reaction has served as a vital experimental tool for acquiring information about molecular structure, since the character of the photodissociative transition can be inferred by measuring the 3D photofragment angular distribution (PAD). While theoretical understanding of this process has gradually evolved from classical considerations to a fully quantum approach, experiments to date have not yet revealed the full quantum nature of this process. In my talk I will describe recent experiments involving the photodissociation of ultracold, optical lattice-trapped, and fully quantum state-resolved 88Sr2 molecules. Optical absorption images of the PADs produced in these experiments reveal features which are inherently quantum mechanical in nature, such as matter-wave interference between output channels, and are sensitive to the quantum statistics of the molecular wavefunctions. The results of these experiments cannot be predicted using quasiclassical methods. Instead, we describe our results with a fully quantum mechanical model yielding new intuition about ultracold chemistry.

On the Relative "Transparency" of Gas-phase Coronene Molecules to Low-energy Electrons: Effects on the Interstellar Medium

NASA Astrophysics Data System (ADS)

Carelli, F.; Gianturco, F. A.

2011-12-01

Free, gas-phase polycyclic aromatic hydrocarbons (PAHs) are understood to play an important role in the interstellar medium (ISM), as they are thought to significantly contribute to both diffused and unidentified infrared interstellar bands. They are also considered fundamental blocks of the interstellar dust, whose nature has important implications for a plethora of physical and chemical nanoscopic processes within the ISM. Since free electrons represent a versatile alternative way to transport energy in the interstellar space, in this paper we compute from quantum scattering methods the angular redistributions of free electrons by gas-phase coronene molecules, the latter of which are believed to be one of the most representative PAHs, in order to assess their role in describing the efficiency of electron deflection by this molecule. The associated rates can provide useful information about the coupling mechanism between external radio-frequency fields and complex molecular plasmas containing neutral and ionized PAHs. They can also yield information on the possible presence of such species in the dust phase of the medium.

The hydrogen molecule under the reaction microscope: single photon double ionization at maximum cross section and threshold (doubly differential cross sections)

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

Weber, Thorsten; Foucar, Lutz; Jahnke, Till

In this paper, we studied the photo double ionization of hydrogen molecules in the threshold region (50 eV) and the complete photo fragmentation of deuterium molecules at maximum cross section (75 eV) with single photons (linearly polarized) from the Advanced Light Source, using the reaction microscope imaging technique. The 3D-momentum vectors of two recoiling ions and up to two electrons were measured in coincidence. We present the kinetic energy sharing between the electrons and ions, the relative electron momenta, the azimuthal and polar angular distributions of the electrons in the body-fixed frame. We also present the dependency of the kineticmore » energy release in the Coulomb explosion of the two nuclei on the electron emission patterns. We find that the electronic emission in the body-fixed frame is strongly influenced by the orientation of the molecular axis to the polarization vector and the internuclear distance as well as the electronic energy sharing. Finally, traces of a possible breakdown of the Born–Oppenheimer approximation are observed near threshold.« less

Accessing the molecular frame through strong-field alignment of distributions of gas phase molecules

NASA Astrophysics Data System (ADS)

Reid, Katharine L.

2018-03-01

A rationale for creating highly aligned distributions of molecules is that it enables vector properties referenced to molecule-fixed axes (the molecular frame) to be determined. In the present work, the degree of alignment that is necessary for this to be achieved in practice is explored. Alignment is commonly parametrized in experiments by a single parameter, ?, which is insufficient to enable predictive calculations to be performed. Here, it is shown that, if the full distribution of molecular axes takes a Gaussian form, this single parameter can be used to determine the complete set of alignment moments needed to characterize the distribution. In order to demonstrate the degree of alignment that is required to approach the molecular frame, the alignment moments corresponding to a few chosen values of ? are used to project a model molecular frame photoelectron angular distribution into the laboratory frame. These calculations show that ? needs to approach 0.9 in order to avoid significant blurring to be caused by averaging. This article is part of the theme issue `Modern theoretical chemistry'.

Myosin conformational states determined by single fluorophore polarization

PubMed Central

Warshaw, David M.; Hayes, Eric; Gaffney, Donald; Lauzon, Anne-Marie; Wu, Junru; Kennedy, Guy; Trybus, Kathleen; Lowey, Susan; Berger, Christopher

1998-01-01

Muscle contraction is powered by the interaction of the molecular motor myosin with actin. With new techniques for single molecule manipulation and fluorescence detection, it is now possible to correlate, within the same molecule and in real time, conformational states and mechanical function of myosin. A spot-confocal microscope, capable of detecting single fluorophore polarization, was developed to measure orientational states in the smooth muscle myosin light chain domain during the process of motion generation. Fluorescently labeled turkey gizzard smooth muscle myosin was prepared by removal of endogenous regulatory light chain and re-addition of the light chain labeled at cysteine-108 with the 6-isomer of iodoacetamidotetramethylrhodamine (6-IATR). Single myosin molecule fluorescence polarization data, obtained in a motility assay, provide direct evidence that the myosin light chain domain adopts at least two orientational states during the cyclic interaction of myosin with actin, a randomly disordered state, most likely associated with myosin whereas weakly bound to actin, and an ordered state in which the light chain domain adopts a finite angular orientation whereas strongly bound after the powerstroke. PMID:9653135

Attosecond control of dissociative ionization of O{sub 2} molecules

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

Siu, W.; Kelkensberg, F.; Gademann, G.

We demonstrate that dissociative ionization of O{sub 2} can be controlled by the relative delay between an attosecond pulse train (APT) and a copropagating infrared (IR) field. Our experiments reveal a dependence of both the branching ratios between a range of electronic states and the fragment angular distributions on the extreme ultraviolet (XUV) to IR time delay. The observations go beyond adiabatic propagation of dissociative wave packets on IR-induced quasistatic potential energy curves and are understood in terms of an IR-induced coupling between electronic states in the molecular ion.

Exchange-Dominated Pure Spin Current Transport in Alq3 Molecules.

PubMed

Jiang, S W; Liu, S; Wang, P; Luan, Z Z; Tao, X D; Ding, H F; Wu, D

2015-08-21

We address the controversy over the spin transport mechanism in Alq3 utilizing spin pumping in the Y3Fe5O12/Alq3/Pd system. An unusual angular dependence of the inverse spin Hall effect is found. It, however, disappears when the microwave magnetic field is fully in the sample plane, excluding the presence of the Hanle effect. Together with the quantitative temperature-dependent measurements, these results provide compelling evidence that the pure spin current transport in Alq3 is dominated by the exchange-mediated mechanism.

Ordered and disordered dynamics in monolayers of rolling particles.

PubMed

Kim, Byungsoo; Putkaradze, Vakhtang

2010-12-10

We consider the ordered and disordered dynamics for monolayers of rolling self-interacting particles modeling water molecules. The rolling constraint represents a simplified model of a strong, but rapidly decaying bond with the surface. We show the existence and nonlinear stability of ordered lattice states, as well as disturbance propagation through and chaotic vibrations of these states. We study the dynamics of disordered gas states and show that there is a surprising and universal linear connection between distributions of angular and linear velocity, allowing definition of temperature.

Recombination of H3(+) and D3(+) Ions in a Flowing Afterglow Plasma

NASA Technical Reports Server (NTRS)

Gougousi, T.; Johnsen, R.; Golde, M. F.

1995-01-01

The analysis of flowing afterglow plasmas containing H3(+) or D3(+) ions indicates that the de-ionization of such plasmas does not occur by simple dissociative recombination of ions with electrons. An alternative model of de-ionization is proposed in which electrons are captured into H3(**) auto-ionization Rydberg states that are stabilized by collisional mixing of the Rydberg molecules' angular momenta. The proposed mechanism would enable de-ionization to occur without the need for dissociative recombination by the mechanisms of potential-surface crossings.

Switchable molecular magnets

PubMed Central

SATO, Osamu

2012-01-01

Various molecular magnetic compounds whose magnetic properties can be controlled by external stimuli have been developed, including electrochemically, photochemically, and chemically tunable bulk magnets as well as a phototunable antiferromagnetic phase of single chain magnet. In addition, we present tunable paramagnetic mononuclear complexes ranging from spin crossover complexes and valence tautomeric complexes to Co complexes in which orbital angular momentum can be switched. Furthermore, we recently developed several switchable clusters and one-dimensional coordination polymers. The switching of magnetic properties can be achieved by modulating metals, ligands, and molecules/ions in the second sphere of the complexes. PMID:22728438

Rabi like angular splitting in Surface Plasmon Polariton - Exciton interaction in ATR configuration

NASA Astrophysics Data System (ADS)

Hassan, Heba; Abdallah, T.; Negm, S.; Talaat, H.

2018-05-01

We have studied the coupling of propagating Surface Plasmon Polaritons (SPP) on silver films and excitons in CdS quantum dots (QDs). We employed the Kretschmann-Raether configuration of the attenuated total reflection (ATR) to propagate the SPP on silver film of thickness 47.5 nm at three different wavelengths. The CdS QD have been chemically synthesized with particular size such that its exciton of energy would resonate with SPP. High resolution transmission electron microscopy (HRTEM) and scan tunneling microscopy (STM) were used to measure the corresponding QDs size and confirm its shape. Further confirmation of the size has been performed by the effective mass approximation (EMA) model utilizing the band gap of the prepared QDs. The band gaps have been measured through UV-vis absorption spectra as well as scan tunneling spectroscopy (STS). The coupling has been observed as two branching dips in the ATR spectra indicating Rabi like splitting. To the best of our knowledge, this is the first time that Rabi interaction is directly observed in an ATR angular spectra. This observation is attributed to the use a high resolution angular scan (±0.005°), in addition to the Doppler width of the laser line as well as the energy distribution of the excitons. The effect of three different linker molecules (TOPO, HDA), (Pyridine) and (Tri-butylamine) as surface ligands, on SPP-Exciton interaction has been examined.

Precision Measurements with a Molecular Clock

NASA Astrophysics Data System (ADS)

Grier, Andrew; McDonald, Mickey; McGuyer, Bart; Iwata, Geoffrey; Apfelbeck, Florian; Tarallo, Marco; Zelevinsky, Tanya

2015-05-01

We report on recent results obtained with photoassociated Sr2 molecules confined in a lattice. Sr2 has a range of electronically excited bound states which are readily accessible with optical wavelengths using the narrow 1S0->3P1 intercombination line. As in Nat. Phys. 11, 32, we measure the lifetimes of the narrow, deeply-bound subradiant states in the 1g (1S0+3P1 dissociative limit) potential, allowing for coherent control of molecules and a comparison with theoretical predictions of the lifetimes and transition strengths of these states. Next, we study ultracold photodissociation of Sr2 molecules through abortion of one and two photons near the atomic intercombination line. This allows us to observe the vector character of transition elements through the angular dissociation pattern and to directly measure barrier heights in the excited state potentials. Finally, as shown in PRL 114, 023001, we demonstrate that in a non-magic lattice, a narrow transition can be used to measure the trapped gas temperature through the linewidth of the spectral feature corresponding to the carrier transitions. We use this technique to measure the temperature of Sr2 molecules to 10x higher precision than with standard techniques. We discuss future prospects with this molecular lattice clock. Funding from NIST, ARO, and NSF IGERT.

Utilization of UV and IR Supercontinua in Gas-Phase Subpicosecond Kinetic Spectroscopy

NASA Astrophysics Data System (ADS)

Glownia, J. H.; Misewich, J.; Sorokin, P. P.

Through the work of photochemists extending over many decades, there now exists a wealth of information on the various reactions that photoexcited gas phase molecules undergo. Most of this information relates to the product molecules that are formed, either as the direct result of a primary photochemical act, such as photodissociation, or through subsequent secondary reactions, involving collisions with other molecules in the gas. Recently, there has been an extensive effort directed at determining the exact energy distributions of the primary products formed in photodissociation. With the use of nanosecond tunable-laser techniques, such as laser-induced fluorescence (LIF) and coherent anti-Stokes Raman spectroscopy (CARS), scientists have successfully determined the nascent electronic, vibrational, and rotational energy distributions of various diatomic fragments such as CN, OH, NO, and O2 that are directly formed in the photodissociation of many kinds of molecules. The ready availability of high-quality, tunable, nanosecond lasers has made determination of the above-mentioned collisionless energy distributions a relatively straightforward process. The determination of product translational energies has long effectively been handled by angularly resolved time-of-flight (TOF) spectroscopy, or by sub-Doppler resolution spectroscopy, including a recently improved version of the latter, velocity-aligned Doppler spectroscopy (Xu et al., 1986).

Semiclassical theory of the self-consistent vibration-rotation fields and its application to the bending-rotation interaction in the H{sub 2}O molecule

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

Skalozub, A.S.; Tsaune, A.Ya.

1994-12-01

A new approach for analyzing the highly excited vibration-rotation (VR) states of nonrigid molecules is suggested. It is based on the separation of the vibrational and rotational terms in the molecular VR Hamiltonian by introducing periodic auxiliary fields. These fields transfer different interactions within a molecule and are treated in terms of the mean-field approximation. As a result, the solution of the stationary Schroedinger equation with the VR Hamiltonian amounts to a quantization of the Berry phase in a problem of the molecular angular-momentum motion in a certain periodic VR field (rotational problem). The quantization procedure takes into account themore » motion of the collective vibrational variables in the appropriate VR potentials (vibrational problem). The quantization rules, the mean-field configurations of auxiliary interactions, and the solutions to the Schrodinger equations for the vibrational and rotational problems are self-consistently connected with one another. The potentialities of the theory are demonstrated by the bending-rotation interaction modeled by the Bunker-Landsberg potential function in the H{sub 2} molecule. The calculations are compared with both the results of the exact computations and those of other approximate methods. 32 refs., 4 tabs.« less

Detection and characterization of the tin dihydride (SnH2 and SnD2) molecule in the gas phase

NASA Astrophysics Data System (ADS)

Smith, Tony C.; Clouthier, Dennis J.

2018-01-01

The SnH2 and SnD2 molecules have been detected for the first time in the gas phase by laser-induced fluorescence (LIF) and emission spectroscopic techniques through the à 1B1-X ˜ 1A1 electronic transition. These reactive species were prepared in a pulsed electric discharge jet using (CH3)4Sn or SnH4/SnD4 precursors diluted in high pressure argon. Transitions to the electronic excited state of the jet-cooled molecules were probed with LIF, and the ground state energy levels were measured from single rovibronic level emission spectra. The LIF spectrum of SnD2 afforded sufficient rotational structure to determine the ground and excited state geometries: r0″ = 1.768 Å, θ0″ = 91.0°, r0' = 1.729 Å, θ0' = 122.9°. All of the observed LIF bands show evidence of a rotational-level-dependent predissociation process which rapidly decreases the fluorescence yield and lifetime with increasing rotational angular momentum in each excited vibronic level. This behavior is analogous to that observed in SiH2 and GeH2 and is suggested to lead to the formation of ground state tin atoms and hydrogen molecules.

Nuclear magnetic resonance of laser-polarized noble gases in molecules, materials and organisms

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

Goodson, Boyd McLean

1999-12-01

Conventional nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI) are fundamentally challenged by the insensitivity that stems from the ordinarily low spin polarization achievable in even the strongest NMR magnets. However, by transferring angular momentum from laser light to electronic and nuclear spins, optical pumping methods can increase the nuclear spin polarization of noble gases by several orders of magnitude, thereby greatly enhancing their NMR sensitivity. This dissertation is primarily concerned with the principles and practice of optically pumped nuclear magnetic resonance (OPNMR). The enormous sensitivity enhancement afforded by optical pumping noble gases can be exploited to permitmore » a variety of novel NMR experiments across many disciplines. Many such experiments are reviewed, including the void-space imaging of organisms and materials, NMR and MRI of living tissues, probing structure and dynamics of molecules in solution and on surfaces, and zero-field NMR and MRI.« less

Conformational effects on circular dichroism in the photoelectron angular distribution.

PubMed

Di Tommaso, Devis; Stener, Mauro; Fronzoni, Giovanna; Decleva, Piero

2006-04-10

The B-spline density-functional method has been applied to the conformers of the (1R, 2R)-1,2-dibromo-1,2-dichloro-1,2-difluoroethane molecule. The cross section, asymmetry, and dichroic parameters relative to core and valence orbitals, which do not change their nature along the conformational curve, have been systematically studied. While the cross section and the asymmetry parameter are weakly affected, the dichroic parameter appears to be rather sensitive to the particular conformer of the molecule, suggesting that this dynamical property could be a useful tool for conformational analysis. The computational method has also been applied to methyl rotation in methyloxirane. Unexpected and dramatic sensitivity of the dichroic-parameter profile to the methyl rotation, both in the core and valence states, has been found. Boltzmann averaging over the conformers reproduces quite closely the profiles previously obtained for the minimum-energy conformation, which is in good agreement with the experimental results.

Communication: Photoionization of degenerate orbitals for randomly oriented molecules: The effect of time-reversal symmetry on recoil-ion momentum angular distributions

NASA Astrophysics Data System (ADS)

Suzuki, Yoshi-Ichi

2018-04-01

The photoelectron asymmetry parameter β, which characterizes the direction of electrons ejected from a randomly oriented molecular ensemble by linearly polarized light, is investigated for degenerate orbitals. We show that β is totally symmetric under the symmetry operation of the point group of a molecule, and it has mixed properties under time reversal. Therefore, all degenerate molecular orbitals, except for the case of degeneracy due to time reversal, have the same β (Wigner-Eckart theorem). The exceptions are e-type complex orbitals of the Cn, Sn, Cnh, T, and Th point groups, and calculations on boric acid (C3h symmetry) are performed as an example. However, including those point groups, all degenerate orbitals have the same β if those orbitals are real. We discuss the implications of this operator formalism for molecular alignment and photoelectron circular dichroism.

Communication: Multiple-property-based diabatization for open-shell van der Waals molecules

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

Karman, Tijs; Avoird, Ad van der; Groenenboom, Gerrit C., E-mail: gerritg@theochem.ru.nl

2016-03-28

We derive a new multiple-property-based diabatization algorithm. The transformation between adiabatic and diabatic representations is determined by requiring a set of properties in both representations to be related by a similarity transformation. This set of properties is determined in the adiabatic representation by rigorous electronic structure calculations. In the diabatic representation, the same properties are determined using model diabatic states defined as products of undistorted monomer wave functions. This diabatic model is generally applicable to van der Waals molecules in arbitrary electronic states. Application to locating seams of conical intersections and collisional transfer of electronic excitation energy is demonstrated formore » O{sub 2} − O{sub 2} in low-lying excited states. Property-based diabatization for this test system included all components of the electric quadrupole tensor, orbital angular momentum, and spin-orbit coupling.« less

The atom-molecule reaction D plus H2 yields HD plus H studied by molecular beams

NASA Technical Reports Server (NTRS)

Geddes, J.; Krause, H. F.; Fite, W. L.

1972-01-01

Collisions between deuterium atoms and hydrogen molecules were studied in a modulated crossed beam experiment. The relative signal intensity and the signal phase for the product HD from reactive collisions permitted determination of both the angular distribution and HD mean velocity as a function of angle. From these a relative differential reactive scattering cross section in center-of-mass coordinates was deduced. The experiment indicates that reactively formed HD which has little or no internal excitation departs from the collision anisotropically, with maximum amplitude 180 deg from the direction of the incident D beam in center-of-mass coordinates, which shows that the D-H-H reacting configuration is short-lived compared to its rotation time. Non reactive scattering of D by H2 was used to assign absolute values to the differential reactive scattering cross sections.

Charles Hard Townes: Remarkable Scientist and Inspiring Teacher

NASA Astrophysics Data System (ADS)

Goldsmith, P. F.

2015-05-01

Charles Townes is renowned for his work elucidating the structure of molecules through microwave spectroscopy and for his invention of the maser and the laser. He also had a lifelong interest in astronomy, and in the later portion of his remarkable and long career devoted himself to astronomical research, pioneering the study of molecules in interstellar space and the development of infrared spectroscopy, first from the ground and then from airborne facilities. His interest in high angular resolution, as well as high spectral resolution observations, led to development of the first infrared spatial interferometer employing coherent signal processing techniques. In this short review I will only touch on some of Townes' many scientific contributions, concentrating on astronomy, and will also give some personal thoughts about how he inspired students in their research, helping to make the "Townes Group" at the University of California, Berkeley, an ideal environment in which to start a career in research.

Electronic spectrum of the UO and UO(+) molecules.

PubMed

Tyagi, Rajni; Zhang, Zhiyong; Pitzer, Russell M

2014-12-18

Electronic theory calculations are applied to the study of the UO molecule and the UO(+) ion. Relativistic effective core potentials are used along with the accompanying valence spin-orbit operators. Polarized double-ς and triple-ς basis sets are used. Molecular orbitals are obtained from state-averaged multiconfiguration self-consistent field calculations and then used in multireference spin-orbit configuration interaction calculations with a number of millions of terms. The ground state of UO has open shells of 5f(3)7s(1), angular momentum Ω = 4, and a spin-orbit-induced avoided crossing near the equilibrium internuclear distance. Many UO excited states are studied with rotational constants, intensities, and experimental comparisons. The ground state of UO(+) is of 5f(3) nature with Ω = 9/2. Many UO(+) excited states are also studied. The open-shell nature of both UO and UO(+) leads to many low-lying excited states.

Excitation enhancement and extraction enhancement with photonic crystals

DOEpatents

Shapira, Ofer; Soljacic, Marin; Zhen, Bo; Chua, Song-Liang; Lee, Jeongwon; Joannopoulos, John

2015-03-03

Disclosed herein is a system for stimulating emission from at least one an emitter, such as a quantum dot or organic molecule, on the surface of a photonic crystal comprising a patterned dielectric substrate. Embodiments of this system include a laser or other source that illuminates the emitter and the photonic crystal, which is characterized by an energy band structure exhibiting a Fano resonance, from a first angle so as to stimulate the emission from the emitter at a second angle. The coupling between the photonic crystal and the emitter may result in spectral and angular enhancement of the emission through excitation and extraction enhancement. These enhancement mechanisms also reduce the emitter's lasing threshold. For instance, these enhancement mechanisms enable lasing of a 100 nm thick layer of diluted organic molecules solution with reduced threshold intensity. This reduction in lasing threshold enables more efficient organic light emitting devices and more sensitive molecular sensing.

Electron stimulated desorption studies of the adsorption and dynamics of molecules on a copper(110) single crystal surface

NASA Astrophysics Data System (ADS)

Mocuta, Dan Mihai

This thesis describes studies of angular distributions produced by the electron stimulated desorption of ions and neutrals from adsorbates on a Cu(110) surface. A new technique, time-of-flight electron stimulated desorption ion angular distribution (TOF-ESDIAD), has been developed and several studies using this method are reported. The low frequency frustrated translation mode of a model system, low coverage CO/Cu(110), is analyzed using TOF-ESDIAD. A simplified model is used to extract the energies of this mode along the two crystal azimuthal directions. A first time measurement of an anisotropy of this mode in the two directions is reported. The same frustrated translational energies giving the same anisotropy have been measured in a helium atom scattering experiment in confirmation of the ESDIAD measurements. An analysis of the TOF distributions of species desorbing from CO/Cu(110) shows that these are Maxwellian. It is shown that CO* and CO+ have similar TOF distributions, indicating a common desorption channel for both species. The ability of ESDIAD to measure chemical bond directions has been put to use in the observation of interadsorbate interactions. It is shown that at high CO coverage on the Cu(110) surface, the CO molecules agglomerate in chains and tilt away from the surface normal. The same phenomenon is observed in the case of NH3, where H+ ions produced by rupturing the N-H bonds of this molecule are imaged. The NH3 molecules can be trapped in a tilted position by cooling the copper surface using liquid helium. It is shown that such a configuration is a precursor to the upright chemisorbed configuration, in which the molecules rotate around the C3v axis. Not only can we image using the electrons, but we can produce new species by electron bombardment. The dissociation of NH3 to NH2 and H has been induced by electrons and the formation of these products is witnessed using ESDIAD. The oxygen induced reconstruction of the Cu(110) surface is studied. The formation of the characteristic striped oxide structure is witnessed using ESDIAD and new details on the interactions between the oxide ions within the stripes are revealed by the ejection directions of the O+ ions produced by electron stimulation. The interaction between the oxide structure and coadsorbed Ar and CO is also described. Aspects on the thermal activation of low frequency vibrational modes of adsorbates are addressed. The thesis concludes with a look at the possible other developments in the use of TOF-ESDIAD.

HF in clusters of molecular hydrogen. I. Size evolution of quantum solvation by parahydrogen molecules.

PubMed

Jiang, Hao; Bacić, Zlatko

2005-06-22

We present a theoretical study of the quantum solvation of the HF molecule by a small number of parahydrogen molecules, having n = 1-13 solvent particles. The minimum-energy cluster structures determined for n = 1-12 have all of the H(2) molecules in the first solvent shell. The first solvent shell closes at n = 12 and its geometry is icosahedral, with the HF molecule at the center. The quantum-mechanical ground-state properties of the clusters are calculated exactly using the diffusion Monte Carlo method. The zero-point energy of (p-H(2))(n)HF clusters is unusually large, amounting to 86% of the potential well depth for n > 7. The radial probability distribution functions (PDFs) confirm that the first solvent shell is complete for n = 12, and that the 13th p-H(2) molecule begins to fill the second solvent shell. The p-H(2) molecules execute large-amplitude motions and are highly mobile, making the solvent cage exceptionally fluxional. The anisotropy of the solvent, very pronounced for small clusters, decreases rapidly with increasing n, so that for n approximately 8-9 the solvent environment is practically isotropic. The analysis of the pair angular PDF reveals that for a given n, the parahydrogen solvent density around the HF is modulated in a pattern which clearly reflects the lowest-energy cluster configuration. The rigidity of the solvent clusters displays an interesting size dependence, increasing from n = 6 to 9, becoming floppier for n = 10, and increasing again up to n = 12, as the solvent shell is filled. The rigidity of the solvent cage appears to reach its maximum for n = 12, the point at which the first solvent shell is closed.

Inelastic electron tunneling mediated by a molecular quantum rotator

NASA Astrophysics Data System (ADS)

Sugimoto, Toshiki; Kunisada, Yuji; Fukutani, Katsuyuki

2017-12-01

Inelastic electron tunneling (IET) accompanying nuclear motion is not only of fundamental physical interest but also has strong impacts on chemical and biological processes in nature. Although excitation of rotational motion plays an important role in enhancing electric conductance at a low bias, the mechanism of rotational excitation remains veiled. Here, we present a basic theoretical framework of IET that explicitly takes into consideration quantum angular momentum, focusing on a molecular H2 rotator trapped in a nanocavity between two metallic electrodes as a model system. It is shown that orientationally anisotropic electrode-rotator coupling is the origin of angular-momentum exchange between the electron and molecule; we found that the anisotropic coupling imposes rigorous selection rules in rotational excitation. In addition, rotational symmetry breaking induced by the anisotropic potential lifts the degeneracy of the energy level of the degenerated rotational state of the quantum rotator and tunes the threshold bias voltage that triggers rotational IET. Our theoretical results provide a paradigm for physical understanding of the rotational IET process and spectroscopy, as well as molecular-level design of electron-rotation coupling in nanoelectronics.

Photonic Interrogation and Control of Nano Processes

NASA Technical Reports Server (NTRS)

Jassemnejad, Baha

2003-01-01

My research activities for the summer of 2003 consisted of two projects: One project was concerned with determining a method for predicting the static and dynamic assembly properties of nano-structures using laser tweezers. The other project was to investigate the generation of Laguerre-Gaussian modes using a spatial light modulator incorporated into an optical tweezers system. Concerning the first project, I initially pursued the approach suggested by my NASA colleague Dr. Art Decker. This approach involved mimicking the model of the structure of atomic nucleus for the assembly of 1 to 100 atoms using allowed quadruple transitions induced by orbital angular momentums of a Laguerre- Gaussian (Doughnut) laser mode. After realizing the inaptness of the nuclear model with the nanostructure model as far as the binding forces and transitions were concerned, I focused on using quantum dot modei. This model was not attuned also for the host lattice influences the electronic structure of the quantum dot. Thus one other option that I decided to pursue was the approach of molecular quantum mechanics. In this approach the nanostructure is treated as a large (10-100 nm) molecule constructed from single element or multi-elements. Subsequent to consultation with Dr. Fred Morales, a chemical engineer at NASA GRC, and Dr. David Ball, a computational chemist at Cleveland State University, I acquired a molecular-quantum computation software, Hyperchem 7.0. This software allows simulation of different molecular structures as far as their static and dynamic behaviors are concerned. The time that I spent on this project was about eight weeks. Once this suitable approach was identified, I realized the need to collaborate with a computational quantum chemist to pursue searching for stable nanostructures in the range of 10-100 nm that we can be assembled using laser tweezers. The second project was about generating laser tweezers that possess orbital angular momentum. As shown, we were able to generate laser tweezers modes of different orbital angular momentum using a spatial light modulator incorporated into a laser tweezers system. The motivation for investigating these types of modes stems from being able to spin particles at high speeds and also to orient two particles in separate traps and then join them together. Also, there has been recent intense interest on fundamental physics research on orbital angular momentum of light. The fact that circularly polarized light may have associated with it angular momentum that relates to the spin of individual photons (spin 0 for the plane polarized light, spin +1 for the right-circularly polarized light and spin -1 for the left-circularly polarized light) was first demonstrated by Beth in 1936. Orbital angular momentum is, however, distinct from spin in that the spin angular momentum of light is intrinsically linked to the behavior of the electric field in the light whereas orbital angular momentum is a consequence of inclined wavefronts. In 1992 L. Allen, et al showed that the Laguerre-Gaussian (LG) modes could possess well-defined orbital angular momentum that can exceed 1 planck's constant, i.e. l plancks constant per photon, where l is the azimuthal index of the mode.

Charge exchange in cometary coma: Discovery of H- ions in the solar wind close to comet 67P/Churyumov-Gerasimenko.

PubMed

Burch, J L; Cravens, T E; Llera, K; Goldstein, R; Mokashi, P; Tzou, C-Y; Broiles, T

2015-07-16

As Rosetta was orbiting comet 67P/Churyumov-Gerasimenko, the Ion and Electron Sensor detected negative particles with angular distributions like those of the concurrently measured solar wind protons but with fluxes of only about 10% of the proton fluxes and energies of about 90% of the proton energies. Using well-known cross sections and energy-loss data, it is determined that the fluxes and energies of the negative particles are consistent with the production of H - ions in the solar wind by double charge exchange with molecules in the coma.

Algorithms for calculating mass-velocity and Darwin relativistic corrections with n-electron explicitly correlated Gaussians with shifted centers

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

Stanke, Monika, E-mail: monika@fizyka.umk.pl; Palikot, Ewa, E-mail: epalikot@doktorant.umk.pl; Adamowicz, Ludwik, E-mail: ludwik@email.arizona.edu

2016-05-07

Algorithms for calculating the leading mass-velocity (MV) and Darwin (D) relativistic corrections are derived for electronic wave functions expanded in terms of n-electron explicitly correlated Gaussian functions with shifted centers and without pre-exponential angular factors. The algorithms are implemented and tested in calculations of MV and D corrections for several points on the ground-state potential energy curves of the H{sub 2} and LiH molecules. The algorithms are general and can be applied in calculations of systems with an arbitrary number of electrons.

The three-body problem with short-range interactions

NASA Astrophysics Data System (ADS)

Nielsen, E.; Fedorov, D. V.; Jensen, A. S.; Garrido, E.

2001-06-01

The quantum mechanical three-body problem is studied for general short-range interactions. We work in coordinate space to facilitate accurate computations of weakly bound and spatially extended systems. Hyperspherical coordinates are used in both the interpretation and as an integral part of the numerical method. Universal properties and model independence are discussed throughout the report. We present an overview of the hyperspherical adiabatic Faddeev equations. The wave function is expanded on hyperspherical angular eigenfunctions which in turn are found numerically using the Faddeev equations. We generalize the formalism to any dimension of space d greater or equal to two. We present two numerical techniques for solving the Faddeev equations on the hypersphere. These techniques are effective for short and intermediate/large distances including use for hard core repulsive potentials. We study the asymptotic limit of large hyperradius and derive the analytic behaviour of the angular eigenvalues and eigenfunctions. We discuss four applications of the general method. We first analyze the Efimov and Thomas effects for arbitrary angular momenta and for arbitrary dimensions d. Second we apply the method to extract the general behaviour of weakly bound three-body systems in two dimensions. Third we illustrate the method in three dimensions by structure computations of Borromean halo nuclei, the hypertriton and helium molecules. Fourth we investigate in three dimensions three-body continuum properties of Borromean halo nuclei and recombination reactions of helium atoms as an example of direct relevance for the stability of Bose-Einstein condensates.

Crossed beam studies of ion-molecule reactions in methane and ammonia

NASA Technical Reports Server (NTRS)

Smith, G. P. K.; Saunders, M.; Cross, R. J., Jr.

1976-01-01

A crossed-beam apparatus is used to measure the product ion velocity and angular distributions for the following ion-molecule reactions in the relative energy range from 2 to 9 eV: CH4(+) + NH3 yields NH4(+) + CH3; CH4(+) + NH3 yields CNH5(+) + H2; NH2(+) + CH4 yields CNH4(+) + H2 (or 2H); and CH3(+) + NH3 yields CNH4(+) + H2 (or 2H). These reactions are also studied by means of deuterium labeling as a further probe of the detailed reaction dynamics. Probability contour plots for the four reactions are constructed in Cartesian velocity space, and product peaks in the plots are discussed. Relative cross sections and Q values are computed for two of the reactions as well as for the corresponding deuterium-labelled reactions. The results show that the present ion-neutral condensation reactions are highly exothermic with a deep well for the internal complex, that little hydrogen scrambling occurs, and that the energy of the reactions is released mainly as internal energy, even to the extent of producing two hydrogen atoms in some cases rather than one hydrogen atom or molecule.

Unambiguous Signature of the Berry Phase in Intense Laser Dissociation of Diatomic Molecules.

PubMed

Bouakline, Foudhil

2018-05-03

We report strong evidence of Berry phase effects in intense laser dissociation of D 2 + molecules, manifested as Aharonov-Bohm-like oscillations in the photofragment angular distribution (PAD). Our calculations show that this interference pattern strongly depends on the parity of the diatom initial rotational state, (-1) j . Indeed, the PAD local maxima (minima) observed in one case ( j odd) correspond to local minima (maxima) in the other case ( j even). Using simple topological arguments, we clearly show that such interference conversion is a direct signature of the Berry phase. The sole effect of the latter on the rovibrational wave function is a sign change of the relative phase between two interfering components, which wind in opposite senses around a light-induced conical intersection (LICI). Therefore, encirclement of the LICI leads to constructive ( j odd) or destructive ( j even) self-interference of the initial nuclear wavepacket in the dissociative limit. To corroborate our theoretical findings, we suggest an experiment of strong-field indirect dissociation of D 2 + molecules, comparing the PAD of the ortho and para molecular species in directions nearly perpendicular to the laser polarization axis.

Alignment of the hydrogen molecule under intense laser fields

DOE PAGES

Lopez, Gary V.; Fournier, Martin; Jankunas, Justin; ...

2017-06-01

Alignment, dissociation and ionization of H 2 molecules in the ground or the electronically excited E,F state of the H 2 molecule are studied and contrasted using the Velocity Mapping Imaging (VMI) technique. Photoelectron images from nonresonant 7-, 8- and 9-photon radiation ionization of H 2 show that the intense laser fields create ponderomotive shifts in the potential energy surfaces and distort the velocity of the emitted electrons that are produced from ionization. Photofragment images of H+ due to the dissociation mechanism that follows the 2-photon excitation into the (E,F; v = 0, J = 0, 1) electronic state showmore » a strong dependence on laser intensity, which is attributed to the high polarizability of the H 2 (E,F) state. For transitions from the J = 0 state, particularly, we observe marked structure in the angular distribution, which we explain as the interference between the prepared J = 0 and Stark-mixed J = 2 rovibrational states of H 2, as the laser intensity increases. Quantification of these effects allows us to extract the molecular polarizability of the H 2 (E,F) state, and yields a value of 103 ± 37 A.U.« less

Alignment of the hydrogen molecule under intense laser fields

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

Lopez, Gary V.; Fournier, Martin; Jankunas, Justin

Alignment, dissociation and ionization of H 2 molecules in the ground or the electronically excited E,F state of the H 2 molecule are studied and contrasted using the Velocity Mapping Imaging (VMI) technique. Photoelectron images from nonresonant 7-, 8- and 9-photon radiation ionization of H 2 show that the intense laser fields create ponderomotive shifts in the potential energy surfaces and distort the velocity of the emitted electrons that are produced from ionization. Photofragment images of H+ due to the dissociation mechanism that follows the 2-photon excitation into the (E,F; v = 0, J = 0, 1) electronic state showmore » a strong dependence on laser intensity, which is attributed to the high polarizability of the H 2 (E,F) state. For transitions from the J = 0 state, particularly, we observe marked structure in the angular distribution, which we explain as the interference between the prepared J = 0 and Stark-mixed J = 2 rovibrational states of H 2, as the laser intensity increases. Quantification of these effects allows us to extract the molecular polarizability of the H 2 (E,F) state, and yields a value of 103 ± 37 A.U.« less

Building Blocks of Dust and Large Organic Molecules: a Coordinated Laboratory and Astronomical Study of AGB Stars

NASA Astrophysics Data System (ADS)

McCarthy, Michael C.; Gottlieb, Carl A.; Cernicharo, Jose

2017-06-01

The increased sensitivity and angular resolution of high-altitude ground-based interferometers in the sub-millimeter band has enabled the physics and chemistry of carbon- and oxygen-rich evolved stars to be re-examined at an unprecedented level of detail. Observations of rotational lines in the inner envelope - the region within a few stellar radii of the central star where the molecular seeds of dust are formed - allows one to critically assess models of dust growth. Interferometric observations of the outer envelope provide stringent tests of neutral and ionized molecule formation. All of the astronomical studies are crucially dependent on precise laboratory measurements of the rotational spectra of new species and of vibrationally excited levels of known molecules and their rare isotopic species. By means of a closely coordinated laboratory and astronomical program, a number of exotic species including the disilicon carbide SiCSi, titanium oxides TiO and TiO_2, and carbon chain anions ranging from CN^- to C_8H^- have recently been observed in evolved stars. This talk will provide overview of these findings, and how they impact current models of the ``chemical laboratories'' of evolved stars. Ongoing laboratory studies of small silicon-bearing molecules such as H_2SiO_2 and vibrationally excited SiC_2 will be highlighted.

High precision optical spectroscopy and quantum state selected photodissociation of ultracold 88Sr2 molecules in an optical lattice

NASA Astrophysics Data System (ADS)

McDonald, Mickey Patrick

Over the past several decades, rapid progress has been made toward the accurate characterization and control of atoms, made possible largely by the development of narrow-linewidth lasers and techniques for trapping and cooling at ultracold temperatures. Extending this progress to molecules will have exciting implications for chemistry, condensed matter physics, and precision tests of physics beyond the Standard Model. These possibilities are all consequences of the richness of molecular structure, which is governed by physics substantially different from that characterizing atomic structure. This same richness of structure, however, increases the complexity of any molecular experiment manyfold over its atomic counterpart, magnifying the difficulty of everything from trapping and cooling to the comparison of theory with experiment. This thesis describes work performed over the past six years to establish the state of the art in manipulation and quantum control of ultracold molecules. Our molecules are produced via photoassociation of ultracold strontium atoms followed by spontaneous decay to a stable ground state. We describe a thorough set of measurements characterizing the rovibrational structure of very weakly bound (and therefore very large) 88Sr2 molecules from several different perspectives, including determinations of binding energies; linear, quadratic, and higher order Zeeman shifts; transition strengths between bound states; and lifetimes of narrow subradiant states. The physical intuition gained in these experiments applies generally to weakly bound diatomic molecules, and suggests extensive applications in precision measurement and metrology. In addition, we present a detailed analysis of the thermally broadened spectroscopic lineshape of molecules in a non-magic optical lattice trap, showing how such lineshapes can be used to directly determine the temperature of atoms or molecules in situ, addressing a long-standing problem in ultracold physics. Finally, we discuss the measurement of photofragment angular distributions produced by photodissociation, leading to an exploration of quantum-state-resolved ultracold chemistry.

Dependencia del tiempo de formación de los planetas gigantes con el tamaño de los planetesimales acretados.

NASA Astrophysics Data System (ADS)

Fortier, A.; Benvenuto, O. G.; Brunini, A.

