Engineering topics
Publications and source records attributed to Meijer, Gerard.
We present the first X-ray photoelectron circular dichroism (PECD) study from a liquid phase sample, exemplified for liquid fenchone at the C 1s edge.
A generalised liquid-phase photoelectron spectroscopy approach is reported, allowing accurate, absolute energy scale ionisation energies of liquid water and aqueous solutions, as well as liquid water's work function to be reported.
We report on the effects of electron collision and indirect ionization processes on the photoemission spectra of liquid water, specifically at photoexcitation and electron kinetic energies well below 30 eV.
We present an experimental and theoretical investigation of rotationally inelastic transitions of OH, prepared in the X{sup 2}Π, v = 0, j = 3/2 F{sub 1}f level, in collisions with molecular hydrogen (H{sub 2} and D{sub 2}). In a crossed beam experiment, the OH radicals were state selected and velocity tuned over the collision energy range 75–155 cm{sup −1} using a Stark decelerator. Relative parity-resolved state-to-state integral cross sections were determined for collisions with normal and para converted H{sub 2}. These cross sections, as well as previous OH–H{sub 2} measurements at 595 cm{sup −1} collision energy by Schreel and ter Meulen [J. Chem. Phys. 105, 4522 (1996)], and OH–D{sub 2} measurements for collision energies 100–500 cm{sup −1} by Kirste et al. [Phys. Rev. A 82, 042717 (2010)], were compared with the results of quantum scattering calculations using recently determined ab initio potential energy surfaces [Ma et al., J. Chem. Phys. 141, 174309 (2014)]. Good agreement between the experimental and computed relative cross sections was found, although some structure seen in the OH(j = 3/2 F{sub 1}f → j = 5/2 F{sub 1}e) + H{sub 2}(j = 0) cross section is not understood.
We report on the design and characterization of a new apparatus for performing quantum-state resolved surface scattering experiments. The apparatus combines optical state-specific molecule preparation with a compact hexapole and a Stark decelerator to prepare carrier gas-free pulses of quantum-state pure CO molecules with velocities controllable between 33 and 1000 m/s with extremely narrow velocity distributions. The ultrahigh vacuum surface scattering chamber includes homebuilt ion and electron detectors, a closed-cycle helium cooled single crystal sample mount capable of tuning surface temperature between 19 and 1337 K, a Kelvin probe for non-destructive work function measurements, a precision leak valve manifold for targeted adsorbate deposition, an inexpensive quadrupole mass spectrometer modified to perform high resolution temperature programmed desorption experiments and facilities to clean and characterize the surface.
We observe a strong influence of molecular vibration and surface temperature on electron emission promoted by the de-excitation of metastable CO(a{sup 3}Π) on a clean Au(111) surface using a molecular beam surface scattering apparatus. The de-excitation is independent of incidence translational energy. These observations appear incompatible with existing theories of metastable particle de-excitation on metal surfaces, which are based on the Auger effect. Instead, they strongly suggest a mechanism involving formation of a transient anion whose lifetime is similar to the vibrational period of the CO molecule.
Polar molecules in selected quantum states can be guided, decelerated, and trapped using electric fields created by microstructured electrodes on a chip. Here we explore how nonadiabatic transitions between levels in which the molecules are trapped and levels in which the molecules are not trapped can be suppressed. We use {sup 12}CO and {sup 13}CO (a {sup 3{Pi}}{sub 1},v=0) molecules, prepared in the upper {Lambda}-doublet component of the J=1 rotational level, and study the trap loss as a function of an offset magnetic field. The experimentally observed suppression (enhancement) of the nonadiabatic transitions for {sup 12}CO ({sup 13}CO) with increasing magnetic field is quantitatively explained.
We present combined experimental and theoretical results on strong-field ionization of oriented carbonyl sulfide molecules by circularly polarized laser pulses. The obtained molecular frame photoelectron angular distributions show pronounced asymmetries perpendicular to the direction of the molecular electric dipole moment. These findings are explained by a tunneling model invoking the laser-induced Stark shifts associated with the dipoles and polarizabilities of the molecule and its unrelaxed cation. The focus of the present article is to understand the strong-field ionization of one-dimensionally-oriented polar molecules, in particular asymmetries in the emission direction of the photoelectrons. In the following article [Phys. Rev. A 83, 023406 (2011)] the focus is to understand strong-field ionization from three-dimensionally-oriented asymmetric top molecules, in particular the suppression of electron emission in nodal planes of molecular orbitals.
