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We present chemical kinetics measurements of the luminol oxydation chemiluminescence reaction at the interface between two aqueous solutions, using liquid jet technology. Free-flowing iquid microjets are a relatively recent development that has found its way into a growing number of applications in spectroscopy and dynamics. A variant thereof, called flat-jet, is obtained when two cylindrical jets of a liquid are crossed, leading to a chain of planar leaf-shaped structures of the flowing liquid. We here show that in the first leaf of this chain the fluids do not exhibit turbulent mixing, providing a clean interface between the liquids from the impinging jets. We also show, using the example of the luminol chemiluminescence reaction, how this setup can be used to obtain kinetics information from friction-less flow and by circumventing the requirement for rapid mixing but by intentionally suppressing all turbulent mixing and instead relying on diffusion.

Review of scientific instruments 93(1), 015101 (2022). doi:10.1063/5.0072346, We present a unique experimental design that enables the measurement of photoelectron circular dichroism (PECD) from chiral molecules in aqueous solution. The effect is revealed from the intensity difference of photoelectron emission into a backward-scattering angle relative to the photon propagation direction when ionizing with circularly polarized light of different helicity. This leads to asymmetries (normalized intensity differences) that depend on the handedness of the chiral sample and exceed the ones in conventional dichroic mechanisms by orders of magnitude. The asymmetry is largest for photon energies within several electron volts above the ionization threshold. A primary aim is to explore the effect of hydration on PECD. The modular and flexible design of our experimental setup EASI (Electronic structure from Aqueous Solutions and Interfaces) also allows for detection of more common photoelectron angular distributions, requiring distinctively different detection geometries and typically using linearly polarized light. A microjet is used for liquid-sample delivery. We describe EASI���s technical features and present two selected experimental results, one based on synchrotron-light measurements and the other performed in the laboratory, using monochromatized He-II �� radiation. The former demonstrates the principal effectiveness of PECD detection, illustrated for prototypic gas-phase fenchone. We also discuss the first data from liquid fenchone. In the second example, we present valence photoelectron spectra from liquid water and NaI aqueous solution, here obtained from a planar-surface microjet (flatjet). This new development features a more favorable symmetry for angle-dependent photoelectron measurements., Published by American Institute of Physics, [S.l.]

A novel traveling-wave Zeeman decelerator based on a double-helix coil geometry capable of decelerating paramagnetic molecules with high efficiency is presented. Moving magnetic traps are generated by applying time-dependent currents through the decelerator coils. Paramagnetic molecules in low-field-seeking Zeeman states are confined inside the moving traps which are decelerated to lower forward velocities. As a prototypical example, we demonstrate the deceleration of OH radicals from an initial velocity of 445 m s-1 down to various final velocities. The experimental results are analyzed and numerically reproduced with the help of trajectory simulations confirming the phase-space stability and efficiency of the deceleration of the molecules in the new device.

International audience; The concept of a novel traveling wave Zeeman deccelerator based on a double-helix wire geometry capable of decelerating paramagnetic species with high efficiency is presented. A moving magnetic trap is created by running time-dependent currents through the decelerator coils. Paramagnetic species in low-field-seeking Zeeman states are confined in the moving traps and transported to the end of the decelerator with programmable velocities. Here, we present the theoretical foundations underlying the working principle of the traveling-trap decelerator. Using trajectory simulations, we characterise the performance of the new device and explore the conditions for phase-space stability of the transported molecules.

Synopsis We developed a new-concept Zeeman decelerator which produces a traveling magnetic trap. Atoms and molecules possessing a magnetic dipole moment, in so-called low field seeking states, are trapped around a node of a propagating wave provided that the initial velocity of the wave matches a velocity populated in the supersonic beam. In addition, three dimensional confinement is achieved by controlling the radial orientation of the trap, which can be done fully independently from its longitudinal motion.

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.

Focusing of molecular beams using an electrostatic hexapole is a mature technique to produce samples of state-selected molecules. The ability to efficiently focus molecules depends on the properties of the molecular species of interest, the length of the hexapole state selector, as well as on the maximum electric field strength that can be achieved in these devices. In particular for species with a small effective dipole moment such as nitric oxide (NO), hexapole state selectors of several meters in length are required to focus the beam. We report on a novel design for an electrostatic hexapole state-selector that allows for a maximum electric field strength of 260 kV/cm, reducing significantly the length of the hexapole that is required to focus the beam. We demonstrate the focusing of a molecular beam of NO radicals (X 2Π1/2, v = 0, J = 1/2, f) using a hexapole of only 30 cm length. A beamstop is integrated inside the hexapole at the geometric center of the device where the molecular trajectories have the largest deviation from the beam axis, effectively blocking the carrier gas of the molecular beam at minimum loss of NO density. The performance of the hexapole state-selector is investigated by state-selective laser induced fluorescence detection, as well as by two-dimensional imaging of the focused packet of NO radicals. The resulting packet of NO radicals has a density of 9 ± 3 × 1010 cm-3 and a state purity of 99%