In the framework of the core instability hypothesis and according to the Nice model for the primordial orbital architecture of the Solar System, we study the formation of the giant planets considering several different laws for the size distribution of the accreted planetesimals. Our results show that, if most of the mass lies in small planetesimals (radii 30 - 100 meters), the formation of Jupiter, Saturn, Uranus and Neptune can be explained by the core instability model, avoiding any conflict with the estimated lifetime of protoplanetary discs. FULL TEXT IN SPANISH

Laser studies of the photodissociation dynamics of cometary radicals

NASA Technical Reports Server (NTRS)

Jackson, William M.

1991-01-01

In the past year, it was shown that in the 193 nm photolysis of C2H, the C2 radical is produced in a variety of electronic, vibrational, and rotational states. The relative population of the vibrational and rotational states of C2(A 1 Pi u), C2(B 1 Sigma g +), and C2(A 3 Pi u) were determined in a static gas cell and in a pulsed molecular beam. It seems as though the original angular momentum of the C2H molecule appears as part of the angular momentum of the C2 radical. A attempt is being made to discover the mathematical relationship that governs this mapping. New information about the bond dissociation energy of the C2 radical was produces. C2(b 3 Sigma g -) and C2( 1 Delta g) were detected in the photolysis of C2H via time resolved infrared emission spectroscopy. In the former case, vibrational excitation up to v'' = 4 is observed. All of the results suggest that the C2 models in comets need to consider the presence of vibrationally excited C2 radicals in comets. The laser induced fluorescence spectra of the C3 was observed as a product of the 193 nm photolysis of allene and propyne. The populations of the rotational levels are identical in both cases. This result has led us to conclude that an isomerization reaction occurs in the photolysis of propyne which leads to the same C3H2 intermediate that is formed in the photolysis of C3H4. Since the former molecule is one of the most abundant in the interstellar medium it is also likely that its precursor is also present in comets. This would explain why C3 is observed in comets.

Surface-enhanced Raman scattering (SERS) by molecules adsorbed at spherical particles: errata

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

Kerker, M.; Wang, D.S.; Chew, H.

1980-12-15

A model for Raman scattering by a molecule adsorbed at the surface of a spherical particle is articulated by treating the molecule as a classical electric dipole. This follows Moskovits's suggestion (J. Chem. Phys. 69, 4159 (1978)) and the experiments by Creighton et al. (J. Chem. Soc. Faraday Trans. II, 75, 790(1979)) that such a system may exhibit SERS simlar to that at roughened electrode surfaces. The molecule is stimulated by a primary field comprised of the incident and near-scattered fields. Emission consists of the dipole field plus a scattered field, each at the shifted frequency. Addition of feedback termsmore » between the dipole and the particle makes only a negligible contribution to the fields. For pyridine adsorbed at the surface of a silver sphere, the 1010 cm/sup -1/ band is enhanced by approx.10/sup 6/ if the radius is much less than the wavelengths and the excitation wavelength is approx.382 nm, a wavelength for which the relative refractive index of silver is close to m = ..sqrt..2i. Detailed results are given for the effect upon the angular distribution and the polarization of the Raman emission of particle size, distance from the surface, excitation wavelength, and location of the molecule upon the surface. These results simulate those observed at roughened silver electrodes and suggest that the mechanism of SERS at those electrodes may resemble the electromagnetic mechanism elucidated here. The authors predict that comparable effects should be observed for fluorescent scattering. 53 references, 9 figures.« less

Quantitative Pointwise Estimate of the Solution of the Linearized Boltzmann Equation

NASA Astrophysics Data System (ADS)

Lin, Yu-Chu; Wang, Haitao; Wu, Kung-Chien

2018-04-01

We study the quantitative pointwise behavior of the solutions of the linearized Boltzmann equation for hard potentials, Maxwellian molecules and soft potentials, with Grad's angular cutoff assumption. More precisely, for solutions inside the finite Mach number region (time like region), we obtain the pointwise fluid structure for hard potentials and Maxwellian molecules, and optimal time decay in the fluid part and sub-exponential time decay in the non-fluid part for soft potentials. For solutions outside the finite Mach number region (space like region), we obtain sub-exponential decay in the space variable. The singular wave estimate, regularization estimate and refined weighted energy estimate play important roles in this paper. Our results extend the classical results of Liu and Yu (Commun Pure Appl Math 57:1543-1608, 2004), (Bull Inst Math Acad Sin 1:1-78, 2006), (Bull Inst Math Acad Sin 6:151-243, 2011) and Lee et al. (Commun Math Phys 269:17-37, 2007) to hard and soft potentials by imposing suitable exponential velocity weight on the initial condition.

Circular dichroism in photoelectron images from aligned nitric oxide molecules

DOE PAGES

Sen, Ananya; Pratt, S. T.; Reid, K. L.

2017-05-03

We have used velocity map photoelectron imaging to study circular dichroism of the photoelectron angular distributions (PADs) of nitric oxide following two-color resonanceenhanced two-photon ionization via selected rotational levels of the A 2Σ +, v' = 0 state. By using a circularly polarized pump beam and a counter-propagating, circularly polarized probe beam, cylindrical symmetry is preserved in the ionization process, and the images can be reconstructed using standard algorithms. The VMI set up enables individual ion rotational states to be resolved with excellent collection efficiency, rendering the measurements considerably simpler to perform than previous measurements conducted with a conventional photoelectronmore » spectrometer. The results demonstrate that circular dichroism is observed even when cylindrical symmetry is maintained, and serve as a reminder that dichroism is a general feature of the multiphoton ionization of atoms and molecules. Furthermore, the observed PADs are in good agreement with calculations based on parameters extracted from previous experimental results obtained by using a time-offlight electron spectrometer.« less

LETTER TO THE EDITOR: Differential electron scattering from the (010) excited vibrational mode of N2O

NASA Astrophysics Data System (ADS)

Akther, P.; Johnstone, W. M.; El-Zein, A. A. A.; Campbell, L.; Teubner, P. J. O.; Brunger, M. J.; Newell, W. R.

2002-11-01

In this letter we report differential superelastic, elastic and inelastic electron scattering measurements from nitrous oxide (N2O) in its (010)* excited vibrational quantum. The incident electron energy was 2.5 eV and the scattered electron angular range was 10°- 40°. Unlike our previous results (1999 J. Phys. B: At. Mol. Opt. Phys. 32 5779) with the isoelectronic molecule carbon dioxide (CO2), where the elastic differential cross sections (DCSs) for scattering from the (010)* mode were 2.3 times larger than those for elastic scattering from the ground (000) state, in N2O the corresponding (010)* elastic cross sections are usually only a fraction of those for the ground state. To the best of our knowledge, the present data are the first DCSs which have been reported in the literature for electron scattering from an excited vibrational level of the N2O molecule.

Rovibrational states of Wigner molecules in spherically symmetric confining potentials

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

Cioslowski, Jerzy

2016-08-07

The strong-localization limit of three-dimensional Wigner molecules, in which repulsively interacting particles are confined by a weak spherically symmetric potential, is investigated. An explicit prescription for computation of rovibrational wavefunctions and energies that are asymptotically exact at this limit is presented. The prescription is valid for systems with arbitrary angularly-independent interparticle and confining potentials, including those involving Coulombic and screened (i.e., Yukawa/Debye) interactions. The necessary derivations are greatly simplified by explicit constructions of the Eckart frame and the parity-adapted primitive wavefunctions. The performance of the new formalism is illustrated with the three- and four-electron harmonium atoms at their strong-correlation limits.more » In particular, the involvement of vibrational modes with the E symmetry is readily pinpointed as the origin of the “anomalous” weak-confinement behavior of the {sup 1}S{sub +} state of the four-electron species that is absent in its {sup 1}D{sub +} companion of the strong-confinement regime.« less

The HD molecule in small and medium cages of clathrate hydrates: Quantum dynamics studied by neutron scattering measurements and computation

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

Colognesi, Daniele; Celli, Milva; Ulivi, Lorenzo, E-mail: lorenzo.ulivi@isc.cnr.it

2014-10-07

We report inelastic neutron scattering (INS) measurements on molecular hydrogen deuteride (HD) trapped in binary cubic (sII) and hexagonal (sH) clathrate hydrates, performed at low temperature using two different neutron spectrometers in order to probe both energy and momentum transfer. The INS spectra of binary clathrate samples exhibit a rich structure containing sharp bands arising from both the rotational transitions and the rattling modes of the guest molecule. For the clathrates with sII structure, there is a very good agreement with the rigorous fully quantum simulations which account for the subtle effects of the anisotropy, angular and radial, of themore » host cage on the HD microscopic dynamics. The sH clathrate sample presents a much greater challenge, due to the uncertainties regarding the crystal structure, which is known only for similar crystals with different promoter, but nor for HD (or H{sub 2}) plus methyl tert-butyl ether (MTBE-d12)« less

Quantitative Pointwise Estimate of the Solution of the Linearized Boltzmann Equation

NASA Astrophysics Data System (ADS)

Lin, Yu-Chu; Wang, Haitao; Wu, Kung-Chien

2018-06-01

We study the quantitative pointwise behavior of the solutions of the linearized Boltzmann equation for hard potentials, Maxwellian molecules and soft potentials, with Grad's angular cutoff assumption. More precisely, for solutions inside the finite Mach number region (time like region), we obtain the pointwise fluid structure for hard potentials and Maxwellian molecules, and optimal time decay in the fluid part and sub-exponential time decay in the non-fluid part for soft potentials. For solutions outside the finite Mach number region (space like region), we obtain sub-exponential decay in the space variable. The singular wave estimate, regularization estimate and refined weighted energy estimate play important roles in this paper. Our results extend the classical results of Liu and Yu (Commun Pure Appl Math 57:1543-1608, 2004), (Bull Inst Math Acad Sin 1:1-78, 2006), (Bull Inst Math Acad Sin 6:151-243, 2011) and Lee et al. (Commun Math Phys 269:17-37, 2007) to hard and soft potentials by imposing suitable exponential velocity weight on the initial condition.

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

Role of electronic correlations in photoionization of NO2 in the vicinity of the 2A1/2B2 conical intersection.

PubMed

Brambila, Danilo S; Harvey, Alex G; Houfek, Karel; Mašín, Zdeněk; Smirnova, Olga

2017-08-02

We present the first ab initio multi-channel photoionization calculations for NO 2 in the vicinity of the 2 A 1 / 2 B 2 conical intersection, for a range of nuclear geometries, using our newly developed set of tools based on the ab initio multichannel R-matrix method. Electronic correlation is included in both the neutral and the scattering states of the molecule via configuration interaction. Configuration mixing is especially important around conical intersections and avoided crossings, both pertinent for NO 2 , and manifests itself via significant variations in photoelectron angular distributions. The method allows for a balanced and accurate description of the photoionization/photorecombination for a number of different ionic channels in a wide range of photoelectron energies up to 100 eV. Proper account of electron correlations is crucial for interpreting time-resolved signals in photoelectron spectroscopy and high harmonic generation (HHG) from polyatomic molecules.

Angle-resolved photoelectron spectroscopy of the chloro-substituted methanes

NASA Astrophysics Data System (ADS)

Keller, P. R.; Taylor, J. W.; Carlson, Thomas A.; Grimm, F. A.

1983-09-01

The angular distribution parameter, β, was determined for the valence orbitals (IP ' 21.2 eV) of CCl 4, CHCl 3, CH 2Cl 2, and CH 3Cl in the 10-30 eV photon energy range using dispersed polarized synchrotron radiation. The energy dependence of β in the photoelectron energy range of 2 to 10 eV for the non-bonding chlorine n(Cl) orbitals of these molecules was found to be similar for all n(Cl) orbitals investigated. The energy dependence of β for the σ orbitals in these molecules was similar to that observed previously for other σ orbitals. The experimental CCl 4 results were compared with theoretical CCl 4 results obtained using the Xα multiple scattering formalism. Theory predicts the existence of two strong shape resonances in each of the valence orbitals of CCl 4. The overall agreement between experiment and theory is evaluated along with the experimental evidence concerning the verification of the predicted shape resonances.

Multi-layer Lanczos iteration approach to calculations of vibrational energies and dipole transition intensities for polyatomic molecules

DOE PAGES

Yu, Hua-Gen

2015-01-28

We report a rigorous full dimensional quantum dynamics algorithm, the multi-layer Lanczos method, for computing vibrational energies and dipole transition intensities of polyatomic molecules without any dynamics approximation. The multi-layer Lanczos method is developed by using a few advanced techniques including the guided spectral transform Lanczos method, multi-layer Lanczos iteration approach, recursive residue generation method, and dipole-wavefunction contraction. The quantum molecular Hamiltonian at the total angular momentum J = 0 is represented in a set of orthogonal polyspherical coordinates so that the large amplitude motions of vibrations are naturally described. In particular, the algorithm is general and problem-independent. An applicationmore » is illustrated by calculating the infrared vibrational dipole transition spectrum of CH₄ based on the ab initio T8 potential energy surface of Schwenke and Partridge and the low-order truncated ab initio dipole moment surfaces of Yurchenko and co-workers. A comparison with experiments is made. The algorithm is also applicable for Raman polarizability active spectra.« less

Spin-based diagnostic of nanostructure in copper phthalocyanine-C60 solar cell blends.

PubMed

Warner, Marc; Mauthoor, Soumaya; Felton, Solveig; Wu, Wei; Gardener, Jules A; Din, Salahud; Klose, Daniel; Morley, Gavin W; Stoneham, A Marshall; Fisher, Andrew J; Aeppli, Gabriel; Kay, Christopher W M; Heutz, Sandrine

2012-12-21

Nanostructure and molecular orientation play a crucial role in determining the functionality of organic thin films. In practical devices, such as organic solar cells consisting of donor-acceptor mixtures, crystallinity is poor and these qualities cannot be readily determined by conventional diffraction techniques, while common microscopy only reveals surface morphology. Using a simple nondestructive technique, namely, continuous-wave electron paramagnetic resonance spectroscopy, which exploits the well-understood angular dependence of the g-factor and hyperfine tensors, we show that in the solar cell blend of C(60) and copper phthalocyanine (CuPc)-for which X-ray diffraction gives no information-the CuPc, and by implication the C(60), molecules form nanoclusters, with the planes of the CuPc molecules oriented perpendicular to the film surface. This information demonstrates that the current nanostructure in CuPc:C(60) solar cells is far from optimal and suggests that their efficiency could be considerably increased by alternative film growth algorithms.

Circular dichroism in photoelectron images from aligned nitric oxide molecules

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

Sen, Ananya; Pratt, S. T.; Reid, K. L.

We have used velocity map photoelectron imaging to study circular dichroism of the photoelectron angular distributions (PADs) of nitric oxide following two-color resonanceenhanced two-photon ionization via selected rotational levels of the A 2Σ +, v' = 0 state. By using a circularly polarized pump beam and a counter-propagating, circularly polarized probe beam, cylindrical symmetry is preserved in the ionization process, and the images can be reconstructed using standard algorithms. The VMI set up enables individual ion rotational states to be resolved with excellent collection efficiency, rendering the measurements considerably simpler to perform than previous measurements conducted with a conventional photoelectronmore » spectrometer. The results demonstrate that circular dichroism is observed even when cylindrical symmetry is maintained, and serve as a reminder that dichroism is a general feature of the multiphoton ionization of atoms and molecules. Furthermore, the observed PADs are in good agreement with calculations based on parameters extracted from previous experimental results obtained by using a time-offlight electron spectrometer.« less

Resonance energy transfer: The unified theory via vector spherical harmonics

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

Grinter, Roger, E-mail: r.grinter@uea.ac.uk; Jones, Garth A., E-mail: garth.jones@uea.ac.uk

2016-08-21

In this work, we derive the well-established expression for the quantum amplitude associated with the resonance energy transfer (RET) process between a pair of molecules that are beyond wavefunction overlap. The novelty of this work is that the field of the mediating photon is described in terms of a spherical wave rather than a plane wave. The angular components of the field are constructed in terms of vector spherical harmonics while Hankel functions are used to define the radial component. This approach alleviates the problem of having to select physically correct solution from non-physical solutions, which seems to be inherentmore » in plane wave derivations. The spherical coordinate system allows one to easily decompose the photon’s fields into longitudinal and transverse components and offers a natural way to analyse near-, intermediate-, and far-zone RET within the context of the relative orientation of the transition dipole moments for the two molecules.« less

Communication: Understanding molecular representations in machine learning: The role of uniqueness and target similarity

NASA Astrophysics Data System (ADS)

Huang, Bing; von Lilienfeld, O. Anatole

2016-10-01

The predictive accuracy of Machine Learning (ML) models of molecular properties depends on the choice of the molecular representation. Inspired by the postulates of quantum mechanics, we introduce a hierarchy of representations which meet uniqueness and target similarity criteria. To systematically control target similarity, we simply rely on interatomic many body expansions, as implemented in universal force-fields, including Bonding, Angular (BA), and higher order terms. Addition of higher order contributions systematically increases similarity to the true potential energy and predictive accuracy of the resulting ML models. We report numerical evidence for the performance of BAML models trained on molecular properties pre-calculated at electron-correlated and density functional theory level of theory for thousands of small organic molecules. Properties studied include enthalpies and free energies of atomization, heat capacity, zero-point vibrational energies, dipole-moment, polarizability, HOMO/LUMO energies and gap, ionization potential, electron affinity, and electronic excitations. After training, BAML predicts energies or electronic properties of out-of-sample molecules with unprecedented accuracy and speed.

Rotational spectroscopy with an optical centrifuge.

PubMed

Korobenko, Aleksey; Milner, Alexander A; Hepburn, John W; Milner, Valery

2014-03-07

We demonstrate a new spectroscopic method for studying electronic transitions in molecules with extremely broad range of angular momentum. We employ an optical centrifuge to create narrow rotational wave packets in the ground electronic state of (16)O2. Using the technique of resonance-enhanced multi-photon ionization, we record the spectrum of multiple ro-vibrational transitions between X(3)Σg(-) and C(3)Πg electronic manifolds of oxygen. Direct control of rotational excitation, extending to rotational quantum numbers as high as N ≳ 120, enables us to interpret the complex structure of rotational spectra of C(3)Πg beyond thermally accessible levels.

Charge exchange in cometary coma: Discovery of H− ions in the solar wind close to comet 67P/Churyumov‐Gerasimenko

PubMed Central

Cravens, T. E.; Llera, K.; Goldstein, R.; Mokashi, P.; Tzou, C.‐Y.; Broiles, T.

2015-01-01

Abstract As Rosetta was orbiting comet 67P/Churyumov‐Gerasimenko, the Ion and Electron Sensor detected negative particles with angular distributions like those of the concurrently measured solar wind protons but with fluxes of only about 10% of the proton fluxes and energies of about 90% of the proton energies. Using well‐known cross sections and energy‐loss data, it is determined that the fluxes and energies of the negative particles are consistent with the production of H− ions in the solar wind by double charge exchange with molecules in the coma. PMID:27656008

Experimental Demonstration of Coherent Control in Quantum Chaotic Systems

NASA Astrophysics Data System (ADS)

Bitter, M.; Milner, V.

2017-01-01

We experimentally demonstrate coherent control of a quantum system, whose dynamics is chaotic in the classical limit. Interaction of diatomic molecules with a periodic sequence of ultrashort laser pulses leads to the dynamical localization of the molecular angular momentum, a characteristic feature of the chaotic quantum kicked rotor. By changing the phases of the rotational states in the initially prepared coherent wave packet, we control the rotational distribution of the final localized state and its total energy. We demonstrate the anticipated sensitivity of control to the exact parameters of the kicking field, as well as its disappearance in the classical regime of excitation.

Comparison of short-range-order in liquid- and rotator-phase states of a simple molecular liquid: A reverse Monte Carlo and molecular dynamics analysis of neutron diffraction data

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

Pardo, Luis Carlos; Tamarit, Josep Lluis; Veglio, Nestor

2007-10-01

The short-range order (SRO) correlations in liquid- and rotator-phase states of carbon tetrachloride are revisited here. The correlation of some angular magnitudes is used to evaluate the positional and orientational correlations in the liquid as well as in the rotator phase. The results show significant similitudes in the relative position of the molecules surrounding a central one but striking differences in their relative orientations, which could explain the changes in SRO between the two phases and the puzzling behavior of the local density in the liquid and rotator phases.

Non-Equilibrium Chemistry of O-Rich AGB Stars as Revealed by ALMA

NASA Astrophysics Data System (ADS)

Wong, Ka Tat

2018-04-01

Chemical models suggest that pulsation driven shocks propagating from the stellar surfaces of oxygen-rich evolved stars to the dust formation zone trigger non-equilibrium chemistry in the shocked gas near the star, including the formation of carbon-bearing molecules in the stellar winds dominated by oxygen-rich chemistry. Recent long-baseline ALMA observations are able to give us a detailed view of the molecular line emission and absorption at an angular resolution of a few stellar radii. I am going to present the latest results from the ALMA observations of IK Tau and o Cet in late 2017, with a particular focus on HCN.

Electronuclear paths in the nuclear conversion of molecular hydrogen in silicon

NASA Astrophysics Data System (ADS)

Ilisca, Ernest; Ghiglieno, Filippo

2017-01-01

The ortho-para conversion of hydrogen molecules oscillating inside tetrahedral cages of silicon compounds relies on the interaction of the nuclear protons with the silicon electrons. At each collision against the cage hard walls, the electron repulsion changes the molecular rotation while projecting a valence electron in the antibonding molecular state dressed by a group of conduction ones. That «bridge» facilitates the hyperfine contact of the electrons with the protons. At room temperature, the angular momentum transfer is enhanced by electron fluctuations that overcome the silicon gap and accelerate the nuclear rates by more than one order of magnitude.

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.

Manipulating the motion of large molecules: Information from the molecular frame

NASA Astrophysics Data System (ADS)

Küpper, Jochen

2011-05-01

Large molecules have complex potential-energy surfaces with many local minima. They exhibit multiple stereoisomers, even at the low temperatures (~1 K) in a molecular beam, with rich intra- and intermolecular dynamics. Over the last years, we have developed methods to manipulate the motion of large, complex molecules and to select their quantum states. We have exploited this state-selectivity, for example, to spatially separate individual structural isomers of complex molecules and to demonstrate unprecedented degrees of laser alignment and mixed-field orientation of these molecules. Such clean, well-defined samples strongly benefit, or simply allow, novel experiments on the dynamics of complex molecules, for instance, femtosecond pump-probe measurements, X-ray or electron diffraction of molecular ensembles (including diffraction-from-within experiments), or tomographic reconstructions of molecular orbitals. These samples could also be very advantageous for metrology applications, such as, for example, matter-wave interferometry or the search for electroweak interactions in chiral molecules. Moreover, they provide an extreme level of control for stereo-dynamically controlled reaction dynamics. We have recently exploited these state-selected and oriented samples to measure photoelectron angular distributions in the molecular frame (MFPADs) from non-resonant femtosecond-laser photoionization and using the X-ray Free-Electron-Laser LCLS. We have also investigated X-ray diffraction imaging and, using ion momentum imaging, the induced radiation damage of these samples using the LCLS. This work was carried out within a collaboration for which J. Küpper, H. Chapman, and D. Rolles are spokespersons. The collaboration consists of CFEL (DESY, MPG, University Hamburg), Fritz-Haber-Institute Berlin, MPI Nuclear Physics Heidelberg, MPG Semi-conductor Lab, Aarhus University, FOM AMOLF Amsterdam, Lund University, MPI Medical Research Heidelberg, TU Berlin, Max Born Institute Berlin, and SLAC Menlo Park, CA, USA. The experiments were carried out using CAMP (designed and built by the MPG-ASG at CFEL) at the LCLS (operated by Stanford University on behalf of the US DOE).

An Angular Overlap Model for Cu(II) Ion in the AMOEBA Polarizable Force Field

PubMed Central

Xiang, Jin Yu; Ponder, Jay W.

2014-01-01

An extensible polarizable force field for transition metal ion was developed based on AMOEBA and the angular overlap model (AOM) with consistent treatment of electrostatics for all atoms. Parameters were obtained by fitting molecular mechanics (MM) energies to various ab initio gas-phase calculations. The results of parameterization were presented for copper (II) ion ligated to water and model fragments of amino acid residues involved in the copper binding sites of type 1 copper proteins. Molecular dynamics (MD) simulations were performed on aqueous copper (II) ion at various temperatures, as well as plastocyanin (1AG6) and azurin (1DYZ). Results demonstrated that the AMOEBA-AOM significantly improves the accuracy of classical MM in a number of test cases when compared to ab initio calculations. The Jahn-Teller distortion for hexa-aqua copper (II) complex was handled automatically without specifically designating axial and in-plane ligands. Analyses of MD trajectories resulted in a 6-coordination first solvation shell for aqueous copper (II) ion and a 1.8ns average residence time of water molecules. The ensemble average geometries of 1AG6 and 1DYZ copper binding sites were in general agreement with X-ray and previous computational studies. PMID:25045338

Theoretical model of chirality-induced helical self-propulsion

NASA Astrophysics Data System (ADS)

Yamamoto, Takaki; Sano, Masaki

2018-01-01

We recently reported the experimental realization of a chiral artificial microswimmer exhibiting helical self-propulsion [T. Yamamoto and M. Sano, Soft Matter 13, 3328 (2017), 10.1039/C7SM00337D]. In the experiment, cholesteric liquid crystal (CLC) droplets dispersed in surfactant solutions swam spontaneously, driven by the Marangoni flow, in helical paths whose handedness is determined by the chirality of the component molecules of CLC. To study the mechanism of the emergence of the helical self-propelled motion, we propose a phenomenological model of the self-propelled helical motion of the CLC droplets. Our model is constructed by symmetry argument in chiral systems, and it describes the dynamics of CLC droplets with coupled time-evolution equations in terms of a velocity, an angular velocity, and a tensor variable representing the symmetry of the helical director field of the droplet. We found that helical motions as well as other chiral motions appear in our model. By investigating bifurcation behaviors between each chiral motion, we found that the chiral coupling terms between the velocity and the angular velocity, the structural anisotropy of the CLC droplet, and the nonlinearity of model equations play a crucial role in the emergence of the helical motion of the CLC droplet.

Metabolic Response of Strawberry (Fragaria x ananassa) Leaves Exposed to the Angular Leaf Spot Bacterium (Xanthomonas fragariae).

PubMed

Kim, Min-Sun; Jin, Jong Sung; Kwak, Youn-Sig; Hwang, Geum-Sook

2016-03-09

Plants have evolved various defense mechanisms against biotic stress. The most common mechanism involves the production of metabolites that act as defense compounds. Bacterial angular leaf spot disease (Xanthomonas fragariae) of the strawberry (Fragaria x ananassa) has become increasingly destructive to strawberry leaves and plant production. In this study, we examined metabolic changes associated with the establishment of long-term bacterial disease stress using UPLC-QTOF mass spectrometry. Infected leaves showed decreased levels of gallic acid derivatives and ellagitannins, which are related to the plant defense system. The levels of phenylalanine, tryptophan, and salicylic acid as precursors of aromatic secondary metabolites were increased in inoculated leaves, whereas levels of coumaric acid, quinic acid, and flavonoids were decreased in infected plants, which are involved in the phenylpropanoid pathway. In addition, phenylalanine ammonia-lyase (PAL) activity, a key enzyme in the phenylpropanoid pathway, was decreased following infection. These results suggest that long-term bacterial disease stress may lead to down-regulation of select molecules of the phenylpropanoid metabolic pathway in strawberry leaves. This approach could be applied to explore the metabolic pathway associated with plant protection/breeding in strawberry leaves.

Photoionization of water molecules by a train of attosecond pulses assisted by a near-infrared laser: delay and polarization control

NASA Astrophysics Data System (ADS)

Martini, Lara; Boll, Diego I. R.; Fojón, Omar A.

2017-08-01

Basic reactions involving water molecules are essential to understand the interaction between radiation and the biological tissue because living cells are composed mostly by water. Therefore, the knowledge of ionization of the latter is crucial in many domains of Biology and Physics. So, we study theoretically the photoionization of water molecules by extreme ultraviolet attopulse trains assisted by lasers in the near-infrared range. We use a separable Coulomb-Volkov model in which the temporal evolution of the system can be divided into three stages allowing spatial and temporal separation for the Coulomb and Volkov final state wavefunctions. First, we analyze photoelectron angular distributions for different delays between the attopulse train and the assistant laser field. We compare our results for water and Ne atoms as they belong to the same isoelectronic series. Moreover, we contrast our calculations with previous theoretical and experimental work for Ar atoms due to the similarities of the orbitals involved in the reaction. Second, we study the effect of varying the relative orientations of the attopulse and laser field polarizations and we compare our predictions with other theories and experiments. We expect these studies contribute to the improvement of polarization experiments and the development of the attopulse trains and assistant laser fields technologies. Finally, we hope our work promote progress on the control of the chemical reactivity of water molecules since this could be useful in different fields such as radiobiology and medical physics.

Stop-Frame Filming and Discovery of Reactions at the Single-Molecule Level by Transmission Electron Microscopy

PubMed Central

2017-01-01

We report an approach, named chemTEM, to follow chemical transformations at the single-molecule level with the electron beam of a transmission electron microscope (TEM) applied as both a tunable source of energy and a sub-angstrom imaging probe. Deposited on graphene, disk-shaped perchlorocoronene molecules are precluded from intermolecular interactions. This allows monomolecular transformations to be studied at the single-molecule level in real time and reveals chlorine elimination and reactive aryne formation as a key initial stage of multistep reactions initiated by the 80 keV e-beam. Under the same conditions, perchlorocoronene confined within a nanotube cavity, where the molecules are situated in very close proximity to each other, enables imaging of intermolecular reactions, starting with the Diels–Alder cycloaddition of a generated aryne, followed by rearrangement of the angular adduct to a planar polyaromatic structure and the formation of a perchlorinated zigzag nanoribbon of graphene as the final product. ChemTEM enables the entire process of polycondensation, including the formation of metastable intermediates, to be captured in a one-shot “movie”. A molecule with a similar size and shape but with a different chemical composition, octathio[8]circulene, under the same conditions undergoes another type of polycondensation via thiyl biradical generation and subsequent reaction leading to polythiophene nanoribbons with irregular edges incorporating bridging sulfur atoms. Graphene or carbon nanotubes supporting the individual molecules during chemTEM studies ensure that the elastic interactions of the molecules with the e-beam are the dominant forces that initiate and drive the reactions we image. Our ab initio DFT calculations explicitly incorporating the e-beam in the theoretical model correlate with the chemTEM observations and give a mechanism for direct control not only of the type of the reaction but also of the reaction rate. Selection of the appropriate e-beam energy and control of the dose rate in chemTEM enabled imaging of reactions on a time frame commensurate with TEM image capture rates, revealing atomistic mechanisms of previously unknown processes. PMID:28191929

Magnetically confined electron beam system for high resolution electron transmission-beam experiments

NASA Astrophysics Data System (ADS)

Lozano, A. I.; Oller, J. C.; Krupa, K.; Ferreira da Silva, F.; Limão-Vieira, P.; Blanco, F.; Muñoz, A.; Colmenares, R.; García, G.

2018-06-01

A novel experimental setup has been implemented to provide accurate electron scattering cross sections from molecules at low and intermediate impact energies (1-300 eV) by measuring the attenuation of a magnetically confined linear electron beam from a molecular target. High-resolution electron energy is achieved through confinement in a magnetic gas trap where electrons are cooled by successive collisions with N2. Additionally, we developed and present a method to correct systematic errors arising from energy and angular resolution limitations. The accuracy of the entire measurement procedure is validated by comparing the N2 total scattering cross section in the considered energy range with benchmark values available in the literature.

Monte Carlo and analytical calculations for characterization of gas bremsstrahlung in ILSF insertion devices

NASA Astrophysics Data System (ADS)

Salimi, E.; Rahighi, J.; Sardari, D.; Mahdavi, S. R.; Lamehi Rachti, M.

2014-12-01

Gas bremsstrahlung is generated in high energy electron storage rings through interaction of the electron beam with the residual gas molecules in vacuum chamber. In this paper, Monte Carlo calculation has been performed to evaluate radiation hazard due to gas bremsstrahlung in the Iranian Light Source Facility (ILSF) insertion devices. Shutter/stopper dimensions is determined and dose rate from the photoneutrons via the giant resonance photonuclear reaction which takes place inside the shutter/stopper is also obtained. Some other characteristics of gas bremsstrahlung such as photon fluence, energy spectrum, angular distribution and equivalent dose in tissue equivalent phantom have also been investigated by FLUKA Monte Carlo code.

The Rotational Excitation Temperature of the 6614 DIB Carrier

NASA Technical Reports Server (NTRS)

Cami, J.; Salama, F.; Jimenez-Vicente, J.; Galazutdinov, G.; Krelowski, J.

2004-01-01

Analysis of high spectral resolution observations of the lambda6614 DIB line profile show systematic variations in the positions of the peaks in the substructure of the profile. These variations can only be understood in the framework of rotational contours of large molecules, where the variations are caused by changes in the rotational excitation temperature. We show that the rotational excitation temperature for the DIB carrier is of the order 10-40 K - much lower than the gas kinetic temperature - indicating that for this particular DIB carrier angular momentum buildup is not very efficient. The rotational constant indicates that the carrier of this DIB is smaller than previously assumed:7-22 C atoms, depending on the geometry.

Angle-resolved photoelectron spectroscopy of formaldehyde and methanol

NASA Astrophysics Data System (ADS)

Keller, P. R.; Taylor, J. W.; Grimm, F. A.; Carlson, Thomas A.

1984-10-01

Angle-resolved photoelectron spectroscopy was employed to obtain the angular distribution parameter, β, for the valence orbitals (IP < 21.1 eV) of formaldehyde and methanol over the 10-30 eV photon energy range using dispersed polarized synchrotron radiation as the excitation source. It was found that the energy dependence of β in the photoelectron energy range between 2 and 10 eV can be related to the molecular-orbital type from which ionization occurs. This generalized energy behavior is discussed with regard to earlier energy-dependence studies on molecules of different orbital character. Evidence is presented for the presence of resonance photoionization phenomena in formaldehyde in agreement with theoretical cross-section calculations.

Wigner molecules: natural orbitals of strongly correlated two-electron harmonium.

PubMed

Cioslowski, Jerzy; Buchowiecki, Marcin

2006-08-14

Explicit asymptotic expressions for natural orbitals and their occupancies are derived for the harmonium atom at the strong-correlation limit at which the confinement strength omega tends to zero. Unlike in systems with moderate correlation effects, the occupancies at the omega-->0 limit (derived from occupation amplitudes with alternating sign patterns) are vanishingly small and asymptotically independent of the angular momentum, forming a geometric progression with the scale factor proportional to omega(1/3) and the common ratio of ca. 0.0186. The radial components of the natural orbitals are given by products of polynomials and Gaussian functions that, as expected, peak at approximately half of the equilibrium interelectron distance.

Kinetic theory analysis of rarefied gas flow through finite length slots

NASA Technical Reports Server (NTRS)

Raghuraman, P.

1972-01-01

An analytic study is made of the flow a rarefied monatomic gas through a two dimensional slot. The parameters of the problem are the ratios of downstream to upstream pressures, the Knudsen number at the high pressure end (based on slot half width) and the length to slot half width ratio. A moment method of solution is used by assuming a discontinuous distribution function consisting of four Maxwellians split equally in angular space. Numerical solutions are obtained for the resulting equations. The characteristics of the transition regime are portrayed. The solutions in the free molecule limit are systematically lower than the results obtained in that limit by more accurate numerical methods.

Electron scattering by highly polar molecules. III - CsCl

NASA Technical Reports Server (NTRS)

Vuskovic, L.; Srivastava, S. K.

1981-01-01

Utilizing a crossed electron-beam-molecular-beam scattering geometry, relative values of differential electron scattering cross sections for cesium chloride at 5 and 20 eV electron impact energies and at scattering angles between 10 and 120 deg have been measured. These relative cross sections have been normalized to the cross section at 15 deg scattering angle calculated by the hybrid S-matrix technique. In the angular range between 0 and 10 deg and between 120 and 180 deg extrapolations have been made to obtain integral and momentum transfer cross sections. An energy-loss spectrum is also presented which gives various spectral features lying between the 4 and 10 eV regions in CsCl.

Underwound DNA under Tension: Structure, Elasticity, and Sequence-Dependent Behaviors

NASA Astrophysics Data System (ADS)

Sheinin, Maxim Y.; Forth, Scott; Marko, John F.; Wang, Michelle D.

2011-09-01

DNA melting under torsion plays an important role in a wide variety of cellular processes. In the present Letter, we have investigated DNA melting at the single-molecule level using an angular optical trap. By directly measuring force, extension, torque, and angle of DNA, we determined the structural and elastic parameters of torsionally melted DNA. Our data reveal that under moderate forces, the melted DNA assumes a left-handed structure as opposed to an open bubble conformation and is highly torsionally compliant. We have also discovered that at low forces melted DNA properties are highly dependent on DNA sequence. These results provide a more comprehensive picture of the global DNA force-torque phase diagram.

Valence and inner-valence shell dissociative photoionization of CO in the 26-33 eV range. II. Molecular-frame and recoil-frame photoelectron angular distributions.

PubMed

Lebech, M; Houver, J C; Raseev, G; dos Santos, A S; Dowek, D; Lucchese, Robert R

2012-03-07

Experimental and theoretical results for molecular-frame photoemission are presented for inner-valence shell photoionization of the CO molecule induced by linearly and circularly polarized light. The experimental recoil frame photoelectron angular distributions (RFPADs) obtained from dissociative photoionization measurements where the velocities of the ionic fragment and photoelectron were detected in coincidence, are compared to RFPADs computed using the multichannel Schwinger configuration interaction method. The formalism for including a finite lifetime of the predissociative ion state is presented for the case of general elliptically polarized light, to obtain the RFPAD rather than the molecular frame photoelectron angular distribution (MFPAD), which would be obtained with the assumption of instantaneous dissociation. We have considered photoionization of CO for the photon energies of 26.0 eV, 29.5 eV, and 32.5 eV. A comparison of experimental and theoretical RFPADs allows us to identify the ionic states detected in the experimental studies. In addition to previously identified states, we found evidence for the 2 (2)Δ state with an ionization potential of 25.3 eV and (2)Σ(+) states with ionization potentials near 32.5 eV. A comparison of the experimental and theoretical RFPADs permits us to estimate predissociative lifetimes of 0.25-1 ps for some of the ion states. Consideration of the MFPADs of a series of (2)Π ion states indicates the importance of inter-channel coupling at low photoelectron kinetic energy and the limitations of a single-channel analysis based on the corresponding Dyson orbitals. © 2012 American Institute of Physics

Stiffness of γ subunit of F(1)-ATPase.

PubMed

Okuno, Daichi; Iino, Ryota; Noji, Hiroyuki

2010-11-01

F(1)-ATPase is a molecular motor in which the γ subunit rotates inside the α(3)β(3) ring upon adenosine triphosphate (ATP) hydrolysis. Recent works on single-molecule manipulation of F(1)-ATPase have shown that kinetic parameters such as the on-rate of ATP and the off-rate of adenosine diphosphate (ADP) strongly depend on the rotary angle of the γ subunit (Hirono-Hara et al. 2005; Iko et al. 2009). These findings provide important insight into how individual reaction steps release energy to power F(1) and also have implications regarding ATP synthesis and how reaction steps are reversed upon reverse rotation. An important issue regarding the angular dependence of kinetic parameters is that the angular position of a magnetic bead rotation probe could be larger than the actual position of the γ subunit due to the torsional elasticity of the system. In the present study, we assessed the stiffness of two different portions of F(1) from thermophilic Bacillus PS3: the internal part of the γ subunit embedded in the α(3)β(3) ring, and the complex of the external part of the γ subunit and the α(3)β(3) ring (and streptavidin and magnetic bead), by comparing rotational fluctuations before and after crosslinkage between the rotor and stator. The torsional stiffnesses of the internal and remaining parts were determined to be around 223 and 73 pNnm/radian, respectively. Based on these values, it was estimated that the actual angular position of the internal part of the γ subunit is one-fourth of the magnetic bead position upon stalling using an external magnetic field. The estimated elasticity also partially explains the accommodation of the intrinsic step size mismatch between F(o) and F(1)-ATPase.