We present a combined experimental and theoretical study on strong-field ionization of a three-dimensionally-oriented asymmetric top molecule, benzonitrile (C{sub 7}H{sub 5}N), by circularly polarized, nonresonant femtosecond laser pulses. Prior to the interaction with the strong field, the molecules are quantum-state selected using a deflector and three-dimensionally (3D) aligned and oriented adiabatically using an elliptically polarized laser pulse in combination with a static electric field. A characteristic splitting in the molecular frame photoelectron momentum distribution reveals the position of the nodal planes of the molecular orbitals from which ionization occurs. The experimental results are supported by a theoretical tunneling model that includes and quantifies the splitting in the momentum distribution. The focus of the present article is to understand strong-field ionization from 3D-oriented asymmetric top molecules, in particular the suppression of electron emission in nodal planes of molecular orbitals. In the preceding article [Dimitrovski et al., Phys. Rev. A 83, 023405 (2011)] the focus is to understand the strong-field ionization of one-dimensionally-oriented polar molecules, in particular asymmetries in the emission direction of the photoelectrons.
We study the focusing of large neutral molecules in a molecular beam using electric fields. Since all quantum states of these molecules are high-field seeking under the practical experimental conditions, alternating gradient (AG) focusing has to be applied. The optimal ac frequency that yields the highest transmission depends on m/{mu}, where {mu} is the dipole moment and m denotes the mass. Therefore, an AG focuser can be used to select species with different m/{mu} ratios, e.g., the conformers of neutral molecules [Phys. Rev. Lett. 100, 133003 (2008)]. Here we demonstrate both theoretically and experimentally how the resolution of such an m/{mu} selector can be optimized.
We present an experimental study on the rotational inelastic scattering of OH (X {sup 2}{Pi}{sub 3/2},J=3/2,f) radicals with He and D{sub 2} at collision energies between 100 and 500 cm{sup -1} in a crossed beam experiment. The OH radicals are state selected and velocity tuned using a Stark decelerator. Relative parity-resolved state-to-state inelastic scattering cross sections are accurately determined. These experiments complement recent low-energy collision studies between trapped OH radicals and beams of He and D{sub 2} that are sensitive to the total (elastic and inelastic) cross sections [Sawyer et al., Phys. Rev. Lett. 101, 203203 (2008)], but for which the measured cross sections could not be reproduced by theoretical calculations [Pavlovic et al., J. Phys. Chem. A 113, 14670 (2009)]. For the OH-He system, our experiments validate the inelastic cross sections determined from rigorous quantum calculations.
We report coherent reflection of thermal He atom beams from various microscopically rough surfaces at grazing incidence. For a sufficiently small normal component k{sub z} of the incident wave vector of the atom the reflection probability is found to be a function of k{sub z} only. This behavior is explained by quantum reflection at the attractive branch of the Casimir-van der Waals interaction potential. For larger values of k{sub z} the overall reflection probability decreases rapidly and is found to also depend on the parallel component k{sub x} of the wave vector. The material specific k{sub x} dependence for this classic reflection at the repulsive branch of the potential is discussed in terms of an averaging out of the surface roughness under grazing incidence conditions.
We report on the observation of emerging beam resonances, well known as Rayleigh-Wood anomalies and threshold resonances in photon and electron diffraction, respectively, in an atom-optical diffraction experiment. Diffraction of He atom beams reflected from a blazed ruled grating at grazing incidence has been investigated. The total reflectivity of the grating as well as the intensities of the diffracted beams reveal anomalies at the Rayleigh angles of incidence, i.e., when another diffracted beam emerges parallel to the grating surface. The observed anomalies are discussed in terms of the classical wave-optical model of Rayleigh and Fano.
A decelerator is presented where polar neutral molecules are guided and decelerated using the principle of traveling electric potential wells, such that molecules are confined in stable three-dimensional traps throughout. We compare this decelerator with that of Scharfenberg et al. [Phys. Rev. A 79, 023410 (2009)] and we show that the current decelerator provides a substantially larger phase-space acceptance, even at higher acceleration. The mode of operation is described and experimentally demonstrated by guiding and decelerating CO molecules.