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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,009 records · Page 56
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DOE OSTI2014

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

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

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Complete active space second order perturbation theory (CASPT2) study of N({sup 2}D) + H{sub 2}O reaction paths on D{sub 1} and D{sub 0} potential energy surfaces: Direct and roaming pathways

We report reaction paths starting from N({sup 2}D) + H{sub 2}O for doublet spin states, D{sub 0} and D{sub 1}. The potential energy surfaces are explored in an automated fashion using the global reaction route mapping strategy. The critical points and reaction paths have been fully optimized at the complete active space second order perturbation theory level taking all valence electrons in the active space. In addition to direct dissociation pathways that would be dominant, three roaming processes, two roaming dissociation, and one roaming isomerization: (1) H{sub 2}ON → H–O(H)N → H–HON → NO({sup 2}Π) + H{sub 2}, (2) cis-HNOH → HNO–H → H–HNO → NO + H{sub 2}, (3) H{sub 2}NO → H–HNO → HNO–H → trans-HNOH, are confirmed on the D{sub 0} surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Two-component multi-configurational second-order perturbation theory with Kramers restricted complete active space self-consistent field reference function and spin-orbit relativistic effective core potential

We report the formulation and implementation of KRCASPT2, a two-component multi-configurational second-order perturbation theory based on Kramers restricted complete active space self-consistent field (KRCASSCF) reference function, in the framework of the spin-orbit relativistic effective core potential. The zeroth-order Hamiltonian is defined as the sum of nondiagonal one-electron operators with generalized two-component Fock matrix elements as scalar factors. The Kramers symmetry within the zeroth-order Hamiltonian is maintained via the use of a state-averaged density, allowing a consistent treatment of degenerate states. The explicit expressions are derived for the matrix elements of the zeroth-order Hamiltonian as well as for the perturbation vector. The use of a fully variational reference function and nondiagonal operators in relativistic multi-configurational perturbation theory is reported for the first time. A series of initial calculations are performed on the ionization potential and excitation energies of the atoms of the 6p-block; the results display a significant improvement over those from KRCASSCF, showing a closer agreement with experimental results. Accurate atomic properties of the superheavy elements of the 7p-block are also presented, and the electronic structures of the low-lying excited states are compared with those of their lighter homologues.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Multi-direction high-efficiency second harmonic generation in ellipse structure nonlinear photonic crystals

We have designed and fabricated a lithium niobate (LN) nonlinear photonic crystal (NPC) with a two-dimensional (2D) ellipse structure of inverse poling domains. The structure can offer continuously varying reciprocal lattice vectors in different directions to compensate the phase-mismatching during the second harmonic generation (SHG) for diverse pump wavelengths. We consider three propagation directions with large effective nonlinear susceptibility and measure the nonlinear conversion efficiency of SHG. The experimental data are in good agreement with the quantitative calculation results using the effective susceptibility model with pump depletion. With high-efficiency SHG in multiple propagation direction, the 2D ellipse structure of LN NPC has the potential to realize various broadband nonlinear frequency conversion processes in different propagation direction with a single crystal.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Optimal control of a Cope rearrangement by coupling the reaction path to a dissipative bath or a second active mode

We compare the strategy found by the optimal control theory in a complex molecular system according to the active subspace coupled to the field. The model is the isomerization during a Cope rearrangement of Thiele’s ester that is the most stable dimer obtained by the dimerization of methyl-cyclopentadienenylcarboxylate. The crudest partitioning consists in retaining in the active space only the reaction coordinate, coupled to a dissipative bath of harmonic oscillators which are not coupled to the field. The control then fights against dissipation by accelerating the passage across the transition region which is very wide and flat in a Cope reaction. This mechanism has been observed in our previous simulations [Chenel et al., J. Phys. Chem. A 116, 11273 (2012)]. We compare here, the response of the control field when the reaction path is coupled to a second active mode. Constraints on the integrated intensity and on the maximum amplitude of the fields are imposed limiting the control landscape. Then, optimum field from one-dimensional simulation cannot provide a very high yield. Better guess fields based on the two-dimensional model allow the control to exploit different mechanisms providing a high control yield. By coupling the reaction surface to a bath, we confirm the link between the robustness of the field against dissipation and the time spent in the delocalized states above the transition barrier.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Approximate spin projected spin-unrestricted density functional theory method: Application to diradical character dependences of second hyperpolarizabilities