Ionization and dissociation of molecular ion beams by intense ultrafast laser pulses

NASA Astrophysics Data System (ADS)

Ben-Itzhak, Itzik

2007-06-01

Laser-induced dissociation and ionization of a diatomic molecular-ion beam were simultaneously measured using coincidence 3D momentum imaging, with direct separation of the two processes even where the fragment kinetic energy is the same for both processes. We mainly focus on the fundamental H2^+ molecule in 7-135 fs laser pulses having 10^13-10^15 W/cm^2 peak intensity. At high intensities the kinetic energy release (KER) distribution following ionization of H2^+ was measured to be broad and structureless. Its centroid shifts toward higher energies as the laser intensity is increased indicating that ionization shifts to smaller internuclear distances. In contrast, a surprising structure is observed near the ionization threshold, which we call above threshold Coulomb explosion (ATCE) [1]. The angular distributions of the two H^+ fragments are strongly peaked along the laser polarization, and the angular distribution is described well by [cos^2θ]^n, where n is the number of photons predicted by our ATCE model [1]. Our data indicates that n varies with the laser wavelength as predicted by the model. The KER and angular distributions of H2^+ dissociation change dramatically with decreasing pulse width over the 7-135 fs range in contrast to the reported trend for longer pulses. Others contributing to this work: A.M. Sayler, P.Q. Wang, J. McKenna, B. Gaire, Nora G. Johnson, E. Parke, K.D. Carnes, and B.D. Esry. Thank are due to Professor Zenghu Chang for providing the intense laser beams and Dr. Charles Fehrenbach for his help with the ion beams. [1] B.D. Esry, A.M. Sayler, P.Q. Wang, K.D. Carnes, and I. Ben-Itzhak, Phys. Rev. Lett. 97, 013003 (2006).

Drag coefficient Variability and Thermospheric models

NASA Astrophysics Data System (ADS)

Moe, Kenneth

Satellite drag coefficients depend upon a variety of factors: The shape of the satellite, its altitude, the eccentricity of its orbit, the temperature and mean molecular mass of the ambient atmosphere, and the time in the sunspot cycle. At altitudes where the mean free path of the atmospheric molecules is large compared to the dimensions of the satellite, the drag coefficients can be determined from the theory of free-molecule flow. The dependence on altitude is caused by the concentration of atomic oxygen which plays an important role by its ability to adsorb on the satellite surface and thereby affect the energy loss of molecules striking the surface. The eccentricity of the orbit determines the satellite velocity at perigee, and therefore the energy of the incident molecules relative to the energy of adsorption of atomic oxygen atoms on the surface. The temperature of the ambient atmosphere determines the extent to which the random thermal motion of the molecules influences the momentum transfer to the satellite. The time in the sunspot cycle affects the ambient temperature as well as the concentration of atomic oxygen at a particular altitude. Tables and graphs will be used to illustrate the variability of drag coefficients. Before there were any measurements of gas-surface interactions in orbit, Izakov and Cook independently made an excellent estimate that the drag coefficient of satellites of compact shape would be 2.2. That numerical value, independent of altitude, was used by Jacchia to construct his model from the early measurements of satellite drag. Consequently, there is an altitude dependent bias in the model. From the sparce orbital experiments that have been done, we know that the molecules which strike satellite surfaces rebound in a diffuse angular distribution with an energy loss given by the energy accommodation coefficient. As more evidence accumulates on the energy loss, more realistic drag coefficients are being calculated. These improved drag coefficients help evaluate the biases in present models. Moreover, they make possible the derivation of accurate densities from accelerometer measurements.

Exchange interaction and tunneling-induced transparency in coupled quantum dots

NASA Astrophysics Data System (ADS)

Borges, H. S.; Alcalde, A. M.; Ulloa, Sergio E.

2014-11-01

We investigate the optical response of quantum dot molecules coherently driven by polarized laser light. Our description includes the splitting in excitonic levels caused by isotropic and anisotropic exchange interactions. We consider interdot transitions mediated by hole tunneling between states with the same total angular momentum and between bright and dark exciton states as allowed by spin-flip hopping between the dots in the molecule. Using realistic experimental parameters we demonstrate that the excitonic states coupled by tunneling exhibit a rich and controllable optical response. We show that through the appropriate control of an external electric field and light polarization, the tunneling coupling establishes an efficient destructive quantum interference path that creates a transparency window in the absorption spectra whenever states of appropriate symmetry are mixed by the carrier tunneling. We explore the relevant parameter space that allows probing this phenomenon in experiments. Controlled variation in applied field and laser detuning would allow the optical characterization of spin-preserving and spin-flip hopping amplitudes in such systems by measuring the width of the tunneling-induced transparency windows.

Spectroscopic FITS to the Alma Science Verification Band 6 Survey of the Orion Hot Core and Compact Ridge

NASA Astrophysics Data System (ADS)

Nagarajan, Satyakumar; McMillan, James P.; Burkhardt, Andrew M.; Neese, Christopher F.; De Lucia, Frank C.; Remijan, Anthony

2016-06-01

Individual spectral lines in astrophysical data are ordinarily assigned by comparison with line frequency and intensities predicted by catalogs. Here we seek to fit the spectra of specific sources within Orion KL that are first selected by ALMA's angular resolution and then by Doppler velocity class. For each molecule in this study, astrophysical reference lines are selected. Subsequent analyses of individual velocity components provide the astrophysical column density and temperature for these velocity regimes. These column densities and temperatures are then combined with results from the complete experimental spectra obtained from our laboratory spectra to model the molecule's contribution to the entire astrophysical spectrum [1]. Effects due to optical thickness and spectral overlap are included in the analyses. Examples for ethyl cyanide in the hot core and methanol in the compact ridge will be presented. [1] J. P. McMillan, S. M. Fortman, C. F. Neese, and F. C. De Lucia, "The Complete, Temperature Resolved Experi- mental Spectrum of Methanol (CH3OH) between 214.6 and 265.4 GHz," Astrophys. J., vol. 795, pp. 56(1-9), 2014.

Influence of light-induced conical intersection on the photodissociation dynamics of D2(+) starting from individual vibrational levels.

PubMed

Halász, Gábor J; Csehi, András; Vibók, Ágnes; Cederbaum, Lorenz S

2014-12-26

Previous works have shown that dressing of diatomic molecules by standing or by running laser waves gives rise to the appearance of so-called light-induced conical intersections (LICIs). Because of the strong nonadiabatic couplings, the existence of such LICIs may significantly change the dynamical properties of a molecular system. In our former paper (J. Phys. Chem. A 2013, 117, 8528), the photodissociation dynamics of the D(2)(+) molecule were studied in the LICI framework starting the initial vibrational nuclear wave packet from the superposition of all the vibrational states initially produced by ionizing D(2). The present work complements our previous investigation by letting the initial nuclear wave packets start from different individual vibrational levels of D(2)(+), in particular, above the energy of the LICI. The kinetic energy release spectra, the total dissociation probabilities, and the angular distributions of the photofragments are calculated and discussed. An interesting phenomenon has been found in the spectra of the photofragments. Applying the light-induced adiabatic picture supported by LICI, explanations are given for the unexpected structure of the spectra.

Viscous properties of isotropic fluids composed of linear molecules: departure from the classical Navier-Stokes theory in nano-confined geometries.

PubMed

Hansen, J S; Daivis, Peter J; Todd, B D

2009-10-01

In this paper we present equilibrium molecular-dynamics results for the shear, rotational, and spin viscosities for fluids composed of linear molecules. The density dependence of the shear viscosity follows a stretched exponential function, whereas the rotational viscosity and the spin viscosities show approximately power-law dependencies. The frequency-dependent shear and spin viscosities are also studied. It is found that viscoelastic behavior is first manifested in the shear viscosity and that the real part of the spin viscosities features a maximum for nonzero frequency. The calculated transport coefficients are used together with the extended Navier-Stokes equations to investigate the effect of the coupling between the intrinsic angular momentum and linear momentum for highly confined fluids. Both steady and oscillatory flows are studied. It is shown, for example, that the fluid flow rate for Poiseuille flow is reduced by up to 10% in a 2 nm channel for a buta-triene fluid at density 236 kg m(-3) and temperature 306 K. The coupling effect may, therefore, become very important for nanofluidic applications.

Tracing the Origins of Nitrogen Bearing Organics Toward Orion KL with Alma

NASA Astrophysics Data System (ADS)

Carroll, Brandon; Crockett, Nathan; Wilkins, Olivia H.; Bergin, Edwin; Blake, Geoffrey

2017-06-01

A comprehensive analysis of a broadband 1.2 THz wide spectral survey of the Orion Kleinmann-Low nebula (Orion KL) has shown that nitrogen bearing complex organics trace systematically hotter gas than O-bearing organics toward this source. The origin of this O/N dichotomy remains a mystery. If complex molecules originate from grain surfaces, N-bearing species may be more difficult to remove from grain surfaces than O-bearing organics. Theoretical studies, however, have shown that hot (T=300 K) gas phase chemistry can produce high abundances of N-bearing organics while suppressing the formation of O-bearing complex molecules. In order to distinguish these distinct formation pathways we have obtained extremely high angular resolution observations of methyl cyanide (CH_3CN) using the Atacama Large Millimeter/Submillimeter Array (ALMA) toward Orion KL. By simultaneously imaging ^{13}CH_3CN and CH_2DCN we map the temperature structure and D/H ratio of CH_3CN. We will present updated results of these observations and discuss their implications for the formation of N-bearing organics in the interstellar medium.

Tracing the Origins of Nitrogen Bearing Organics Toward Orion KL with Alma

NASA Astrophysics Data System (ADS)

Carroll, Brandon; Crockett, Nathan; Bergin, Edwin; Blake, Geoffrey

2016-06-01

A comprehensive analysis of a broadband 1.2 THz wide spectral survey of the Orion Kleinmann-Low nebula (Orion KL) from the Herschel Space Telescope has shown that nitrogen bearing complex organics trace systematically hotter gas than O-bearing organics toward this source. The origin of this O/N dichotomy remains a mystery. If complex molecules originate from grain surfaces, N-bearing species may be more difficult to remove from grain surfaces than O-bearing organics. Theoretical studies, however, have shown that hot (T=300 K) gas phase chemistry can produce high abundances of N-bearing organics while suppressing the formation of O-bearing complex molecules. In order to distinguish these distinct formation pathways we have obtained extremely high angular resolution observations of methyl cyanide (CH_3CN) using the Atacama Large Millimeter/Submillimeter Array (ALMA) toward Orion KL. By simultaneously imaging 13CH_3CN and CH_2DCN we map the temperature structure and D/H ratio of CH_3CN. We will present the initial results of these observations and discuss their implications for the formation of N-bearing organics in the interstellar medium.

Fine-structure-resolution for Rovibrational Excitation of CN Due to H2

NASA Astrophysics Data System (ADS)

Byrd, Nat; Yang, Benhui H.; Stancil, Phillip C.

2018-06-01

Diatomic molecules can be readily excited in interstellar environments exposed to intense UV radiation, such as the inner rim of a protoplanetary disk. Non-thermal populations of excited rovibrational levels can result, for example, following decay from electronically excited states to the electronic ground state. Competition between radiative decay and collisional processes, mostly due to H2, determine the resulting rovibrational emission spectrum. For CN, and other open-shell molecules, the resulting spectrum will be complicated due to fine-structure splitting of the rotational levels. In some cases, fine-structure resolution has been previously computed for rotational transitions in atom- or diatom-diatom collisional processes. Here we present the first fine-structure resolution for vibrational deexcitation for CN colliding with H2. The collisional cross sections were computed using a 6D potential energy surface with a full close-coupling approach. Fine-structure resolution is obtained by adopting an angular momentum recoupling scheme to transform the scattering matrices to a recoupled basis. Here we present low-energy calculations for the v=1 to 0 transition.This work was supported by NASA Grant NNX16AF09G.

Solvation of Na^+ in water from first-principles molecular dynamics

NASA Astrophysics Data System (ADS)

White, J. A.; Schwegler, E.; Galli, G.; Gygi, F.

2000-03-01

We have carried out ab initio molecular dynamics (MD) simulations of the Na^+ ion in water with an MD cell containing a single alkali ion and 53 water molecules. The electron-electron and electron-ion interactions were modeled by density functional theory with a generalized gradient approximation for the exchange-correlation functional. The computed radial distribution functions, coordination numbers, and angular distributions are consistent with available experimental data. The first solvation shell contains 5.2±0.6 water molecules, with some waters occasionally exchanging with those of the second shell. The computed Na^+ hydration number is larger than that from calculations for water clusters surrounding an Na^+ ion, but is consistent with that derived from x-ray measurements. Our results also indicate that the first hydration shell is better defined for Na^+ than for K^+ [1], as indicated by the first minimum in the Na-O pair distribution function. [1] L.M. Ramaniah, M. Bernasconi, and M. Parrinello, J. Chem. Phys. 111, 1587 (1999). This work was performed for DOE under contract W-7405-ENG-48.

Crystal structure of di-bromo-meth-oxy-seselin (DBMS), a photobiologically active pyran-ocoumarin.

PubMed

Bauri, A K; Foro, Sabine; Rahman, A F M M

2017-05-01

The title compound, C 15 H 14 Br 2 O 4 [systematic name: rac -(9 S ,10 R )-3,9-dibromo-10-methoxy-8,8-dimethyl-9,10-dihydropyrano[2,3- h ]chromen-2(8 H )-one], is a pyran-ocoumarin derivative formed by the bromination of seselin, which is a naturally occurring angular pyran-ocoumarin isolated from the Indian herb Trachyspermum stictocarpum . In the mol-ecule, the benzo-pyran ring system is essentially planar, with a maximum deviation of 0.044 (2) Å for the O atom. The di-hydro-pyran ring is in a half-chair conformation and the four essentially planar atoms of this ring form a dihedral angle of 4.6 (2)° with the benzo-pyran ring system. In the crystal, mol-ecules are linked by weak C-H⋯O hydrogen bonds, forming chains propagating along [010]. In addition, π-π stacking inter-actions, with centroid-centroid distances of 3.902 (2) and 3.908 (2) Å, link the hydrogen-bonded chains into layers parallel to (001).

Angular-dependent EDMR linewidth for spin-dependent space charge limited conduction in a polycrystalline pentacene

NASA Astrophysics Data System (ADS)

Fukuda, Kunito; Asakawa, Naoki

2017-08-01

Spin-dependent space charge limited carrier conduction in a Schottky barrier diode using polycrystalline p-type π-conjugated molecular pentacene is explored using multiple-frequency electrically detected magnetic resonance (EDMR) spectroscopy with a variable-angle configuration. The measured EDMR spectra are decomposed into two components derived respectively from mobile and trapped positive polarons. The linewidth of the EDMR signal for the trapped polarons increases with increasing resonance magnetic field for an in-plane configuration where the normal vector of the device substrate is perpendicular to the resonance magnetic field, while it is independent of the field for an out-of-plane configuration. This difference is consistent with the pentacene arrangement on the device substrate, where pentacene molecules exhibit a uniaxial orientation on the out-of-substrate plane. By contrast, the mobile polarons do not show anisotropic behavior with respect to the resonance magnetic field, indicating that the anisotropic effect is averaged out owing to carrier motion. These results suggest that the orientational arrangements of polycrystalline pentacene molecules in a nano thin film play a crucial role in spin-dependent electrical conduction.

Picosecond absorption anisotropy of polymethine and squarylium dyes in liquid and polymeric media

NASA Astrophysics Data System (ADS)

Przhonska, Olga V.; Hagan, David J.; Novikov, Evgueni; Lepkowicz, Richard; Van Stryland, Eric W.; Bondar, Mikhail V.; Slominsky, Yuriy L.; Kachkovski, Alexei D.

2001-11-01

Time-resolved excitation-probe polarization measurements are performed for polymethine and squarylium dyes in ethanol and an elastopolymer of polyurethane acrylate (PUA). These molecules exhibit strong excited-state absorption in the visible, which results in reverse saturable absorption (RSA). In pump-probe experiments, we observe a strong angular dependence of the RSA decay kinetics upon variation of the angle between pump and probe polarizations. The difference in absorption anisotropy kinetics in ethanol and PUA is detected and analyzed. Anisotropy decay curves in ethanol follow a single exponential decay leading to complete depolarization of the excited state. We also observe complete depolarization in PUA, in which case the anisotropy decay follows a double exponential behavior. Possible rotations in the PUA polymeric matrix are connected with the existence of local microcavities of free volume. We believe that the fast decay component is connected with the rotation of molecular fragments and the slower decay component is connected with the rotation of entire molecules in local microcavities, which is possible because of the elasticity of the polymeric material.

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

Asthalter,T.; Sergueev, I.; Van Burck, U.

The low- and high-temperature phases of octamethyl ferrocene were studied in detail, using high-resolution X-ray powder diffraction, differential scanning calorimetry and nuclear resonant scattering, in particular the novel technique of synchrotron radiation perturbed angular correlations (SRPAC). Much as in the case of an analogous but more unsymmetrical molecule, octamethyl ethinyl ferrocene, the high-temperature phase possesses the space group R{bar 3}m source with lattice parameters a = b = 12.5568(1) Angstroms, c = 9.6045(1) Angstroms, which in the rhombohedral setting correspond to a = 7.9251(1) Angstroms, {alpha}=104.79 degrees. An increase of the volume per formula unit of about 12% across themore » phase transition is observed. The rotation of the electric field gradient, which can be identified with the rotation of the entire molecule within the lattice, follows Arrhenius behavior with a high activation energy of (40.3 {+-} 3.3)kJ mol{sup -1}. Whereas precursor effects and a change in activation energy were observed for octamethyl ethinyl ferrocene, no such effects are observed for octamethyl ferrocene. We relate this difference to the absence of the ethinyl substituent in octamethyl ferrocene.« less

Spin squeezing a cold molecule

NASA Astrophysics Data System (ADS)

Bhattacharya, M.

2015-12-01

In this article we present a concrete proposal for spin squeezing the cold ground-state polar paramagnetic molecule OH, a system currently under fine control in the laboratory. In contrast to existing work, we consider a single, noninteracting molecule with angular momentum greater than 1 /2 . Starting from an experimentally relevant effective Hamiltonian, we identify an adiabatic regime where different combinations of static electric and magnetic fields can be used to realize the single-axis twisting Hamiltonian of Kitagawa and Ueda [M. Kitagawa and M. Ueda, Phys. Rev. A 47, 5138 (1993), 10.1103/PhysRevA.47.5138], the uniform field Hamiltonian proposed by Law et al. [C. K. Law, H. T. Ng, and P. T. Leung, Phys. Rev. A 63, 055601 (2001), 10.1103/PhysRevA.63.055601], and a model of field propagation in a Kerr medium considered by Agarwal and Puri [G. S. Agarwal and R. R. Puri, Phys. Rev. A 39, 2969 (1989), 10.1103/PhysRevA.39.2969]. We then consider the situation in which nonadiabatic effects are quite large and show that the effective Hamiltonian supports spin squeezing even in this case. We provide analytical expressions as well as numerical calculations, including optimization of field strengths and accounting for the effects of field misalignment. Our results have consequences for applications such as precision spectroscopy, techniques such as magnetometry, and stereochemical effects such as the orientation-to-alignment transition.

Enhanced Raman Scattering on In-plane Anisotropic Layered Materials

DOE PAGES

Liang, Liangbo; Meunier, Vincent; Sumpter, Bobby G.; ...

2015-11-19

Surface-enhanced Raman scattering (SERS) on two-dimensional (2D) layered materials has provided a unique platform to study the chemical mechanism (CM) of the enhancement due to its natural separation from electromagnetic enhancement. The CM stems from the basic charge interactions between the substrate and molecules. Despite the extensive studies of the energy alignment between 2D materials and molecules, an understanding of how the electronic properties of the substrate are explicitly involved in the charge interaction is still unclear. Lately, a new group of 2D layered materials with anisotropic structure, including orthorhombic black phosphorus (BP) and triclinic rhenium disulphide (ReS2), has attractedmore » great interest due to their unique anisotropic electrical and optical properties. Herein, we report a unique anisotropic Raman enhancement on few-layered BP and ReS2 using copper phthalocyanine (CuPc) molecules as a Raman probe, which is absent on isotropic graphene and h-BN. According to detailed Raman tensor analysis and density functional theory calculations, anisotropic charge interactions due to the anisotropic carrier mobilities of the 2D materials are responsible for the angular dependence of the Raman enhancement. Our findings not only provide new insights into the CM process in SERS, but also open up new avenues for the exploration and application of the electronic properties of anisotropic 2D layered materials.« less

Change in resonance parameters of a linear molecule as it bends: Evidence in electron-impact vibrational transitions of hot COS and CO2 molecules*

NASA Astrophysics Data System (ADS)

Hoshino, Masamitsu; Ishijima, Yohei; Kato, Hidetoshi; Mogi, Daisuke; Takahashi, Yoshinao; Fukae, Katsuya; Limão-Vieira, Paulo; Tanaka, Hiroshi; Shimamura, Isao

2016-04-01

Inelastic and superelastic electron-impact vibrational excitation functions of hot carbonyl sulphide COS (and hot CO2) are measured for electron energies from 0.5 to 3.0 eV (1.5 to 6.0 eV) and at a scattering angle of 90°. Based on the vibrational populations and the principle of detailed balance, these excitation functions are decomposed into contributions from state-to-state vibrational transitions involving up to the second bending overtone (030) in the electronically ground state. Both the 2Π resonance for COS around 1.2 eV and the 2Πu resonance for CO2 around 3.8 eV are shifted to lower energies as the initial vibrational state is excited in the bending mode. The width of the resonance hump for COS changes only little as the molecule bends, whereas that of the overall boomerang resonance for CO2 becomes narrower. The angular distribution of the electrons resonantly scattered by hot COS and hot CO2 is also measured. The different shapes depending on the vibrational transitions and gas temperatures are discussed in terms of the symmetry of the vibrational wave functions. Contribution to the Topical Issue "Advances in Positron and Electron Scattering", edited by Paulo Limao-Vieira, Gustavo Garcia, E. Krishnakumar, James Sullivan, Hajime Tanuma and Zoran Petrovic.

The Renner effect in triatomic molecules with application to CH+, MgNC and NH2.

PubMed

Jensen, Per; Odaka, Tina Erica; Kraemer, W P; Hirano, Tsuneo; Bunker, P R

2002-03-01

We have developed a computational procedure, based on the variational method, for the calculation of the rovibronic energies of a triatomic molecule in an electronic state that become degenerate at the linear nuclear configuration. In such an electronic state the coupling caused by the electronic orbital angular momentum is very significant and it is called the Renner effect. We include it, and the effect of spin-orbit coupling, in our program. We have developed the procedure to the point where spectral line intensities can be calculated so that absorption and emission spectra can be simulated. In order to gain insight into the nature of the eigenfunctions, we have introduced and calculated the overall bending probability density function f(p) of the states. By projecting the eigenfunctions onto the Born-Oppenheimer basis, we have determined the probability density functions f+(rho) and f-(rho) associated with the individual Born-Oppenheimer states phi(-)elec and phi(+)elec. At a given temperature the Boltzmann averaged value of the f(p) over all the eigenstates gives the bending probability distribution function F(rho), and this can be related to the result of a Coulomb Explosion Imaging (CEI) experiment. We review our work and apply it to the molecules CH2+, MgNC and NH2, all of which are of astrophysical interest.

An optical apparatus for rotation and trapping

PubMed Central

Gutiérrez-Medina, Braulio; Andreasson, Johan O. L.; Greenleaf, William J.; LaPorta, Arthur; Block, Steven M.

2010-01-01

We present details of the design, construction and testing of a single-beam optical tweezers apparatus capable of measuring and exerting torque, as well as force, on microfabricated, optically anisotropic particles (an ‘optical torque wrench’). The control of angular orientation is achieved by rotating the linear polarization of a trapping laser with an electro-optic modulator (EOM), which affords improved performance over previous designs. The torque imparted to the trapped particle is assessed by measuring the difference between left- and right-circular components of the transmitted light, and constant torque is maintained by feeding this difference signal back into a custom-designed electronic servo loop. The limited angular range of the EOM (±180°) is extended by rapidly reversing the polarization once a threshold angle is reached, enabling the torque clamp to function over unlimited, continuous rotations at high bandwidth. In addition, we developed particles suitable for rotation in this apparatus using microfabrication techniques. Altogether, the system allows for the simultaneous application of forces (~0.1–100 pN) and torques (~1–10,000 pN nm) in the study of biomolecules. As a proof of principle, we demonstrate how our instrument can be used to study the supercoiling of single DNA molecules. PMID:20627165

Photonic orbital angular momentum in starlight. Further analysis of the 2011 Starfire Optical Range Observations

NASA Astrophysics Data System (ADS)

Oesch, Denis W.; Sanchez, Darryl J.

2014-07-01

Context. Each attempt by the Atmospheric Simulation and Adaptive-optics Laboratory Testbed (ASALT) research group to detect turbulence-induced photonic orbital angular momentum (POAM) has been successful, spanning laboratory, simulation and field experiments, with the possible exception of the 2011 Starfire Optical Range (SOR) astronomical observations, a search for POAM induced by astronomical sources. Aims: The purposes of this work are to discuss how POAM from astronomical turbulent assemblages of molecules or atoms (TAMA) would appear in observations and then to reanalyze the data from the 2011 SOR observations using a more refined technique as a demonstration of POAM in starlight. Methods: This work uses the method of projections used previously in analysis of terrestrial data. Results: Using the method of projections, the noise floor of the system was reevaluated and is found to be no greater than 1%. Reevaluation of the 2011 SOR observations reveals that a POAM signal is evident in all of the data. Conclusions: POAM signals have been found in every instance of extended propagation through turbulence conducted by the ASALT research group, including the 2011 SOR observations. POAM is an inevitable result of the propagation of optical waves through turbulence. We express our gratitude to the Air Force Office of Scientific Research for their support of this research.

Angle-Dependent Atomic Force Microscopy Single-Chain Pulling of Adsorbed Macromolecules from Planar Surfaces Unveils the Signature of an Adsorption-Desorption Transition.

PubMed

Grebíková, Lucie; Whittington, Stuart G; Vancso, Julius G

2018-05-23

The adsorption-desorption behavior of polymer chains is at the heart of macromolecular surface science and technology. With the current developments in atomic force microscopy (AFM), it has now become possible to address the desorption problem from the perspective of a single macromolecule. Here, we report on desorption of single polymer chains on planar surfaces by AFM-based single molecule force spectroscopy (SMFS) as a function of the pulling angle with respect to the surface-normal direction. SMFS experiments were performed in water with various substrates using different polymers covalently attached to the AFM probe tip. End-grafting at the AFM tip was achieved by surface-initiated polymerization using initiator functionalized tips. We found that the desorption force increases with a decreasing pulling angle, i.e., an enhanced adhesion of the polymer chain was observed. The magnitude of the desorption force shows a weak angular dependence at pulling angles close to the surface normal. A significant increase of the force is observed at shallower pulling from a certain pulling angle. This behavior carries the signature of an adsorption-desorption transition. The angular dependence of the normalized desorption force exhibits a universal behavior. We compared and interpreted our results using theoretical predictions for single-chain adsorption-desorption transitions.

Angle-Dependent Atomic Force Microscopy Single-Chain Pulling of Adsorbed Macromolecules from Planar Surfaces Unveils the Signature of an Adsorption–Desorption Transition

PubMed Central

2018-01-01

The adsorption–desorption behavior of polymer chains is at the heart of macromolecular surface science and technology. With the current developments in atomic force microscopy (AFM), it has now become possible to address the desorption problem from the perspective of a single macromolecule. Here, we report on desorption of single polymer chains on planar surfaces by AFM-based single molecule force spectroscopy (SMFS) as a function of the pulling angle with respect to the surface-normal direction. SMFS experiments were performed in water with various substrates using different polymers covalently attached to the AFM probe tip. End-grafting at the AFM tip was achieved by surface-initiated polymerization using initiator functionalized tips. We found that the desorption force increases with a decreasing pulling angle, i.e., an enhanced adhesion of the polymer chain was observed. The magnitude of the desorption force shows a weak angular dependence at pulling angles close to the surface normal. A significant increase of the force is observed at shallower pulling from a certain pulling angle. This behavior carries the signature of an adsorption–desorption transition. The angular dependence of the normalized desorption force exhibits a universal behavior. We compared and interpreted our results using theoretical predictions for single-chain adsorption–desorption transitions. PMID:29712430

Bessel Fourier Orientation Reconstruction (BFOR): An Analytical Diffusion Propagator Reconstruction for Hybrid Diffusion Imaging and Computation of q-Space Indices

PubMed Central

Hosseinbor, A. Pasha; Chung, Moo K.; Wu, Yu-Chien; Alexander, Andrew L.

2012-01-01

The ensemble average propagator (EAP) describes the 3D average diffusion process of water molecules, capturing both its radial and angular contents. The EAP can thus provide richer information about complex tissue microstructure properties than the orientation distribution function (ODF), an angular feature of the EAP. Recently, several analytical EAP reconstruction schemes for multiple q-shell acquisitions have been proposed, such as diffusion propagator imaging (DPI) and spherical polar Fourier imaging (SPFI). In this study, a new analytical EAP reconstruction method is proposed, called Bessel Fourier orientation reconstruction (BFOR), whose solution is based on heat equation estimation of the diffusion signal for each shell acquisition, and is validated on both synthetic and real datasets. A significant portion of the paper is dedicated to comparing BFOR, SPFI, and DPI using hybrid, non-Cartesian sampling for multiple b-value acquisitions. Ways to mitigate the effects of Gibbs ringing on EAP reconstruction are also explored. In addition to analytical EAP reconstruction, the aforementioned modeling bases can be used to obtain rotationally invariant q-space indices of potential clinical value, an avenue which has not yet been thoroughly explored. Three such measures are computed: zero-displacement probability (Po), mean squared displacement (MSD), and generalized fractional anisotropy (GFA). PMID:22963853

Scattering of low-energetic atoms and molecules from a boron-doped CVD diamond surface

NASA Astrophysics Data System (ADS)

Allenbach, M.; Neuland, M. B.; Riedo, A.; Wurz, P.

2018-01-01

For the detection of low energetic neutral atoms for the remote sensing of space plasmas, charge state conversion surfaces are used to ionize the neutrals for their subsequent measurement. We investigated a boron-doped Chemical Vapor Deposition (CVD) diamond sample for its suitability to serve as a conversion surface on future space missions, such as NASA's Interstellar Mapping and Acceleration Probe. For H and O atoms incident on conversion surface with energies ranging from 195 to 1000 eV and impact angles from 6° to 15° we measured the angular scattering distributions and the ionization yields. Atomic force microscope and laser ablation ionization mass spectrometry analyses were applied to further characterize the sample. Based on a figure-of-merit, which included the ionization yield and angular scatter distribution, the B-doped CVD surface was compared to other, previously characterized conversion surfaces, including e.g. an undoped CVD diamond with a metallized backside. For particle energies below 390 eV the performance of the B-doped CVD conversion surfaces is comparable to surfaces studied before. For higher energies the figure-of-merit indicates a superior performance. From our studies we conclude that the B-doped CVD diamond sample is well suited for its application on future space missions.

Non-mechanical beam steering in the mid-wave infrared

NASA Astrophysics Data System (ADS)

Frantz, Jesse A.; Myers, Jason D.; Bekele, Robel Y.; Spillmann, Christopher M.; Naciri, Jawad; Kolacz, Jakub S.; Gotjen, Henry; Shaw, Leslie B.; Sanghera, Jasbinder S.; Sodergren, Bennett; Wang, Ying-Ju; Rommel, Scott D.; Anderson, Mike; Davis, Scott R.; Ziemkiewicz, Michael

2017-05-01

The mid-wave infrared (MWIR) portion of the electromagnetic spectrum is critically important for a variety of applications such as LIDAR and chemical sensing. Concerning the latter, the MWIR is often referred to as the "molecular fingerprint" region owing to the fact that many molecules display distinctive vibrational absorptions in this region, making it useful for gas detection. To date, steering MWIR radiation typically required the use of mechanical devices such as gimbals, which are bulky, slow, power-hungry, and subject to mechanical failure. We present the first non-mechanical beam steerer capable of continuous angular tuning in the MWIR. These devices, based on refractive, electro-optic waveguides, provide angular steering in two dimensions without relying on moving parts. Previous work has demonstrated non-mechanical beam steering (NMBS) in the short-wave infrared (SWIR) and near infrared (NIR) using a waveguide in which a portion of the propagating light is evanescently coupled to a liquid crystal (LC) layer in which the refractive index is voltage-tuned. We have extended this NMBS technology into the MWIR by employing chalcogenide glass waveguides and LC materials that exhibit high MWIR transparency. As a result, we have observed continuous, 2D MWIR steering for the first time with a magnitude of 2.74° in-plane and 0.3° out-of-plane.

Excitation of vibrational quanta in furfural by intermediate-energy electrons

NASA Astrophysics Data System (ADS)

Jones, D. B.; Neves, R. F. C.; Lopes, M. C. A.; da Costa, R. F.; Varella, M. T. do N.; Bettega, M. H. F.; Lima, M. A. P.; García, G.; Blanco, F.; Brunger, M. J.

2015-12-01

We report cross sections for electron-impact excitation of vibrational quanta in furfural, at intermediate incident electron energies (20, 30, and 40 eV). The present differential cross sections are measured over the scattered electron angular range 10°-90°, with corresponding integral cross sections subsequently being determined. Furfural is a viable plant-derived alternative to petrochemicals, being produced via low-temperature plasma treatment of biomass. Current yields, however, need to be significantly improved, possibly through modelling, with the present cross sections being an important component of such simulations. To the best of our knowledge, there are no other cross sections for vibrational excitation of furfural available in the literature, so the present data are valuable for this important molecule.

Hybrid and Constrained Resolution-of-Identity Techniques for Coulomb Integrals.

PubMed

Duchemin, Ivan; Li, Jing; Blase, Xavier

2017-03-14

The introduction of auxiliary bases to approximate molecular orbital products has paved the way to significant savings in the evaluation of four-center two-electron Coulomb integrals. We present a generalized dual space strategy that sheds a new light on variants over the standard density and Coulomb-fitting schemes, including the possibility of introducing minimization constraints. We improve in particular the charge- or multipole-preserving strategies introduced respectively by Baerends and Van Alsenoy that we compare to a simple scheme where the Coulomb metric is used for lowest angular momentum auxiliary orbitals only. We explore the merits of these approaches on the basis of extensive Hartree-Fock and MP2 calculations over a standard set of medium size molecules.

Dynamical properties of the hydration shell of fully deuterated myoglobin

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

Achterhold, Klaus; Parak, Fritz G.; Ostermann, Andreas

2011-10-15

Freeze-dried perdeuterated sperm whale myoglobin was kept in a water-saturated atmosphere in order to obtain a hydration degree of 335 {sup 1}H{sub 2}O molecules per one myoglobin molecule. Incoherent neutron scattering was performed at the neutron spectrometer TOFTOF at the FRM II in an angular range of q from 0.6 to 1.8 A{sup -1} and a temperature range from 4 to 297 K. We used neutrons with a wavelength of {lambda}{alpha}E 6 A and an energy resolution of about 65 {mu}eV corresponding to motions faster than 10 ps. At temperatures above 225 K, broad lines appear in the spectra causedmore » by quasielastic scattering. For an explanation of these lines, we assumed that there are only two types of protons, those that are part of the hydration water (72%) and those that belong to the protein (28%). The protons of the hydration water were analyzed with the diffusion model of Singwi and Sjoelander [Phys. Rev. 119, 863 (1960)]. In this model, a water molecule stays for a time {tau}{sub 0} in a bound state performing oscillatory motions. Thereafter, the molecule performs free diffusion for the time {tau}{sub 1} in a nonbound state followed again by the oscillatory motions for {tau}{sub 0} and so forth. We used the general formulation with no simplifications as {tau}{sub 0}>>{tau}{sub 1} or {tau}{sub 1}>>{tau}{sub 0}. At room temperature, we obtained {tau}{sub 0} {alpha}E 104 ps and {tau}{sub 1} {alpha}E 37 ps. For the protein bound hydrogen, the dynamics is described by a Brownian oscillator where the protons perform overdamped motions in limited space.« less

Exploring Molecular Complexity in the Interstellar Medium with Alma

NASA Astrophysics Data System (ADS)

Belloche, Arnaud

2017-06-01

The search for complex organic molecules (COMs) in the interstellar medium (ISM) relies heavily on the progress made in the laboratory to record and characterize the rotational spectra of these molecules. Almost 200 different molecules have been identified in the ISM so far, in particular thanks to millimeter-wavelength observations of the star-forming molecular cloud core Sgr B2(N) in the Galactic Center region. The advent of the Atacama Large Millimeter/submillimeter Array (ALMA) has recently opened a new door to explore the molecular complexity of the ISM. Thanks to its high angular resolution, the spectral confusion of star-forming cores can be reduced, and its tremendous sensitivity allows astronomers to detect molecules of low abundance that could not be probed by previous generations of telescopes. I will present results of the EMoCA survey conducted toward Sgr B2(N) with ALMA. The main goal of this spectral line survey is to decipher the molecular content of Sgr B2(N) in order to test the predictions of astrochemical numerical simulations and gain insight into the chemical processes at work in the ISM. I will in particular report on the tentative detection of N-methylformamide, on the deuterium fractionation of COMs, and on the detection of a branched alkyl molecule in the ISM. The latter detection has unveiled a new domain in the structures available to the chemistry of star-forming regions and established a further connection to the COMs found in meteorites. A. Belloche, A. A. Meshcheryakov, R. T. Garrod et al. 2017, A&A, in press, DOI: 10.1051/0004-6361/201629724 A. Belloche, H. S. P. Müller, R. T. Garrod, and K. M. Menten 2016, A&A, 587, A91 A. Belloche, R. T. Garrod, H. S. P. Müller, and K. M. Menten 2014, Science, 345, 1584 R. T. Garrod, A. Belloche, H. S. P. Müller, and K. M. Menten 2017, A&A, in press, DOI: 10.1051/0004-6361/201630254.

Radiation from an accelerating neutral body: The case of rotation

NASA Astrophysics Data System (ADS)

Yarman, Tolga; Arik, Metin; Kholmetskii, Alexander L.

2013-11-01

When an object is bound at rest to an attractional field, its rest mass (owing to the law of energy conservation, including the mass and energy equivalence of the Special Theory of Relativity) must decrease. The mass deficiency coming into play indicates a corresponding rest energy discharge. Thus, bringing an object to a rotational motion means that the energy transferred for this purpose serves to extract just as much rest mass (or similarly "rest energy", were the speed of light in empty space taken to be unity) out of it. Here, it is shown that during angular acceleration, photons of fundamental energy are emitted, while the object is kept on being delivered to a more and more intense rotational accelerational field, being the instantaneous angular velocity of the rotating object. This fundamental energy, as seen, does not depend on anything else (such as the mass or charge of the object), and it is in harmony with Bohr's Principle of Correspondence. This means at the same time, that emission will be achieved, as long as the angular velocity keeps on increasing, and will cease right after the object reaches a stationary rotational motion (a constant centrifugal acceleration), but if the object were brought to rotation in vacuum with no friction. By the same token, one can affirm that even the rotation at a macroscopic level is quantized, and can only take on "given angular velocities" (which can only be increased, bit by bit). The rate of emission of photons of concern is, on the other hand, proportional to the angular acceleration of the object, similarly to the derivative of the tangential acceleration with respect to time. It is thus constant for a "constant angular acceleration", although the energy of the emitted photons will increase with increasing , until the rotation reaches a stationary level, after which we expect no emission --let us stress-- if the object is in rotation in vacuum, along with no whatsoever friction (such as the case of a rotating diatomic molecule, for instance). If the object reaches its final state in a given medium, say air, and "friction" is present, such as the case of a dental drill, then energy should keep being supplied to it, to overcome friction, which is present either inside the "inner mechanism of rotation" or in its surroundings. In other words, the object in the latter case, would be constantly subject to a friction force, countering its motion, and tending to make it fall to lower rotational energy states. Any fluctuations in the power supply, on the other hand, will slow down the rotating object, no matter how indiscernibly. The small decrease in the rotational velocity is yet reincreased by restoring the power supply, thus perpetually securing a stationary rotational motion. Thereby, the object in this final state, due to fluctuations in either friction or power supply, or both, shall further be expected to emit a radiation of energy , where is the final angular velocity of the object in rotation. What is more is that our team has very successfully measured what is predicted here, and they will report their experimental results in a subsequent article. The approach presented here seems to shed light on the mysterious sonoluminescence. It also triggers the possibility of sensing earthquakes due to radiation that should be emitted by the faults, on which the seismic stress keeps increasing until the crackdown. By the same token, also two colliding (neutral) objects are expected to emit radiation.

Efficient molecular density functional theory using generalized spherical harmonics expansions.

