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Henrik Haak

Publications and source records attributed to Henrik Haak.

15 recordsLinked to original sources

Continuous thermochemical sources of AlF molecules

The AlF molecule, currently subject to laser cooling and trapping efforts, has the advantage that it can be efficiently produced in a thermochemical reaction between sublimated aluminum trifluoride and aluminum metal. Here we present a series of experiments with continuous molecular beam sources of AlF, utilising this reaction. We demonstrate a compact AlF molecular beam oven whose total far-field brightness is $5\times 10^{15}$ molecules per steradian per second at 923~K, just below the melting temperature of aluminum metal. The continuous output from the oven begins to exceed the peak brightness of a jet-cooled, ablation-based supersonic AlF source for the $v=0$, $J=7$ level, and we obtain an excellent signal-to-noise ratio with the oven in pulsed laser ionisation spectroscopy experiments. By delivering flux from the oven into a cryogenic Ne buffer gas cell, we lower the rotational temperature of the beam to around 30~K and reduce its most probable forward velocity from 600~ms$^{-1}$ to 200~ms$^{-1}$. In addition, we demonstrate that AlF can be made in a simple dispenser package, and observe that molecules thermalise to the laboratory temperature after colliding with vacuum chamber walls of the experiment. The resulting transient AlF vapour may enable direct loading of a molecular magneto-optical trap.

physics.atom-ph

Non-equilibrium state during proton-deuteron exchange at a liquid-liquid interface

Proton-deuteron exchange is a very fast process, even across macroscopic length scales. Here we directly and quantitatively measure the formation of HDO within the first 100 microseconds of the reaction at the liquid-liquid interface between D$_2$O and H$_2$O, using a fast-flowing liquid flat jet combined with infrared spectroscopic imaging. We demonstrate that, at early stages HDO formation is reaction-limited, set by the low concentration of the hydroxide and hydronium ions that mediate the exchange. As the ion concentration rises, the rate rapidly approaches the diffusion limit. The reaction rate constant we extract is consistent with the picosecond timescale of the elementary proton-deuteron exchange. Access to these microsecond kinetics reveals a non-equilibrium state in the early H$_2$O/D$_2$O interface: the two liquids are fully mixed by diffusion, yet the HDO concentration remains well below equilibrium. Quantitative imaging of reactant and product concentrations at well-defined liquid-liquid interfaces, as introduced here, will enable the study of fast kinetics across a wide range of chemical reactions.

physics.chem-ph

Imaging Temperature and Thickness of Thin Planar Liquid Water Jets in Vacuum

We present spatially resolved measurements of the temperature of a flat liquid water microjet for varying pressures, from vacuum to 100% relative humidity. The entire jet surface is probed in a single shot by a high-resolution infrared camera. Obtained 2D images are substantially influenced by the temperature of the apparatus on the opposite side of the IR camera; a protocol to correct for the thermal background radiation is presented. In vacuum, we observe cooling rates due to water evaporation on the order of 105 K/s. For our system, this corresponds to a temperature decrease of approximately 15 K between upstream and downstream positions of the flowing leaf. Making reasonable assumptions on the absorption of the thermal background radiation in the flatjet we can extend our analysis to infer a thickness map. For a reference system our value for the thickness is in good agreement with the one reported from white light interferometry.

cond-mat.soft

Imaging of chemical kinetics at the water-water interface in a free-flowing liquid flat-jet

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.

physics.chem-ph

A setup for studies of photoelectron circular dichroism from chiral molecules in aqueous solution

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 (PADs), 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 $α$ 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.

physics.chem-ph

A New Design for a Traveling-Wave Zeeman Decelerator: I. Theory

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.

physics.chem-ph

A New Design for a Traveling-Wave Zeeman Decelerator: II. Experiment

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 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.

physics.chem-ph

A traveling wave decelerator for neutral polar molecules

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.

physics.atom-ph

An electrostatic elliptical mirror for neutral polar molecules

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.

physics.atom-ph

Rotational-state-specific guiding of large molecules

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/$Δ$\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.

physics.atm-clus

Slowing polar molecules using a wire Stark decelerator

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.

physics.atom-ph

Deceleration of neutral molecules in macroscopic traveling traps

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.

physics.atom-ph

Operation of a Stark decelerator with optimum acceptance

With a Stark decelerator, beams of neutral polar molecules can be accelerated, guided at a constant velocity, or decelerated. The effectiveness of this process is determined by the 6D volume in phase space from which molecules are accepted by the Stark decelerator. Couplings between the longitudinal and transverse motion of the molecules in the decelerator can reduce this acceptance. These couplings are nearly absent when the decelerator operates such that only every third electric field stage is used for deceleration, while extra transverse focusing is provided by the intermediate stages. For many applications, the acceptance of a Stark decelerator in this so-called $s=3$ mode significantly exceeds that of a decelerator in the conventionally used ($s=1$) mode. This has been experimentally verified by passing a beam of OH radicals through a 2.6 meter long Stark decelerator. The experiments are in quantitative agreement with the results of trajectory calculations, and can qualitatively be explained with a simple model for the 6D acceptance. These results imply that the 6D acceptance of a Stark decelerator in the $s=3$ mode of operation approaches the optimum value, i.e. the value that is obtained when any couplings are neglected.

physics.atm-clus

Alternating gradient focusing and deceleration of large molecules

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.

physics.atom-ph

Compact in-place gate valve for molecular beam experiments

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.

physics.ins-det