We develop a novel method for the calculation and the analysis of the one-electron reduced densities in open-shell molecular systems using the natural orbitals and approximate spin projected occupation numbers obtained from broken symmetry (BS), i.e., spin-unrestricted (U), density functional theory (DFT) calculations. The performance of this approximate spin projection (ASP) scheme is examined for the diradical character dependence of the second hyperpolarizability (γ) using several exchange-correlation functionals, i.e., hybrid and long-range corrected UDFT schemes. It is found that the ASP-LC-UBLYP method with a range separating parameter μ = 0.47 reproduces semi-quantitatively the strongly-correlated [UCCSD(T)] result for p-quinodimethane, i.e., the γ variation as a function of the diradical character.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Prospects of using the second-order perturbation theory of the MP2 type in the theory of electron scattering by polyatomic molecules

So far the second-order perturbation theory has been only applied to the hydrogen molecule. No application was attempted for another molecule, probably because of technical difficulties of such calculations. The purpose of this contribution is to show that the calculations of this type are now feasible on larger polyatomic molecules even on commonly used computers.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

The effects of magnetohydrodynamic and radiation on flow of second grade fluid past an infinite inclined plate in porous medium

An analysis of the exact solutions of second grade fluid problem for unsteady magnetohydrodynamic (MHD) flows past an infinite inclined plate in a porous medium is presented. It is assumed that the bounding infinite inclined plate has a constant temperature with radiation effects. Based on Boussinesq approximation the expressions for dimensionless velocity, temperature and concentration are obtained by using Laplace transform method. The derived solutions satisfying the involved differential equations, and all the boundary and initial conditions. The influence of various parameters on the velocity has been illustrated graphically and analyzed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Solution of second order quasi-linear boundary value problems by a wavelet method

A wavelet Galerkin method based on expansions of Coiflet-like scaling function bases is applied to solve second order quasi-linear boundary value problems which represent a class of typical nonlinear differential equations. Two types of typical engineering problems are selected as test examples: one is about nonlinear heat conduction and the other is on bending of elastic beams. Numerical results are obtained by the proposed wavelet method. Through comparing to relevant analytical solutions as well as solutions obtained by other methods, we find that the method shows better efficiency and accuracy than several others, and the rate of convergence can even reach orders of 5.8.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Relaxation approximations to second-order traffic flow models by high-resolution schemes

A relaxation-type approximation of second-order non-equilibrium traffic models, written in conservation or balance law form, is considered. Using the relaxation approximation, the nonlinear equations are transformed to a semi-linear diagonilizable problem with linear characteristic variables and stiff source terms with the attractive feature that neither Riemann solvers nor characteristic decompositions are in need. In particular, it is only necessary to provide the flux and source term functions and an estimate of the characteristic speeds. To discretize the resulting relaxation system, high-resolution reconstructions in space are considered. Emphasis is given on a fifth-order WENO scheme and its performance. The computations reported demonstrate the simplicity and versatility of relaxation schemes as numerical solvers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Enhancement in the structure quality of ZnO nanorods by diluted Co dopants: Analyses via optical second harmonic generation

We report a systematic study about the effect of cobalt concentration in the growth solution over the crystallization, growth, and optical properties of hydrothermally synthesized Zn{sub 1−x}Co{sub x}O [0 ≤ x ≤ 0.40, x is the weight (wt.) % of Co in the growth solution] nanorods. Dilute Co concentration of 1 wt. % in the growth solution enhances the bulk crystal quality of ZnO nanorods, and high wt. % leads to distortion in the ZnO lattice that depresses the crystallization, growth as well as the surface structure quality of ZnO. Although, Co concentration in the growth solution varies from 1 to 40 wt. %, the real doping concentration is limited to 0.28 at. % that is due to the low growth temperature of 80 °C. The enhancement in the crystal quality of ZnO nanorods at dilute Co concentration in the solution is due to the strain relaxation that is significantly higher for ZnO nanorods prepared without, and with high wt. % of Co in the growth solution. Second harmonic generation is used to investigate the net dipole distribution from these coatings, which provides detailed information about bulk and surface structure quality of ZnO nanorods at the same time. High quality ZnO nanorods are fabricated by a low-temperature (80 °C) hydrothermal synthesis method, and no post synthesis treatment is needed for further crystallization. Therefore, this method is advantageous for the growth of high quality ZnO coatings on plastic substrates that may lead toward its application in flexible electronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Evidence and detailed study of a second-order phase transition in the (C{sub 6}H{sub 11}NH{sub 3}){sub 2}[PbI{sub 4}] organic-inorganic hybrid material