PubMed

Ding, Lu; Levesque, Maximilien; Borgis, Daniel; Belloni, Luc

2017-09-07

We show that generalized spherical harmonics are well suited for representing the space and orientation molecular density in the resolution of the molecular density functional theory. We consider the common system made of a rigid solute of arbitrary complexity immersed in a molecular solvent, both represented by molecules with interacting atomic sites and classical force fields. The molecular solvent density ρ(r,Ω) around the solute is a function of the position r≡(x,y,z) and of the three Euler angles Ω≡(θ,ϕ,ψ) describing the solvent orientation. The standard density functional, equivalent to the hypernetted-chain closure for the solute-solvent correlations in the liquid theory, is minimized with respect to ρ(r,Ω). The up-to-now very expensive angular convolution products are advantageously replaced by simple products between projections onto generalized spherical harmonics. The dramatic gain in speed of resolution enables to explore in a systematic way molecular solutes of up to nanometric sizes in arbitrary solvents and to calculate their solvation free energy and associated microscopic solvent structure in at most a few minutes. We finally illustrate the formalism by tackling the solvation of molecules of various complexities in water.

EPR Studies of Magnetically Dilute Ga-Doped Single Crystals of Fe18 Antiferromagnetic Molecular Wheels

NASA Astrophysics Data System (ADS)

Henderson, John; Ramsey, Christopher; Del Barco, Enrique; Stamatatos, Theocharis; Christou, George

2008-03-01

Studies of the quantum dynamics of the electron spins in solid state systems has gained considerable interest recently due to their potential for use as quantum computing substrates. One class of materials, molecular magnets, are of particular importance, owing to the seemingly limitless array of spin configurations due to synthetic chemical flexibility. Efforts are currently devoted to minimizing decoherence times by diminishing dipolar effects. In this regard, we have carried out EPR measurements on small single crystals of 0.5% Ga doped Fe18 molecular antiferromagnetic wheels at temperatures down to 300 mK using planar resonators patterned on GaAs wafers. This system constitutes a dilute sample of S = 5/2 molecules dispersed within a sea of S = 0 (at low temperature) molecules, which significantly reduces dipolar interactions and might provide a means of observing Rabi oscillations in crystals of molecular magnets. Detailed angular dependence studies reveal significant anisotropy with D = 500 mK and E = 20 mK. The presence of second order anisotropy (E) is very unusual for such a high symmetry system and its interpretation will be discussed. Pulsed-EPR measurements and doping concentration dependence will also be discussed.

Photodissociation of ultracold diatomic strontium molecules with quantum state control.

PubMed

McDonald, M; McGuyer, B H; Apfelbeck, F; Lee, C-H; Majewska, I; Moszynski, R; Zelevinsky, T

2016-07-07

Chemical reactions at ultracold temperatures are expected to be dominated by quantum mechanical effects. Although progress towards ultracold chemistry has been made through atomic photoassociation, Feshbach resonances and bimolecular collisions, these approaches have been limited by imperfect quantum state selectivity. In particular, attaining complete control of the ground or excited continuum quantum states has remained a challenge. Here we achieve this control using photodissociation, an approach that encodes a wealth of information in the angular distribution of outgoing fragments. By photodissociating ultracold (88)Sr2 molecules with full control of the low-energy continuum, we access the quantum regime of ultracold chemistry, observing resonant and nonresonant barrier tunnelling, matter-wave interference of reaction products and forbidden reaction pathways. Our results illustrate the failure of the traditional quasiclassical model of photodissociation and instead are accurately described by a quantum mechanical model. The experimental ability to produce well-defined quantum continuum states at low energies will enable high-precision studies of long-range molecular potentials for which accurate quantum chemistry models are unavailable, and may serve as a source of entangled states and coherent matter waves for a wide range of experiments in quantum optics.

Probing Cometary Chemistry with ALMA

NASA Technical Reports Server (NTRS)

Milam, Stefanie N.

2010-01-01

Comets are considered to bear the record of the primitive Solar nebula as remnants of planetesimals that formed the outer planets. To date there are just over two dozen known cometary species compared to the >150 known interstellar molecules. This is likely due to the challenges posed when attempting to measure the composition of these small bodies. With the significant improvement in sensitivity, ALMA will likely enable the detection of new molecules to help us gain better understanding of the chemical complexity found in comets. This advancement in sensitivity will also assist in the measurement of isotope ratios in various species. These values are imperative for determining the conditions during cometary formation as well as provide insight into ongoing speculations of parent species, the possible delivery of H2O to Earth, and a direct comparison to protostellar disk chemistry. The high angular resolution obtained with ALMA will be capable of resolving any compact distributions or density enhancements in the more extended distribution that may lead to a better understanding of the formation of these species in the outer coma. By studying comet compositions we gain insight into the composition of the early Solar System as well as their astrobiological implications.

High field ESR study of the pi-d interaction effect in beta-(BDA-TTP)2MCl4 (M=Fe, Ga)

NASA Astrophysics Data System (ADS)

Tokumoto, Takahisa; Vantol, J.; Brunel, L.-C.; Choi, E. S.; Brooks, J. S.; Kaihatsu, T.; Akutsu, H.; Yamada, J.

2007-03-01

Novel magnetic organic conductors with pi-d interaction have commanded attention since the discovery of field induced superconductivity. One of them, beta-(BDA-TTP)2FeCl4, has alternating donor molecules and quasi 2D electrical properties. Previous studies of electrical and magnetic properties show an M-I transition at 120K and an AF transition at TN=8.5K, suggesting an exchange interaction between the conduction electrons and the Fe^3+ d-electrons. The properties of beta-(BDA-TTP)2GaCl4 are similar with exception of the absence of the AF transition, which is apparently due to the absence of pi-d exchange interaction. We report angular/temperature dependent 240GHz quasi optical ESR measurements on both compounds to probe the magnetic properties. The Ga compound signals follow the donor molecule structure, and show no magnetic order at any temperature. The Fe compound signals are quite different from the Ga compound, and exhibit AF behavior below TN. The difference of Fe and Ga compounds will be discussed in terms of the interaction between localized and itinerant magnetic moments.

Water evaporation: a transition path sampling study.

PubMed

Varilly, Patrick; Chandler, David

2013-02-07

We use transition path sampling to study evaporation in the SPC/E model of liquid water. On the basis of thousands of evaporation trajectories, we characterize the members of the transition state ensemble (TSE), which exhibit a liquid-vapor interface with predominantly negative mean curvature at the site of evaporation. We also find that after evaporation is complete, the distributions of translational and angular momenta of the evaporated water are Maxwellian with a temperature equal to that of the liquid. To characterize the evaporation trajectories in their entirety, we find that it suffices to project them onto just two coordinates: the distance of the evaporating molecule to the instantaneous liquid-vapor interface and the velocity of the water along the average interface normal. In this projected space, we find that the TSE is well-captured by a simple model of ballistic escape from a deep potential well, with no additional barrier to evaporation beyond the cohesive strength of the liquid. Equivalently, they are consistent with a near-unity probability for a water molecule impinging upon a liquid droplet to condense. These results agree with previous simulations and with some, but not all, recent experiments.

Learning about Biomolecular Solvation from Water in Protein Crystals.

PubMed

Altan, Irem; Fusco, Diana; Afonine, Pavel V; Charbonneau, Patrick

2018-03-08

Water occupies typically 50% of a protein crystal and thus significantly contributes to the diffraction signal in crystallography experiments. Separating its contribution from that of the protein is, however, challenging because most water molecules are not localized and are thus difficult to assign to specific density peaks. The intricateness of the protein-water interface compounds this difficulty. This information has, therefore, not often been used to study biomolecular solvation. Here, we develop a methodology to surmount in part this difficulty. More specifically, we compare the solvent structure obtained from diffraction data for which experimental phasing is available to that obtained from constrained molecular dynamics (MD) simulations. The resulting spatial density maps show that commonly used MD water models are only partially successful at reproducing the structural features of biomolecular solvation. The radial distribution of water is captured with only slightly higher accuracy than its angular distribution, and only a fraction of the water molecules assigned with high reliability to the crystal structure is recovered. These differences are likely due to shortcomings of both the water models and the protein force fields. Despite these limitations, we manage to infer protonation states of some of the side chains utilizing MD-derived densities.

Simulation of diatomic gas-wall interaction and accommodation coefficients for negative ion sources and accelerators.

PubMed

Sartori, E; Brescaccin, L; Serianni, G

2016-02-01

Particle-wall interactions determine in different ways the operating conditions of plasma sources, ion accelerators, and beams operating in vacuum. For instance, a contribution to gas heating is given by ion neutralization at walls; beam losses and stray particle production-detrimental for high current negative ion systems such as beam sources for fusion-are caused by collisional processes with residual gas, with the gas density profile that is determined by the scattering of neutral particles at the walls. This paper shows that Molecular Dynamics (MD) studies at the nano-scale can provide accommodation parameters for gas-wall interactions, such as the momentum accommodation coefficient and energy accommodation coefficient: in non-isothermal flows (such as the neutral gas in the accelerator, coming from the plasma source), these affect the gas density gradients and influence efficiency and losses in particular of negative ion accelerators. For ideal surfaces, the computation also provides the angular distribution of scattered particles. Classical MD method has been applied to the case of diatomic hydrogen molecules. Single collision events, against a frozen wall or a fully thermal lattice, have been simulated by using probe molecules. Different modelling approximations are compared.

Simulation of diatomic gas-wall interaction and accommodation coefficients for negative ion sources and accelerators

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

Sartori, E., E-mail: emanuele.sartori@igi.cnr.it; Serianni, G.; Brescaccin, L.

2016-02-15

Particle-wall interactions determine in different ways the operating conditions of plasma sources, ion accelerators, and beams operating in vacuum. For instance, a contribution to gas heating is given by ion neutralization at walls; beam losses and stray particle production—detrimental for high current negative ion systems such as beam sources for fusion—are caused by collisional processes with residual gas, with the gas density profile that is determined by the scattering of neutral particles at the walls. This paper shows that Molecular Dynamics (MD) studies at the nano-scale can provide accommodation parameters for gas-wall interactions, such as the momentum accommodation coefficient andmore » energy accommodation coefficient: in non-isothermal flows (such as the neutral gas in the accelerator, coming from the plasma source), these affect the gas density gradients and influence efficiency and losses in particular of negative ion accelerators. For ideal surfaces, the computation also provides the angular distribution of scattered particles. Classical MD method has been applied to the case of diatomic hydrogen molecules. Single collision events, against a frozen wall or a fully thermal lattice, have been simulated by using probe molecules. Different modelling approximations are compared.« less

Unraveling the formation of HCPH(X2A') molecules in extraterrestrial environments: crossed molecular beam study of the reaction of carbon atoms, C(3Pj), with phosphine, PH3(X1A1).

PubMed

Guo, Y; Gu, X; Zhang, F; Sun, B J; Tsai, M F; Chang, A H H; Kaiser, R I

2007-05-03

The reaction between ground state carbon atoms, C(3P(j)), and phosphine, PH3(X(1)A1), was investigated at two collision energies of 21.1 and 42.5 kJ mol(-1) using the crossed molecular beam technique. The chemical dynamics extracted from the time-of-flight spectra and laboratory angular distributions combined with ab initio calculations propose that the reaction proceeds on the triplet surface via an addition of atomic carbon to the phosphorus atom. This leads to a triplet CPH3 complex. A successive hydrogen shift forms an HCPH2 intermediate. The latter was found to decompose through atomic hydrogen emission leading to the cis/trans-HCPH(X(2)A') reaction products. The identification of cis/trans-HCPH(X(2)A') molecules under single collision conditions presents a potential pathway to form the very first carbon-phosphorus bond in extraterrestrial environments like molecular clouds and circumstellar envelopes, and even in the postplume chemistry of the collision of comet Shoemaker-Levy 9 with Jupiter.

Nuclear conversion theory: molecular hydrogen in non-magnetic insulators

NASA Astrophysics Data System (ADS)

Ilisca, Ernest; Ghiglieno, Filippo

2016-09-01

The hydrogen conversion patterns on non-magnetic solids sensitively depend upon the degree of singlet/triplet mixing in the intermediates of the catalytic reaction. Three main `symmetry-breaking' interactions are brought together. In a typical channel, the electron spin-orbit (SO) couplings introduce some magnetic excitations in the non-magnetic solid ground state. The electron spin is exchanged with a molecular one by the electric molecule-solid electron repulsion, mixing the bonding and antibonding states and affecting the molecule rotation. Finally, the magnetic hyperfine contact transfers the electron spin angular momentum to the nuclei. Two families of channels are considered and a simple criterion based on the SO coupling strength is proposed to select the most efficient one. The denoted `electronic' conversion path involves an emission of excitons that propagate and disintegrate in the bulk. In the other denoted `nuclear', the excited electron states are transients of a loop, and the electron system returns to its fundamental ground state. The described model enlarges previous studies by extending the electron basis to charge-transfer states and `continui' of band states, and focuses on the broadening of the antibonding molecular excited state by the solid conduction band that provides efficient tunnelling paths for the hydrogen conversion. After working out the general conversion algebra, the conversion rates of hydrogen on insulating and semiconductor solids are related to a few molecule-solid parameters (gap width, ionization and affinity potentials) and compared with experimental measures.

Stern-Gerlach-like approach to electron orbital angular momentum measurement

DOE PAGES

Harvey, Tyler R.; Grillo, Vincenzo; McMorran, Benjamin J.

2017-02-28

Many methods now exist to prepare free electrons into orbital-angular-momentum states, and the predicted applications of these electron states as probes of materials and scattering processes are numerous. The development of electron orbital-angular-momentum measurement techniques has lagged behind. We show that coupling between electron orbital angular momentum and a spatially varying magnetic field produces an angular-momentum-dependent focusing effect. We propose a design for an orbital-angular-momentum measurement device built on this principle. As the method of measurement is noninterferometric, the device works equally well for mixed, superposed, and pure final orbital-angular-momentum states. The energy and orbital-angular-momentum distributions of inelastically scattered electronsmore » may be simultaneously measurable with this technique.« less

Stern-Gerlach-like approach to electron orbital angular momentum measurement

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

Harvey, Tyler R.; Grillo, Vincenzo; McMorran, Benjamin J.

Many methods now exist to prepare free electrons into orbital-angular-momentum states, and the predicted applications of these electron states as probes of materials and scattering processes are numerous. The development of electron orbital-angular-momentum measurement techniques has lagged behind. We show that coupling between electron orbital angular momentum and a spatially varying magnetic field produces an angular-momentum-dependent focusing effect. We propose a design for an orbital-angular-momentum measurement device built on this principle. As the method of measurement is noninterferometric, the device works equally well for mixed, superposed, and pure final orbital-angular-momentum states. The energy and orbital-angular-momentum distributions of inelastically scattered electronsmore » may be simultaneously measurable with this technique.« less

Linear and angular control of circular walking in healthy older adults and subjects with cerebellar ataxia.

PubMed

Goodworth, Adam D; Paquette, Caroline; Jones, Geoffrey Melvill; Block, Edward W; Fletcher, William A; Hu, Bin; Horak, Fay B

2012-05-01

Linear and angular control of trunk and leg motion during curvilinear navigation was investigated in subjects with cerebellar ataxia and age-matched control subjects. Subjects walked with eyes open around a 1.2-m circle. The relationship of linear to angular motion was quantified by determining the ratios of trunk linear velocity to trunk angular velocity and foot linear position to foot angular position. Errors in walking radius (the ratio of linear to angular motion) also were quantified continuously during the circular walk. Relative variability of linear and angular measures was compared using coefficients of variation (CoV). Patterns of variability were compared using power spectral analysis for the trunk and auto-covariance analysis for the feet. Errors in radius were significantly increased in patients with cerebellar damage as compared to controls. Cerebellar subjects had significantly larger CoV of feet and trunk in angular, but not linear, motion. Control subjects also showed larger CoV in angular compared to linear motion of the feet and trunk. Angular and linear components of stepping differed in that angular, but not linear, foot placement had a negative correlation from one stride to the next. Thus, walking in a circle was associated with more, and a different type of, variability in angular compared to linear motion. Results are consistent with increased difficulty of, and role of the cerebellum in, control of angular trunk and foot motion for curvilinear locomotion.

Cortical fibers orientation mapping using in-vivo whole brain 7 T diffusion MRI.

PubMed

Gulban, Omer F; De Martino, Federico; Vu, An T; Yacoub, Essa; Uğurbil, Kamil; Lenglet, Christophe

2018-05-10

Diffusion MRI of the cortical gray matter is challenging because the micro-environment probed by water molecules is much more complex than within the white matter. High spatial and angular resolutions are therefore necessary to uncover anisotropic diffusion patterns and laminar structures, which provide complementary (e.g. to anatomical and functional MRI) microstructural information about the cortex architectonic. Several ex-vivo and in-vivo MRI studies have recently addressed this question, however predominantly with an emphasis on specific cortical areas. There is currently no whole brain in-vivo data leveraging multi-shell diffusion MRI acquisition at high spatial resolution, and depth dependent analysis, to characterize the complex organization of cortical fibers. Here, we present unique in-vivo human 7T diffusion MRI data, and a dedicated cortical depth dependent analysis pipeline. We leverage the high spatial (1.05 mm isotropic) and angular (198 diffusion gradient directions) resolution of this whole brain dataset to improve cortical fiber orientations mapping, and study neurites (axons and/or dendrites) trajectories across cortical depths. Tangential fibers in superficial cortical depths and crossing fiber configurations in deep cortical depths are identified. Fibers gradually inserting into the gyral walls are visualized, which contributes to mitigating the gyral bias effect. Quantitative radiality maps and histograms in individual subjects and cortex-based aligned datasets further support our results. Copyright © 2018 Elsevier Inc. All rights reserved.

Submillimeter Spectroscopy of the Out-Of Bending State ν_{20} of C_2H_5CN

NASA Astrophysics Data System (ADS)

Pearson, John C.; Brauer, Carolyn S.; Yu, Shanshan; Drouin, Brian J.

2009-06-01

Propionitrile is a well known interstellar molecule that is a closely associated with warm dust near ultra compact H_{II} regions. In these regions the C_2H_5CN column can reach 10^{17} and the rotational temperature often equals the vibrational temperature and exceeds 200 K, populating all the low-lying vibrational states. The rotational spectrum of the third lowest excited vibrational state, the 378 cm^{-1} out-of-plane bending state, ν_{20}, of propionitrile, which was previously identified at millimeter wavelengths in both the laboratory and the interstellar medium, has been characterized to high angular momentum quantum numbers. This state is surprisingly isolated considering its proximity to the overtone of the in-plane bend, 2ν_{13}, the excited torsional state of the in-plane bend, ν_{13}+ν_{21}, and the second excited torsional state, 2ν_{21}, which lie approximately 35 cm^{-1} higher. The only surprising aspect is the presence of significantly larger torsional A-E splitting than observed in either the ground state or the ν_{13} in the absence of a resonance with ν_{21}. Because ν_{20} has been observed in high mass star forming cores in the millimeter, its higher angular momentum lines are known to be a major source of line confusion in high mass star forming cores. The spectrum, constants and determined barriers will be presented.

Imaging electronic motions by ultrafast electron diffraction

NASA Astrophysics Data System (ADS)

Shao, Hua-Chieh; Starace, Anthony F.

2017-08-01

Recently ultrafast electron diffraction and microscopy have reached unprecedented temporal resolution, and transient structures with atomic precision have been observed in various reactions. It is anticipated that these extraordinary advances will soon allow direct observation of electronic motions during chemical reactions. We therefore performed a series of theoretical investigations and simulations to investigate the imaging of electronic motions in atoms and molecules by ultrafast electron diffraction. Three prototypical electronic motions were considered for hydrogen atoms. For the case of a breathing mode, the electron density expands and contracts periodically, and we show that the time-resolved scattering intensities reflect such changes of the charge radius. For the case of a wiggling mode, the electron oscillates from one side of the nucleus to the other, and we show that the diffraction images exhibit asymmetric angular distributions. The last case is a hybrid mode that involves both breathing and wiggling motions. Owing to the demonstrated ability of ultrafast electrons to image these motions, we have proposed to image a coherent population transfer in lithium atoms using currently available femtosecond electron pulses. A frequency-swept laser pulse adiabatically drives the valence electron of a lithium atom from the 2s to 2p orbitals, and a time-delayed electron pulse maps such motion. Our simulations show that the diffraction images reflect this motion both in the scattering intensities and the angular distributions.

New vibration-rotation code for tetraatomic molecules exhibiting wide-amplitude motion: WAVR4

NASA Astrophysics Data System (ADS)

Kozin, Igor N.; Law, Mark M.; Tennyson, Jonathan; Hutson, Jeremy M.

2004-11-01

A general computational method for the accurate calculation of rotationally and vibrationally excited states of tetraatomic molecules is developed. The resulting program is particularly appropriate for molecules executing wide-amplitude motions and isomerizations. The program offers a choice of coordinate systems based on Radau, Jacobi, diatom-diatom and orthogonal satellite vectors. The method includes all six vibrational dimensions plus three rotational dimensions. Vibration-rotation calculations with reduced dimensionality in the radial degrees of freedom are easily tackled via constraints imposed on the radial coordinates via the input file. Program summaryTitle of program: WAVR4 Catalogue number: ADUN Program summary URL:http://cpc.cs.qub.ac.uk/summaries/ADUN Program obtainable from: CPC Program Library, Queen's University of Belfast, N. Ireland Licensing provisions: Persons requesting the program must sign the standard CPC nonprofit use license Computer: Developed under Tru64 UNIX, ported to Microsoft Windows and Sun Unix Operating systems under which the program has been tested: Tru64 Unix, Microsoft Windows, Sun Unix Programming language used: Fortran 90 Memory required to execute with typical data: case dependent No. of lines in distributed program, including test data, etc.: 11 937 No. of bytes in distributed program, including test data, etc.: 84 770 Distribution format: tar.gz Nature of physical problem: WAVR4 calculates the bound ro-vibrational levels and wavefunctions of a tetraatomic system using body-fixed coordinates based on generalised orthogonal vectors. Method of solution: The angular coordinates are treated using a finite basis representation (FBR) based on products of spherical harmonics. A discrete variable representation (DVR) [1] based on either Morse-oscillator-like or spherical-oscillator functions [2] is used for the radial coordinates. Matrix elements are computed using an efficient Gaussian quadrature in the angular coordinates and the DVR approximation in the radial coordinates. The solution of the secular problem is carried through a series of intermediate diagonalisations and truncations. Restrictions on the complexity of the problem: (1) The size of the final Hamiltonian matrix that can be practically diagonalised; (2) The DVR approximation for a radial coordinate fails for values of the coordinate near zero—this is remedied only for one radial coordinate by using analytical integration. Typical running time: problem-dependent Unusual features of the program: A user-supplied subroutine to evaluate the potential energy is a program requirement. External routines: BLAS and LAPACK are required. References: [1] J.C. Light, I.P. Hamilton, J.V. Lill, J. Chem. Phys. 92 (1985) 1400. [2] J.R. Henderson, C.R. Le Sueur, J. Tennyson, Comp. Phys. Comm. 75 (1993) 379.

Airborne Laser Polar Nephelometer

NASA Technical Reports Server (NTRS)

Grams, Gerald W.

1973-01-01

A polar nephelometer has been developed at NCAR to measure the angular variation of the intensity of light scattered by air molecules and particles. The system has been designed for airborne measurements using outside air ducted through a 5-cm diameter airflow tube; the sample volume is that which is common to the intersection of a collimated source beam and the detector field of view within the airflow tube. The source is a linearly polarized helium-neon laser beam. The optical system defines a collimated field-of-view (0.5deg half-angle) through a series of diaphragms located behind a I72-mm focal length objective lens. A photomultiplier tube is located immediately behind an aperture in the focal plane of the objective lens. The laser beam is mechanically chopped (on-off) at a rate of 5 Hz; a two-channel pulse counter, synchronized to the laser output, measures the photomultiplier pulse rate with the light beam both on and off. The difference in these measured pulse rates is directly proportional to the intensity of the scattered light from the volume common to the intersection of the laser beam and the detector field-of-view. Measurements can be made at scattering angles from 15deg to 165deg with reference to the direction of propagation of the light beam. Intermediate angles are obtained by selecting the angular increments desired between these extreme angles (any multiple of 0.1deg can be selected for the angular increment; 5deg is used in normal operation). Pulses provided by digital circuits control a stepping motor which sequentially rotates the detector by pre-selected angular increments. The synchronous photon-counting system automatically begins measurement of the scattered-light intensity immediately after the rotation to a new angle has been completed. The instrument has been flown on the NASA Convair 990 airborne laboratory to obtain data on the complex index of refraction of atmospheric aerosols. A particle impaction device is operated simultaneously to collect particles from the same airflow tube used to make the scattered-light measurements. A size distribution function is obtained by analysis of the particles collected by the impaction device. Calculated values of the angular variation of the scattered-light intensity are obtained by applying Mie scattering theory to the observed size distribution function and assuming different values of the complex index of refraction of the particles. The calculated values are then compared with data on the actual variation of the scattered-light intensity obtained with the polar nephelometer. The most probable value of the complex refractive index is that which provides the best fit between the experimental light scattering data and the parameters calculated from the observed size distribution function.

Variable Mixed Orbital Character in the Photoelectron Angular Distribution of NO_{2}

NASA Astrophysics Data System (ADS)

Laws, Benjamin A.; Cavanagh, Steven J.; Lewis, Brenton R.; Gibson, Stephen T.

2017-06-01

NO_{2} a key component of photochemical smog and an important species in the Earth's atmosphere, is an example of a molecule which exhibits significant mixed orbital character in the HOMO. In photoelectron experiments the geometric properties of the parent anion orbital are reflected in the photoelectron angular distribution (PAD), an area of research that has benefited largely from the ability of velocity-map imaging (VMI) to simultaneously record both the energetic and angular information, with 100% collection efficiency. Photoelectron spectra of NO_{2}^{-}, taken over a range of wavelengths (355nm-520nm) with the ANU's VMI spectrometer, reveal an anomalous jump in the anisotropy parameter near threshold. Consequently, the orbital behavior of NO_{2}^{-} appears to be quite different near threshold compared to detachment at higher photon energies. This surprising effect is due to the Wigner Threshold law, which causes p orbital character to dominate the photodetachment cross-section near threshold, before the mixed s/d orbital character becomes significant at higher electron kinetic energies. By extending recent work on binary character models to form a more general expression, the variable mixed orbital character of NO_{2}^{-} is able to be described. This study provides the first multi-wavelength NO_{2} anisotropy data, which is shown to be in decent agreement with much earlier zero-core model predictions of the anisotropy parameter. K. J. Reed, A. H. Zimmerman, H. C. Andersen, and J. I. Brauman, J. Chem. Phys. 64, 1368, (1976). doi:10.1063/1.432404 D. Khuseynov, C. C. Blackstone, L. M. Culberson, and A. Sanov, J. Chem. Phys. 141, 124312, (2014). doi:10.1063/1.4896241 W. B. Clodius, R. M. Stehman, and S. B. Woo, Phys. Rev. A. 28, 760, (1983). doi:10.1103/PhysRevA.28.760 Research supported by the Australian Research Council Discovery Project Grant DP160102585

Water reorientation in the hydration shells of hydrophilic and hydrophobic solutes

NASA Astrophysics Data System (ADS)

Laage, Damien; Stirnemann, Guillaume; Hynes, James T.

2010-06-01

We discuss some key aspects of our recent theoretical work on water reorientation dynamics, which is important in a wide range of phenomena, including aqueous phase chemical reactions, protein folding, and drug binding to proteins and DNA. It is shown that, contrary to the standard conception that these dynamics are diffusional, the reorientation of a water molecule occurs by sudden, large amplitude angular jumps. The mechanism involves the exchange of one hydrogen bond for another by the reorienting water, and the process can be fruitfully viewed as a chemical reaction. The results for reorientation times, which can be well described analytically, are discussed in the context of the molecular level interpretation of recent ultrafast infrared spectroscopic results, focusing on the concepts of structure making/breaking and solvent ‘icebergs’.

Multisite Interactions in Lattice-Gas Models

NASA Astrophysics Data System (ADS)

Einstein, T. L.; Sathiyanarayanan, R.

For detailed applications of lattice-gas models to surface systems, multisite interactions often play at least as significant a role as interactions between pairs of adatoms that are separated by a few lattice spacings. We recall that trio (3-adatom, non-pairwise) interactions do not inevitably create phase boundary asymmetries about half coverage. We discuss a sophisticated application to an experimental system and describe refinements in extracting lattice-gas energies from calculations of total energies of several different ordered overlayers. We describe how lateral relaxations complicate matters when there is direct interaction between the adatoms, an issue that is important when examining the angular dependence of step line tensions. We discuss the connector model as an alternative viewpoint and close with a brief account of recent work on organic molecule overlayers.

ISS and TPD study of the adsorption and interaction of CO and H2 on polycrystalline Pt

NASA Technical Reports Server (NTRS)

Melendez, Orlando; Hoflund, Gar B.; Schryer, David R.

1990-01-01

The adsorption and interaction of CO and H2 on polycrystalline Pt has been studied using ion scattering spectroscopy (ISS) and temperature programmed desorption (TPD). The ISS results indicate that the initial CO adsorption on Pt takes place very rapidly and saturates the Pt surface with coverage close to a monolayer. ISS also shows that the CO molecules adsorb at an angular orientation from the surface normal and perhaps parallel to the surface. A TPD spectrum obtained after coadsorbing C-12 O-16 and C-13 O-18 on Pt shows no isotopic mixing, which is indicative of molecular CO adsorption. TPD spectra obtained after coadsorbing H2 and CO on polycrystalline Pt provides evidence for the formation of a CO-H surface species.

Numerical Simulation of Rarefied Plume Flow Exhausting from a Small Nozzle

NASA Astrophysics Data System (ADS)

Hyakutake, Toru; Yamamoto, Kyoji

2003-05-01

This paper describes the numerical studies of a rarefied plume flow expanding through a nozzle into a vacuum, especially focusing on investigating the nozzle performance, the angular distributions of molecular flux in the nozzle plume and the influence of the backflow contamination for the variation of nozzle geometries and gas/surface interaction models. The direct simulation Monte Carlo (DSMC) method is employed for determining inside the nozzle and in the nozzle plume. The simulation results indicate that the half-angle of the diverging section in the highest thrust coefficient is 25° - 30° and this value varies with the expansion ratio of the nozzle. The descent of the half-angle brings about the increase of the molecules that are scattered in the backflow region.

Dynamic resonances in the reaction of fluorine atoms with hydrogen molecules

NASA Astrophysics Data System (ADS)

Neumark, D. M.; Wodtke, A. M.; Robinson, G. N.; Hayden, C. C.; Lee, Y. T.

1984-05-01

The reactions of F + H2, HD and D2 were studied in high resolution crossed molecular beams experiments. Center of mass translational energy and angular distributions were determined for each product vibrational state. In the F + H2 reaction, the v = 3 product showed intense forward scattering while the v = 2 product was backward peaked. The results suggest that dynamical resonances play an important role in the reaction dynamics of this system. In the F + HD reaction, the strong forward scattering of HF products and backward scattering of DF products is in agreement with the prediction of a stronger resonance effect for HF formation. The effect of the H2 rotational excitation and the reactivity of F((2)P/sub 1/2/) are also discussed.

Whole-body angular momentum during stair ascent and descent.

PubMed

Silverman, Anne K; Neptune, Richard R; Sinitski, Emily H; Wilken, Jason M

2014-04-01

The generation of whole-body angular momentum is essential in many locomotor tasks and must be regulated in order to maintain dynamic balance. However, angular momentum has not been investigated during stair walking, which is an activity that presents a biomechanical challenge for balance-impaired populations. We investigated three-dimensional whole-body angular momentum during stair ascent and descent and compared it to level walking. Three-dimensional body-segment kinematic and ground reaction force (GRF) data were collected from 30 healthy subjects. Angular momentum was calculated using a 13-segment whole-body model. GRFs, external moment arms and net joint moments were used to interpret the angular momentum results. The range of frontal plane angular momentum was greater for stair ascent relative to level walking. In the transverse and sagittal planes, the range of angular momentum was smaller in stair ascent and descent relative to level walking. Significant differences were also found in the ground reaction forces, external moment arms and net joint moments. The sagittal plane angular momentum results suggest that individuals alter angular momentum to effectively counteract potential trips during stair ascent, and reduce the range of angular momentum to avoid falling forward during stair descent. Further, significant differences in joint moments suggest potential neuromuscular mechanisms that account for the differences in angular momentum between walking conditions. These results provide a baseline for comparison to impaired populations that have difficulty maintaining dynamic balance, particularly during stair ascent and descent. Copyright © 2014 Elsevier B.V. All rights reserved.

A proposed measurement of optical orbital and spin angular momentum and its implications for photon angular momentum

NASA Astrophysics Data System (ADS)

Leader, Elliot

2018-04-01

The expression for the total angular momentum carried by a laser optical vortex beam, splits, in the paraxial approximation, into two terms which seem to represent orbital and spin angular momentum respectively. There are, however, two very different competing versions of the formula for the spin angular momentum, one based on the use of the Poynting vector, as in classical electrodynamics, the other related to the canonical expression for the angular momentum which occurs in Quantum Electrodynamics. I analyze the possibility that a sufficiently sensitive optical measurement could decide which of these corresponds to the actual physical angular momentum carried by the beam.

A Computational Technique to Determine the Angular Displacement, Velocity and Momentum of a Human Body.

ERIC Educational Resources Information Center

Hay, James G.; Wilson, Barry D.

The angular momentum of a human body derived from both the angular velocity and angular displacement, utilizing cinematographic records has not been adequately assessed, prior to this study. Miller (1970) obtained the angular momentum but only during the airborne phase of activity. The method used by Ramey (1973) involved a force platform, but…

Difference in perception of angular displacement according to applied waveforms.

PubMed

Kushiro, Keisuke; Goto, Fumiyuki

2013-05-01

This study shows that the differences in the waveforms of angular rotation affect the perception and memory of angular displacement. During daily life, when we turn our head during various activities, our brain calculates how much angular displacement our head has undergone. However, how we obtain an accurate estimation of this angular displacement remains unclarified. This study aims to clarify this issue by investigating the perception and memory of passive rotation for three different waveforms of angular velocity rotation (sinusoidal (sine), triangle, and step). Thirteen healthy young subjects sitting on a servo-controlled chair were passively rotated at 60° or 120° about the earth-vertical axis by using one of these three angular velocity waveforms. They then attempted to reproduce the rotation angle by rotating the chair in the same direction in which they had been passively rotated using a handheld controller. The gain (reproduced angle/passively rotated angle) was calculated and used for the evaluation of the perception and memory of angular rotation. The gain for step rotation was larger than that for sine and triangle rotations, with statistical significance. This confirms that the difference in the waveforms of angular rotation affects the perception and memory of angular displacement.

CONNECTING ANGULAR MOMENTUM AND GALACTIC DYNAMICS: THE COMPLEX INTERPLAY BETWEEN SPIN, MASS, AND MORPHOLOGY

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

Teklu, Adelheid F.; Remus, Rhea-Silvia; Dolag, Klaus

The evolution and distribution of the angular momentum of dark matter (DM) halos have been discussed in several studies over the past decades. In particular, the idea arose that angular momentum conservation should allow us to infer the total angular momentum of the entire DM halo from measuring the angular momentum of the baryonic component, which is populating the center of the halo, especially for disk galaxies. To test this idea and to understand the connection between the angular momentum of the DM halo and its galaxy, we use a state-of-the-art, hydrodynamical cosmological simulation taken from the set of Magneticummore » Pathfinder simulations. Thanks to the inclusion of the relevant physical processes, the improved underlying numerical methods, and high spatial resolution, we successfully produce populations of spheroidal and disk galaxies self-consistently. Thus, we are able to study the dependence of galactic properties on their morphology. We find that (1) the specific angular momentum of stars in disk and spheroidal galaxies as a function of their stellar mass compares well with observational results; (2) the specific angular momentum of the stars in disk galaxies is slightly smaller compared to the specific angular momentum of the cold gas, in good agreement with observations; (3) simulations including the baryonic component show a dichotomy in the specific stellar angular momentum distribution when splitting the galaxies according to their morphological type (this dichotomy can also be seen in the spin parameter, where disk galaxies populate halos with slightly larger spin compared to spheroidal galaxies); (4) disk galaxies preferentially populate halos in which the angular momentum vector of the DM component in the central part shows a better alignment to the angular momentum vector of the entire halo; and (5) the specific angular momentum of the cold gas in disk galaxies is approximately 40% smaller than the specific angular momentum of the total DM halo and shows a significant scatter.« less

Optical angular momentum and atoms

PubMed Central

2017-01-01

Any coherent interaction of light and atoms needs to conserve energy, linear momentum and angular momentum. What happens to an atom’s angular momentum if it encounters light that carries orbital angular momentum (OAM)? This is a particularly intriguing question as the angular momentum of atoms is quantized, incorporating the intrinsic spin angular momentum of the individual electrons as well as the OAM associated with their spatial distribution. In addition, a mechanical angular momentum can arise from the rotation of the entire atom, which for very cold atoms is also quantized. Atoms therefore allow us to probe and access the quantum properties of light’s OAM, aiding our fundamental understanding of light–matter interactions, and moreover, allowing us to construct OAM-based applications, including quantum memories, frequency converters for shaped light and OAM-based sensors. This article is part of the themed issue ‘Optical orbital angular momentum’. PMID:28069766

Vibration signal correction of unbalanced rotor due to angular speed fluctuation

NASA Astrophysics Data System (ADS)

Cao, Hongrui; He, Dong; Xi, Songtao; Chen, Xuefeng

2018-07-01

The rotating speed of a rotor is hardly constant in practice due to angular speed fluctuation, which affects the balancing accuracy of the rotor. In this paper, the effect of angular speed fluctuation on vibration responses of the unbalanced rotor is analyzed quantitatively. Then, a vibration signal correction method based on zoom synchrosqueezing transform (ZST) and tacholess order tracking is proposed. The instantaneous angular speed (IAS) of the rotor is extracted by the ZST firstly and then used to calculate the instantaneous phase. The vibration signal is further resampled in angular domain to reduce the effect of angular speed fluctuation. The signal obtained in angular domain is transformed into order domain using discrete Fourier transform (DFT) to estimate the amplitude and phase of the vibration signal. Simulated and experimental results show that the proposed method can successfully correct the amplitude and phase of the vibration signal due to angular speed fluctuation.

Quantum treatment of the capture of an atom by a fast nucleus incident on a molecule

NASA Astrophysics Data System (ADS)

Shakeshaft, Robin; Spruch, Larry

1980-04-01

The classical double-scattering model of Thomas for the capture of electrons from atoms by fast ions yields a cross section σ which dominates over the single scattering contribution for sufficiently fast ions. The magnitude of the classical double-scattering σ differs, however, from its quantum-mechanical (second-Born) analog by an order of magnitude. Further, a "fast ion" means an ion of some MeV, and at those energies the cross sections are very low. On the other hand, as noted by Bates, Cook, and Smith, the double-scattering cross section for the capture of atoms from molecules by fast ions dominates over the single-scattering contribution for incident ions of very much lower energy; roughly, one must have the velocity of the incident projectile much larger than a characteristic internal velocity of the particles in the target. It follows that we are in the asymptotic domain not at about 10 MeV but at about 100 eV. For the reaction H+ + CH4-->H+2 + CH3 with incident proton energies of 70 to 150 eV, the peak in the angular distribution as determined experimentally is at almost precisely the value predicted by the classical model, but the theoretical total cross section is about 30 times too large. Using a quantum version of the classical model, which involves the same kinematics and therefore preserves the agreement with the angular distribution, we obtain somewhat better agreement with the experimental total cross section, by a factor of about 5. (To obtain very good agreement, one may have to perform a really accurate calculation of large-angle elastic scattering of protons and H atoms by CH3, and take into account interference effects.) In the center-of-mass frame, for sufficiently high incident energy, the first of the two scatterings involves the scattering of H+ by H through an angle of very close to 90°, and it follows that the nuclei of the emergent H+2 ion will almost all be in the singlet state. We have also calculated the cross section for the reaction D+ + CH4-->(HD)+ + CH3.

Polarization Catastrophe Contributing to Rotation and Tornadic Motion in Cumulo-Nimbus Clouds

NASA Astrophysics Data System (ADS)

Handel, P. H.

