arXiv subjects

Sebastiaan Y. T. van de Meerakker

Publications and source records attributed to Sebastiaan Y. T. van de Meerakker.

At least 37 records · Page 2Linked to original sources

arXiv2017

A new concept multi-stage Zeeman decelerator

We present a new concept for a multi-stage Zeeman decelerator that is optimized particularly for applications in molecular beam scattering experiments. The decelerator consists of a series of alternating hexapoles and solenoids, that effectively decouple the transverse focusing and longitudinal deceleration properties of the decelerator. It can be operated in a deceleration and acceleration mode, as well as in a hybrid mode that makes it possible to guide a particle beam through the decelerator at constant speed. The deceleration features phase stability, with a relatively large six-dimensional phase-space acceptance. The separated focusing and deceleration elements result in an unequal partitioning of this acceptance between the longitudinal and transverse directions. This is ideal in scattering experiments, which typically benefit from a large longitudinal acceptance combined with narrow transverse distributions. We demonstrate the successful experimental implementation of this concept using a Zeeman decelerator consisting of an array of 25 hexapoles and 24 solenoids. The performance of the decelerator in acceleration, deceleration and guiding modes is characterized using beams of metastable Helium ($^3S$) atoms. Up to 60 % of the kinetic energy was removed for He atoms that have an initial velocity of 520 m/s. The hexapoles consist of permanent magnets, whereas the solenoids are produced from a single hollow copper capillary through which cooling liquid is passed. The solenoid design allows for excellent thermal properties, and enables the use of readily available and cheap electronics components to pulse high currents through the solenoids. The Zeeman decelerator demonstrated here is mechanically easy to build, can be operated with cost-effective electronics, and can run at repetition rates up to 10 Hz

physics.atom-ph↗

arXiv2016

Direct probe of anisotropy in atom-molecule collisions via quantum scattering resonances

Anisotropy is a fundamental property of particle interactions. It occupies a central role in cold and ultra-cold molecular processes, where long range forces have been found to significantly depend on orientation in ultra-cold polar molecule collisions. Recent experiments have demonstrated the emergence of quantum phenomena such as scattering resonances in the cold collisions regime due to quantization of the intermolecular degrees of freedom. Although these states have been shown to be sensitive to interaction details, the effect of anisotropy on quantum resonances has eluded experimental observation so far. Here, we directly measure the anisotropy in atom-molecule interactions via quantum resonances by changing the quantum state of the internal molecular rotor. We observe that a quantum scattering resonance at a collision energy of $k_B$ x 270 mK appears in the Penning ionization of molecular hydrogen with metastable helium only if the molecule is rotationally excited. We use state of the art ab initio and multichannel quantum molecular dynamics calculations to show that the anisotropy contributes to the effective interaction only for $H_2$ molecules in the first excited rotational state, whereas rotationally ground state $H_2$ interacts purely isotropically with metastable helium. Control over the quantum state of the internal molecular rotation allows us to switch the anisotropy on or off and thus disentangle the isotropic and anisotropic parts of the interaction. These quantum phenomena provide a challenging benchmark for even the most advanced theoretical descriptions, highlighting the advantage of using cold collisions to advance the microscopic understanding of particle interactions.

physics.chem-ph↗

arXiv2015

Imaging resonances in low-energy NO-He inelastic collisions

In molecular collisions, resonances occur at specific energies where the colliding particles temporarily form quasi-bound complexes, resulting in rapid variations in the energy dependence of scattering cross sections. Experimentally, it has proven challenging to observe such scattering resonances, especially in differential cross sections. We report the observation of resonance fingerprints in the state-to-state differential cross sections for inelastic NO-He collisions in the 13 to 19 cm$^{-1}$ energy range with 0.3 cm$^{-1}$ resolution. The observed structures were in excellent agreement with quantum scattering calculations. They were analyzed by separating the resonance contributions to the differential cross sections from the background through a partitioning of the multichannel scattering matrix. This revealed the partial wave composition of the resonances, and their evolution during the collision.

physics.atm-clus↗

arXiv2014

High-resolution imaging of velocity-controlled molecular collisions using counterpropagating beams

We present ultrahigh-resolution measurements of state-to-state inelastic differential cross sections for NO-Ne and NO-Ar collisions, obtained by combining the Stark deceleration and velocity map imaging techniques. We show that for counterpropagating crossed beam geometries, the effect of the velocity spreads of the reagent beams on the angular resolution of the images is minimized. Futhermore, the counterpropagating geometry results in images that are symmetric with respect to the relative velocity vector. This allows for the use of inverse Abel transformation methods that enhance the resolution further. State-resolved diffraction oscillations in the differential cross sections are measured with an angular resolution approaching 0.3$^\circ$. Distinct structures observed in the cross sections gauge the quality of recent \emph{ab initio} potential energy surfaces for NO-rare gas atom collisions with unprecedented precision.