The thermal properties of the organic-inorganic hybrid material (C{sub 6}H{sub 11}NH{sub 3}){sub 2}[PbI{sub 4}] are investigated using diffuse reflectivity, spectroscopic ellipsometry, differential scanning calorimetry, Raman spectroscopy, and X-ray diffraction. The diffuse reflectivity, performed in heating mode, clearly evidences the presence of a singularity at 336 K. This is confirmed by the temperature dependence of the spectroscopic ellipsometry spectra, which points out a second-order phase transition at 336 K with a critical exponent ∼0.5. Differential scanning calorimetry measurements on a polycrystalline powder of (C{sub 6}H{sub 11}NH{sub 3}){sub 2}[PbI{sub 4}] show a reversible phase transition detected at T{sub C} = 336 K without hysteresis. Raman spectroscopy data suggest that this transition arises from a change in the interactions between inorganic sheets (([PbI{sub 4}]{sup 2−}){sub ∞}) and organic protonated molecules ([C{sub 6}H{sub 11}NH{sub 3}]{sup +}). The structural analysis from power X-ray diffraction reveals an incomplete order-disorder transition of the cyclohexylammonium cation, causing a subtle contraction of the inter-plane distance. The transition results from repulsive close contacts between the organic molecules in the interlayer spacing.

36 MATERIALS SCIENCE↗
DOE OSTI2015

A way for studying the impact of PEDOT:PSS interface layer on carrier transport in PCDTBT:PC{sub 71}BM bulk hetero junction solar cells by electric field induced optical second harmonic generation measurement

Electric-field-induced optical second-harmonic generation (EFISHG) measurement was employed to study the impact of poly(3,4-ethylenedioxythiophene)-polystyrene sulfonate (PEDOT:PSS) interface layer on the carrier transport mechanism of the PCDTBT:PC{sub 71}BM bulk heterojunction (BHJ) organic solar cells (OSCs). We revealed that the electric fields in the PCDTBT and PC{sub 71}BM were allowed to be measured individually by choosing fundamental laser wavelengths of 1000 nm and 1060 nm, respectively, in dark and under illumination. The results showed that the direction of the internal electric fields in the PCDTBT:PC{sub 71}BM BHJ layer is reversed by introducing the PEDOT:PSS layer, and this results in longer electron transport time in the BHJ layer. We conclude that TR-EFISHG can be used as a novel way for studying the impact of interfacial layer on the transport of electrons and holes in the bulk-heterojunction OSCs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Isotropic octupolar second harmonic generation response in LaBGeO{sub 5} glass-ceramic with spherulitic precipitation

A spherulitic crystallization of the crystalline phase LaBGeO{sub 5} is generated in the 25La{sub 2}O{sub 3}-25B{sub 2}O{sub 3}-50 GeO{sub 2} glass system. Linear and nonlinear optical properties of lanthanum borogermanate glass-ceramic have been investigated at both macroscopic and microscopic scales. Polarized μ-Raman analysis has evidenced a radial distribution of the crystallites along the c-axis inside spherulites, whereas polarized μ-Second Harmonic Generation (SHG) analysis revealed intensity maxima perpendicularly to the c-axis crystallites orientation. Polarized SHG mapping of a spherulite indicate that no dipolar response along the c-axis oriented crystallites occurs despite the individual dipolar symmetry C{sub 3} of the crystallites. At a larger mm scale, the isotropic scattering of spherulites recorded from macroscopic SHG experiment in the forward direction is consistent with an average coherent octupolar response per spherulite. These SHG analyses at different scale are both in accordance with radial antiferroelectric orientation along the c-axis of crystallites inside each spherulite.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Forces and stress in second order Møller-Plesset perturbation theory for condensed phase systems within the resolution-of-identity Gaussian and plane waves approach