2007-05-01

When the concentration of sub-micron ice particles in a cloud exceeds 2.5E21 per cubic cm, divided by the squared average number of water molecules per crystallite, the polarization catastrophe occurs. Then all ice crystallites nucleated on aerosol dust particles align their dipole moments in the same direction, and a large polarization vector field is generated in the cloud. Often this vector field has a radial component directed away from the vertical axis of the cloud. It is induced by the pre-existing electric field caused by the charged screening layers at the cloud surface, the screening shell of the cloud. The presence of a vertical component of the magnetic field of the earth creates a density of linear momentum G=DxB in the azimuthal direction, where D=eE+P is the electric displacement vector and e is the vacuum permittivity. This linear momentum density yields an angular momentum density vector directed upward in the nordic hemisphere, if the polarization vector points away from the vertical axis of the cloud. When the cloud becomes colloidally unstable, the crystallites grow beyond the size limit at which they still could carry a large ferroelectric saturation dipole moment, and the polarization vector quickly disappears. Then the cloud begins to rotate with an angular momentum that has the same direction. Due to the large average number of water molecules in a crystallite, the polarization catastrophe (PC) is present in practically all clouds, and is compensated by masking charges. In cumulo-nimbus (thunder-) clouds the collapse of the PC is rapid, and the masking charges lead to lightning, and in the upper atmosphere also to sprites, elves, and blue jets. In stratus clouds, however, the collapse is slow, and only leads to reverse polarity in dissipating clouds (minus on the bottom), as compared with growing clouds (plus on the bottom, because of the excess polarization charge). References: P.H. Handel: "Polarization Catastrophe Theory of Cloud Electricity", J. Geophysical Research 90, 5857-5863 (1985). P.H. Handel and P.B. James: "Polarization Catastrophe Model of Static Electrification and Spokes in the B-Ring of Saturn", Geophys. Res. Lett. 10, 1-4 (1983).

Angular-Rate Estimation Using Quaternion Measurements

NASA Technical Reports Server (NTRS)

Azor, Ruth; Bar-Itzhack, Y.; Deutschmann, Julie K.; Harman, Richard R.

1998-01-01

In most spacecraft (SC) there is a need to know the SC angular rate. Precise angular rate is required for attitude determination, and a coarse rate is needed for attitude control damping. Classically, angular rate information is obtained from gyro measurements. These days, there is a tendency to build smaller, lighter and cheaper SC, therefore the inclination now is to do away with gyros and use other means and methods to determine the angular rate. The latter is also needed even in gyro equipped satellites when performing high rate maneuvers whose angular-rate is out of range of the on board gyros or in case of gyro failure. There are several ways to obtain the angular rate in a gyro-less SC. When the attitude is known, one can differentiate the attitude in whatever parameters it is given and use the kinematics equation that connects the derivative of the attitude with the satellite angular-rate and compute the latter. Since SC usually utilize vector measurements for attitude determination, the differentiation of the attitude introduces a considerable noise component in the computed angular-rate vector.

The clinical features of angular cheilitis occurring during orthodontic treatment: a multi-centre observational study.

PubMed

Cross, David; Eide, May L; Kotinas, Anastasios

2010-06-01

To report the prevalence and clinical features of angular cheilitis occurring in patients undergoing orthodontic treatment. Cross-sectional, observational study. Three centres were involved; Glasgow Dental Hospital and two specialist orthodontic practices, one in Scotland and one in Greece. Six hundred and sixty consecutive patients undergoing orthodontic treatment were examined over a 9 month period. The presence and absence of angular cheilitis was recorded. A six-point clinical scale was used to describe the clinical features of angular cheilitis when present. Chi-squared tests were used to investigate the association between the presence of angular cheilitis and oral hygiene level/appliance type. Eleven per cent of orthodontic patients in this Western European population, showed signs of angular cheilitis. No correlation was found between the presence of angular cheilitis and gender. Good oral hygiene was associated with a reduced prevalence (P<0.01). Angular cheilitis is a multifactorial condition that can occur in a small percentage of patients during orthodontic treatment. Good oral hygiene may be associated with a reduced risk. A new clinical grade of angular cheilitis is suggested that may help future research. Further studies are required to investigate the microbiological features associated with angular cheilitis occurring in orthodontic patients, as well as associations with medical conditions, such as asthma.

Polycyclic aromatic hydrocarbons in model bacterial membranes - Langmuir monolayer studies.

PubMed

Broniatowski, Marcin; Binczycka, Martyna; Wójcik, Aneta; Flasiński, Michał; Wydro, Paweł

2017-12-01

High molecular weight polycyclic aromatic hydrocarbons (HMW-PAHs) are persistent organic pollutants which due to their limited biodegradability accumulate in soils where their increased presence can lead to the impoverishment of the decomposer organisms. As very hydrophobic PAHs easily penetrate cellular membranes of soil bacteria and can be incorporated therein, changing the membrane fluidity and other functions which in consequence can lead to the death of the organism. The structure and size of PAH molecule can be crucial for its membrane activity; however the correlation between PAH structure and its interaction with phospholipids have not been investigated so far. In our studies we applied phospholipid Langmuir monolayers as model bacterial membranes and investigated how the incorporation of six structurally different PAH molecules change the membrane texture and physical properties. In our studies we registered surface pressure and surface potential isotherms upon the monolayer compression, visualized the monolayer texture with the application of Brewster angle microscopy and searched the ordering of the film-forming molecules with molecular resolution with the application of grazing incidence X-ray diffraction (GIXD) method. It turned out that the phospholipid-PAH interactions are strictly structure dependent. Four and five-ring PAHs of the angular or cluster geometry can be incorporated into the model membranes changing profoundly their textures and fluidity; whereas linear or large cluster PAHs cannot be incorporated and separate from the lipid matrix. The observed phenomena were explained based on structural similarities of the applied PAHs with membrane steroids and hopanoids. Copyright © 2017. Published by Elsevier B.V.

Protostellar Interferometric Line Survey (PILS): Constraining the formation of complex organic molecules with ALMA

NASA Astrophysics Data System (ADS)

Jorgensen, Jes K.; Coutens, Audrey; Bourke, Tyler L.; Favre, Cecile; Garrod, Robin; Lykke, Julie; Mueller, Holger; Oberg, Karin I.; Schmalzl, Markus; van der Wiel, Matthijs; van Dishoeck, Ewine; Wampfler, Susanne F.

2015-08-01

Understanding how, when and where complex organic and potentially prebiotic molecules are formed is a fundamental goal of astrochemistry and an integral part of origins of life studies. Already now ALMA is showing its capabilities for studies of the chemistry of solar-type stars with its high sensitivity for faint lines, high spectral resolution which limits line confusion, and high angular resolution making it possible to study the structure of young protostars on solar-system scales. We here present the first results from a large unbiased survey “Protostellar Interferometric Line Survey (PILS)” targeting one of the astrochemical template sources, the low-mass protostellar binary IRAS 16293-2422. The survey is more than an order of magnitude more sensitive than previous surveys of the source and provide imaging down to 25 AU scales (radius) around each of the two components of the binary. An example of one of the early highlights from the survey is unambiguous detections of the (related) prebiotic species glycolaldehyde, ethylene glycol (two lowest energy conformers), methyl formate and acetic acid. The glycolaldehyde-ethylene glycol abundance ratio is high in comparison to comets and other protostars - but agrees with previous measurements, e.g., in the Galactic Centre clouds possibly reflecting different environments and/or evolutionary histories. Complete mapping of this and other chemical networks in comparison with detailed chemical models and laboratory experiments will reveal the origin of complex organic molecules in a young protostellar system and investigate the link between these protostellar stages and the early Solar System.

SU-E-T-472: Improvement of IMRT QA Passing Rate by Correcting Angular Dependence of MatriXX

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

Chen, Q; Watkins, W; Kim, T

2015-06-15

Purpose: Multi-channel planar detector arrays utilized for IMRT-QA, such as the MatriXX, exhibit an incident-beam angular dependent response which can Result in false-positive gamma-based QA results, especially for helical tomotherapy plans which encompass the full range of beam angles. Although MatriXX can use with gantry angle sensor to provide automatically angular correction, this sensor does not work with tomotherapy. The purpose of the study is to reduce IMRT-QA false-positives by correcting for the MatriXX angular dependence. Methods: MatriXX angular dependence was characterized by comparing multiple fixed-angle irradiation measurements with corresponding TPS computed doses. For 81 Tomo-helical IMRT-QA measurements, two differentmore » correction schemes were tested: (1) A Monte-Carlo dose engine was used to compute MatriXX signal based on the angular-response curve. The computed signal was then compared with measurement. (2) Uncorrected computed signal was compared with measurements uniformly scaled to account for the average angular dependence. Three scaling factor (+2%, +2.5%, +3%) were tested. Results: The MatriXX response is 8% less than predicted for a PA beam even when the couch is fully accounted for. Without angular correction, only 67% of the cases pass the >90% points γ<1 (3%, 3mm). After full angular correction, 96% of the cases pass the criteria. Of three scaling factors, +2% gave the highest passing rate (89%), which is still less than the full angular correction method. With a stricter γ(2%,3mm) criteria, the full angular correction method was still able to achieve the 90% passing rate while the scaling method only gives 53% passing rate. Conclusion: Correction for the MatriXX angular dependence reduced the false-positives rate of our IMRT-QA process. It is necessary to correct for the angular dependence to achieve the IMRT passing criteria specified in TG129.« less

Factors influencing perceived angular velocity.

PubMed

Kaiser, M K; Calderone, J B

1991-11-01

The assumption that humans are able to perceive and process angular kinematics is critical to many structure-from-motion and optical flow models. The current studies investigate this sensitivity, and examine several factors likely to influence angular velocity perception. In particular, three factors are considered: (1) the extent to which perceived angular velocity is determined by edge transitions of surface elements, (2) the extent to which angular velocity estimates are influenced by instantaneous linear velocities of surface elements, and (3) whether element-velocity effects are related to three-dimensional (3-D) tangential velocities or to two-dimensional (2-D) image velocities. Edge-transition rate biased angular velocity estimates only when edges were highly salient. Element velocities influenced perceived angular velocity; this bias was related to 2-D image velocity rather than 3-D tangential velocity. Despite these biases, however, judgments were most strongly determined by the true angular velocity. Sensitivity to this higher order motion parameter was surprisingly good, for rotations both in depth (y-axis) and parallel to the line of sight (z-axis).

AtlasCBS: a web server to map and explore chemico-biological space

NASA Astrophysics Data System (ADS)

Cortés-Cabrera, Álvaro; Morreale, Antonio; Gago, Federico; Abad-Zapatero, Celerino

2012-09-01

New approaches are needed that can help decrease the unsustainable failure in small-molecule drug discovery. Ligand Efficiency Indices (LEI) are making a great impact on early-stage compound selection and prioritization. Given a target-ligand database with chemical structures and associated biological affinities/activities for a target, the AtlasCBS server generates two-dimensional, dynamical representations of its contents in terms of LEI. These variables allow an effective decoupling of the chemical (angular) and biological (radial) components. BindingDB, PDBBind and ChEMBL databases are currently implemented. Proprietary datasets can also be uploaded and compared. The utility of this atlas-like representation in the future of drug design is highlighted with some examples. The web server can be accessed at http://ub.cbm.uam.es/atlascbs and https://www.ebi.ac.uk/chembl/atlascbs.

Internal Energy Dependence of Molecular Condensation Coefficients Determined from Molecular Beam Surface Scattering Experiments

DOE R&D Accomplishments Database

Sibener, S. J.; Lee, Y. T.

1978-05-01

An experiment was performed which confirms the existence of an internal mode dependence of molecular sticking probabilities for collisions of molecules with a cold surface. The scattering of a velocity selected effusive beam of CCl{sub 4} from a 90 K CC1{sub 4} ice surface has been studied at five translational velocities and for two different internal temperatures. At a surface temperature of 90 K (approx. 99% sticking probability) a four fold increase in reflected intensity was observed for the internally excited (560 K) CC1{sub 4} relative to the room temperature (298 K) CC1{sub 4} at a translational velocity of 2.5 X 10{sup 4} cm/sec. For a surface temperature of 90 K all angular distributions were found to peak 15{sup 0} superspecularly independent of incident velocity.

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

Electron scattering by highly polar molecules. II - LiF

NASA Technical Reports Server (NTRS)

Vuskovic, L.; Srivastavas, S. K.; Trajmar, S.

1978-01-01

The crossed electron-beam - molecular-beam scattering technique has been used to measure relative values of differential 'elastic' scattering cross sections at electron impact energies of 5.4 and 20 eV for the angular range from 20 to 130 deg. The absolute values of these cross sections have been obtained by normalization to the classical perturbation theory of Dickinson (1977) at a scattering angle of 40 deg. These differential cross sections have then been used to calculate the integral and momentum-transfer cross sections. An energy-loss spectrum at 100 eV electron impact energy and 15 deg scattering angle has also been obtained. Two weak features at the energy losses of 6.74 and 8.82 eV appear. Their energy positions are compared with the recent calculations of Kahn et al. (1974).

Single molecule fate of HIV-1 envelope reveals late-stage viral lattice incorporation.

PubMed

Buttler, Carmen A; Pezeshkian, Nairi; Fernandez, Melissa V; Aaron, Jesse; Norman, Sofya; Freed, Eric O; van Engelenburg, Schuyler B

2018-05-10

Human immunodeficiency virus type 1 (HIV-1) assembly occurs on the inner leaflet of the host cell plasma membrane, incorporating the essential viral envelope glycoprotein (Env) within a budding lattice of HIV-1 Gag structural proteins. The mechanism by which Env incorporates into viral particles remains poorly understood. To determine the mechanism of recruitment of Env to assembly sites, we interrogate the subviral angular distribution of Env on cell-associated virus using multicolor, three-dimensional (3D) superresolution microscopy. We demonstrate that, in a manner dependent on cell type and on the long cytoplasmic tail of Env, the distribution of Env is biased toward the necks of cell-associated particles. We postulate that this neck-biased distribution is regulated by vesicular retention and steric complementarity of Env during independent Gag lattice formation.

Single-photon Coulomb explosion of methanol using broad bandwidth ultrafast EUV pulses.

PubMed

Luzon, Itamar; Jagtap, Krishna; Livshits, Ester; Lioubashevski, Oleg; Baer, Roi; Strasser, Daniel

2017-05-31

Single-photon Coulomb explosion of methanol is instigated using the broad bandwidth pulse achieved through high-order harmonics generation. Using 3D coincidence fragment imaging of one molecule at a time, the kinetic energy release (KER) and angular distributions of the products are measured in different Coulomb explosion (CE) channels. Two-body CE channels breaking either the C-O or the C-H bonds are described as well as a proton migration channel forming H 2 O + , which is shown to exhibit higher KER. The results are compared to intense-field Coulomb explosion measurements in the literature. The interpretation of broad bandwidth single-photon CE data is discussed and supported by ab initio calculations of the predominant C-O bond breaking CE channel. We discuss the importance of these findings for achieving time resolved imaging of ultrafast dynamics.

Steric-electronic effects in malarial peptides inducing sterile immunity

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

Moreno-Vranich, Armando; Patarroyo, Manuel E., E-mail: mepatarr@mail.com; Universidad Nacional de Colombia, Bogota

Highlights: Black-Right-Pointing-Pointer Is it evident that the residues position are relevant regarding of {phi} angular value. Black-Right-Pointing-Pointer The geometry considered for detailing the alterations undergone by HABPs. Black-Right-Pointing-Pointer The inter planar interactions ruled by clashes between the atoms making them up. -- Abstract: Conserved Plasmodium falciparum high activity binding peptides' (HABPs) most relevant proteins involved in malaria parasite invasion are immunologically silent; critical binding residues must therefore be specifically replaced to render them highly immunogenic and protection-inducing. Such changes have a tremendous impact on these peptides' steric-electronic effects, such as modifications to peptide length peptide bonds and electronic orbitals' disposition,more » to allow a better fit into immune system MHCII molecules and better interaction with the TCR which might account for the final immunological outcome.« less

AtlasCBS: a web server to map and explore chemico-biological space.

PubMed

Cortés-Cabrera, Alvaro; Morreale, Antonio; Gago, Federico; Abad-Zapatero, Celerino

2012-09-01

New approaches are needed that can help decrease the unsustainable failure in small-molecule drug discovery. Ligand Efficiency Indices (LEI) are making a great impact on early-stage compound selection and prioritization. Given a target-ligand database with chemical structures and associated biological affinities/activities for a target, the AtlasCBS server generates two-dimensional, dynamical representations of its contents in terms of LEI. These variables allow an effective decoupling of the chemical (angular) and biological (radial) components. BindingDB, PDBBind and ChEMBL databases are currently implemented. Proprietary datasets can also be uploaded and compared. The utility of this atlas-like representation in the future of drug design is highlighted with some examples. The web server can be accessed at http://ub.cbm.uam.es/atlascbs and https://www.ebi.ac.uk/chembl/atlascbs.

Quadratic Finite Element Method for 1D Deterministic Transport

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

Tolar, Jr., D R; Ferguson, J M

2004-01-06

In the discrete ordinates, or SN, numerical solution of the transport equation, both the spatial ({und r}) and angular ({und {Omega}}) dependences on the angular flux {psi}{und r},{und {Omega}}are modeled discretely. While significant effort has been devoted toward improving the spatial discretization of the angular flux, we focus on improving the angular discretization of {psi}{und r},{und {Omega}}. Specifically, we employ a Petrov-Galerkin quadratic finite element approximation for the differencing of the angular variable ({mu}) in developing the one-dimensional (1D) spherical geometry S{sub N} equations. We develop an algorithm that shows faster convergence with angular resolution than conventional S{sub N} algorithms.

Mitigation of radiation-pressure-induced angular instability of a Fabry-Perot cavity consisting of suspended mirrors

NASA Astrophysics Data System (ADS)

Nagano, Koji; Enomoto, Yutaro; Nakano, Masayuki; Furusawa, Akira; Kawamura, Seiji

2016-12-01

To observe radiation pressure noise in optical cavities consisting of suspended mirrors, high laser power is necessary. However, because the radiation pressure on the mirrors could cause an angular anti-spring effect, the high laser power could induce angular instability to the cavity. An angular control system using radiation pressure as an actuator, which was previously invented to reduce the anti-spring effect for the low power case, was applied to the higher power case where the angular instability would occur. As a result the angular instability was mitigated. It was also demonstrated that the cavity was unstable without this control system.

Break-technique handheld dynamometry: relation between angular velocity and strength measurements.

PubMed

Burns, Stephen P; Spanier, David E

2005-07-01

To determine whether the muscle strength, as measured with break-technique handheld dynamometry (HHD), is dependent on the angular velocity achieved during testing and to compare reliability at different angular velocities. Repeated-measures study. Participants underwent HHD by using make-technique (isometric) and break-technique (eccentric) dynamometry at 3 prespecified angular velocities. Elbow movement was recorded with an electrogoniometer. Inpatient spinal cord injury unit. Convenience sample of 20 persons with tetraplegia with weakness of elbow flexors or extensors. Not applicable. Elbow angular velocity and muscle strength recorded during HHD. With the break technique, angular velocities averaging 15 degrees , 33 degrees , and 55 degrees /s produced 16%, 30%, and 51% greater strength measurements, respectively, than velocities recorded by using the make technique (all P < .006 for comparisons between successive techniques). The intraclass correlation coefficient for intrarater reliability was .89 or greater for all testing techniques. Greater strength is recorded with faster angular velocities during HHD. Differences in angular velocity may explain the wide range previously reported for break- versus make-technique strength measurements. Variation in angular velocity is a potential source of variability in serial HHD strength measurements, and for this reason the make technique may be preferable.

Rapidly-Indexing Incremental-Angle Encoder

NASA Technical Reports Server (NTRS)

Christon, Philip R.; Meyer, Wallace W.

1989-01-01

Optoelectronic system measures relative angular position of shaft or other device to be turned, also measures absolute angular position after device turned through small angle. Relative angular position measured with fine resolution by optoelectronically counting finely- and uniformly-spaced light and dark areas on encoder disk as disk turns past position-sensing device. Also includes track containing coarsely- and nonuniformly-spaced light and dark areas, angular widths varying in proportion to absolute angular position. This second track provides gating and indexing signal.

Layered crystal structure, conformational and vibrational properties of 2,2,2-trichloroethoxysulfonamide: An experimental and theoretical study

NASA Astrophysics Data System (ADS)

Gil, Diego M.; Piro, Oscar E.; Echeverría, Gustavo A.; Tuttolomondo, María E.; Altabef, Aída Ben

2013-12-01

The molecular structure of 2,2,2-trichloroethoxysulfonamide, CCl3CH2OSO2NH2, has been determined in the solid state by X-ray diffraction data and in the gas phase by ab initio (MP2) and DFT calculations. The substance crystallizes in the monoclinic P21/c space group with a = 9.969(3) Å, b = 22.914(6) Å, c = 7.349(2) Å, β = 91.06(3)°, and Z = 8 molecules per unit cell. There are two independent, but closely related molecular conformers in the crystal asymmetric unit. They only differ in the angular orientation of the sulfonamide (sbnd SO2NH2) group. The conformers are arranged in the lattice as center-symmetric Nsbnd H⋯O(sulf)-bonded dimers. Neighboring dimers are linked through further Nsbnd H⋯O(sulf) bonds giving rise to a crystal layered structure. The solid state infrared and Raman spectra have been recorded and the observed bands assigned to the molecular vibration modes. Also, the thermal behavior of the substance was investigated by TG-DT analysis. The stability of the molecule arising from hyper-conjugative interactions and charge delocalization has been analyzed using natural bond (NBO) analysis.

Molecular Dynamics Simulation of Carbon Nanotube Based Gears

NASA Technical Reports Server (NTRS)

Han, Jie; Globus, Al; Jaffe, Richard; Deardorff, Glenn; Chancellor, Marisa K. (Technical Monitor)

1996-01-01

We used molecular dynamics to investigate the properties and design space of molecular gears fashioned from carbon nanotubes with teeth added via a benzyne reaction known to occur with C60. A modified, parallelized version of Brenner's potential was used to model interatomic forces within each molecule. A Leonard-Jones 6-12 potential was used for forces between molecules. One gear was powered by forcing the atoms near the end of the buckytube to rotate, and a second gear was allowed.to rotate by keeping the atoms near the end of its buckytube on a cylinder. The meshing aromatic gear teeth transfer angular momentum from the powered gear to the driven gear. A number of gear and gear/shaft configurations were simulated. Cases in vacuum and with an inert atmosphere were examined. In an extension to molecular dynamics technology, some simulations used a thermostat on the atmosphere while the hydrocarbon gear's temperature was allowed to fluctuate. This models cooling the gears with an atmosphere. Results suggest that these gears can operate at up to 50-100 gigahertz in a vacuum or inert atmosphere at room temperature. The failure mode involves tooth slip, not bond breaking, so failed gears can be returned to operation by lowering temperature and/or rotation rate. Videos and atomic trajectory files in xyz format are presented.

High-resolution vacuum-ultraviolet photoabsorption spectra of 1-butyne and 2-butyne

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

Jacovella, U.; Holland, D. M. P.; Boyé-Péronne, S.

2015-07-21

The absolute photoabsorption cross sections of 1- and 2-butyne have been recorded at high resolution by using the vacuum-ultraviolet Fourier-Transform spectrometer at the SOLEIL Synchrotron. Both spectra show more resolved structure than previously observed, especially in the case of 2-butyne. In this work, we assess the potential importance of Rydberg states with higher values of orbital angular momentum, l, than are typically observed in photoabsorption experiments from ground state molecules. We show how the character of the highest occupied molecular orbitals in 1- and 2-butyne suggests the potential importance of transitions to such high-l (l = 3 and 4) Rydbergmore » states. Furthermore, we use theoretical calculations of the partial wave composition of the absorption cross section just above the ionization threshold and the principle of continuity of oscillator strength through an ionization threshold to support this conclusion. The new absolute photoabsorption cross sections are discussed in light of these arguments, and the results are consistent with the expectations. This type of argument should be valuable for assessing the potential importance of different Rydberg series when sufficiently accurate direct quantum chemical calculations are difficult, for example, in the n ≥ 5 manifolds of excited states of larger molecules.« less

Hydrogenic molecular transitions in double concentric quantum donuts by changing geometrical parameters

NASA Astrophysics Data System (ADS)

Ospina-Londoño, D. A.; Fulla, M. R.; Marín, J. H.

2013-03-01

In this work it is considered a versatile model to study two different ionization processes starting from a D20 homonuclear hydrogenic molecule confined in double concentric quantum donuts. Very narrow quantum donut circular cross sections are considered to separate the radial and angular variables in the D20 Hamiltonian by using the well-known adiabatic approximation D20 total energy as a function of the inter donor spacing and the outer donut center line radius is calculated. The salient features of an artificial D20 hydrogenic molecule such as the dissociation energy and the equilibrium length are strongly dependent on the quantum donut geometrical parameters. By increasing systematically the quantum donut outer center line radius, it is possible to understand a first ionization process: D20→D2++e-. A second ionization process D20→D-+D+ can be carried out by fixing the first donor position and gradually moving away the second one. The results obtained in this study are in good agreement with those previously obtained in the limiting cases of very large inter donor separation. The model proposed here is computationally economical and provides a realistic description of both ionization processes and the few-particle system confined in double concentric quantum donuts.

Advanced Structural Analyses by Third Generation Synchrotron Radiation Powder Diffraction

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

Sakata, M.; Aoyagi, S.; Ogura, T.

2007-01-19

Since the advent of the 3rd generation Synchrotron Radiation (SR) sources, such as SPring-8, the capabilities of SR powder diffraction increased greatly not only in an accurate structure refinement but also ab initio structure determination. In this study, advanced structural analyses by 3rd generation SR powder diffraction based on the Large Debye-Scherrer camera installed at BL02B2, SPring-8 is described. Because of high angular resolution and high counting statistics powder data collected at BL02B2, SPring-8, ab initio structure determination can cope with a molecular crystals with 65 atoms including H atoms. For the structure refinements, it is found that a kindmore » of Maximum Entropy Method in which several atoms are omitted in phase calculation become very important to refine structural details of fairy large molecule in a crystal. It should be emphasized that until the unknown structure is refined very precisely, the obtained structure by Genetic Algorithm (GA) or some other ab initio structure determination method using real space structural knowledge, it is not possible to tell whether the structure obtained by the method is correct or not. In order to determine and/or refine crystal structure of rather complicated molecules, we cannot overemphasize the importance of the 3rd generation SR sources.« less

Phase space barriers and dividing surfaces in the absence of critical points of the potential energy: Application to roaming in ozone

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

Mauguière, Frédéric A. L., E-mail: frederic.mauguiere@bristol.ac.uk; Collins, Peter, E-mail: peter.collins@bristol.ac.uk; Wiggins, Stephen, E-mail: stephen.wiggins@mac.com

We examine the phase space structures that govern reaction dynamics in the absence of critical points on the potential energy surface. We show that in the vicinity of hyperbolic invariant tori, it is possible to define phase space dividing surfaces that are analogous to the dividing surfaces governing transition from reactants to products near a critical point of the potential energy surface. We investigate the problem of capture of an atom by a diatomic molecule and show that a normally hyperbolic invariant manifold exists at large atom-diatom distances, away from any critical points on the potential. This normally hyperbolic invariantmore » manifold is the anchor for the construction of a dividing surface in phase space, which defines the outer or loose transition state governing capture dynamics. We present an algorithm for sampling an approximate capture dividing surface, and apply our methods to the recombination of the ozone molecule. We treat both 2 and 3 degrees of freedom models with zero total angular momentum. We have located the normally hyperbolic invariant manifold from which the orbiting (outer) transition state is constructed. This forms the basis for our analysis of trajectories for ozone in general, but with particular emphasis on the roaming trajectories.« less

Theoretical and experimental study on electron interactions with chlorobenzene: Shape resonances and differential cross sections

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

Barbosa, Alessandra Souza; Laboratório de Colisões Atómicas e Moleculares, CEFITEC, Departamento de Física, Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa, 2829-516 Caparica; Varella, Márcio T. do N.

2016-08-28

In this work, we report theoretical and experimental cross sections for elastic scattering of electrons by chlorobenzene (ClB). The theoretical integral and differential cross sections (DCSs) were obtained with the Schwinger multichannel method implemented with pseudopotentials (SMCPP) and the independent atom method with screening corrected additivity rule (IAM-SCAR). The calculations with the SMCPP method were done in the static-exchange (SE) approximation, for energies above 12 eV, and in the static-exchange plus polarization approximation, for energies up to 12 eV. The calculations with the IAM-SCAR method covered energies up to 500 eV. The experimental differential cross sections were obtained in themore » high resolution electron energy loss spectrometer VG-SEELS 400, in Lisbon, for electron energies from 8.0 eV to 50 eV and angular range from 7{sup ∘} to 110{sup ∘}. From the present theoretical integral cross section (ICS) we discuss the low-energy shape-resonances present in chlorobenzene and compare our computed resonance spectra with available electron transmission spectroscopy data present in the literature. Since there is no other work in the literature reporting differential cross sections for this molecule, we compare our theoretical and experimental DCSs with experimental data available for the parent molecule benzene.« less

Temperature dependent CO2 behavior in microporous 1-D channels of a metal-organic framework with multiple interaction sites

PubMed Central

Kim, Dongwook; Park, Jaehun; Kim, Yung Sam; Lah, Myoung Soo

2017-01-01

The MOF with the encapsulated CO2 molecule shows that the CO2 molecule is ligated to the unsaturated Cu(II) sites in the cage using its Lewis basic oxygen atom via an angular η1-(OA) coordination mode and also interacts with Lewis basic nitrogen atoms of the tetrazole ligands using its Lewis acidic carbon atom. Temperature dependent structure analyses indicate the simultaneous weakening of both interactions as temperature increases. Infrared spectroscopy of the MOF confirmed that the CO2 interaction with the framework is temperature dependent. The strength of the interaction is correlated to the separation of the two bending peaks of the bound CO2 rather than the frequency shift of the asymmetric stretching peak from that of free CO2. The encapsulated CO2 in the cage is weakly interacting with the framework at around ambient temperatures and can have proper orientation for wiggling out of the cage through the narrow portals so that the reversible uptake can take place. On the other hand, the CO2 in the cage is restrained at a specific orientation at 195 K since it interacts with the framework strong enough using the multiple interaction sites so that adsorption process is slightly restricted and desorption process is almost clogged. PMID:28128298

Tensor distribution function

NASA Astrophysics Data System (ADS)

Leow, Alex D.; Zhu, Siwei

2008-03-01

Diffusion weighted MR imaging is a powerful tool that can be employed to study white matter microstructure by examining the 3D displacement profile of water molecules in brain tissue. By applying diffusion-sensitizing gradients along a minimum of 6 directions, second-order tensors (represetnted by 3-by-3 positive definiite matrices) can be computed to model dominant diffusion processes. However, it has been shown that conventional DTI is not sufficient to resolve more complicated white matter configurations, e.g. crossing fiber tracts. More recently, High Angular Resolution Diffusion Imaging (HARDI) seeks to address this issue by employing more than 6 gradient directions. To account for fiber crossing when analyzing HARDI data, several methodologies have been introduced. For example, q-ball imaging was proposed to approximate Orientation Diffusion Function (ODF). Similarly, the PAS method seeks to reslove the angular structure of displacement probability functions using the maximum entropy principle. Alternatively, deconvolution methods extract multiple fiber tracts by computing fiber orientations using a pre-specified single fiber response function. In this study, we introduce Tensor Distribution Function (TDF), a probability function defined on the space of symmetric and positive definite matrices. Using calculus of variations, we solve for the TDF that optimally describes the observed data. Here, fiber crossing is modeled as an ensemble of Gaussian diffusion processes with weights specified by the TDF. Once this optimal TDF is determined, ODF can easily be computed by analytical integration of the resulting displacement probability function. Moreover, principle fiber directions can also be directly derived from the TDF.

Incorporation of Hydrogen Bond Angle Dependency into the Generalized Solvation Free Energy Density Model.

PubMed

Ma, Songling; Hwang, Sungbo; Lee, Sehan; Acree, William E; No, Kyoung Tai

2018-04-23

To describe the physically realistic solvation free energy surface of a molecule in a solvent, a generalized version of the solvation free energy density (G-SFED) calculation method has been developed. In the G-SFED model, the contribution from the hydrogen bond (HB) between a solute and a solvent to the solvation free energy was calculated as the product of the acidity of the donor and the basicity of the acceptor of an HB pair. The acidity and basicity parameters of a solute were derived using the summation of acidities and basicities of the respective acidic and basic functional groups of the solute, and that of the solvent was experimentally determined. Although the contribution of HBs to the solvation free energy could be evenly distributed to grid points on the surface of a molecule, the G-SFED model was still inadequate to describe the angle dependency of the HB of a solute with a polarizable continuum solvent. To overcome this shortcoming of the G-SFED model, the contribution of HBs was formulated using the geometric parameters of the grid points described in the HB coordinate system of the solute. We propose an HB angle dependency incorporated into the G-SFED model, i.e., the G-SFED-HB model, where the angular-dependent acidity and basicity densities are defined and parametrized with experimental data. The G-SFED-HB model was then applied to calculate the solvation free energies of organic molecules in water, various alcohols and ethers, and the log P values of diverse organic molecules, including peptides and a protein. Both the G-SFED model and the G-SFED-HB model reproduced the experimental solvation free energies with similar accuracy, whereas the distributions of the SFED on the molecular surface calculated by the G-SFED and G-SFED-HB models were quite different, especially for molecules having HB donors or acceptors. Since the angle dependency of HBs was included in the G-SFED-HB model, the SFED distribution of the G-SFED-HB model is well described as compared to that of the G-SFED model.

Maximum angular accuracy of pulsed laser radar in photocounting limit.

PubMed

Elbaum, M; Diament, P; King, M; Edelson, W

1977-07-01

To estimate the angular position of targets with pulsed laser radars, their images may be sensed with a fourquadrant noncoherent detector and the image photocounting distribution processed to obtain the angular estimates. The limits imposed on the accuracy of angular estimation by signal and background radiation shot noise, dark current noise, and target cross-section fluctuations are calculated. Maximum likelihood estimates of angular positions are derived for optically rough and specular targets and their performances compared with theoretical lower bounds.

Measures and models for angular correlation and angular-linear correlation. [correlation of random variables

NASA Technical Reports Server (NTRS)

Johnson, R. A.; Wehrly, T.

1976-01-01

Population models for dependence between two angular measurements and for dependence between an angular and a linear observation are proposed. The method of canonical correlations first leads to new population and sample measures of dependence in this latter situation. An example relating wind direction to the level of a pollutant is given. Next, applied to pairs of angular measurements, the method yields previously proposed sample measures in some special cases and a new sample measure in general.

Symmetry-Based Techniques for Qualitative Understanding of Rovibrational Effects in Spherical-Top Molecular Spectra and Dynamics

NASA Astrophysics Data System (ADS)

Mitchell, Justin Chadwick

2011-12-01

Using light to probe the structure of matter is as natural as opening our eyes. Modern physics and chemistry have turned this art into a rich science, measuring the delicate interactions possible at the molecular level. Perhaps the most commonly used tool in computational spectroscopy is that of matrix diagonalization. While this is invaluable for calculating everything from molecular structure and energy levels to dipole moments and dynamics, the process of numerical diagonalization is an opaque one. This work applies symmetry and semi-classical techniques to elucidate numerical spectral analysis for high-symmetry molecules. Semi-classical techniques, such as the Potential Energy Surfaces, have long been used to help understand molecular vibronic and rovibronic spectra and dynamics. This investigation focuses on newer semi-classical techniques that apply Rotational Energy Surfaces (RES) to rotational energy level clustering effects in high-symmetry molecules. Such clusters exist in rigid rotor molecules as well as deformable spherical tops. This study begins by using the simplicity of rigid symmetric top molecules to clarify the classical-quantum correspondence of RES semi-classical analysis and then extends it to a more precise and complete theory of modern high-resolution spectra. RES analysis is extended to molecules having more complex and higher rank tensorial rotational and rovibrational Hamiltonians than were possible to understand before. Such molecules are shown to produce an extraordinary range of rotational level clusters, corresponding to a panoply of symmetries ranging from C4v to C2 and C1 (no symmetry) with a corresponding range of new angular momentum localization and J-tunneling effects. Using RES topography analysis and the commutation duality relations between symmetry group operators in the lab-frame to those in the body-frame, it is shown how to better describe and catalog complex splittings found in rotational level clusters. Symmetry character analysis is generalized to give analytic eigensolutions. An appendix provides vibrational analogies. For the first time, interactions between molecular vibrations (polyads) are described semi-classically by multiple RES. This is done for the nu 3/2nu4 dyad of CF4. The nine-surface RES topology of the U(9)-dyad agrees with both computational and experimental work. A connection between this and a simpler U(2) example is detailed in an Appendix.

Motion fading is driven by perceived, not actual angular velocity.

PubMed

Kohler, P J; Caplovitz, G P; Hsieh, P-J; Sun, J; Tse, P U

2010-06-01

After prolonged viewing of a slowly drifting or rotating pattern under strict fixation, the pattern appears to slow down and then momentarily stop. Here we examine the relationship between such 'motion fading' and perceived angular velocity. Using several different dot patterns that generate emergent virtual contours, we demonstrate that whenever there is a difference in the perceived angular velocity of two patterns of dots that are in fact rotating at the same angular velocity, there is also a difference in the time to undergo motion fading for those two patterns. Conversely, whenever two patterns show no difference in perceived angular velocity, even if in fact rotating at different angular velocities, we find no difference in the time to undergo motion fading. Thus, motion fading is driven by the perceived rather than actual angular velocity of a rotating stimulus. Copyright (c) 2010 Elsevier Ltd. All rights reserved.

Angular Positioning Sensor for Space Mechanisms

NASA Astrophysics Data System (ADS)

Steiner, Nicolas; Chapuis, Dominique

2013-09-01

Angular position sensors are used on various rotating mechanisms such as solar array drive mechanisms, antenna pointing mechanisms, scientific instruments, motors or actuators.Now a days, potentiometers and encoders are mainly used for angular measurement purposes. Both of them have their own pros and cons.As alternative, Ruag Space Switzerland Nyon (RSSN) is developing and qualifying two innovative technologies of angular position sensors which offer easy implementation, medium to very high lifetime and high flexibility with regards to the output signal shape/type.The Brushed angular position sensor uses space qualified processes which are already flying on RSSN's sliprings for many years. A large variety of output signal shape can be implemented to fulfill customer requirements (digital, analog, customized, etc.).The contactless angular position sensor consists in a new radiation hard Application Specific Integrated Circuit (ASIC) based on the Hall effect and providing the angular position without complex processing algorithm.

Variation in Angular Velocity and Angular Acceleration of a Particle in Rectilinear Motion

ERIC Educational Resources Information Center

Mashood, K. K.; Singh, V. A.

2012-01-01

We discuss the angular velocity ([image omitted]) and angular acceleration ([image omitted]) associated with a particle in rectilinear motion with constant acceleration. The discussion was motivated by an observation that students and even teachers have difficulty in ascribing rotational motion concepts to a particle when the trajectory is a…

47 CFR 73.128 - AM stereophonic broadcasting.

Code of Federal Regulations, 2014 CFR

2014-10-01

... magnitude of the nth term of the difference signal ωsn=the nth order angular velocity of the sum signal ωdn=the nth order angular velocity of the difference signal ωc=the angular velocity of the carrier... presence of envelope modulation. (5) Maximum angular modulation, which occurs on negative peaks of the left...

System and method for correcting attitude estimation

NASA Technical Reports Server (NTRS)

Josselson, Robert H. (Inventor)

2010-01-01

A system includes an angular rate sensor disposed in a vehicle for providing angular rates of the vehicle, and an instrument disposed in the vehicle for providing line-of-sight control with respect to a line-of-sight reference. The instrument includes an integrator which is configured to integrate the angular rates of the vehicle to form non-compensated attitudes. Also included is a compensator coupled across the integrator, in a feed-forward loop, for receiving the angular rates of the vehicle and outputting compensated angular rates of the vehicle. A summer combines the non-compensated attitudes and the compensated angular rates of the to vehicle to form estimated vehicle attitudes for controlling the instrument with respect to the line-of-sight reference. The compensator is configured to provide error compensation to the instrument free-of any feedback loop that uses an error signal. The compensator may include a transfer function providing a fixed gain to the received angular rates of the vehicle. The compensator may, alternatively, include a is transfer function providing a variable gain as a function of frequency to operate on the received angular rates of the vehicle.

The effects of obesity on balance recovery using an ankle strategy.