physics.atom-ph↗

arXiv2013

Stark deceleration of NO radicals

We report on the Stark deceleration of a pulsed molecular beam of NO radicals. Stark deceleration of this chemically important species has long been considered unfeasible due to its small electric dipole moment of 0.16 D. We prepared the NO radicals in the X 2Π3/2, v=0, J=3/2 spin-orbit excited state from the X 2Π1/2, v=0, J=1/2 ground state by Franck-Condon pumping via the A 2Σ+ state. The larger effective dipole moment in the J=3/2 level of the X 2Π3/2, v=0 state, in combination with a 316-stages-long Stark decelerator, allowed us to decelerate NO radicals from 315.0 m/s to 229.2 m/s, thus removing 47 % of their kinetic energy. The measured time-of-flight profiles of the NO radicals exiting the decelerator show good agreement with the outcome of numerical trajectory simulations.

physics.chem-ph↗

arXiv2012

Scattering resonances in slow NH${}_3$-He collisions

We theoretically study slow collisions of NH$_3$ molecules with He atoms, where we focus in particular on the observation of scattering resonances. We calculate state-to-state integral and differential cross sections for collision energies ranging from 10${}^{-4}$ cm$^{-1}$ to 130 cm$^{-1}$, using fully converged quantum close-coupling calculations. To describe the interaction between the NH${}_3$ molecules and the He atoms, we present a four-dimensional potential energy surface, based on an accurate fit of 4180 {\it ab initio} points. Prior to collision, we consider the ammonia molecules to be in their antisymmetric umbrella state with angular momentum $j=1$ and projection $k=1$, which is a suitable state for Stark deceleration. We find pronounced shape and Feshbach resonances, especially for inelastic collisions into the symmetric umbrella state with $j=k=1$. We analyze the observed resonant structures in detail by looking at scattering wavefunctions, phase shifts, and lifetimes. Finally, we discuss the prospects for observing the predicted scattering resonances in future crossed molecular beam experiments with a Stark-decelerated NH$_3$ beam.

physics.chem-ph↗

arXiv2012

Quantum-state resolved bimolecular collisions of velocity-controlled OH with NO radicals

Whereas atom-molecule collisions have been studied with complete quantum state resolution, interactions between two state-selected molecules have proven much harder to probe. Here, we report the measurement of state-resolved inelastic scattering cross sections for collisions between two open-shell molecules that are both prepared in a single quantum state. Stark-decelerated OH radicals were scattered with hexapole-focused NO radicals in a crossed beam configuration. Rotationally and spin-orbit inelastic scattering cross sections were measured on an absolute scale for collision energies between 70 and 300 cm$^{-1}$. These cross sections show fair agreement with quantum coupled-channels calculations using a set of coupled model potential energy surfaces based on ab initio calculations for the long-range non-adiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes.

physics.chem-ph↗

arXiv2012

Magnetic dipole transitions in the OH $A\,^2Σ^+ \leftarrow X\,^2Π$ system

We report on the observation of magnetic dipole allowed transitions in the well-characterized $A\,^2Σ^+ - X\,^2Π$ band system of the OH radical. A Stark decelerator in combination with microwave Rabi spectroscopy is used to control the populations in selected hyperfine levels of both $Λ$-doublet components of the $X\,^2Π_{3/2},v=0,J=3/2$ ground state. Theoretical calculations presented in this paper predict that the magnetic dipole transitions in the $ν'=1 \leftarrow ν=0$ band are weaker than the electric dipole transitions by a factor of $2.58\times 10^3$ only, i.e., much less than commonly believed. Our experimental data confirm this prediction.

physics.chem-ph↗

arXiv2012

Resonances in rotationally inelastic scattering of OH($X^2Π$) with helium and neon

We present detailed calculations on resonances in rotationally and spin-orbit inelastic scattering of OH ($X\,^2Π, j=3/2, F_1, f$) radicals with He and Ne atoms. We calculate new \emph{ab initio} potential energy surfaces for OH-He, and the cross sections derived from these surfaces compare favorably with the recent crossed beam scattering experiment of Kirste \emph{et al.} [Phys. Rev. A \textbf{82}, 042717 (2010)]. We identify both shape and Feshbach resonances in the integral and differential state-to-state scattering cross sections, and we discuss the prospects for experimentally observing scattering resonances using Stark decelerated beams of OH radicals.

physics.atom-ph↗

arXiv2011

Scattering of Stark-decelerated OH radicals with rare-gas atoms

We present a combined experimental and theoretical study on the rotationally inelastic scattering of OH ($X\,^2Π_{3/2}, J=3/2, f$) radicals with the collision partners He, Ne, Ar, Kr, Xe, and D$_2$ as a function of the collision energy between $\sim 70$ cm$^{-1}$ and 400~cm$^{-1}$. The OH radicals are state selected and velocity tuned prior to the collision using a Stark decelerator, and field-free parity-resolved state-to-state inelastic relative scattering cross sections are measured in a crossed molecular beam configuration. For all OH-rare gas atom systems excellent agreement is obtained with the cross sections predicted by close-coupling scattering calculations based on accurate \emph{ab initio} potential energy surfaces. This series of experiments complements recent studies on the scattering of OH radicals with Xe [Gilijamse \emph{et al.}, Science {\bf 313}, 1617 (2006)], Ar [Scharfenberg \emph{et al.}, Phys. Chem. Chem. Phys. {\bf 12}, 10660 (2010)], He, and D$_2$ [Kirste \emph{et al.}, Phys. Rev. A {\bf 82}, 042717 (2010)]. A comparison of the relative scattering cross sections for this set of collision partners reveals interesting trends in the scattering behavior.