The forces acting on the atoms as well as the stress tensor are crucial ingredients for calculating the structural and dynamical properties of systems in the condensed phase. Here, these derivatives of the total energy are evaluated for the second-order Møller-Plesset perturbation energy (MP2) in the framework of the resolution of identity Gaussian and plane waves method, in a way that is fully consistent with how the total energy is computed. This consistency is non-trivial, given the different ways employed to compute Coulomb, exchange, and canonical four center integrals, and allows, for example, for energy conserving dynamics in various ensembles. Based on this formalism, a massively parallel algorithm has been developed for finite and extended system. The designed parallel algorithm displays, with respect to the system size, cubic, quartic, and quintic requirements, respectively, for the memory, communication, and computation. All these requirements are reduced with an increasing number of processes, and the measured performance shows excellent parallel scalability and efficiency up to thousands of nodes. Additionally, the computationally more demanding quintic scaling steps can be accelerated by employing graphics processing units (GPU’s) showing, for large systems, a gain of almost a factor two compared to the standard central processing unit-only case. In this way, the evaluation of the derivatives of the RI-MP2 energy can be performed within a few minutes for systems containing hundreds of atoms and thousands of basis functions. With good time to solution, the implementation thus opens the possibility to perform molecular dynamics (MD) simulations in various ensembles (microcanonical ensemble and isobaric-isothermal ensemble) at the MP2 level of theory. Geometry optimization, full cell relaxation, and energy conserving MD simulations have been performed for a variety of molecular crystals including NH{sub 3}, CO{sub 2}, formic acid, and benzene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Polyanalytic relativistic second Bargmann transforms

We construct coherent states through special superpositions of eigenstates of the relativistic isotonic oscillator. In each superposition, the coefficients are chosen to be L{sup 2}-eigenfunctions of a σ-weight Maass Laplacian on the Poincaré disk, which are associated with the eigenvalue 4m(σ−1−m), m∈Z{sub +}∩[0,(σ−1)/2]. For each nonzero m, the associated coherent states transform constitutes the m-true-polyanalytic extension of a relativistic version of the second Bargmann transform, whose integral kernel is expressed in terms of a special Appel-Kampé de Fériet’s hypergeometric function. The obtained results could be used to extend the known semi-classical analysis of quantum dynamics of the relativistic isotonic oscillator.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Lagrangian formulation of irreversible thermodynamics and the second law of thermodynamics

We show that the equations which describe irreversible evolution of a system can be derived from a variational principle. We suggest a Lagrangian, which depends on the properties of the normal and the so-called “mirror-image” system. The Lagrangian is symmetric in time and therefore compatible with microscopic reversibility. The evolution equations in the normal and mirror-imaged systems are decoupled and describe therefore independent irreversible evolution of each of the systems. The second law of thermodynamics follows from a symmetry of the Lagrangian. Entropy increase in the normal system is balanced by the entropy decrease in the mirror-image system, such that there exists an “integral of evolution” which is a constant. The derivation relies on the property of local equilibrium, which states that the local relations between the thermodynamic quantities in non-equilibrium are the same as in equilibrium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Determination of vibrational and rotational temperatures in highly constricted nitrogen plasmas by fitting the second positive system of N{sub 2} molecules

Highly constricted plasmas are an active research area because of their ability to generate high activity of plasma beams, which exhibit potential in applications of material processing and film deposition. In this study, optical emission spectroscopy was used to study the highly constricted nitrogen plasma created at low pressure. The vibrational and rotational temperatures of molecules were determined by fitting the second positive system of nitrogen molecule. Under the conditions of the power densities as high as 7 ∼ 85 W/cm{sup 3} and the pressures of 2 ∼ 200 Pa, the determined rotational temperature was found to be relatively low, increasing from 350 to 700 K and the vibrational temperature keeping at ∼ 5000 K. The analysis of dissipated power revealed that ∼ 80 % of input power is dissipated for the nitrogen molecule dissociation and the creation/loss of ions at the tube wall, producing an as high as 10{sup 12} ∼ 10{sup 13} cm{sup −3} plasma with the nitrogen dissociation degrees of 2%∼15%. With the increase in the discharge pressure, more input power was found to be dissipated in the dissociation of nitrogen molecules instead of creation of ions, resulting in a higher density of radicals.

36 MATERIALS SCIENCE↗