PubMed

Matrangola, Sara L; Madigan, Michael L

2011-06-01

Obesity is associated with an increased risk of falls. The purpose of this study was to investigate the effects of obesity on balance recovery using an ankle strategy. In addition, computer simulations to understand how increased inertia and weight associated with obesity independently influence balance recovery. Ten normal weight (BMI: 22.7±0.6 kg/m(2)) and ten obese (BMI: 32.2±2.2 kg/m(2)) adult male subjects participated in the study. Subjects recovered balance using an ankle strategy after three types of postural perturbations: an initial angular displacement, an initial angular velocity from the natural stance, and an initial angular velocity from a prescribed position. Balance recovery was quantified by the largest initial angular displacement or angular velocity from which balance could be recovered. Obesity impaired balance recovery from perturbations involving an initial angular velocity, but not from an initial angular displacement. Similarly, computer simulations determined that increased inertia is beneficial to balance recovery when there is little to no initial angular velocity. These findings indicate that the effects of obesity on balance recovery are dependent on the type of perturbation, and that increased inertia associated with obesity can be beneficial for perturbations that involve little to no initial angular velocity. Copyright © 2011 Elsevier B.V. All rights reserved.

Generation of vertical angular momentum in single, double, and triple-turn pirouette en dehors in ballet.

PubMed

Kim, Jemin; Wilson, Margaret A; Singhal, Kunal; Gamblin, Sarah; Suh, Cha-Young; Kwon, Young-Hoo

2014-09-01

The purpose of this study was to investigate the vertical angular momentum generation strategies used by skilled ballet dancers in pirouette en dehors. Select kinematic parameters of the pirouette preparation (stance depth, vertical center-of-mass motion range, initial shoulder line position, shoulder line angular displacement, and maximum trunk twist angle) along with vertical angular momentum parameters during the turn (maximum momentums of the whole body and body parts, and duration and rate of generation) were obtained from nine skilled collegiate ballet dancers through a three-dimensional motion analysis and compared among three turn conditions (single, double, and triple). A one-way ('turn') multivariate analysis of variance of the kinematic parameters and angular momentum parameters of the whole body and a two-way analysis of variance ('turn' × 'body') of the maximum angular momentums of the body parts were conducted. Significant 'turn' effects were observed in the kinematic/angular momentum parameters (both the preparation and the turn) (p <  0.05). As the number of turns increased, skilled dancers generated larger vertical angular momentums by predominantly increasing the rate of momentum generation using rotation of the upper trunk and arms. The trail (closing) arm showed the largest contribution to whole-body angular momentum followed by the lead arm.

Massive star formation by accretion. II. Rotation: how to circumvent the angular momentum barrier?

NASA Astrophysics Data System (ADS)

Haemmerlé, L.; Eggenberger, P.; Meynet, G.; Maeder, A.; Charbonnel, C.; Klessen, R. S.

2017-06-01

Context. Rotation plays a key role in the star-formation process, from pre-stellar cores to pre-main-sequence (PMS) objects. Understanding the formation of massive stars requires taking into account the accretion of angular momentum during their PMS phase. Aims: We study the PMS evolution of objects destined to become massive stars by accretion, focusing on the links between the physical conditions of the environment and the rotational properties of young stars. In particular, we look at the physical conditions that allow the production of massive stars by accretion. Methods: We present PMS models computed with a new version of the Geneva Stellar Evolution code self-consistently including accretion and rotation according to various accretion scenarios for mass and angular momentum. We describe the internal distribution of angular momentum in PMS stars accreting at high rates and we show how the various physical conditions impact their internal structures, evolutionary tracks, and rotation velocities during the PMS and the early main sequence. Results: We find that the smooth angular momentum accretion considered in previous studies leads to an angular momentum barrier and does not allow the formation of massive stars by accretion. A braking mechanism is needed in order to circumvent this angular momentum barrier. This mechanism has to be efficient enough to remove more than two thirds of the angular momentum from the inner accretion disc. Due to the weak efficiency of angular momentum transport by shear instability and meridional circulation during the accretion phase, the internal rotation profiles of accreting stars reflect essentially the angular momentum accretion history. As a consequence, careful choice of the angular momentum accretion history allows circumvention of any limitation in mass and velocity, and production of stars of any mass and velocity compatible with structure equations.

Characterization of thigh and shank segment angular velocity during jump landing tasks commonly used to evaluate risk for ACL injury.

PubMed

Dowling, Ariel V; Favre, Julien; Andriacchi, Thomas P

2012-09-01

The dynamic movements associated with anterior cruciate ligament (ACL) injury during jump landing suggest that limb segment angular velocity can provide important information for understanding the conditions that lead to an injury. Angular velocity measures could provide a quick and simple method of assessing injury risk without the constraints of a laboratory. The objective of this study was to assess the inter-subject variations and the sensitivity of the thigh and shank segment angular velocity in order to determine if these measures could be used to characterize jump landing mechanisms. Additionally, this study tested the correlation between angular velocity and the knee abduction moment. Thirty-six healthy participants (18 male) performed drop jumps with bilateral and unilateral landing. Thigh and shank angular velocities were measured by a wearable inertial-based system, and external knee moments were measured using a marker-based system. Discrete parameters were extracted from the data and compared between systems. For both jumping tasks, the angular velocity curves were well defined movement patterns with high inter-subject similarity in the sagittal plane and moderate to good similarity in the coronal and transverse planes. The angular velocity parameters were also able to detect differences between the two jumping tasks that were consistent across subjects. Furthermore, the coronal angular velocities were significantly correlated with the knee abduction moment (R of 0.28-0.51), which is a strong indicator of ACL injury risk. This study suggested that the thigh and shank angular velocities, which describe the angular dynamics of the movement, should be considered in future studies about ACL injury mechanisms.

Singularity in the Laboratory Frame Angular Distribution Derived in Two-Body Scattering Theory

ERIC Educational Resources Information Center

Dick, Frank; Norbury, John W.

2009-01-01

The laboratory (lab) frame angular distribution derived in two-body scattering theory exhibits a singularity at the maximum lab scattering angle. The singularity appears in the kinematic factor that transforms the centre of momentum (cm) angular distribution to the lab angular distribution. We show that it is caused in the transformation by the…

Stellar Rotation on the Main Sequence

NASA Astrophysics Data System (ADS)

Soderblom, D.; Murdin, P.

2000-11-01

The conservation of ANGULAR MOMENTUM is the one effective counterbalance to the inexorable pull of gravity in the universe, and so everything rotates. Stars acquire their angular momentum when they form, and, indeed, the manner in which nearly all this initial angular momentum is dissipated remains poorly understood, but without substantial angular momentum loss an interstellar cloud could never ...

The Physics and Chemistry of Oxygen-Rich Circumstellar Envelopes as Traced by Simple Molecules

NASA Astrophysics Data System (ADS)

Wong, Ka Tat

2018-04-01

The physics and chemistry of the circumstellar envelopes (CSEs) of evolved stars are not fully understood despite decades of research. This thesis addresses two issues in the study of the CSEs of oxygen-rich (O-rich) evolved stars. In the first project, the ammonia (NH3) chemistry of O-rich stars is investigated with multi-wavelength observations; in the second project, the extended atmosphere and inner wind of the archetypal asymptotic giant branch (AGB) star o Ceti (Mira) is studied with high-angular resolution observations. One of the long-standing mysteries in circumstellar chemistry is the perplexing overabundance of the NH3 molecule. NH3 in O-rich evolved stars has been found in much higher abundance, by several orders of magnitude, than that expected in equilibrium chemistry. Several mechanisms have been suggested in the literature to explain this high NH3 abundance, including shocks in the inner wind, photodissociation of nitrogen by interstellar ultraviolet radiation, and nitrogen enrichment in stellar nucleosynthesis; however, none of these suggestions can fully explain the abundances of NH3 and various other molecular species in the CSEs of O-rich stars. In order to investigate the distribution of NH3 in O-rich CSEs, observations of the spectral lines of NH3 from a diverse sample of evolved stars and in different wavelength regimes are necessary. In this thesis, the NH3 line emission and absorption from four O-rich stars are studied. These targets include the AGB star IK Tauri, the pre-planetary nebula OH 231.8+4.2, the red supergiant VY Canis Majoris, and the yellow hypergiant IRC +10420. The amount of NH3 observational data has increased drastically thanks to the recent advancement of instrumentation. Observations of NH3 rotational line emission at submillimetre/far-infrared wavelengths were possible with the Herschel Space Observatory (2009–2013). The new wideband correlator in the upgraded Karl G. Janksy Very Large Array (VLA) provided data of multiple radio inversion lines of NH3. Furthermore, mid-infrared absorption of NH3 has been observed by the NASA Infrared Telescope Facility (IRTF) for IK Tau and VY CMa. Full radiative transfer modelling including mid-infrared pumping to the first vibrationally excited state (v2=1) has been carried out to reproduce the observed emission and absorption spectra and to retrieve the NH3 abundances in the targets. It is found that the NH3 emission in the CSEs of the targets arises from localised spatial-kinematic structures in which the gas density may be higher than in the surrounding gas. Circumstellar shocks may contribute to, but cannot fully account for, the formation of the molecule. Besides circumstellar chemistry, our understanding of the dust formation and wind-driving mechanisms of oxygen-rich evolved stars is still incomplete. One of the obstacles in the past was the difficulty in imaging the dust condensation and wind acceleration zones due to the lack of high-angular resolution instruments. Thanks to the Atacama Large Millimeter/submillimeter Array (ALMA), which has the longest baseline of about 15 km, we are now able to produce high-fidelity images at unprecedented angular resolutions of tens of milliarcseconds (mas) in the (sub)millimetre regime. Such angular resolutions, which are comparable to the stellar radii of nearby objects, are necessary to understand the gas dynamics and chemical evolution in the pulsating atmosphere and dust formation zone of nearby AGB stars. The eponymous Mira-type long-period variable, o Cet, was observed as a Science Verification target during the first ALMA Long Baseline Campaign that took place in 2014. The observations produced images of the stellar radio photosphere and the molecular transitions of SiO and H2O at an angular resolution of about 30 mas near 220 GHz (1.3 mm). The millimetre stellar disc of o Cet was resolved and modelled. More importantly, this is the first time that molecular line absorption against the background stellar continuum has been clearly imaged in the (sub)millimetre wavelength regime. Through radiative transfer modelling of the SiO and H2O line absorption and emission, it is found that during the ALMA observations, the extended atmosphere of the star exhibited infall motions in general with a shock front of velocity

Spin-to-orbit conversion at acousto-optic diffraction of light: conservation of optical angular momentum.

PubMed

Skab, Ihor; Vlokh, Rostyslav

2012-04-01

Acousto-optic diffraction of light in optically active cubic crystals is analyzed from the viewpoint of conservation of optical angular momentum. It is shown that the availability of angular momentum in the diffracted optical beam can be necessarily inferred from the requirements of angular momentum conservation law. As follows from our analysis, a circularly polarized diffracted wave should bear an orbital angular momentum. The efficiency of the spin-to-orbit momentum conversion is governed by the efficiency of acousto-optic diffraction.

Angular behavior of synchrotron radiation harmonics.

PubMed

Bagrov, V G; Bulenok, V G; Gitman, D M; Jara, Jose Acosta; Tlyachev, V B; Jarovoi, A T

2004-04-01

The detailed analysis of angular dependence of the synchrotron radiation (SR) is presented. Angular distributions of linear and circular polarization integrated over all harmonics, well known for relativistic electron energies, are extended to include radiation from electrons that are not fully relativistic. In particular, we analyze the angular dependence of the integral SR intensity and peculiarities of the angular dependence of the first harmonics SR. Studying spectral SR intensities, we have discovered their unexpected angular behavior, completely different from that of the integral SR intensity; namely, for any given synchrotron frequency, maxima of the spectral SR intensities recede from the orbit plane with increasing particle energy. Thus, in contrast with the integral SR intensity, the spectral ones have the tendency to deconcentrate themselves on the orbit plane.

There are many ways to spin a photon: Half-quantization of a total optical angular momentum

PubMed Central

Ballantine, Kyle E.; Donegan, John F.; Eastham, Paul R.

2016-01-01

The angular momentum of light plays an important role in many areas, from optical trapping to quantum information. In the usual three-dimensional setting, the angular momentum quantum numbers of the photon are integers, in units of the Planck constant ħ. We show that, in reduced dimensions, photons can have a half-integer total angular momentum. We identify a new form of total angular momentum, carried by beams of light, comprising an unequal mixture of spin and orbital contributions. We demonstrate the half-integer quantization of this total angular momentum using noise measurements. We conclude that for light, as is known for electrons, reduced dimensionality allows new forms of quantization. PMID:28861467

Physical angular momentum separation for QED

NASA Astrophysics Data System (ADS)

Sun, Weimin

2017-04-01

We study the non-uniqueness problem of the gauge-invariant angular momentum separation for the case of QED, which stems from the recent controversy concerning the proper definitions of the orbital angular momentum and spin operator of the individual parts of a gauge field system. For the free quantum electrodynamics without matter, we show that the basic requirement of Euclidean symmetry selects a unique physical angular momentum separation scheme from the multitude of the possible angular momentum separation schemes constructed using the various gauge-invariant extensions (GIEs). Based on these results, we propose a set of natural angular momentum separation schemes for the case of interacting QED by invoking the formalism of asymptotic fields. Some perspectives on such a problem for the case of QCD are briefly discussed.

Implementing a Low-Cost Long-Range Unmanned Underwater Vehicle: The SeaDiver Glider

DTIC Science & Technology

2007-01-09

25 2. Position estimation.............................................................................26 3. Angular ...calculation velocity..............................................................27 4. Angular calculation position...25 Figure 14. Angular Positions.............................................................................................27

Angular momentum of dwarf galaxies

NASA Astrophysics Data System (ADS)

Kurapati, Sushma; Chengalur, Jayaram N.; Pustilnik, Simon; Kamphuis, Peter

2018-05-01

Mass and specific angular momentum are two fundamental physical parameters of galaxies. We present measurements of the baryonic mass and specific angular momentum of 11 void dwarf galaxies derived from neutral hydrogen (HI) synthesis data. Rotation curves were measured using 3D and 2D tilted ring fitting routines, and the derived curves generally overlap within the error bars, except in the central regions where, as expected, the 3D routines give steeper curves. The specific angular momentum of void dwarfs is found to be high compared to an extrapolation of the trends seen for higher mass bulge-less spirals, but comparable to that of other dwarf irregular galaxies that lie outside of voids. As such, our data show no evidence for a dependence of the specific angular momentum on the large scale environment. Combining our data with the data from the literature, we find a baryonic threshold of ˜109.1 M⊙ for this increase in specific angular momentum. Interestingly, this threshold is very similar to the mass threshold below which the galaxy discs start to become systematically thicker. This provides qualitative support to the suggestion that the thickening of the discs, as well as the increase in specific angular momentum, are both results of a common physical mechanism, such as feedback from star formation. Quantitatively, however, the amount of star formation observed in our dwarfs appears insufficient to produce the observed increase in specific angular momentum. It is hence likely that other processes, such as cold accretion of high angular momentum gas, also play a role in increasing the specific angular momentum.

Identification of trunk and pelvis movement compensations in patients with transtibial amputation using angular momentum separation.

PubMed

Gaffney, Brecca M; Murray, Amanda M; Christiansen, Cory L; Davidson, Bradley S

2016-03-01

Patients with unilateral dysvascular transtibial amputation (TTA) have a higher risk of developing low back pain than their healthy counterparts, which may be related to movement compensations used in the absence of ankle function. Assessing components of segmental angular momentum provides a unique framework to identify and interpret these movement compensations alongside traditional observational analyses. Angular momentum separation indicates two components of total angular momentum: (1) transfer momentum and (2) rotational momentum. The objective of this investigation was to assess movement compensations in patients with dysvascular TTA, patients with diabetes mellitus (DM), and healthy controls (HC) by examining patterns of generating and arresting trunk and pelvis segmental angular momenta during gait. We hypothesized that all groups would demonstrate similar patterns of generating/arresting total momentum and transfer momentum in the trunk and pelvis in reference to the groups (patients with DM and HC). We also hypothesized that patients with amputation would demonstrate different (larger) patterns of generating/arresting rotational angular momentum in the trunk. Patients with amputation demonstrated differences in trunk and pelvis transfer angular momentum in the sagittal and transverse planes in comparison to the reference groups, which indicates postural compensations adopted during walking. However, patients with amputation demonstrated larger patterns of generating and arresting of trunk and pelvis rotational angular momentum in comparison to the reference groups. These segmental rotational angular momentum patterns correspond with high eccentric muscle demands needed to arrest the angular momentum, and may lead to consequential long-term effects such as low back pain. Copyright © 2016 Elsevier B.V. All rights reserved.

Optical spin-to-orbital angular momentum conversion in ultra-thin metasurfaces with arbitrary topological charges

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

Bouchard, Frédéric; De Leon, Israel; Schulz, Sebastian A.

Orbital angular momentum associated with the helical phase-front of optical beams provides an unbounded “space” for both classical and quantum communications. Among the different approaches to generate and manipulate orbital angular momentum states of light, coupling between spin and orbital angular momentum allows a faster manipulation of orbital angular momentum states because it depends on manipulating the polarisation state of light, which is simpler and generally faster than manipulating conventional orbital angular momentum generators. In this work, we design and fabricate an ultra-thin spin-to-orbital angular momentum converter, based on plasmonic nano-antennas and operating in the visible wavelength range that ismore » capable of converting spin to an arbitrary value of orbital angular momentum ℓ. The nano-antennas are arranged in an array with a well-defined geometry in the transverse plane of the beam, possessing a specific integer or half-integer topological charge q. When a circularly polarised light beam traverses this metasurface, the output beam polarisation switches handedness and the orbital angular momentum changes in value by ℓ=±2qℏ per photon. We experimentally demonstrate ℓ values ranging from ±1 to ±25 with conversion efficiencies of 8.6% ± 0.4%. Our ultra-thin devices are integratable and thus suitable for applications in quantum communications, quantum computations, and nano-scale sensing.« less

Analysis of the geodetic residuals as differences between geodetic and sum of the atmospheric and ocean excitation of polar motion

NASA Astrophysics Data System (ADS)

Kolaczek, B.; Pasnicka, M.; Nastula, J.

2012-12-01

Up to now studies of geophysical excitation of polar motion containing AAM (Atmospheric Angular Momentum), OAM (Oceanic Angular Momentum) and HAM (Hydrological Angular Momentum) excitation functions of polar motion have not achieved the total agreement between geophysical and determined geodetic excitation (GAM, Geodetic AngularMomentum) functions of polar motion...

A goal-based angular adaptivity method for thermal radiation modelling in non grey media

NASA Astrophysics Data System (ADS)

Soucasse, Laurent; Dargaville, Steven; Buchan, Andrew G.; Pain, Christopher C.

2017-10-01

This paper investigates for the first time a goal-based angular adaptivity method for thermal radiation transport, suitable for non grey media when the radiation field is coupled with an unsteady flow field through an energy balance. Anisotropic angular adaptivity is achieved by using a Haar wavelet finite element expansion that forms a hierarchical angular basis with compact support and does not require any angular interpolation in space. The novelty of this work lies in (1) the definition of a target functional to compute the goal-based error measure equal to the radiative source term of the energy balance, which is the quantity of interest in the context of coupled flow-radiation calculations; (2) the use of different optimal angular resolutions for each absorption coefficient class, built from a global model of the radiative properties of the medium. The accuracy and efficiency of the goal-based angular adaptivity method is assessed in a coupled flow-radiation problem relevant for air pollution modelling in street canyons. Compared to a uniform Haar wavelet expansion, the adapted resolution uses 5 times fewer angular basis functions and is 6.5 times quicker, given the same accuracy in the radiative source term.

Analysis of angular momentum properties of photons emitted in fundamental atomic processes

NASA Astrophysics Data System (ADS)

Zaytsev, V. A.; Surzhykov, A. S.; Shabaev, V. M.; Stöhlker, Th.

2018-04-01

Many atomic processes result in the emission of photons. Analysis of the properties of emitted photons, such as energy and angular distribution as well as polarization, is regarded as a powerful tool for gaining more insight into the physics of corresponding processes. Another characteristic of light is the projection of its angular momentum upon propagation direction. This property has attracted a special attention over the past decades due to studies of twisted (or vortex) light beams. Measurements being sensitive to this projection may provide valuable information about the role of angular momentum in the fundamental atomic processes. Here we describe a simple theoretical method for determination of the angular momentum properties of the photons emitted in various atomic processes. This method is based on the evaluation of expectation value of the total angular momentum projection operator. To illustrate the method, we apply it to the textbook examples of plane-wave, spherical-wave, and Bessel light. Moreover, we investigate the projection of angular momentum for the photons emitted in the process of the radiative recombination with ionic targets. It is found that the recombination photons do carry a nonzero projection of the orbital angular momentum.

Angular Spacing Control for Segmented Data Pages in Angle-Multiplexed Holographic Memory

NASA Astrophysics Data System (ADS)

Kinoshita, Nobuhiro; Muroi, Tetsuhiko; Ishii, Norihiko; Kamijo, Koji; Kikuchi, Hiroshi; Shimidzu, Naoki; Ando, Toshio; Masaki, Kazuyoshi; Shimizu, Takehiro

2011-09-01

To improve the recording density of angle-multiplexed holographic memory, it is effective to increase the numerical aperture of the lens and to shorten the wavelength of the laser source as well as to increase the multiplexing number. The angular selectivity of a hologram, which determines the multiplexing number, is dependent on the incident angle of not only the reference beam but also the signal beam to the holographic recording medium. The actual signal beam, which is a convergent or divergent beam, is regarded as the sum of plane waves that have different propagation directions, angular selectivities, and optimal angular spacings. In this paper, focusing on the differences in the optimal angular spacing, we proposed a method to control the angular spacing for each segmented data page. We investigated the angular selectivity of a hologram and crosstalk for segmented data pages using numerical simulation. The experimental results showed a practical bit-error rate on the order of 10-3.

Amplification of Angular Rotations Using Weak Measurements

NASA Astrophysics Data System (ADS)

Magaña-Loaiza, Omar S.; Mirhosseini, Mohammad; Rodenburg, Brandon; Boyd, Robert W.

2014-05-01

We present a weak measurement protocol that permits a sensitive estimation of angular rotations based on the concept of weak-value amplification. The shift in the state of a pointer, in both angular position and the conjugate orbital angular momentum bases, is used to estimate angular rotations. This is done by an amplification of both the real and imaginary parts of the weak-value of a polarization operator that has been coupled to the pointer, which is a spatial mode, via a spin-orbit coupling. Our experiment demonstrates the first realization of weak-value amplification in the azimuthal degree of freedom. We have achieved effective amplification factors as large as 100, providing a sensitivity that is on par with more complicated methods that employ quantum states of light or extremely large values of orbital angular momentum.

Angular-domain scattering interferometry.

PubMed

Shipp, Dustin W; Qian, Ruobing; Berger, Andrew J

2013-11-15

We present an angular-scattering optical method that is capable of measuring the mean size of scatterers in static ensembles within a field of view less than 20 μm in diameter. Using interferometry, the method overcomes the inability of intensity-based models to tolerate the large speckle grains associated with such small illumination areas. By first estimating each scatterer's location, the method can model between-scatterer interference as well as traditional single-particle Mie scattering. Direct angular-domain measurements provide finer angular resolution than digitally transformed image-plane recordings. This increases sensitivity to size-dependent scattering features, enabling more robust size estimates. The sensitivity of these angular-scattering measurements to various sizes of polystyrene beads is demonstrated. Interferometry also allows recovery of the full complex scattered field, including a size-dependent phase profile in the angular-scattering pattern.

Dynamo magnetic field-induced angular momentum transport in protostellar nebulae - The 'minimum mass' protosolar nebula

NASA Technical Reports Server (NTRS)

Stepinski, T. F.; Levy, E. H.

1990-01-01

Magnetic torques can produce angular momentum redistribution in protostellar nebulas. Dynamo magnetic fields can be generated in differentially rotating and turbulent nebulas and can be the source of magnetic torques that transfer angular momentum from a protostar to a disk, as well as redistribute angular momentum within a disk. A magnetic field strength of 100-1000 G is needed to transport the major part of a protostar's angular momentum into a surrounding disk in a time characteristic of star formation, thus allowing formation of a solar-system size protoplanetary nebula in the usual 'minimum-mass' model of the protosolar nebula. This paper examines the possibility that a dynamo magnetic field could have induced the needed angular momentum transport from the proto-Sun to the protoplanetary nebula.

Separation of spin and orbital angular coherence momenta in the second-order coherence theory of vector electromagnetic fields.

PubMed

Wang, Wei; Takeda, Mitsuo

2007-09-15

In analogy with the separation of the total optical angular momentum into a spin and an orbital part in electrodynamics, we introduce a new concept of spin and orbital angular coherence momenta into the general coherence theory of vector electromagnetic fields. The properties of the newly introduced spin and orbital angular coherence momenta are investigated through the decomposition of the total coherence angular momentum into the sum of these two components, and their separate conservations have been derived for what is believed to be the first time.

The creation of photonic orbital angular momentum in electromagnetic waves propagating through turbulence

NASA Astrophysics Data System (ADS)

Sanchez, D. J.; Oesch, D. W.; Reynolds, O. R.

2013-08-01

Context. We have recently shown that the phenomenon known as "branch points" in AO are markers for photons carrying orbital angular momentum (OAM). In doing so, we have demonstrated that atmospheric turbulence creates well defined OAM states in beams propagating through it. Aims: In this paper, we extend our previous research to include any astrophysical turbulent assemblage of molecules or atoms (TAMA), demonstrating that these clouds, similar to Earth's atmosphere, also create photonic orbital angular momentum (POAM) in electromagnetic waves propagating through them. A TAMA is any gaseous cloud with a varying density and therefore variation in its index of refraction, which includes but is not limited to stellar envelopes, circumstellar disks, molecular clouds, planetary atmospheres, and the interstellar medium. Methods: We applied our previous theoretical, simulation, and laboratory results to astrophysical TAMAs. Additionally, we demonstrated how sensors designed for AO can be used to measure this POAM flux. Results: Our results apply to light propagating through any TAMA. Since TAMA are ubiquitous in the cosmos, steady, long lasting POAM fluxes will be ubiquitous as well. Conclusions: Our results, which include theory, benchtop laboratory data, and wave optic simulation, indicate that, under the right conditions, POAM fluxes can reach over 50% of the total photon flux. An initial set of on-sky experimental observations appear to corroborate the laboratory results with two of the five stars, HR 1529 and HR 1577, showing POAM fluxes of 3% ± 1% and 2% ± 1% of the total flux, and a third, HR 1895, with a PAOM flux of up to 17% ± 2% of the total flux. We express our gratitude to the Air Force Office of Scientific Research for their support of this research.Appendices are available in electronic form at http://www.aanda.orgData referred to in measurements are only available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (ftp://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/556/A130

MIRO Computational Model

NASA Technical Reports Server (NTRS)

Broderick, Daniel

2010-01-01

A computational model calculates the excitation of water rotational levels and emission-line spectra in a cometary coma with applications for the Micro-wave Instrument for Rosetta Orbiter (MIRO). MIRO is a millimeter-submillimeter spectrometer that will be used to study the nature of cometary nuclei, the physical processes of outgassing, and the formation of the head region of a comet (coma). The computational model is a means to interpret the data measured by MIRO. The model is based on the accelerated Monte Carlo method, which performs a random angular, spatial, and frequency sampling of the radiation field to calculate the local average intensity of the field. With the model, the water rotational level populations in the cometary coma and the line profiles for the emission from the water molecules as a function of cometary parameters (such as outgassing rate, gas temperature, and gas and electron density) and observation parameters (such as distance to the comet and beam width) are calculated.

Three dimensional chiral plasmon rulers based on silver nanorod trimers.

PubMed

Han, Chunrui; Yang, Lechen; Ye, Piao; Parrott, Edward P J; Pickwell-Macpherson, Emma; Tam, Wing Yim

2018-04-16

The symmetry dependences of plasmon excitation modes are studied in 3D silver nanorod trimers. The degenerate plasmon modes split into chiral modes by breaking the inversion and mirror symmetry of the nanorod trimer through translation and/or rotation of the middle rod. With a translation operation, successive evolution of the circular dichroism (CD) spectrum can be achieved through gradual breaking of the inversion symmetry. An additional rotation operation produces even dramatic spectral changes due to breaking a quasi-mirror symmetry resulted from the same angular distance of the middle rod to the top and bottom rods. Especially, pairs of new chiral modes can be excited due to the contact of the middle rod with the top-bottom rod pair. The spectral changes in the simulations, which are also demonstrated experimentally, envision the 3D chiral nanorod trimer system as plasmon ruler for spatial configuration retrieval and dynamic bio-process analysis at the single molecule level.

NGC 2024: Far-infrared and radio molecular observations

NASA Technical Reports Server (NTRS)

Thronson, H. A., Jr.; Lada, C. J.; Schwartz, P. R.; Smith, H. A.; Smith, J.; Glaccum, W.; Harper, D. A.; Loewenstein, R. F.

1984-01-01

Far infrared continuum and millimeter wave molecular observations are presented for the infrared and radio source NGC 2024. The measurements are obtained at relatively high angular resolution, enabling a description of the source energetics and mass distribution in greater detail than previously reported. The object appears to be dominated by a dense ridge of material, extended in the north/south direction and centered on the dark lane that is seen in visual photographs. Maps of the source using the high density molecules CS and HCN confirm this picture and allow a description of the core structure and molecular abundances. The radio molecular and infrared observations support the idea that an important exciting star in NGC 2024 has yet to be identified and is centered on the dense ridge about 1' south of the bright mid infrared source IRS 2. The data presented here allows a presentation of a model for the source.

Harmonium: An Ultrafast Vacuum Ultraviolet Facility.

PubMed

Arrell, Christopher A; Ojeda, José; Longetti, Luca; Crepaldi, Alberto; Roth, Silvan; Gatti, Gianmarco; Clark, Andrew; van Mourik, Frank; Drabbels, Marcel; Grioni, Marco; Chergui, Majed

2017-05-31

Harmonium is a vacuum ultraviolet (VUV) photon source built within the Lausanne Centre for Ultrafast Science (LACUS). Utilising high harmonic generation, photons from 20-110 eV are available to conduct steady-state or ultrafast photoelectron and photoion spectroscopies (PES and PIS). A pulse preserving monochromator provides either high energy resolution (70 meV) or high temporal resolution (40 fs). Three endstations have been commissioned for: a) PES of liquids; b) angular resolved PES (ARPES) of solids and; c) coincidence PES and PIS of gas phase molecules or clusters. The source has several key advantages: high repetition rate (up to 15 kHz) and high photon flux (1011 photons per second at 38 eV). The capabilities of the facility complement the Swiss ultrafast and X-ray community (SwissFEL, SLS, NCCR MUST, etc.) helping to maintain Switzerland's leading role in ultrafast science in the world.

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.

An Organic Vortex Laser.

PubMed

Stellinga, Daan; Pietrzyk, Monika E; Glackin, James M E; Wang, Yue; Bansal, Ashu K; Turnbull, Graham A; Dholakia, Kishan; Samuel, Ifor D W; Krauss, Thomas F

2018-03-27

Optical vortex beams are at the heart of a number of novel research directions, both as carriers of information and for the investigation of optical activity and chiral molecules. Optical vortex beams are beams of light with a helical wavefront and associated orbital angular momentum. They are typically generated using bulk optics methods or by a passive element such as a forked grating or a metasurface to imprint the required phase distribution onto an incident beam. Since many applications benefit from further miniaturization, a more integrated yet scalable method is highly desirable. Here, we demonstrate the generation of an azimuthally polarized vortex beam directly by an organic semiconductor laser that meets these requirements. The organic vortex laser uses a spiral grating as a feedback element that gives control over phase, handedness, and degree of helicity of the emitted beam. We demonstrate vortex beams up to an azimuthal index l = 3 that can be readily multiplexed into an array configuration.

Pulsed electron nuclear double resonance studies of the photoexcited triplet state of pentacene in p-terphenyl crystals at room temperature.

PubMed

Yago, Tomoaki; Link, Gerhard; Kothe, Gerd; Lin, Tien-Sung

2007-09-21

Pulsed electron nuclear double resonance (ENDOR) using a modified Davies-type [Phys. Lett. 47A, 1 (1974)] sequence is employed to study the hyperfine (HF) structure of the photoexcited triplet state of pentacene dispersed in protonated and deuterated p-terphenyl single crystals. The strong electron spin polarization and long phase memory time of triplet pentacene enable us to perform the ENDOR measurements on the S=1 spin system at room temperature. Proton HF tensor elements and spin density values of triplet pentacene are extracted from a detailed angular-dependent study in which the orientation of the magnetic field is varied systematically in two different pentacene planes. Analysis reveals that the pentacene molecule is no longer planar in the p-terphenyl host lattice. The distortion is more pronounced in the deuterated crystal where the unit cell dimensions are slightly smaller than those of the protonated crystal.

Chiral optical response of planar and symmetric nanotrimers enabled by heteromaterial selection.

PubMed

Banzer, Peter; Woźniak, Paweł; Mick, Uwe; De Leon, Israel; Boyd, Robert W

2016-10-13

Chirality is an intriguing property of certain molecules, materials or artificial nanostructures, which allows them to interact with the spin angular momentum of the impinging light field. Due to their chiral geometry, they can distinguish between left- and right-hand circular polarization states or convert them into each other. Here we introduce an approach towards optical chirality, which is observed in individual two-dimensional and geometrically mirror-symmetric nanostructures. In this scheme, the chiral optical response is induced by the chosen heterogeneous material composition of a particle assembly and the corresponding resonance behaviour of the constituents it is built from, which breaks the symmetry of the system. As a proof of principle, we investigate such a structure composed of individual silicon and gold nanoparticles both experimentally, as well as numerically. Our proposed concept constitutes an approach for designing two-dimensional chiral media tailored at the nanoscale, allowing for high tunability of their optical response.

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 .

`Twisted' electrons

NASA Astrophysics Data System (ADS)

Larocque, Hugo; Kaminer, Ido; Grillo, Vincenzo; Leuchs, Gerd; Padgett, Miles J.; Boyd, Robert W.; Segev, Mordechai; Karimi, Ebrahim

2018-04-01

Electrons have played a significant role in the development of many fields of physics during the last century. The interest surrounding them mostly involved their wave-like features prescribed by the quantum theory. In particular, these features correctly predict the behaviour of electrons in various physical systems including atoms, molecules, solid-state materials, and even in free space. Ten years ago, new breakthroughs were made, arising from the new ability to bestow orbital angular momentum (OAM) to the wave function of electrons. This quantity, in conjunction with the electron's charge, results in an additional magnetic property. Owing to these features, OAM-carrying, or twisted, electrons can effectively interact with magnetic fields in unprecedented ways and have motivated materials scientists to find new methods for generating twisted electrons and measuring their OAM content. Here, we provide an overview of such techniques along with an introduction to the exciting dynamics of twisted electrons.

Diversity‐Oriented Synthesis of Natural‐Product‐like Libraries Containing a 3‐Methylbenzofuran Moiety for the Discovery of New Chemical Elicitors

PubMed Central

He, Xingrui; Chen, Xia; Lin, Songbo; Mo, Xiaochang; Zhou, Pengyong; Zhang, Zhihao; Lu, Yaoyao; Yang, Yu; Gu, Haining

2016-01-01

Abstract Natural products are a major source of biological molecules. The 3‐methylfuran scaffold is found in a variety of plant secondary metabolite chemical elicitors that confer host‐plant resistance against insect pests. Herein, the diversity‐oriented synthesis of a natural‐product‐like library is reported, in which the 3‐methylfuran core is fused in an angular attachment to six common natural product scaffolds—coumarin, chalcone, flavone, flavonol, isoflavone and isoquinolinone. The structural diversity of this library is assessed computationally using cheminformatic analysis. Phenotypic high‐throughput screening of β‐glucuronidase activity uncovers several hits. Further in vivo screening confirms that these hits can induce resistance in rice to nymphs of the brown planthopper Nilaparvata lugens. This work validates the combination of diversity‐oriented synthesis and high‐throughput screening of β‐glucuronidase activity as a strategy for discovering new chemical elicitors. PMID:28168155

Indirect double photoionization of water

NASA Astrophysics Data System (ADS)

Resccigno, T. N.; Sann, H.; Orel, A. E.; Dörner, R.

2011-05-01

The vertical double ionization thresholds of small molecules generally lie above the dissociation limits corresponding to formation of two singly charged fragments. This gives the possibility of populating singly charged molecular ions by photoionization in the Franck-Condon region at energies below the lowest dication state, but above the dissociation limit into two singly charged fragment ions. This process can produce a superexcited neutral fragment that autoionizes at large internuclear separation. We study this process in water, where absorption of a photon produces an inner-shell excited state of H2O+ that fragments to H++OH*. The angular distribution of secondary electrons produced by OH* when it autoionizes produces a characteristic asymmetric pattern that reveals the distance, and therefore the time, at which the decay takes place. LBNL, Berkeley, CA, J. W. Goethe Universität, Frankfurt, Germany. Work performed under auspices of US DOE and supported by OBES, Div. of Chemical Sciences.

Analytical interatomic potential for modeling nonequilibrium processes in the W-C-H system

NASA Astrophysics Data System (ADS)

Juslin, N.; Erhart, P.; Träskelin, P.; Nord, J.; Henriksson, K. O. E.; Nordlund, K.; Salonen, E.; Albe, K.

2005-12-01

A reactive interatomic potential based on an analytical bond-order scheme is developed for the ternary system W-C-H. The model combines Brenner's hydrocarbon potential with parameter sets for W-W, W-C, and W-H interactions and is adjusted to materials properties of reference structures with different local atomic coordinations including tungsten carbide, W-H molecules, as well as H dissolved in bulk W. The potential has been tested in various scenarios, such as surface, defect, and melting properties, none of which were considered in the fitting. The intended area of application is simulations of hydrogen and hydrocarbon interactions with tungsten, which have a crucial role in fusion reactor plasma-wall interactions. Furthermore, this study shows that the angular-dependent bond-order scheme can be extended to second nearest-neighbor interactions, which are relevant in body-centered-cubic metals. Moreover, it provides a possibly general route for modeling metal carbides.

A global ab initio potential for HCN/HNC, exact vibrational energies, and comparison to experiment

NASA Technical Reports Server (NTRS)

Bentley, Joseph A.; Bowman, Joel M.; Gazdy, Bela; Lee, Timothy J.; Dateo, Christopher E.

1992-01-01

An ab initio (i.e., from first principles) calculation of vibrational energies of HCN and HNC is reported. The vibrational calculations were done with a new potential derived from a fit to 1124 ab initio electronic energies which were calculated using the highly accurate CCSD(T) coupled-cluster method in conjunction with a large atomic natural orbital basis set. The properties of this potential are presented, and the vibrational calculations are compared to experiment for 54 vibrational transitions, 39 of which are for zero total angular momentum, J = 0, and 15 of which are for J = 1. The level of agreement with experiment is unprecedented for a triatomic with two nonhydrogen atoms, and demonstrates the capability of the latest computational methods to give reliable predictions on a strongly bound triatomic molecule at very high levels of vibrational excitation.

Communication: Reactivity borrowing in the mode selective chemistry of H + CHD3 → H2 + CD3

NASA Astrophysics Data System (ADS)

Ellerbrock, Roman; Manthe, Uwe

2017-12-01

Quantum state-resolved reaction probabilities for the H + CHD3 → H2 + CD3 reaction are calculated by accurate full-dimensional quantum dynamics calculations using the multi-layer multi-configurational time-dependent Hartree approach and the quantum transition state concept. Reaction probabilities of various ro-vibrational states of the CHD3 reactant are investigated for vanishing total angular momentum. While the reactivity of the different vibrational states of CHD3 mostly follows intuitive patterns, an unusually large reaction probability is found for CHD3 molecules triply excited in the CD3 umbrella-bending vibration. This surprising reactivity can be explained by a Fermi resonance-type mixing of the single CH-stretch excited and the triple CD3 umbrella-bend excited vibrational states of CHD3. These findings show that resonant energy transfer can significantly affect the mode-selective chemistry of CHD3 and result in counter-intuitive reactivity patterns.

Mass-Selective Chiral Analysis

NASA Astrophysics Data System (ADS)

Boesl, Ulrich; Kartouzian, Aras

2016-06-01

Three ways of realizing mass-selective chiral analysis are reviewed. The first is based on the formation of diastereomers that are of homo- and hetero- type with respect to the enantiomers of involved chiral molecules. This way is quite well-established with numerous applications. The other two ways are more recent developments, both based on circular dichroism (CD). In one, conventional or nonlinear electronic CD is linked to mass spectrometry (MS) by resonance-enhanced multiphoton ionization. The other is based on CD in the angular distribution of photoelectrons, which is measured in combination with MS via photoion photoelectron coincidence. Among the many important applications of mass-selective chiral analysis, this review focuses on its use as an analytical tool for the development of heterogeneous enantioselective chemical catalysis. There exist other approaches to combine chiral analysis and mass-selective detection, such as chiral chromatography MS, which are not discussed here.