Focusing optics for neutral molecules finds application in shaping and steering molecular beams. Here we present an electrostatic elliptical mirror for polar molecules consisting of an array of microstructured gold electrodes deposited on a glass substrate. Alternating positive and negative voltages applied to the electrodes create a repulsive potential for molecules in low-field-seeking states. The equipotential lines are parallel to the substrate surface, which is bent in an elliptical shape. The mirror is characterized by focusing a beam of metastable CO molecules and the results are compared to the outcome of trajectory simulations., Comment: 5 pages, 4 figures

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 have designed and implemented a new Stark decelerator based on wire electrodes, which is suitable for ultrahigh vacuum applications. The 100 deceleration stages are fashioned out of 0.6 mm diameter tantalum and the array's total length is 110 mm, approximately 10 times smaller than a conventional Stark decelerator with the same number of electrode pairs. Using the wire decelerator, we have removed more than 90% of the kinetic energy from metastable CO molecules in a beam., updated version, added journal reference

A new type of 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. This new decelerator is superior to the best currently operational decelerator (Scharfenberg et al., Phys.Rev.A 79, 023410(2009)), providing a substantially larger acceptance even at higher accelerations. The mode of operation is described and experimentally demonstrated by guiding and decelerating CO molecules., 10 pages, 3 figures

We have focused and decelerated benzonitrile (C$_7$H$_5$N) molecules from a molecular beam, using an array of time-varying inhomogeneous electric fields in alternating gradient configuration. Benzonitrile is prototypical for large asymmetric top molecules that exhibit rich rotational structure and a high density of states. At the rotational temperature of 3.5 K in the pulsed molecular beam, many rotational states are populated. Benzonitrile molecules in their absolute ground state are decelerated from 320 m/s to 289 m/s, and similar changes in velocity are obtained for excited rotational states. All measurements agree well with the outcome of trajectory calculations. These experiments demonstrate that such large polyatomic molecules are amenable to the powerful method of Stark deceleration., Comment: 5 pages, 4 figures, revtex4

A linear AC trap for polar molecules in high-field seeking states has been devised and implemented, and its characteristics have been investigated both experimentally and theoretically. The trap is loaded with slow 15ND₃ molecules in their ground state (para-ammonia) from a Stark decelerator. The trap's geometry offers optimal access as well as improved loading. We present measurements of the dependence of the trap's performance on the switching frequency, which exhibit a characteristic structure due to nonlinear resonance effects. The molecules are found to oscillate in the trap under the influence of the trapping forces, which were analyzed using 3D numerical simulations. On the basis of expansion measurements, molecules with a velocity and a position spread of 2.1 m/s and 0.4 mm, respectively, are still accepted by the trap. This corresponds to a temperature of 2.0 mK. From numerical simulations, we find the phase-space volume that can be confined by the trap (the acceptance) to be 50 mm³ (m/s)³.

A high vacuum gate valve for skimmed molecular beam experiments is described. It is designed with a very short extent of only 10 mm along the molecular beam axis to minimize the distance between the molecular beam source and the experiment to provide the maximum molecular flux to the experiment. At the same time it provides free space on both sides of the skimmer to not disturb the supersonic expansion in front of the skimmer, to give optical access to the full distance between beam source and skimmer, and to allow for placing electrostatic devices very close behind the skimmer. The gate valve allows to maintain high vacuum conditions (10^{-8} mbar) in the experimental chamber while the source chamber is brought up to atmospheric pressure for modifications or maintenance. The valve can be operated from outside the vacuum chamber while maintaining vacuum conditions in all chambers., RevTeX; 3 pages, 3 figures

A beam of polar molecules can be focused and transported through an ac electric quadrupole guide. At a given ac frequency, the transmission of the guide depends on the mass-to-dipole-moment (m/\textmu) ratio of the molecular quantum state. Here we present a detailed characterization of the m/\textmu selector, using a pulsed beam of benzonitrile (C$_6$H$_5$CN) molecules in combination with rotational quantum state resolved detection. The arrival time distribution as well as the transverse velocity distribution of the molecules exiting the selector are measured as a function of ac frequency. The \textmu/$\Delta$\textmu resolution of the selector can be controlled by the applied ac waveforms and a value of up to 20 can be obtained with the present setup. This is sufficient to exclusively transmit molecules in the absolute ground state of benzonitrile, or rather in quantum states that have the same m/\textmu value as the ground state. The operation characteristics of the m/\textmu selector are in quantitative agreement with the outcome of trajectory simulations.

Recently, a decelerator for neutral polar molecules has been presented that operates on the basis of macroscopic, three-dimensional, traveling electrostatic traps (Osterwalder et al., Phys. Rev. A 81, 051401 (2010)). In the present paper, a complete description of this decelerator is given, with emphasis on the electronics and the mechanical design. Experimental results showing the transverse velocity distributions of guided molecules are shown and compared to trajectory simulations. An assessment of non-adiabatic losses is made by comparing the deceleration signals from 13-CO with those from 12-CO and with simulated signals., 10 pages, 7 figures