arXiv subjects

Gerard Meijer

Publications and source records attributed to Gerard Meijer.

At least 73 records · Page 4Linked to original sources

arXiv2010

Catching proteins in liquid helium droplets

An experimental approach is presented that allows for the incorporation of large mass/charge selected ions in liquid helium droplets. It is demonstrated that droplets can be efficiently doped with a mass/charge selected amino acid as well as with the much bigger m$\approx$12 000 amu protein Cytochrome C in selected charge states. The sizes of the ion-doped droplets are determined via electrostatic deflection. Under the experimental conditions employed, the observed droplet sizes are very large and range, dependent on the incorporated ion, from 10$^{10}$ helium atoms for protonated Phenylalanine to 10$^{12}$ helium atoms for Cytochrome C. As a possible explanation, a simple model based on the size- and internal energy-dependence of the pickup efficiency is given.

physics.atm-clus↗

arXiv2010

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↗

arXiv2010

CO adsorption on neutral iridium clusters

The adsorption of carbon monoxide on neutral iridium clusters in the size range of n = 3 to 21 atoms is investigated with infrared multiple photon dissociation spectroscopy. For each cluster size only a single v(CO) band is present with frequencies in the range between 1962 cm-1 (n = 8) and 1985 cm-1 (n = 18) which can be attributed to an atop binding geometry. This behaviour is compared to the CO binding geometries on clusters of other group 9 and 10 transition metals as well as to that on extended surfaces. The preference of Ir for atop binding is rationalized by relativistic effects on the electronic structure of the later 5d metals.

physics.chem-ph↗

arXiv2010

Microwave Lens for Polar Molecules

We here report on the implementation of a microwave lens for neutral polar molecules suitable to focus molecules both in low-field-seeking and in high-field-seeking states. By using the TE_11m modes of a 12 cm long cylindrically symmetric microwave resonator, Stark-decelerated ammonia molecules are transversally confined. We investigate the focusing properties of this microwave lens as a function of the molecules' velocity, the detuning of the microwave frequency from the molecular resonance frequency, and the microwave power. Such a microwave lens can be seen as a first important step towards further microwave devices, such as decelerators and traps.

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↗

arXiv2010

Coherent reflection of He atom beams from rough surfaces at near-grazing incidence

We here report coherent reflection of thermal He atom beams from various microscopically rough surfaces at grazing incidence. For a sufficiently small normal component $k_z$ of the incident wave-vector of the atom the reflection probability is found to be a function of $k_z$ only. This behavior is explained by quantum-reflection at the attractive branch of the Casimir-van der Waals interaction potential. For larger values of $k_z$ the overall reflection probability decreases rapidly and is found to also depend on the parallel component $k_x$ of the wave-vector. The material specific $k_x$ dependence for this classical reflection at the repulsive branch of the potential is explained qualitatively in terms of the averaging-out of the surface roughness under grazing incidence conditions.

physics.atom-ph↗

arXiv2010

Emerging beam resonances in atom diffraction from a reflection grating

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 merges parallel to the grating surface. The observed anomalies are discussed in terms of the classical wave-optical model of Rayleigh and Fano.

physics.atom-ph↗

arXiv2010

Photoelectron angular distributions from strong-field ionization of oriented molecules

The combination of photoelectron spectroscopy and ultrafast light sources is on track to set new standards for detailed interrogation of dynamics and reactivity of molecules. A crucial prerequisite for further progress is the ability to not only detect the electron kinetic energy, as done in traditional photoelectron spectroscopy, but also the photoelectron angular distributions (PADs) in the molecular frame. Here carbonylsulfide (OCS) and benzonitrile molecules, fixed in space by combined laser and electrostatic fields, are ionized with intense, circularly polarized, 30 femtosecond laser pulses. For 1-dimensionally oriented OCS the molecular frame PADs exhibit pronounced anisotropies, perpendicular to the fixed permanent dipole moment, that are absent in PADs from randomly oriented molecules. For 3-dimensionally oriented benzonitrile additional striking structures appear due to suppression of electron emission in nodal planes of the fixed electronic orbitals. Our theoretical analysis, relying on tunneling ionization theory, shows that the PADs reflect nodal planes, permanent dipole moments and polarizabilities of both the neutral molecule and its cation. The calculated results are exponentially sensitive to changes in these molecular properties thereby pointing to exciting opportunities for time-resolved probing of valence electrons dynamics by intense circularly polarized pulses. Molecular frame PADs from oriented molecules will prove important in other contexts notably in emerging free-electron-laser studies where localized inner shell electrons are knocked off by x-ray pulses.

physics.atom-ph↗

arXiv2010

Alternating Gradient Focusing and Deceleration of Polar Molecules

Beams of polar molecules can be focused using an array of electrostatic lenses in alternating gradient (AG) configuration. They can also be accelerated or decelerated by applying an appropriate high voltage switching sequence to the lenses. AG focusing is applicable to molecules in both low-field and high-field-seeking states and is particularly well suited to the problem of decelerating heavy molecules and those in their ground rotational state. We describe the principles of AG deceleration and set out criteria to be followed in decelerator design, construction and operation. We calculate the longitudinal and transverse focusing properties of a decelerator, and exemplify this by 2D-imaging studies of a decelerated beam of metastable CO molecules.