physics.atm-clus↗

arXiv2010

Multiple packets of neutral molecules revolving for over a mile

The level of control that one has over neutral molecules in beams dictates their possible applications. Here we experimentally demonstrate that state-selected, neutral molecules can be kept together in a few mm long packet for a distance of over one mile. This is accomplished in a circular arrangement of 40 straight electrostatic hexapoles through which the molecules propagate over 1000 times. Up to 19 packets of molecules have simultaneously been stored in this ring structure. This brings the realization of a molecular low-energy collider within reach.

physics.chem-ph↗

arXiv2010

Low-energy inelastic collisions of OH radicals with He atoms and D$_2$ molecules

We present an experimental study on the rotational inelastic scattering of OH ($X^2Π_{3/2}, J=3/2, f$) radicals with He and D$_2$ at collision energies between 100 and 500 cm$^{-1}$ 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$_2$ that are sensitive to the total (elastic and inelastic) cross sections (Sawyer \emph{et al.}, \emph{Phys. Rev. Lett.} \textbf{2008}, \emph{101}, 203203), but for which the measured cross sections could not be reproduced by theoretical calculations (Pavlovic \emph{et al.}, \emph{J. Phys. Chem. A} \textbf{2009}, \emph{113}, 14670). For the OH-He system, our experiments validate the inelastic cross sections determined from rigorous quantum calculations.

physics.atom-ph↗

arXiv2009

Loading Stark-decelerated molecules into electrostatic quadrupole traps

Beams of neutral polar molecules in a low-field seeking quantum state can be slowed down using a Stark decelerator, and can subsequently be loaded and confined in electrostatic quadrupole traps. The efficiency of the trap loading process is determined by the ability to couple the decelerated packet of molecules into the trap without loss of molecules and without heating. We discuss the inherent difficulties to obtain ideal trap loading, and describe and compare different trap loading strategies. A new "split-endcap" quadrupole trap design is presented that enables improved trap loading efficiencies. This is experimentally verified by comparing the trapping of OH radicals using the conventional and the new quadrupole trap designs.

physics.atom-ph↗

arXiv2008

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↗

arXiv2008

Reflection of OH molecules from magnetic mirrors

We have reflected a Stark-decelerated beam of OH molecules under normal incidence from mirrors consisting of permanent magnets. Two different types of magnetic mirrors have been demonstrated. A long-range flat mirror made from a large disc magnet has been used to spatially focus the reflected beam in the longitudinal direction ("bunching"). A short-range curved mirror composed of an array of small cube magnets allows for transverse focusing of the reflected beam.

physics.chem-ph↗

arXiv2008

The radiative lifetime of metastable CO ($a^3Π, v=0$)

We present a combined experimental and theoretical study on the radiative lifetime of CO in the $a^3Π_{1,2}, v=0$ state. CO molecules in a beam are prepared in selected rotational levels of this metastable state, Stark-decelerated and electrostatically trapped. From the phosphorescence decay in the trap, the radiative lifetime is measured to be $2.63\pm0.03$ ms for the $a^3Π_1, v=0, J=1$ level. From spin-orbit coupling between the $a^3Π$ and the $A^1Π$ state a 20% longer radiative lifetime of 3.16 ms is calculated for this level. It is concluded that coupling to other $^1Π$ states contributes to the observed phosphorescence rate of metastable CO.

physics.atom-ph↗

arXiv2008

Electrostatic trapping of metastable NH molecules

We report on the Stark deceleration and electrostatic trapping of $^{14}$NH ($a ^1Δ$) radicals. In the trap, the molecules are excited on the spin-forbidden $A ^3Π\leftarrow a ^1Δ$ transition and detected via their subsequent fluorescence to the $X ^3Σ^-$ ground state. The 1/e trapping time is 1.4 $\pm$ 0.1 s, from which a lower limit of 2.7 s for the radiative lifetime of the $a ^1Δ, v=0,J=2$ state is deduced. The spectral profile of the molecules in the trapping field is measured to probe their spatial distribution. Electrostatic trapping of metastable NH followed by optical pumping of the trapped molecules to the electronic ground state is an important step towards accumulation of these radicals in a magnetic trap.

physics.atom-ph↗

arXiv2007

Optical pumping of trapped neutral molecules by blackbody radiation

Optical pumping by blackbody radiation is a feature shared by all polar molecules and fundamentally limits the time that these molecules can be kept in a single quantum state in a trap. To demonstrate and quantify this, we have monitored the optical pumping of electrostatically trapped OH and OD radicals by room-temperature blackbody radiation. Transfer of these molecules to rotationally excited states by blackbody radiation at 295 K limits the $1/e$ trapping time for OH and OD in the $X^{2}Π_{3/2},v''=0,J''=3/2(f)$ state to 2.8 s and 7.1 s, respectively.

physics.atom-ph↗