Stereodynamics in state-resolved scattering at the gas–liquid interface

PubMed Central

Perkins, Bradford G.; Nesbitt, David J.

2008-01-01

Stereodynamics at the gas–liquid interface provides insight into the important physical interactions that directly influence heterogeneous chemistry at the surface and within the bulk liquid. We investigate molecular beam scattering of CO2 from a liquid perfluoropolyether (PFPE) surface in vacuum [incident energy Einc = 10.6(8) kcal/mol, incident angle θinc = 60°] to specifically reveal rotational angular-momentum directions for scattered molecules. Experimentally, internal quantum state populations and MJ distributions are probed by high-resolution polarization-modulated infrared laser spectroscopy. Analysis of J-state populations reveals dual-channel scattering dynamics characterized by a two-temperature Boltzmann distribution for trapping–desorption and impulsive scattering. In addition, molecular dynamics simulations of CO2 + fluorinated self-assembled monolayers have been used to model CO2 + PFPE dynamics. Experimental results and molecular dynamics simulations reveal highly oriented CO2 distributions that preferentially scatter with “top spin” as a strongly increasing function of J state. PMID:18678907

Accurate quantum wave packet calculations for the F + HCl → Cl + HF reaction on the ground 1(2)A' potential energy surface.

PubMed

Bulut, Niyazi; Kłos, Jacek; Alexander, Millard H

2012-03-14

We present converged exact quantum wave packet calculations of reaction probabilities, integral cross sections, and thermal rate coefficients for the title reaction. Calculations have been carried out on the ground 1(2)A' global adiabatic potential energy surface of Deskevich et al. [J. Chem. Phys. 124, 224303 (2006)]. Converged wave packet reaction probabilities at selected values of the total angular momentum up to a partial wave of J = 140 with the HCl reagent initially selected in the v = 0, j = 0-16 rovibrational states have been obtained for the collision energy range from threshold up to 0.8 eV. The present calculations confirm an important enhancement of reactivity with rotational excitation of the HCl molecule. First, accurate integral cross sections and rate constants have been calculated and compared with the available experimental data.

Prediction of Lunar Reconnaissance Orbiter Reaction Wheel Assembly Angular Momentum Using Regression Analysis

NASA Technical Reports Server (NTRS)

DeHart, Russell

2017-01-01

This study determines the feasibility of creating a tool that can accurately predict Lunar Reconnaissance Orbiter (LRO) reaction wheel assembly (RWA) angular momentum, weeks or even months into the future. LRO is a three-axis stabilized spacecraft that was launched on June 18, 2009. While typically nadir-pointing, LRO conducts many types of slews to enable novel science collection. Momentum unloads have historically been performed approximately once every two weeks with the goal of maintaining system total angular momentum below 70 Nms; however flight experience shows the models developed before launch are overly conservative, with many momentum unloads being performed before system angular momentum surpasses 50 Nms. A more accurate model of RWA angular momentum growth would improve momentum unload scheduling and decrease the frequency of these unloads. Since some LRO instruments must be deactivated during momentum unloads and in the case of one instrument, decontaminated for 24 hours there after a decrease in the frequency of unloads increases science collection. This study develops a new model to predict LRO RWA angular momentum. Regression analysis of data from October 2014 to October 2015 was used to develop relationships between solar beta angle, slew specifications, and RWA angular momentum growth. The resulting model predicts RWA angular momentum using input solar beta angle and mission schedule data. This model was used to predict RWA angular momentum from October 2013 to October 2014. Predictions agree well with telemetry; of the 23 momentum unloads performed from October 2013 to October 2014, the mean and median magnitude of the RWA total angular momentum prediction error at the time of the momentum unloads were 3.7 and 2.7 Nms, respectively. The magnitude of the largest RWA total angular momentum prediction error was 10.6 Nms. Development of a tool that uses the models presented herein is currently underway.

On the structure and dynamics of the hydrated sulfite ion in aqueous solution--an ab initio QMCF MD simulation and large angle X-ray scattering study.

PubMed

Eklund, Lars; Hofer, Thomas S; Pribil, Andreas B; Rode, Bernd M; Persson, Ingmar

2012-05-07

Theoretical ab initio quantum mechanical charge field molecular dynamics (QMCF MD) formalism has been applied in conjunction to experimental large angle X-ray scattering to study the structure and dynamics of the hydrated sulfite ion in aqueous solution. The results show that there is a considerable effect of the lone electron-pair on sulfur concerning structure and dynamics in comparison with the sulfate ion with higher oxidation number and symmetry of the hydration shell. The S-O bond distance in the hydrated sulfite ion has been determined to 1.53(1) Å by both methods. The hydrogen bonds between the three water molecules bound to each sulfite oxygen are only slightly stronger than those in bulk water. The sulfite ion can therefore be regarded as a weak structure maker. The water exchange rate is somewhat slower for the sulfite ion than for the sulfate ion, τ(0.5) = 3.2 and 2.6 ps, respectively. An even more striking observation in the angular radial distribution (ARD) functions is that the for sulfite ion the water exchange takes place in close vicinity of the lone electron-pair directed at its sides, while in principle no water exchange did take place of the water molecules hydrogen bound to sulfite oxygens during the simulation time. This is also confirmed when detailed pathway analysis is conducted. The simulation showed that the water molecules hydrogen bound to the sulfite oxygens can move inside the hydration shell to the area outside the lone electron-pair and there be exchanged. On the other hand, for the hydrated sulfate ion in aqueous solution one can clearly see from the ARD that the distribution of exchange events is symmetrical around the entire hydration sphere.

An investigation of electronic states of some molecules and molecular cations using mass analyzed threshold ionization and photoinduced Rydberg ionization spectroscopy

NASA Astrophysics Data System (ADS)

Hofstein, Jason David

1999-11-01

Mass analyzed threshold ionization (MATI) experiments have enabled mapping of the n-dependent Rydberg state survival probability for a series of molecules. Utilizing vacuum and extreme ultraviolet (VUV/XUV) photons, one photon Rydberg manifold spectra of argon, hydrogen chloride, nitrogen, benzene, and oxygen were produced, and the prospects of photoinduced Rydberg ionization (PIRI) experiments examined. It was found that the widths of Rydberg manifolds for the molecules studied are quite different. Hydrogen chloride and nitrogen have the narrowest manifold width, followed by benzene, and then oxygen. These varying widths are most strongly correlated with the angular momentum (i.e., quantum defect) of the initially prepared Rydberg orbital. PIRI experiments required the use of a static cell, rather than a molecular jet assembly, for the more efficient production of higher amounts of VUV/XUV radiation, and hence more Rydberg signal needed to observe PIRI. Armed with the ability to produce tunable VUV/XUV radiation, and to determine the feasibility of a PIRI experiment, the MATI and fragment PIRI spectra of trans-1,3-butadiene (BD) were recorded. The MATI spectrum is vibrationally resolved and was analyzed with the help of ab initio calculations and other published results. The fragment PIRI spectrum of the A<==X transition of BD+ is not vibrationally resolved, but information regarding the wavelength dependence of fragmentation pathways has been gathered and interpreted. It was found that at low photodissociation photon energies, production of C3H3+ dominates, but at higher photon energies, C2H4 + is also produced. The production of each fragment showed a definite PIRI wavelength dependence.

Huygens-Fresnel picture for electron-molecule elastic scattering★

NASA Astrophysics Data System (ADS)

Baltenkov, Arkadiy S.; Msezane, Alfred Z.

2017-11-01

The elastic scattering cross sections for a slow electron by C2 and H2 molecules have been calculated within the framework of the non-overlapping atomic potential model. For the amplitudes of the multiple electron scattering by a target the wave function of the molecular continuum is represented as a combination of a plane wave and two spherical waves generated by the centers of atomic spheres. This wave function obeys the Huygens-Fresnel principle according to which the electron wave scattering by a system of two centers is accompanied by generation of two spherical waves; their interaction creates a diffraction pattern far from the target. Each of the Huygens waves, in turn, is a superposition of the partial spherical waves with different orbital angular momenta l and their projections m. The amplitudes of these partial waves are defined by the corresponding phases of electron elastic scattering by an isolated atomic potential. In numerical calculations the s- and p-phase shifts are taken into account. So the number of interfering electron waves is equal to eight: two of which are the s-type waves and the remaining six waves are of the p-type with different m values. The calculation of the scattering amplitudes in closed form (rather than in the form of S-matrix expansion) is reduced to solving a system of eight inhomogeneous algebraic equations. The differential and total cross sections of electron scattering by fixed-in-space molecules and randomly oriented ones have been calculated as well. We conclude by discussing the special features of the S-matrix method for the case of arbitrary non-spherical potentials. Contribution to the Topical Issue "Low energy positron and electron interactions", edited by James Sullivan, Ron White, Michael Bromley, Ilya Fabrikant, and David Cassidy.

Characteristics of energy exchange between inter- and intramolecular degrees of freedom in crystalline 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) with implications for coarse-grained simulations of shock waves in polyatomic molecular crystals

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

Kroonblawd, Matthew P.; Sewell, Thomas D., E-mail: sewellt@missouri.edu; Maillet, Jean-Bernard, E-mail: jean-bernard.maillet@cea.fr

2016-02-14

In this report, we characterize the kinetics and dynamics of energy exchange between intramolecular and intermolecular degrees of freedom (DoF) in crystalline 1,3,5-triamino-2,4,6-trinitrobenzene (TATB). All-atom molecular dynamics (MD) simulations are used to obtain predictions for relaxation from certain limiting initial distributions of energy between the intra- and intermolecular DoF. The results are used to parameterize a coarse-grained Dissipative Particle Dynamics at constant Energy (DPDE) model for TATB. Each TATB molecule in the DPDE model is represented as an all-atom, rigid-molecule mesoparticle, with explicit external (molecular translational and rotational) DoF and coarse-grained implicit internal (vibrational) DoF. In addition to conserving linearmore » and angular momentum, the DPDE equations of motion conserve the total system energy provided that particles can exchange energy between their external and internal DoF. The internal temperature of a TATB molecule is calculated using an internal equation of state, which we develop here, and the temperatures of the external and internal DoF are coupled using a fluctuation-dissipation relation. The DPDE force expression requires specification of the input parameter σ that determines the rate at which energy is exchanged between external and internal DoF. We adjusted σ based on the predictions for relaxation processes obtained from MD simulations. The parameterized DPDE model was employed in large-scale simulations of shock compression of TATB. We show that the rate of energy exchange governed by σ can significantly influence the transient behavior of the system behind the shock.« less

Why are ionic liquid ions mainly associated in water? A Car-Parrinello study of 1-ethyl-3-methyl-imidazolium chloride water mixture

NASA Astrophysics Data System (ADS)

Spickermann, C.; Thar, J.; Lehmann, S. B. C.; Zahn, S.; Hunger, J.; Buchner, R.; Hunt, P. A.; Welton, T.; Kirchner, B.

2008-09-01

In this study we present the results of a first principles molecular dynamics simulation of a single 1-ethyl-3-methyl-imidazolium chloride [C2C1im][Cl] ion pair dissolved in 60 water molecules. We observe a preference of the in plane chloride coordination with respect to the cation ring plane as compared to the energetic slightly more demanding on top coordination. Evaluation of the different radial distribution functions demonstrates that the structure of the hydration shell around the ion pair differs significantly from bulk water and that no true ion pair dissociation in terms of completely autonomous solvation shells takes place on the timescale of the simulation. In addition, dipole moment distributions of the solvent in distinct solvation shells around different functional parts of the [C2C1im][Cl] ion pair are calculated from maximally localized Wannier functions. The analysis of these distributions gives evidence for a depolarization of water molecules close to the hydrophobic parts of the cation as well as close to the anion. Examination of the angular distribution of different OH(H2O )-X angles in turn shows a linear coordination of chloride accompanied by a tangential orientation of water molecules around the hydrophobic groups, being a typical feature of hydrophobic hydration. Based on these orientational aspects, a structural model for the obvious preference of ion pair association is developed, which justifies the associating behavior of solvated [C2C1im][Cl] ions in terms of an energetically favorable interface between the solvation shells of the anion and the hydrophobic parts of the cation.

Why are ionic liquid ions mainly associated in water? A Car-Parrinello study of 1-ethyl-3-methyl-imidazolium chloride water mixture.

PubMed

Spickermann, C; Thar, J; Lehmann, S B C; Zahn, S; Hunger, J; Buchner, R; Hunt, P A; Welton, T; Kirchner, B

2008-09-14

In this study we present the results of a first principles molecular dynamics simulation of a single 1-ethyl-3-methyl-imidazolium chloride [C(2)C(1)im][Cl] ion pair dissolved in 60 water molecules. We observe a preference of the in plane chloride coordination with respect to the cation ring plane as compared to the energetic slightly more demanding on top coordination. Evaluation of the different radial distribution functions demonstrates that the structure of the hydration shell around the ion pair differs significantly from bulk water and that no true ion pair dissociation in terms of completely autonomous solvation shells takes place on the timescale of the simulation. In addition, dipole moment distributions of the solvent in distinct solvation shells around different functional parts of the [C(2)C(1)im][Cl] ion pair are calculated from maximally localized Wannier functions. The analysis of these distributions gives evidence for a depolarization of water molecules close to the hydrophobic parts of the cation as well as close to the anion. Examination of the angular distribution of different OH(H(2)O)-X angles in turn shows a linear coordination of chloride accompanied by a tangential orientation of water molecules around the hydrophobic groups, being a typical feature of hydrophobic hydration. Based on these orientational aspects, a structural model for the obvious preference of ion pair association is developed, which justifies the associating behavior of solvated [C(2)C(1)im][Cl] ions in terms of an energetically favorable interface between the solvation shells of the anion and the hydrophobic parts of the cation.

Towards a coherent view at infrared wavelengths of mass loss in Betelgeuse

NASA Astrophysics Data System (ADS)

Kervella, P.; Perrin, G.; Montargès, M.; Haubois, X.

2013-05-01

The violent convective motions, low surface gravity, and high brightness of red supergiants combine to trigger an intense stellar wind. As the distance from the star increases, the standard scenario is that the ejected material forms molecules, then dust particles. But this general picture is still fragmentary. Our goal is to assemble a better understanding of mass loss in Betelgeuse, considered as a prototype for its class, from its photosphere to the interface of its wind with the interstellar medium. Thanks to its proximity ( ≈ 197 pc), it is ideally suited for such a detailed study. Over the past few years, our team obtained an extensive set of observations of Betelgeuse from high angular resolution instruments, probing a broad range of spatial scales: 1) interferometric imaging of its photosphere and close envelope in the near- and thermal-IR domains (IOTA/IONIC), 2) adaptive optics "lucky imaging" of its compact molecular envelope (VLT/NACO, 1.0-2.2 μm), and 3) diffraction-limited imaging of its dusty envelope (VLT/VISIR, 8-20 μm). From our interferometric data, we detect the presence of spots at the surface of the star, as well as CO and H2O molecules, and dust particles close to the star. Within 6 R⋆, the flux distribution of the envelope is compatible with the presence of the CN molecule. At a few arcseconds from the central star, we observe a complex dusty envelope probably containing O-rich dust (e.g. silicates, alumina). We present an overview of these recent observational results and ongoing work. They provide new hints on the physical and chemical mechanisms through which Betelgeuse interacts with its environment.

Final Report for Department of Energy Project DE-SC0012198

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

Lucchese, Robert; Poliakoff, Erwin; Trallero-Herrero, Carlos

The study of the motion of atoms in molecules is important to understanding many areas of physical and life sciences. Such motion occurs on many different times scales, with electronic motion occurring on a sub-femtosecond time scale, and simple vibrational motion in tens to hundreds of femtoseconds. One way to follow such processes in real time is by the use of short-pulsed lasers, and in particular by studying time-resolved photoionization and the related process of high-harmonic generation (HHG). Thus there has been much effort to develop the tools necessary to probe molecular systems using short pulse lasers and understanding themore » sensitivity of the different possible probes to the time dependent geometric structure as well as the electronic structure of molecules. Our research has particularly focused on the connection between high-field processes and the more traditional weak field photoionization processes. Strong field and weak field processes can be connected through models that involve the same matrix elements. We have demonstrated in our study of HHG from SF6 that the spectrum is sensitive to the interplay between the angular dependence of the ionization step and recombination step. In our study of rescattering spectroscopy, we have shown that with a combination of experiment and theory, we can use this high-field spectroscopy to determine molecular structure in molecules such as C2H4. We have also developed new computational tools based on overset grids to enable studies on larger molecular systems which use much more robust numerical approaches so that the resulting code can be a tool that non-specialists can use to study related systems.« less

Angular multiplexing holograms of four images recorded on photopolymer films with recording-film-thickness-dependent holographic characteristics

NASA Astrophysics Data System (ADS)

Osabe, Keiichi; Kawai, Kotaro

2017-03-01

In this study, angular multiplexing hologram recording photopolymer films were studied experimentally. The films contained acrylamide as a monomer, eosin Y as a sensitizer, and triethanolamine as a promoter in a polyvinyl alcohol matrix. In order to determine the appropriate thickness of the photopolymer films for angular multiplexing, photopolymer films with thicknesses of 29-503 μm were exposed to two intersecting beams of a YVO laser at a wavelength of 532 nm to form a holographic grating with a spatial frequency of 653 line/mm. The diffraction efficiencies as a function of the incident angle of reconstruction were measured. A narrow angular bandwidth and high diffraction efficiency are required for angular multiplexing; hence, we define the Q value, which is the diffraction efficiency divided by half the bandwidth. The Q value of the films depended on the thickness of the films, and was calculated based on the measured diffraction efficiencies. The Q value of a 297-μm-thick film was the highest of the all films. Therefore, the angular multiplexing experiments were conducted using 300-μm-thick films. In the angular multiplexing experiments, the object beam transmitted by a square aperture was focused by a Fourier transform lens and interfered with a reference beam. The maximum order of angular multiplexing was four. The signal intensity that corresponds to the squared-aperture transmission and the noise intensity that corresponds to transmission without the square aperture were measured. The signal intensities decreased as the order of angular multiplexing increased, and the noise intensities were not dependent on the order of angular multiplexing.

A Detailed Motion Analysis of the Angular Velocity Between the Vocal Folds During Throat Clearing Using High-speed Digital Imaging.

PubMed

Iwahashi, Toshihiko; Ogawa, Makoto; Hosokawa, Kiyohito; Kato, Chieri; Inohara, Hidenori

2016-11-01

To assess the angular velocity between the vocal folds just before the compression phase of throat clearing (TC) using high-speed digital imaging (HSDI) of the larynx. Twenty normal healthy adults (13 males and seven females) were enrolled in the study. Each participant underwent transnasal laryngo-fiberscopy, and was asked to perform weak/strong TC followed by a comfortable, sustained vowel phonation while recording an HSDI movie (4000 frames/s) of the larynx. Using a motion analysis, the changes in the vocal fold angle and angular velocity during vocal fold adduction were assessed. Subsequently, we calculated the average angular velocities in the ranges of 100-80%, 80-20%, and 20-0% from all of the angular changes. The motion analysis demonstrated that the changes in the angular velocity resulted in polynomial-like and sigmoid curves during TC and vowel phonation, respectively. The angular velocities during weak TC were significantly higher in the 20-0%, 80-20%, and 100-80% regions (in order); the 80-20% angular velocity in vocal fold adduction during phonation was highest. The 20-0% angular velocity during strong TC was more than twofold higher than 20-0% angular velocity during phonation. The present results confirmed that the closing motions of the vocal folds accelerate throughout the precompression closing phase of a TC episode, and decelerate just before the impact between the vocal folds at the onset of phonation, suggesting that the vocal fold velocity generated by TC is sufficient to damage the laryngeal tissues. Copyright © 2016 The Voice Foundation. Published by Elsevier Inc. All rights reserved.

Jet angularity measurements for single inclusive jet production

NASA Astrophysics Data System (ADS)

Kang, Zhong-Bo; Lee, Kyle; Ringer, Felix

2018-04-01

We study jet angularity measurements for single-inclusive jet production at the LHC. Jet angularities depend on a continuous parameter a allowing for a smooth interpolation between different traditional jet shape observables. We establish a factorization theorem within Soft Collinear Effective Theory (SCET) where we consistently take into account in- and out-of-jet radiation by making use of semi-inclusive jet functions. For comparison, we elaborate on the differences to jet angularities measured on an exclusive jet sample. All the necessary ingredients for the resummation at next-to-leading logarithmic (NLL) accuracy are presented within the effective field theory framework. We expect semiinclusive jet angularity measurements to be feasible at the LHC and we present theoretical predictions for the relevant kinematic range. In addition, we investigate the potential impact of jet angularities for quark-gluon discrimination.

A new open-loop fiber optic gyro error compensation method based on angular velocity error modeling.

PubMed

Zhang, Yanshun; Guo, Yajing; Li, Chunyu; Wang, Yixin; Wang, Zhanqing

2015-02-27

With the open-loop fiber optic gyro (OFOG) model, output voltage and angular velocity can effectively compensate OFOG errors. However, the model cannot reflect the characteristics of OFOG errors well when it comes to pretty large dynamic angular velocities. This paper puts forward a modeling scheme with OFOG output voltage u and temperature T as the input variables and angular velocity error Δω as the output variable. Firstly, the angular velocity error Δω is extracted from OFOG output signals, and then the output voltage u, temperature T and angular velocity error Δω are used as the learning samples to train a Radial-Basis-Function (RBF) neural network model. Then the nonlinear mapping model over T, u and Δω is established and thus Δω can be calculated automatically to compensate OFOG errors according to T and u. The results of the experiments show that the established model can be used to compensate the nonlinear OFOG errors. The maximum, the minimum and the mean square error of OFOG angular velocity are decreased by 97.0%, 97.1% and 96.5% relative to their initial values, respectively. Compared with the direct modeling of gyro angular velocity, which we researched before, the experimental results of the compensating method proposed in this paper are further reduced by 1.6%, 1.4% and 1.42%, respectively, so the performance of this method is better than that of the direct modeling for gyro angular velocity.

A New Open-Loop Fiber Optic Gyro Error Compensation Method Based on Angular Velocity Error Modeling

PubMed Central

Zhang, Yanshun; Guo, Yajing; Li, Chunyu; Wang, Yixin; Wang, Zhanqing

2015-01-01

With the open-loop fiber optic gyro (OFOG) model, output voltage and angular velocity can effectively compensate OFOG errors. However, the model cannot reflect the characteristics of OFOG errors well when it comes to pretty large dynamic angular velocities. This paper puts forward a modeling scheme with OFOG output voltage u and temperature T as the input variables and angular velocity error Δω as the output variable. Firstly, the angular velocity error Δω is extracted from OFOG output signals, and then the output voltage u, temperature T and angular velocity error Δω are used as the learning samples to train a Radial-Basis-Function (RBF) neural network model. Then the nonlinear mapping model over T, u and Δω is established and thus Δω can be calculated automatically to compensate OFOG errors according to T and u. The results of the experiments show that the established model can be used to compensate the nonlinear OFOG errors. The maximum, the minimum and the mean square error of OFOG angular velocity are decreased by 97.0%, 97.1% and 96.5% relative to their initial values, respectively. Compared with the direct modeling of gyro angular velocity, which we researched before, the experimental results of the compensating method proposed in this paper are further reduced by 1.6%, 1.4% and 1.2%, respectively, so the performance of this method is better than that of the direct modeling for gyro angular velocity. PMID:25734642

Closed-form integrator for the quaternion (euler angle) kinematics equations

NASA Technical Reports Server (NTRS)

Whitmore, Stephen A. (Inventor)

2000-01-01

The invention is embodied in a method of integrating kinematics equations for updating a set of vehicle attitude angles of a vehicle using 3-dimensional angular velocities of the vehicle, which includes computing an integrating factor matrix from quantities corresponding to the 3-dimensional angular velocities, computing a total integrated angular rate from the quantities corresponding to a 3-dimensional angular velocities, computing a state transition matrix as a sum of (a) a first complementary function of the total integrated angular rate and (b) the integrating factor matrix multiplied by a second complementary function of the total integrated angular rate, and updating the set of vehicle attitude angles using the state transition matrix. Preferably, the method further includes computing a quanternion vector from the quantities corresponding to the 3-dimensional angular velocities, in which case the updating of the set of vehicle attitude angles using the state transition matrix is carried out by (a) updating the quanternion vector by multiplying the quanternion vector by the state transition matrix to produce an updated quanternion vector and (b) computing an updated set of vehicle attitude angles from the updated quanternion vector. The first and second trigonometric functions are complementary, such as a sine and a cosine. The quantities corresponding to the 3-dimensional angular velocities include respective averages of the 3-dimensional angular velocities over plural time frames. The updating of the quanternion vector preserves the norm of the vector, whereby the updated set of vehicle attitude angles are virtually error-free.

Design and Calibration of the ARL Mach 3 High Reynolds Number Facility

DTIC Science & Technology

1975-01-01

degrees Rankine. Test rhombus determinations included lateral and longitudinal Mach number distributions and flow angularity measurements. A...43 3. THE TUNNEL EMPTY MACH NUMBER DISTRIBUTION 45 4. THE CENTERLINE RMS MACH NUMBER 46 5. FLOW ANGULARITY MEASUREMENTS 46 6. BLOCKAGE TESTS... Angularity Wedge Scale Drawing of Flow Angularity Cone Normalized Surface Pressure Difference versus Angle of Attack at xp/xr = - 0.690 for po

On Angular Momentum

DOE R&D Accomplishments Database

Schwinger, J.

1952-01-26

The commutation relations of an arbitrary angular momentum vector can be reduced to those of the harmonic oscillator. This provides a powerful method for constructing and developing the properties of angular momentum eigenvectors. In this paper many known theorems are derived in this way, and some new results obtained. Among the topics treated are the properties of the rotation matrices; the addition of two, three, and four angular momenta; and the theory of tensor operators.

GALACTIC ANGULAR MOMENTUM IN THE ILLUSTRIS SIMULATION: FEEDBACK AND THE HUBBLE SEQUENCE

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

Genel, Shy; Fall, S. Michael; Snyder, Gregory F.

We study the stellar angular momentum of thousands of galaxies in the Illustris cosmological simulation, which captures gravitational and gas dynamics within galaxies, as well as feedback from stars and black holes. We find that the angular momentum of the simulated galaxies matches observations well, and in particular two distinct relations are found for late-type versus early-type galaxies. The relation for late-type galaxies corresponds to the value expected from full conservation of the specific angular momentum generated by cosmological tidal torques. The relation for early-type galaxies corresponds to retention of only ∼30% of that, but we find that those early-typemore » galaxies with low angular momentum at z = 0 nevertheless reside at high redshift on the late-type relation. Some of them abruptly lose angular momentum during major mergers. To gain further insight, we explore the scaling relations in simulations where the galaxy formation physics is modified with respect to the fiducial model. We find that galactic winds with high mass-loading factors are essential for obtaining the high angular momentum relation typical for late-type galaxies, while active galactic nucleus feedback largely operates in the opposite direction. Hence, feedback controls the stellar angular momentum of galaxies, and appears to be instrumental for establishing the Hubble sequence.« less

Optimal simulations of ultrasonic fields produced by large thermal therapy arrays using the angular spectrum approach

PubMed Central

Zeng, Xiaozheng; McGough, Robert J.

2009-01-01

The angular spectrum approach is evaluated for the simulation of focused ultrasound fields produced by large thermal therapy arrays. For an input pressure or normal particle velocity distribution in a plane, the angular spectrum approach rapidly computes the output pressure field in a three dimensional volume. To determine the optimal combination of simulation parameters for angular spectrum calculations, the effect of the size, location, and the numerical accuracy of the input plane on the computed output pressure is evaluated. Simulation results demonstrate that angular spectrum calculations performed with an input pressure plane are more accurate than calculations with an input velocity plane. Results also indicate that when the input pressure plane is slightly larger than the array aperture and is located approximately one wavelength from the array, angular spectrum simulations have very small numerical errors for two dimensional planar arrays. Furthermore, the root mean squared error from angular spectrum simulations asymptotically approaches a nonzero lower limit as the error in the input plane decreases. Overall, the angular spectrum approach is an accurate and robust method for thermal therapy simulations of large ultrasound phased arrays when the input pressure plane is computed with the fast nearfield method and an optimal combination of input parameters. PMID:19425640

Demonstrating the conservation of angular momentum using spherical magnets

NASA Astrophysics Data System (ADS)

Lindén, Johan; Slotte, Joakim; Källman, Kjell-Mikael

2018-01-01

An experimental setup for demonstrating the conservation of angular momentum of rotating spherical magnets is described. Two spherical Nd-Fe-B magnets are placed on a double inclined plane and projected towards each other with pre-selected impact parameters ranging from zero to a few tens of millimeters. After impact, the two magnets either revolve vigorously around the common center of mass or stop immediately, depending on the value of the impact parameter. Using a pick-up coil connected to an oscilloscope, the angular frequency for the rotating magnets was measured, and an estimate for the angular momentum was obtained. A high-speed video camera captured the impact and was used for measuring linear and angular velocities of the magnets. A very good agreement between the initial angular momentum before the impact and the final angular momentum of the revolving dumbbell is observed. The two rotating magnets, and the rotating electromagnetic field emanating from them, can also be viewed as a toy model for the newly discovered gravitational waves, where two black holes collide after revolving around each other. (Enhanced online)

Professional tennis players' serve: correlation between segmental angular momentums and ball velocity.

PubMed

Martin, Caroline; Kulpa, Richard; Delamarche, Paul; Bideau, Benoit

2013-03-01

The purpose of the study was to identify the relationships between segmental angular momentum and ball velocity between the following events: ball toss, maximal elbow flexion (MEF), racket lowest point (RLP), maximal shoulder external rotation (MER), and ball impact (BI). Ten tennis players performed serves recorded with a real-time motion capture. Mean angular momentums of the trunk, upper arm, forearm, and the hand-racket were calculated. The anteroposterior axis angular momentum of the trunk was significantly related with ball velocity during the MEF-RLP, RLP-MER, and MER-BI phases. The strongest relationships between the transverse-axis angular momentums and ball velocity followed a proximal-to-distal timing sequence that allows the transfer of angular momentum from the trunk (MEF-RLP and RLP-MER phases) to the upper arm (RLP-MER phase), forearm (RLP-MER and MER-BI phases), and the hand-racket (MER-BI phase). Since sequence is crucial for ball velocity, players should increase angular momentums of the trunk during MEF-MER, upper arm during RLP-MER, forearm during RLP-BI, and the hand-racket during MER-BI.

Angular Rate Sensing with GyroWheel Using Genetic Algorithm Optimized Neural Networks.

PubMed

Zhao, Yuyu; Zhao, Hui; Huo, Xin; Yao, Yu

2017-07-22

GyroWheel is an integrated device that can provide three-axis control torques and two-axis angular rate sensing for small spacecrafts. Large tilt angle of its rotor and de-tuned spin rate lead to a complex and non-linear dynamics as well as difficulties in measuring angular rates. In this paper, the problem of angular rate sensing with the GyroWheel is investigated. Firstly, a simplified rate sensing equation is introduced, and the error characteristics of the method are analyzed. According to the analysis results, a rate sensing principle based on torque balance theory is developed, and a practical way to estimate the angular rates within the whole operating range of GyroWheel is provided by using explicit genetic algorithm optimized neural networks. The angular rates can be determined by the measurable values of the GyroWheel (including tilt angles, spin rate and torque coil currents), the weights and the biases of the neural networks. Finally, the simulation results are presented to illustrate the effectiveness of the proposed angular rate sensing method with GyroWheel.

Forming Disc Galaxies In Major Mergers: Radial Density Profiles And Angular Momentum

NASA Astrophysics Data System (ADS)

Peschken, Nicolas; Athanassoula, E.; Rodionov, S. A.; Lambert, J. C.

2017-06-01

In Athanassoula et al. (2016), we used high resolution N-body hydrodynamical simulations to model the major merger between two disc galaxies with a hot gaseous halo each, and showed that the remnant is a spiral galaxy. The two discs are destroyed by the collision, but after the merger, accretion from the surrounding gaseous halo allows the building of a new disc in the remnant galaxy. In Peschken et al. (2017), we used these simulations to study the radial surface density profiles of the remnant galaxies with downbending profiles (type II), i.e. composed of an inner and an outer exponential disc separated by a break. We analyzed the effect of angular momentum on these profiles, and found that the inner and outer disc scalelengths, as well as the break radius, all increase linearly with the total angular momentum of the initial merging system. Following the angular momentum redistribution in our simulations, we find that the disc angular momentum is acquired via accretion from the gaseous halo. Furthermore, high angular momentum systems give more angular momentum to their discs, which affects directly their radial density profile.

Effects of aggregate angularity on mix design characteristics and pavement performance.

DOT National Transportation Integrated Search

2009-12-01

This research targeted two primary purposes: to estimate current aggregate angularity test methods and to evaluate current : aggregate angularity requirements in the Nebraska asphalt mixture/pavement specification. To meet the first research : object...

Thermal Ion Upwelling in the High-Altitude Ionosphere

DTIC Science & Technology

1990-01-01

hard sphere collisions) while Vst is the momentum transfer collision frequency between all the other species t and a single s species particle. For... angular dimensions of day side entrance region off of Od degrees towards evening Od angular dimensions of day side entrance region off of 0d...degrees towards morning + angular dimensions of night side exit region off of on towards degrees On degre morning On angular dimensions of night side exit

Angular width of the Cherenkov radiation with inclusion of multiple scattering

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

Zheng, Jian, E-mail: jzheng@ustc.edu.cn

2016-06-15

Visible Cherenkov radiation can offer a method of the measurement of the velocity of charged particles. The angular width of the radiation is important since it determines the resolution of the velocity measurement. In this article, the angular width of Cherenkov radiation with inclusion of multiple scattering is calculated through the path-integral method, and the analytical expressions are presented. The condition that multiple scattering processes dominate the angular distribution is obtained.

Interpreting angular momentum transfer between electromagnetic multipoles using vector spherical harmonics.

PubMed

Grinter, Roger; Jones, Garth A

2018-02-01

The transfer of angular momentum between a quadrupole emitter and a dipole acceptor is investigated theoretically. Vector spherical harmonics are used to describe the angular part of the field of the mediating photon. Analytical results are presented for predicting angular momentum transfer between the emitter and absorber within a quantum electrodynamical framework. We interpret the allowability of such a process, which appears to violate conservation of angular momentum, in terms of the breakdown of the isotropy of space at the point of photon absorption (detection). That is, collapse of the wavefunction results in loss of all angular momentum information. This is consistent with Noether's Theorem and demystifies some common misconceptions about the nature of the photon. The results have implications for interpreting the detection of photons from multipole sources and offers insight into limits on information that can be extracted from quantum measurements in photonic systems.

Creating high-purity angular-momentum-state Rydberg atoms by a pair of unipolar laser pulses

NASA Astrophysics Data System (ADS)

Xin, PeiPei; Cheng, Hong; Zhang, ShanShan; Wang, HanMu; Xu, ZiShan; Liu, HongPing

2018-04-01

We propose a method of producing high-purity angular-momentum-state Rydberg atoms by a pair of unipolar laser pulses. The first positive-polarity optical half-cycle pulse is used to prepare an excited-state wave packet while the second one is less intense, but with opposite polarity and time delayed, and is employed to drag back the escaping free electron and clip the shape of the bound Rydberg wave packet, selectively increasing or decreasing a fraction of the angular-momentum components. An intelligent choice of laser parameters such as phase and amplitude helps us to control the orbital-angular-momentum composition of an electron wave packet with more facility; thus, a specified angular-momentum state with high purity can be achieved. This scheme of producing high-purity angular-momentum-state Rydberg atoms has significant application in quantum-information processing.

Angular momentum conservation law in light-front quantum field theory

DOE PAGES

Chiu, Kelly Yu-Ju; Brodsky, Stanley J.

2017-03-31

We prove the Lorentz invariance of the angular momentum conservation law and the helicity sum rule for relativistic composite systems in the light-front formulation. We explicitly show that j 3, the z -component of the angular momentum remains unchanged under Lorentz transformations generated by the light-front kinematical boost operators. The invariance of j 3 under Lorentz transformations is a feature unique to the front form. Applying the Lorentz invariance of the angular quantum number in the front form, we obtain a selection rule for the orbital angular momentum which can be used to eliminate certain interaction vertices in QED andmore » QCD. We also generalize the selection rule to any renormalizable theory and show that there exists an upper bound on the change of orbital angular momentum in scattering processes at any fixed order in perturbation theory.« less

Aliasing Detection and Reduction Scheme on Angularly Undersampled Light Fields.

PubMed

Xiao, Zhaolin; Wang, Qing; Zhou, Guoqing; Yu, Jingyi

2017-05-01

When using plenoptic camera for digital refocusing, angular undersampling can cause severe (angular) aliasing artifacts. Previous approaches have focused on avoiding aliasing by pre-processing the acquired light field via prefiltering, demosaicing, reparameterization, and so on. In this paper, we present a different solution that first detects and then removes angular aliasing at the light field refocusing stage. Different from previous frequency domain aliasing analysis, we carry out a spatial domain analysis to reveal whether the angular aliasing would occur and uncover where in the image it would occur. The spatial analysis also facilitates easy separation of the aliasing versus non-aliasing regions and angular aliasing removal. Experiments on both synthetic scene and real light field data sets (camera array and Lytro camera) demonstrate that our approach has a number of advantages over the classical prefiltering and depth-dependent light field rendering techniques.

Gait event detection using linear accelerometers or angular velocity transducers in able-bodied and spinal-cord injured individuals.

PubMed

Jasiewicz, Jan M; Allum, John H J; Middleton, James W; Barriskill, Andrew; Condie, Peter; Purcell, Brendan; Li, Raymond Che Tin

2006-12-01

We report on three different methods of gait event detection (toe-off and heel strike) using miniature linear accelerometers and angular velocity transducers in comparison to using standard pressure-sensitive foot switches. Detection was performed with normal and spinal-cord injured subjects. The detection of end contact (EC), normally toe-off, and initial contact (IC) normally, heel strike was based on either foot linear accelerations or foot sagittal angular velocity or shank sagittal angular velocity. The results showed that all three methods were as accurate as foot switches in estimating times of IC and EC for normal gait patterns. In spinal-cord injured subjects, shank angular velocity was significantly less accurate (p<0.02). We conclude that detection based on foot linear accelerations or foot angular velocity can correctly identify the timing of IC and EC events in both normal and spinal-cord injured subjects.

Angular momentum conservation law in light-front quantum field theory

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

Chiu, Kelly Yu-Ju; Brodsky, Stanley J.

We prove the Lorentz invariance of the angular momentum conservation law and the helicity sum rule for relativistic composite systems in the light-front formulation. We explicitly show that j 3, the z -component of the angular momentum remains unchanged under Lorentz transformations generated by the light-front kinematical boost operators. The invariance of j 3 under Lorentz transformations is a feature unique to the front form. Applying the Lorentz invariance of the angular quantum number in the front form, we obtain a selection rule for the orbital angular momentum which can be used to eliminate certain interaction vertices in QED andmore » QCD. We also generalize the selection rule to any renormalizable theory and show that there exists an upper bound on the change of orbital angular momentum in scattering processes at any fixed order in perturbation theory.« less

Angular momentum conservation law in light-front quantum field theory

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

Chiu, Kelly Yu-Ju; Brodsky, Stanley J.

We prove the Lorentz invariance of the angular momentum conservation law and the helicity sum rule for relativistic composite systems in the light-front formulation. We explicitly show that j 3 , the z -component of the angular momentum remains unchanged under Lorentz transformations generated by the light-front kinematical boost operators. The invariance of j 3 under Lorentz transformations is a feature unique to the front form. Applying the Lorentz invariance of the angular quantum number in the front form, we obtain a selection rule for the orbital angular momentum which can be used to eliminate certain interaction vertices in QEDmore » and QCD. We also generalize the selection rule to any renormalizable theory and show that there exists an upper bound on the change of orbital angular momentum in scattering processes at any fixed order in perturbation theory.« less

Light's Darkness

ScienceCinema

Padgett, Miles [University of Glasgow, Glasgow, Scotland

2017-12-09

Optical vortices and orbital angular momentum are currently topical subjects in the optics literature. Although seemingly esoteric, they are, in fact, the generic state of light and arise whenever three or more plane waves interfere. To be observed by eye the light must be monochromatic. Laser speckle is one such example, where the optical energy circulates around each black spot, giving a local orbital angular momentum. This talk with report three on-going studies. First, when considering a volume of interfering waves, the laser specs map out threads of complete darkness embedded in the light. Do these threads form loops? Links? Or even knots? Second, when looking through a rapidly spinning window, the image of the world on the other side is rotated: true or false? Finally, the entanglement of orbital angular momentum states means measuring how the angular position of one photons sets the angular momentum of another: is this an angular version of the EPR (Einstein, Podolsky, and Rosen) paradox?

Large-visual-angle microstructure inspired from quantitative design of Morpho butterflies' lamellae deviation using the FDTD/PSO method.

PubMed

Wang, Wanlin; Zhang, Wang; Chen, Weixin; Gu, Jiajun; Liu, Qinglei; Deng, Tao; Zhang, Di

2013-01-15

The wide angular range of the treelike structure in Morpho butterfly scales was investigated by finite-difference time-domain (FDTD)/particle-swarm-optimization (PSO) analysis. Using the FDTD method, different parameters in the Morpho butterflies' treelike structure were studied and their contributions to the angular dependence were analyzed. Then a wide angular range was realized by the PSO method from quantitatively designing the lamellae deviation (Δy), which was a crucial parameter with angular range. The field map of the wide-range reflection in a large area was given to confirm the wide angular range. The tristimulus values and corresponding color coordinates for various viewing directions were calculated to confirm the blue color in different observation angles. The wide angular range realized by the FDTD/PSO method will assist us in understanding the scientific principles involved and also in designing artificial optical materials.

Optical and microwave control of resonance fluorescence and squeezing spectra in a polar molecule

NASA Astrophysics Data System (ADS)

Antón, M. A.; Maede-Razavi, S.; Carreño, F.; Thanopulos, I.; Paspalakis, E.

2017-12-01

A two-level quantum emitter with broken inversion symmetry simultaneously driven by an optical field and a microwave field that couples to the permanent dipole's moment is presented. We focus to a situation where the angular frequency of the microwave field is chosen such that it closely matches the Rabi frequency of the optical field, the so-called Rabi resonance condition. Using a series of unitary transformations we obtain an effective Hamiltonian in the double-dressed basis which results in easily solvable Bloch equations which allow us to derive analytical expressions for the spectrum of the scattered photons. We analyze the steady-state population inversion of the system which shows a distinctive behavior at the Rabi resonance with regard to an ordinary two-level nonpolar system. We show that saturation can be produced even in the case that the optical field is far detuned from the transition frequency, and we demonstrate that this behavior can be controlled through the intensity and the angular frequency of the microwave field. The spectral properties of the scattered photons are analyzed and manifest the emergence of a series of Mollow-like triplets which may be spectrally broadened or narrowed for proper values of the amplitude and/or frequency of the low-frequency field. We also analyze the phase-dependent spectrum which reveals that a significant enhancement or suppression of the squeezing at certain sidebands can be produced. These quantum phenomena are illustrated in a recently synthesized molecular complex with high nonlinear optical response although they can also occur in other quantum systems with broken inversion symmetry.

Wind and Temperature Spectrometry of the Upper Atmosphere in Low-Earth Orbit

NASA Technical Reports Server (NTRS)

Herrero, Federico

2011-01-01

Wind and Temperature Spectrometry (WATS) is a new approach to measure the full wind vector, temperature, and relative densities of major neutral species in the Earth's thermosphere. The method uses an energy-angle spectrometer moving through the tenuous upper atmosphere to measure directly the angular and energy distributions of the air stream that enters the spectrometer. The angular distribution gives the direction of the total velocity of the air entering the spectrometer, and the energy distribution gives the magnitude of the total velocity. The wind velocity vector is uniquely determined since the measured total velocity depends on the wind vector and the orbiting velocity vector. The orbiting spectrometer moves supersonically, Mach 8 or greater, through the air and must point within a few degrees of its orbital velocity vector (the ram direction). Pointing knowledge is critical; for example, pointing errors 0.1 lead to errors of about 10 m/s in the wind. The WATS method may also be applied without modification to measure the ion-drift vector, ion temperature, and relative ion densities of major ionic species in the ionosphere. In such an application it may be called IDTS: Ion-Drift Temperature Spectrometry. A spectrometer-based coordinate system with one axis instantaneously pointing along the ram direction makes it possible to transform the Maxwellian velocity distribution of the air molecules to a Maxwellian energy-angle distribution for the molecular flux entering the spectrometer. This implementation of WATS is called the gas kinetic method (GKM) because it is applied to the case of the Maxwellian distribution. The WATS method follows from the recognition that in a supersonic platform moving at 8,000 m/s, the measurement of small wind velocities in the air on the order of a few 100 m/s and less requires precise knowledge of the angle of incidence of the neutral atoms and molecules. The same is true for the case of ion-drift measurements. WATS also provides a general approach that can obtain non-equilibrium distributions as may exist in the upper regions of the thermosphere, above 500 km and into the exosphere. Finally, WATS serves as a mass spectrometer, with very low mass resolution of roughly 1 part in 3, but easily separating atomic oxygen from molecular nitrogen.

Whole-body angular momentum during stair walking using passive and powered lower-limb prostheses.

PubMed

Pickle, Nathaniel T; Wilken, Jason M; Aldridge, Jennifer M; Neptune, Richard R; Silverman, Anne K

2014-10-17

Individuals with a unilateral transtibial amputation have a greater risk of falling compared to able-bodied individuals, and falling on stairs can lead to serious injuries. Individuals with transtibial amputations have lost ankle plantarflexor muscle function, which is critical for regulating whole-body angular momentum to maintain dynamic balance. Recently, powered prostheses have been designed to provide active ankle power generation with the goal of restoring biological ankle function. However, the effects of using a powered prosthesis on the regulation of whole-body angular momentum are unknown. The purpose of this study was to use angular momentum to evaluate dynamic balance in individuals with a transtibial amputation using powered and passive prostheses relative to able-bodied individuals during stair ascent and descent. Ground reaction forces, external moment arms, and joint powers were also investigated to interpret the angular momentum results. A key result was that individuals with an amputation had a larger range of sagittal-plane angular momentum during prosthetic limb stance compared to able-bodied individuals during stair ascent. There were no significant differences in the frontal, transverse, or sagittal-plane ranges of angular momentum or maximum magnitude of the angular momentum vector between the passive and powered prostheses during stair ascent or descent. These results indicate that individuals with an amputation have altered angular momentum trajectories during stair walking compared to able-bodied individuals, which may contribute to an increased fall risk. The results also suggest that a powered prosthesis provides no distinct advantage over a passive prosthesis in maintaining dynamic balance during stair walking. Copyright © 2014 Elsevier Ltd. All rights reserved.

Forming disc galaxies in major mergers - III. The effect of angular momentum on the radial density profiles of disc galaxies

NASA Astrophysics Data System (ADS)

Peschken, N.; Athanassoula, E.; Rodionov, S. A.

2017-06-01

We study the effect of angular momentum on the surface density profiles of disc galaxies, using high-resolution simulations of major mergers whose remnants have downbending radial density profiles (type II). As described in the previous papers of this series, in this scenario, most of the disc mass is acquired after the collision via accretion from a hot gaseous halo. We find that the inner and outer disc scalelengths, as well as the break radius, correlate with the total angular momentum of the initial merging system, and are larger for high-angular momentum systems. We follow the angular momentum redistribution in our simulated galaxies, and find that like the mass, the disc angular momentum is acquired via accretion, I.e. to the detriment of the gaseous halo. Furthermore, high-angular momentum systems give more angular momentum to their discs, which directly affects their radial density profile. Adding simulations of isolated galaxies to our sample, we find that the correlations are valid also for disc galaxies evolved in isolation. We show that the outer part of the disc at the end of the simulation is populated mainly by inside-out stellar migration, and that in galaxies with higher angular momentum, stars travel radially further out. This, however, does not mean that outer disc stars (in type II discs) were mostly born in the inner disc. Indeed, generally the break radius increases over time, and not taking this into account leads to overestimating the number of stars born in the inner disc.

Avoiding fractional electrons in subsystem DFT based ab-initio molecular dynamics yields accurate models for liquid water and solvated OH radical

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

Genova, Alessandro, E-mail: alessandro.genova@rutgers.edu; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu; Ceresoli, Davide, E-mail: davide.ceresoli@cnr.it

2016-06-21

In this work we achieve three milestones: (1) we present a subsystem DFT method capable of running ab-initio molecular dynamics simulations accurately and efficiently. (2) In order to rid the simulations of inter-molecular self-interaction error, we exploit the ability of semilocal frozen density embedding formulation of subsystem DFT to represent the total electron density as a sum of localized subsystem electron densities that are constrained to integrate to a preset, constant number of electrons; the success of the method relies on the fact that employed semilocal nonadditive kinetic energy functionals effectively cancel out errors in semilocal exchange–correlation potentials that aremore » linked to static correlation effects and self-interaction. (3) We demonstrate this concept by simulating liquid water and solvated OH{sup •} radical. While the bulk of our simulations have been performed on a periodic box containing 64 independent water molecules for 52 ps, we also simulated a box containing 256 water molecules for 22 ps. The results show that, provided one employs an accurate nonadditive kinetic energy functional, the dynamics of liquid water and OH{sup •} radical are in semiquantitative agreement with experimental results or higher-level electronic structure calculations. Our assessments are based upon comparisons of radial and angular distribution functions as well as the diffusion coefficient of the liquid.« less

Energetic ion, atom, and molecule reactions and excitation in low-current H2 discharges: H(alpha) Doppler profiles.

PubMed

Petrović, Z Lj; Phelps, A V

2009-12-01

Absolute spectral emissivities for Doppler broadened H(alpha) profiles are measured and compared with predictions of energetic hydrogen ion, atom, and molecule behavior in low-current electrical discharges in H2 at very high electric field E to gas density N ratios E/N and low values of Nd , where d is the parallel-plate electrode separation. These observations reflect the energy and angular distributions for the excited atoms and quantitatively test features of multiple-scattering kinetic models in weakly ionized hydrogen in the presence of an electric field that are not tested by the spatial distributions of H(alpha) emission. Absolute spectral intensities agree well with predictions. Asymmetries in Doppler profiles observed parallel to the electric field at 4

Effect of hockey-stick-shaped molecules on the critical behavior at the nematic to isotropic and smectic-A to nematic phase transitions in octylcyanobiphenyl

NASA Astrophysics Data System (ADS)

Chakraborty, Anish; Chakraborty, Susanta; Das, Malay Kumar

2015-03-01

In the field of soft matter research, the characteristic behavior of both nematic-isotropic (N -I ) and smectic-A nematic (Sm -A N ) phase transitions has gained considerable attention due to their several attractive features. In this work, a high-resolution measurement of optical birefringence (Δ n ) has been performed to probe the critical behavior at the N -I and Sm -A N phase transitions in a binary system comprising the rodlike octylcyanobiphenyl and a laterally methyl substituted hockey-stick-shaped mesogen, 4-(3-n -decyloxy-2-methyl-phenyliminomethyl)phenyl 4-n -dodecyloxycinnamate. For the investigated mixtures, the critical exponent β related to the limiting behavior of the nematic order parameter close to the N -I phase transition has come out to be in good conformity with the tricritical hypothesis. Moreover, the yielded effective critical exponents (α', β', γ') characterizing the critical fluctuation near the Sm -A N phase transition have appeared to be nonuniversal in nature. With increasing hockey-stick-shaped dopant concentration, the Sm -A N phase transition demonstrates a strong tendency to be driven towards a first-order nature. Such a behavior has been accounted for by considering a modification of the effective intermolecular interactions and hence the related coupling between the nematic and smectic order parameters, caused by the introduction of the angular mesogenic molecules.

Photoabsorption and S 2p photoionization of the SF6 molecule: resonances in the excitation energy range of 200-280 eV.

PubMed

Stener, M; Bolognesi, P; Coreno, M; O'Keeffe, P; Feyer, V; Fronzoni, G; Decleva, P; Avaldi, L; Kivimäki, A

2011-05-07

Photoabsorption and S 2p photoionization of the SF(6) molecule have been studied experimentally and theoretically in the excitation energy range up to 100 eV above the S 2p ionization potentials. In addition to the well-known 2t(2g) and 4e(g) shape resonances, the spin-orbit-resolved S 2p photoionization cross sections display two weak resonances between 200 and 210 eV, a wide resonance around 217 eV, a Fano-type resonance around 240 eV, and a second wide resonance around 260 eV. Calculations based on time-dependent density functional theory allow us to assign the 217-eV and 260-eV features to the shape resonances in S 2p photoionization. The Fano resonance is caused by the interference between the direct S 2p photoionization channel and the resonant channel that results from the participator decay of the S 2s(-1)6t(1u) excited state. The weak resonances below 210-eV photon energy, not predicted by theory, are tentatively suggested to originate from the coupling between S 2p shake-up photoionization and S 2p single-hole photoionization. The experimental and calculated angular anisotropy parameters for S 2p photoionization are in good agreement.

Avoiding fractional electrons in subsystem DFT based ab-initio molecular dynamics yields accurate models for liquid water and solvated OH radical.

PubMed

Genova, Alessandro; Ceresoli, Davide; Pavanello, Michele

2016-06-21

In this work we achieve three milestones: (1) we present a subsystem DFT method capable of running ab-initio molecular dynamics simulations accurately and efficiently. (2) In order to rid the simulations of inter-molecular self-interaction error, we exploit the ability of semilocal frozen density embedding formulation of subsystem DFT to represent the total electron density as a sum of localized subsystem electron densities that are constrained to integrate to a preset, constant number of electrons; the success of the method relies on the fact that employed semilocal nonadditive kinetic energy functionals effectively cancel out errors in semilocal exchange-correlation potentials that are linked to static correlation effects and self-interaction. (3) We demonstrate this concept by simulating liquid water and solvated OH(•) radical. While the bulk of our simulations have been performed on a periodic box containing 64 independent water molecules for 52 ps, we also simulated a box containing 256 water molecules for 22 ps. The results show that, provided one employs an accurate nonadditive kinetic energy functional, the dynamics of liquid water and OH(•) radical are in semiquantitative agreement with experimental results or higher-level electronic structure calculations. Our assessments are based upon comparisons of radial and angular distribution functions as well as the diffusion coefficient of the liquid.

An AB Initio Study of SbH_2 and BiH_2: the Renner Effect, Spin-Orbit Coupling, Local Mode Vibrations and Rovibronic Energy Level Clustering in SbH_2

NASA Astrophysics Data System (ADS)

Ostojic, Bojana; Schwerdtfeger, Peter; Bunker, Phil; Jensen, Per

2016-06-01

We present the results of ab initio calculations for the lower electronic states of the Group 15 (pnictogen) dihydrides, SbH_2 and BiH_2. For each of these molecules the two lowest electronic states become degenerate at linearity and are therefore subject to the Renner effect. Spin-orbit coupling is also strong in these two heavy-element containing molecules. For the lowest two electronic states of SbH_2, we construct the three dimensional potential energy surfaces and corresponding dipole moment and transition moment surfaces by multi-reference configuration interaction techniques. Including both the Renner effect and spin-orbit coupling, we calculate term values and simulate the rovibrational and rovibronic spectra of SbH_2. Excellent agreement is obtained with the results of matrix isolation infrared spectroscopic studies and with gas phase electronic spectroscopic studies in absorption [1,2]. For the heavier dihydride BiH_2 we calculate bending potential curves and the spin-orbit coupling constant for comparison. For SbH_2 we further study the local mode vibrational behavior and the formation of rovibronic energy level clusters in high angular momentum states. [1] X. Wang, P. F. Souter and L. Andrews, J. Phys. Chem. A 107, 4244-4249 (2003) [2] N. Basco and K. K. Lee, Spectroscopy Letters 1, 13-15 (1968)

Vibrational and rotational transitions in low-energy electron-diatomic-molecule collisions. I - Close-coupling theory in the moving body-fixed frame. II - Hybrid theory and close-coupling theory: An /l subscript z-prime/-conserving close-coupling approximation

NASA Technical Reports Server (NTRS)

Choi, B. H.; Poe, R. T.

1977-01-01

A detailed vibrational-rotational (V-R) close-coupling formulation of electron-diatomic-molecule scattering is developed in which the target molecular axis is chosen to be the z-axis and the resulting coupled differential equation is solved in the moving body-fixed frame throughout the entire interaction region. The coupled differential equation and asymptotic boundary conditions in the body-fixed frame are given for each parity, and procedures are outlined for evaluating V-R transition cross sections on the basis of the body-fixed transition and reactance matrix elements. Conditions are discussed for obtaining identical results from the space-fixed and body-fixed formulations in the case where a finite truncated basis set is used. The hybrid theory of Chandra and Temkin (1976) is then reformulated, relevant expressions and formulas for the simultaneous V-R transitions of the hybrid theory are obtained in the same forms as those of the V-R close-coupling theory, and distorted-wave Born-approximation expressions for the cross sections of the hybrid theory are presented. A close-coupling approximation that conserves the internuclear axis component of the incident electronic angular momentum (l subscript z-prime) is derived from the V-R close-coupling formulation in the moving body-fixed frame.

Anisotropic Coulomb Explosion of CO Ligands in Group 6 Metal Hexacarbonyls: Cr(CO)6, Mo(CO)6, W(CO)6.

PubMed

Tanaka, Hiroki; Nakashima, Nobuaki; Yatsuhashi, Tomoyuki

2016-09-08

Multiple ionization and subsequent Coulomb explosion have been studied for many organic molecules and their clusters; however, the metal complexes, particularly the large Coulombic interactions expected between a metal and its ligands, have not yet been explored. In this study, the angular distribution of CO(+), oxygen, and carbon ions ejected from metal hexacarbonyls (M(CO)6, M: Cr, Mo, W) having Oh symmetry by Coulomb explosion in femtosecond laser fields (>1 × 10(14) W cm(-2)) is investigated. The emissions of oxygen ions are well-explained in terms of the geometric alignment along a line inclined 45° relative to the CO-M-CO axis in a M(CO)4 plane. Unlike the explosion behavior of the oxygen ions located on the outer part of the molecule, the explosion behavior of the carbon ions was affected by the laser intensity, kinetic energy, and metal. This finding that the emission trends of carbon sandwiched between oxygen and metal atoms were the opposite of those for oxygen was explained by the obstruction by oxygen, the deformation of structure in bending coordinates, and the strong interaction with charged metal. The anisotropic Coulomb explosion of metal complexes reflecting their structural symmetry and central metal charge is a promising candidate for use in the investigation of large Coulombic interactions at the molecular level.

A 100 au Wide Bipolar Rotating Shell Emanating from the HH 212 Protostellar Disk: A Disk Wind?

NASA Astrophysics Data System (ADS)

Lee, Chin-Fei; Li, Zhi-Yun; Codella, Claudio; Ho, Paul T. P.; Podio, Linda; Hirano, Naomi; Shang, Hsien; Turner, Neal J.; Zhang, Qizhou

2018-03-01

HH 212 is a Class 0 protostellar system found to host a “hamburger”-shaped dusty disk with a rotating disk atmosphere and a collimated SiO jet at a distance of ∼400 pc. Recently, a compact rotating outflow has been detected in SO and SO2 toward the center along the jet axis at ∼52 au (0.″13) resolution. Here we resolve the compact outflow into a small-scale wide-opening rotating outflow shell and a collimated jet, with the observations in the same S-bearing molecules at ∼16 au (0.″04) resolution. The collimated jet is aligned with the SiO jet, tracing the shock interactions in the jet. The wide-opening outflow shell is seen extending out from the inner disk around the SiO jet and has a width of ∼100 au. It is not only expanding away from the center, but also rotating around the jet axis. The specific angular momentum of the outflow shell is ∼40 au km s‑1. Simple modeling of the observed kinematics suggests that the rotating outflow shell can trace either a disk wind or disk material pushed away by an unseen wind from the inner disk or protostar. We also resolve the disk atmosphere in the same S-bearing molecules, confirming the Keplerian rotation there.

Demonstrating the Direction of Angular Velocity in Circular Motion

NASA Astrophysics Data System (ADS)

Demircioglu, Salih; Yurumezoglu, Kemal; Isik, Hakan

2015-09-01

Rotational motion is ubiquitous in nature, from astronomical systems to household devices in everyday life to elementary models of atoms. Unlike the tangential velocity vector that represents the instantaneous linear velocity (magnitude and direction), an angular velocity vector is conceptually more challenging for students to grasp. In physics classrooms, the direction of an angular velocity vector is taught by the right-hand rule, a mnemonic tool intended to aid memory. A setup constructed for instructional purposes may provide students with a more easily understood and concrete method to observe the direction of the angular velocity. This article attempts to demonstrate the angular velocity vector using the observable motion of a screw mounted to a remotely operated toy car.

Quantum orbital angular momentum of elliptically symmetric light

NASA Astrophysics Data System (ADS)

Plick, William N.; Krenn, Mario; Fickler, Robert; Ramelow, Sven; Zeilinger, Anton

2013-03-01

We present a quantum-mechanical analysis of the orbital angular momentum of a class of recently discovered elliptically symmetric stable light fields—the so-called Ince-Gauss modes. We study, in a fully quantum formalism, how the orbital angular momentum of these beams varies with their ellipticity, and we discover several compelling features, including nonmonotonic behavior, stable beams with real continuous (noninteger) orbital angular momenta, and orthogonal modes with the same orbital angular momenta. We explore, and explain in detail, the reasons for this behavior. These features may have applications in quantum key distribution, atom trapping, and quantum informatics in general—as the ellipticity opens up an alternative way of navigating the spatial photonic Hilbert space.

Fabrication of the planar angular rotator using the CMOS process

NASA Astrophysics Data System (ADS)

Dai, Ching-Liang; Chang, Chien-Liu; Chen, Hung-Lin; Chang, Pei-Zen

2002-05-01

In this investigation we propose a novel planar angular rotator fabricated by the conventional complementary metal-oxide semiconductor (CMOS) process. Following the 0.6 μm single poly triple metal (SPTM) CMOS process, the device is completed by a simple maskless, post-process etching step. The rotor of the planar angular rotator rotates around its geometric center with electrostatic actuation. The proposed design adopts an intelligent mechanism including the slider-crank system to permit simultaneous motion. The CMOS planar angular rotator could be driven with driving voltages of around 40 V. The design proposed here has a shorter response time and longer life, without problems of friction and wear, compared to the more common planar angular micromotor.

Method and system for controlling start of a permanent magnet machine

DOEpatents

Walters, James E.; Krefta, Ronald John

2003-10-28

Method and system for controlling a permanent magnet machine are provided. The method provides a sensor assembly for sensing rotor sector position relative to a plurality of angular sectors. The method further provides a sensor for sensing angular increments in rotor position. The method allows starting the machine in a brushless direct current mode of operation using a calculated initial rotor position based on an initial angular sector position information from the sensor assembly. Upon determining a transition from the initial angular sector to the next angular sector, the method allows switching to a sinusoidal mode of operation using rotor position based on rotor position information from the incremental sensor.

Angular motion estimation using dynamic models in a gyro-free inertial measurement unit.

PubMed

Edwan, Ezzaldeen; Knedlik, Stefan; Loffeld, Otmar

2012-01-01

In this paper, we summarize the results of using dynamic models borrowed from tracking theory in describing the time evolution of the state vector to have an estimate of the angular motion in a gyro-free inertial measurement unit (GF-IMU). The GF-IMU is a special type inertial measurement unit (IMU) that uses only a set of accelerometers in inferring the angular motion. Using distributed accelerometers, we get an angular information vector (AIV) composed of angular acceleration and quadratic angular velocity terms. We use a Kalman filter approach to estimate the angular velocity vector since it is not expressed explicitly within the AIV. The bias parameters inherent in the accelerometers measurements' produce a biased AIV and hence the AIV bias parameters are estimated within an augmented state vector. Using dynamic models, the appended bias parameters of the AIV become observable and hence we can have unbiased angular motion estimate. Moreover, a good model is required to extract the maximum amount of information from the observation. Observability analysis is done to determine the conditions for having an observable state space model. For higher grades of accelerometers and under relatively higher sampling frequency, the error of accelerometer measurements is dominated by the noise error. Consequently, simulations are conducted on two models, one has bias parameters appended in the state space model and the other is a reduced model without bias parameters.

Angular Motion Estimation Using Dynamic Models in a Gyro-Free Inertial Measurement Unit

PubMed Central

Edwan, Ezzaldeen; Knedlik, Stefan; Loffeld, Otmar

2012-01-01

In this paper, we summarize the results of using dynamic models borrowed from tracking theory in describing the time evolution of the state vector to have an estimate of the angular motion in a gyro-free inertial measurement unit (GF-IMU). The GF-IMU is a special type inertial measurement unit (IMU) that uses only a set of accelerometers in inferring the angular motion. Using distributed accelerometers, we get an angular information vector (AIV) composed of angular acceleration and quadratic angular velocity terms. We use a Kalman filter approach to estimate the angular velocity vector since it is not expressed explicitly within the AIV. The bias parameters inherent in the accelerometers measurements' produce a biased AIV and hence the AIV bias parameters are estimated within an augmented state vector. Using dynamic models, the appended bias parameters of the AIV become observable and hence we can have unbiased angular motion estimate. Moreover, a good model is required to extract the maximum amount of information from the observation. Observability analysis is done to determine the conditions for having an observable state space model. For higher grades of accelerometers and under relatively higher sampling frequency, the error of accelerometer measurements is dominated by the noise error. Consequently, simulations are conducted on two models, one has bias parameters appended in the state space model and the other is a reduced model without bias parameters. PMID:22778586

Study of the mode of angular velocity damping for a spacecraft at non-standard situation

NASA Astrophysics Data System (ADS)

Davydov, A. A.; Sazonov, V. V.

2012-07-01

Non-standard situation on a spacecraft (Earth's satellite) is considered, when there are no measurements of the spacecraft's angular velocity component relative to one of its body axes. Angular velocity measurements are used in controlling spacecraft's attitude motion by means of flywheels. The arising problem is to study the operation of standard control algorithms in the absence of some necessary measurements. In this work this problem is solved for the algorithm ensuring the damping of spacecraft's angular velocity. Such a damping is shown to be possible not for all initial conditions of motion. In the general case one of two possible final modes is realized, each described by stable steady-state solutions of the equations of motion. In one of them, the spacecraft's angular velocity component relative to the axis, for which the measurements are absent, is nonzero. The estimates of the regions of attraction are obtained for these steady-state solutions by numerical calculations. A simple technique is suggested that allows one to eliminate the initial conditions of the angular velocity damping mode from the attraction region of an undesirable solution. Several realizations of this mode that have taken place are reconstructed. This reconstruction was carried out using approximations of telemetry values of the angular velocity components and the total angular momentum of flywheels, obtained at the non-standard situation, by solutions of the equations of spacecraft's rotational motion.

A Missile-Borne Angular Velocity Sensor Based on Triaxial Electromagnetic Induction Coils

PubMed Central

Li, Jian; Wu, Dan; Han, Yan

2016-01-01

Aiming to solve the problem of the limited measuring range for angular motion parameters of high-speed rotating projectiles in the field of guidance and control, a self-adaptive measurement method for angular motion parameters based on the electromagnetic induction principle is proposed. First, a framework with type bent “I-shape” is used to design triaxial coils in a mutually orthogonal way. Under the condition of high rotational speed of a projectile, the induction signal of the projectile moving across a geomagnetic field is acquired by using coils. Second, the frequency of the pulse signal is adjusted self-adaptively. Angular velocity and angular displacement are calculated in the form of periodic pulse counting and pulse accumulation, respectively. Finally, on the basis of that principle prototype of the sensor is researched and developed, performance of measuring angular motion parameters are tested on the sensor by semi-physical and physical simulation experiments, respectively. Experimental results demonstrate that the sensor has a wide measuring range of angular velocity from 1 rps to 100 rps with a measurement error of less than 0.3%, and the angular displacement measurement error is lower than 0.2°. The proposed method satisfies measurement requirements for high-speed rotating projectiles with an extremely high dynamic range of rotational speed and high precision, and has definite value to engineering applications in the fields of attitude determination and geomagnetic navigation. PMID:27706039

Goal-based angular adaptivity applied to a wavelet-based discretisation of the neutral particle transport equation

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

Goffin, Mark A., E-mail: mark.a.goffin@gmail.com; Buchan, Andrew G.; Dargaville, Steven

2015-01-15

A method for applying goal-based adaptive methods to the angular resolution of the neutral particle transport equation is presented. The methods are applied to an octahedral wavelet discretisation of the spherical angular domain which allows for anisotropic resolution. The angular resolution is adapted across both the spatial and energy dimensions. The spatial domain is discretised using an inner-element sub-grid scale finite element method. The goal-based adaptive methods optimise the angular discretisation to minimise the error in a specific functional of the solution. The goal-based error estimators require the solution of an adjoint system to determine the importance to the specifiedmore » functional. The error estimators and the novel methods to calculate them are described. Several examples are presented to demonstrate the effectiveness of the methods. It is shown that the methods can significantly reduce the number of unknowns and computational time required to obtain a given error. The novelty of the work is the use of goal-based adaptive methods to obtain anisotropic resolution in the angular domain for solving the transport equation. -- Highlights: •Wavelet angular discretisation used to solve transport equation. •Adaptive method developed for the wavelet discretisation. •Anisotropic angular resolution demonstrated through the adaptive method. •Adaptive method provides improvements in computational efficiency.« less

A Missile-Borne Angular Velocity Sensor Based on Triaxial Electromagnetic Induction Coils.

PubMed

Li, Jian; Wu, Dan; Han, Yan

2016-09-30

Aiming to solve the problem of the limited measuring range for angular motion parameters of high-speed rotating projectiles in the field of guidance and control, a self-adaptive measurement method for angular motion parameters based on the electromagnetic induction principle is proposed. First, a framework with type bent "I-shape" is used to design triaxial coils in a mutually orthogonal way. Under the condition of high rotational speed of a projectile, the induction signal of the projectile moving across a geomagnetic field is acquired by using coils. Second, the frequency of the pulse signal is adjusted self-adaptively. Angular velocity and angular displacement are calculated in the form of periodic pulse counting and pulse accumulation, respectively. Finally, on the basis of that principle prototype of the sensor is researched and developed, performance of measuring angular motion parameters are tested on the sensor by semi-physical and physical simulation experiments, respectively. Experimental results demonstrate that the sensor has a wide measuring range of angular velocity from 1 rps to 100 rps with a measurement error of less than 0.3%, and the angular displacement measurement error is lower than 0.2°. The proposed method satisfies measurement requirements for high-speed rotating projectiles with an extremely high dynamic range of rotational speed and high precision, and has definite value to engineering applications in the fields of attitude determination and geomagnetic navigation.

The Angular Momentum of Baryons and Dark Matter Halos Revisited

NASA Technical Reports Server (NTRS)

Kimm, Taysun; Devriendt, Julien; Slyz, Adrianne; Pichon, Christophe; Kassin, Susan A.; Dubois, Yohan

2011-01-01

Recent theoretical studies have shown that galaxies at high redshift are fed by cold, dense gas filaments, suggesting angular momentum transport by gas differs from that by dark matter. Revisiting this issue using high-resolution cosmological hydrodynamics simulations with adaptive-mesh refinement (AMR), we find that at the time of accretion, gas and dark matter do carry a similar amount of specific angular momentum, but that it is systematically higher than that of the dark matter halo as a whole. At high redshift, freshly accreted gas rapidly streams into the central region of the halo, directly depositing this large amount of angular momentum within a sphere of radius r = 0.1R(sub vir). In contrast, dark matter particles pass through the central region unscathed, and a fraction of them ends up populating the outer regions of the halo (r/R(sub vir) > 0.1), redistributing angular momentum in the process. As a result, large-scale motions of the cosmic web have to be considered as the origin of gas angular momentum rather than its virialised dark matter halo host. This generic result holds for halos of all masses at all redshifts, as radiative cooling ensures that a significant fraction of baryons remain trapped at the centre of the halos. Despite this injection of angular momentum enriched gas, we predict an amount for stellar discs which is in fair agreement with observations at z=0. This arises because the total specific angular momentum of the baryons (gas and stars) remains close to that of dark matter halos. Indeed, our simulations indicate that any differential loss of angular momentum amplitude between the two components is minor even though dark matter halos continuously lose between half and two-thirds of their specific angular momentum modulus as they evolve. In light of our results, a substantial revision of the standard theory of disc formation seems to be required. We propose a new scenario where gas efficiently carries the angular momentum generated by large-scale structure motions deep inside dark matter halos, redistributing it only in the vicinity of the disc.

Vestibular coriolis effect differences modeled with three-dimensional linear-angular interactions.

PubMed

Holly, Jan E

2004-01-01

The vestibular coriolis (or "cross-coupling") effect is traditionally explained by cross-coupled angular vectors, which, however, do not explain the differences in perceptual disturbance under different acceleration conditions. For example, during head roll tilt in a rotating chair, the magnitude of perceptual disturbance is affected by a number of factors, including acceleration or deceleration of the chair rotation or a zero-g environment. Therefore, it has been suggested that linear-angular interactions play a role. The present research investigated whether these perceptual differences and others involving linear coriolis accelerations could be explained under one common framework: the laws of motion in three dimensions, which include all linear-angular interactions among all six components of motion (three angular and three linear). The results show that the three-dimensional laws of motion predict the differences in perceptual disturbance. No special properties of the vestibular system or nervous system are required. In addition, simulations were performed with angular, linear, and tilt time constants inserted into the model, giving the same predictions. Three-dimensional graphics were used to highlight the manner in which linear-angular interaction causes perceptual disturbance, and a crucial component is the Stretch Factor, which measures the "unexpected" linear component.

Low-dimensional organization of angular momentum during walking on a narrow beam.

PubMed

Chiovetto, Enrico; Huber, Meghan E; Sternad, Dagmar; Giese, Martin A

2018-01-08

Walking on a beam is a challenging motor skill that requires the regulation of upright balance and stability. The difficulty in beam walking results from the reduced base of support compared to that afforded by flat ground. One strategy to maintain stability and hence avoid falling off the beam is to rotate the limb segments to control the body's angular momentum. The aim of this study was to examine the coordination of the angular momentum variations during beam walking. We recorded movement kinematics of participants walking on a narrow beam and computed the angular momentum contributions of the body segments with respect to three different axes. Results showed that, despite considerable variability in the movement kinematics, the angular momentum was characterized by a low-dimensional organization based on a small number of segmental coordination patterns. When the angular momentum was computed with respect to the beam axis, the largest fraction of its variation was accounted for by the trunk segment. This simple organization was robust and invariant across all participants. These findings support the hypothesis that control strategies for complex balancing tasks might be easier to understand by investigating angular momentum instead of the segmental kinematics.

Angular Impulse and Balance Regulation During the Golf Swing.

PubMed

Peterson, Travis J; Wilcox, Rand R; McNitt-Gray, Jill L

2016-08-01

Our aim was to determine how skilled players regulate linear and angular impulse while maintaining balance during the golf swing. Eleven highly-skilled golf players performed swings with a 6-iron and driver. Components contributing to linear and angular impulse generated by the rear and target legs (resultant horizontal reaction force [RFh], RFh-angle, and moment arm) were quantified and compared across the group and within a player (α = .05). Net angular impulse generated by both the rear and target legs was greater for the driver than the 6-iron. Mechanisms used to regulate angular impulse generation between clubs varied across players and required coordination between the legs. Increases in net angular impulse with a driver involved increases in target leg RFh. Rear leg RFh-angle was maintained between clubs whereas target leg RFh became more aligned with the target line. Net linear impulse perpendicular to the target line remained near zero, preserving balance, while net linear impulse along the target line decreased in magnitude. These results indicate that the net angular impulse was regulated between clubs by coordinating force generation of the rear and target legs while sustaining balance throughout the task.

Angular-velocity control approach for stance-control orthoses.

PubMed

Lemaire, Edward D; Goudreau, Louis; Yakimovich, Terris; Kofman, Jonathan

2009-10-01

Currently, stance-control knee orthoses require external control mechanisms to control knee flexion during stance and allow free knee motion during the swing phase of gait. A new angular-velocity control approach that uses a rotary-hydraulic device to resist knee flexion when the knee angular velocity passes a preset threshold is presented. This angular-velocity approach for orthotic stance control is based on the premise that knee-flexion angular velocity during a knee-collapse event, such as a stumble or fall, is greater than that during walking. The new hydraulic knee-flexion control device does not require an external control mechanism to switch from free motion to stance control mode. Functional test results demonstrated that the hydraulic angular-velocity activated knee joint provided free knee motion during walking, engaged upon knee collapse, and supported body weight while the end-user recovered to a safe body position. The joint was tested to 51.6 Nm in single loading tests and passed 200,000 repeated loading cycles with a peak load of 88 Nm per cycle. The hydraulic, angular velocity activation approach has potential to improve safety and security for people with lower extremity weakness or when recovering from joint trauma.

A systematic construction of microstate geometries with low angular momentum

NASA Astrophysics Data System (ADS)

Bena, Iosif; Heidmann, Pierre; Ramírez, Pedro F.

2017-10-01

We outline a systematic procedure to obtain horizonless microstate geometries that have the same charges as three-charge five-dimensional black holes with a macroscopically-large horizon area and an arbitrarily-small angular momentum. There are two routes through which such solutions can be constructed: using multi-center Gibbons-Hawking (GH) spaces or using superstratum technology. So far the only solutions corre-sponding to microstate geometries for black holes with no angular momentum have been obtained via superstrata [1], and multi-center Gibbons-Hawking spaces have been believed to give rise only to microstate geometries of BMPV black holes with a large angular mo-mentum [2]. We perform a thorough search throughout the parameter space of smooth horizonless solutions with four GH centers and find that these have an angular momentum that is generally larger than 80% of the cosmic censorship bound. However, we find that solutions with three GH centers and one supertube (which are smooth in six-dimensional supergravity) can have an arbitrarily-low angular momentum. Our construction thus gives a recipe to build large classes of microstate geometries for zero-angular-momentum black holes without resorting to superstratum technology.

Adaptation to vestibular disorientation. IV, Responses to angular acceleration and to bilateral caloric stimulation following unilateral caloric habituation.

DOT National Transportation Integrated Search

1967-01-01

The paper provides information that angular acceleration tests of the vestibular system transcend clinical caloric tests in revealing adaptation to angular accelerations as experienced in rotary motions, including flight situations. The caloric test ...

Evidence for the distribution of angular velocity inside the sun and stars

NASA Technical Reports Server (NTRS)

1972-01-01

A round table discussion of problems of solar and stellar spindown and theory is presented. Observational evidence of the angular momentum of the solar wind is included, emphasizing the distribution of angular velocity inside the sun and stars.

Non-Colinearity of Angular Velocity and Angular Momentum

ERIC Educational Resources Information Center

Burr, A. F.

1974-01-01

Discusses the principles, construction, and operation of an apparatus which serves to demonstrate the non-colinearity of the angular velocity and momentum vectors as well as the inertial tensors. Applications of the apparatus to teaching of advanced undergraduate mechanics courses are recommended. (CC)

D = 5 Einstein-Maxwell-Chern-Simons black holes.

PubMed

Kunz, Jutta; Navarro-Lérida, Francisco

2006-03-03

Five-dimensional Einstein-Maxwell-Chern-Simons theory with a Chern-Simons coefficient lambda = 1 has supersymmetric black holes with a vanishing horizon angular velocity but finite angular momentum. Here supersymmetry is associated with a borderline between stability and instability, since for lambda > 1 a rotational instability arises, where counterrotating black holes appear, whose horizon rotates in the opposite sense to the angular momentum. For lambda > 2 black holes are no longer uniquely characterized by their global charges, and rotating black holes with vanishing angular momentum appear.

Opto-Mechanical Design of a Chromotomographic Imager Direct-Vision Prism Element

DTIC Science & Technology

2013-03-01

The paramount conclusion to be made from these relationships is that the angular dispersion must be known for all wavelengths of interest in order to...respect to the range of angular spread of approximately 4◦ seen in Figure 3.4, the angular error in the measurement is as much as 2.4 minutes of arc...angle is the maximum angular difference between the surface normal, N̂, and the incident ray direction vector, î, for which refraction occurs across a

On the study of angular velocity in mass asymmetry nuclei

NASA Astrophysics Data System (ADS)

Kaur, Kamaldeep; Kumar, Suneel

2018-05-01

Using isospin-dependent quantum molecular dynamics (IQMD) model, the role of angular velocity (Wy) has been explored by changing the mass asymmetric content of the colliding nuclei at the incident energy of 50 MeV/nucleon for centrality 0.25