physics.atom-ph↗

arXiv2010

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↗

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↗

arXiv2009

Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields

Supersonic beams of polar molecules are deflected using inhomogeneous electric fields. The quantum-state selectivity of the deflection is used to spatially separate molecules according to their quantum state. A detailed analysis of the deflection and the obtained quantum-state selection is presented. The rotational temperatures of the molecular beams are determined from the spatial beam profiles and are all approximately 1 K. Unprecedented degrees of laser-induced alignment $(<\cos^2θ_{2D}>=0.972)$ and orientation of iodobenzene molecules are demonstrated when the state-selected samples are used. Such state-selected and oriented molecules provide unique possibilities for many novel experiments in chemistry and physics.

physics.chem-ph↗

arXiv2009

Laser-induced 3D alignment and orientation of quantum-state-selected molecules

A strong inhomogeneous static electric field is used to spatially disperse a rotationally cold supersonic beam of 2,6-difluoroiodobenzene molecules according to their rotational quantum state. The molecules in the lowest lying rotational states are selected and used as targets for 3-dimensional alignment and orientation. The alignment is induced in the adiabatic regime with an elliptically polarized, intense laser pulse and the orientation is induced by the combined action of the laser pulse and a weak static electric field. We show that the degree of 3-dimensional alignment and orientation is strongly enhanced when rotationally state-selected molecules, rather than molecules in the original molecular beam, are used as targets.

physics.chem-ph↗

arXiv2009

Manipulating the motion of large neutral molecules

Large molecules have complex potential-energy surfaces with many local minima. They exhibit multiple stereo-isomers, even at very low temperatures. In this paper we discuss the different approaches for the manipulation of the motion of large and complex molecules, like amino acids or peptides, and the prospects of state- and conformer-selected, focused, and slow beams of such molecules for studying their molecular properties and for fundamental physics studies. Accepted for publication in Faraday Disc. 142 (2009), DOI: 10.1039/b820045a

physics.atom-ph↗

arXiv2009

Nonadiabatic transitions in electrostatically trapped ammonia molecules

Nonadiabatic transitions are known to be major loss channels for atoms in magnetic traps, but have thus far not been experimentally reported upon for trapped molecules. We have observed and quantified losses due to nonadiabatic transitions for three isotopologues of ammonia in electrostatic traps, by comparing the trapping times in traps with a zero and a non-zero electric field at the center. Nonadiabatic transitions are seen to dominate the overall loss rate even for samples at relatively high temperatures of 10-50 mK.

physics.atom-ph↗

arXiv2008

A Stark decelerator on a chip

A microstructured array of 1254 electrodes on a substrate has been configured to generate an array of local minima of electric field strength with a periodicity of 120 $μ$m about 25 $μ$m above the substrate. By applying sinusoidally varying potentials to the electrodes, these minima can be made to move smoothly along the array. Polar molecules in low-field seeking quantum states can be trapped in these traveling potential wells. Recently, we experimentally demonstrated this by transporting metastable CO molecules at constant velocities above the substrate [Phys. Rev. Lett. 100 (2008) 153003]. Here, we outline and experimentally demonstrate how this microstructured array can be used to decelerate polar molecules directly from a molecular beam. For this, the sinusoidally varying potentials need to be switched on when the molecules arrive above the chip, their frequency needs to be chirped down in time, and they need to be switched off before the molecules leave the chip again. Deceleration of metastable CO molecules from an initial velocity of 360 m/s to a final velocity as low as 240 m/s is demonstrated in the 15-35 mK deep potential wells above the 5 cm long array of electrodes. This corresponds to a deceleration of almost $10^5$ $g$, and about 85 cm$^{-1}$ of kinetic energy is removed from the metastable CO molecules in this process.

physics.atom-ph↗

arXiv2008

Quantum reflection of helium atom beams from a microstructured grating

We observe high-resolution diffraction patterns of a thermal-energy helium-atom beam reflected from a microstructured surface grating at grazing incidence. The grating consists of 10-$μ$m-wide Cr strips patterned on a quartz substrate and has a periodicity of 20 $μ$m. Fully-resolved diffraction peaks up to the $7^{\rm th}$ order are observed at grazing angles up to 20 mrad. With changes in de Broglie wavelength or grazing angle the relative diffraction intensities show significant variations which shed light on the nature of the atom-surface interaction potential. The observations are explained in terms of quantum reflection at the long-range attractive Casimir-van der Waals potential.

physics.atom-ph↗

arXiv2008

Nature of Ar bonding to small Co_n^+ clusters and its effect on the structure determination by far-infrared absorption spectroscopy

Far-infrared vibrational spectroscopy by multiple photon dissociation has proven to be a very useful technique for the structural fingerprinting of small metal clusters. Contrary to previous studies on cationic V, Nb and Ta clusters, measured vibrational spectra of small cationic cobalt clusters show a strong dependence on the number of adsorbed Ar probe atoms, which increases with decreasing cluster size. Focusing on the series Co_4^+ to Co_8^+ we therefore use density-functional theory to analyze the nature of the Ar-Co_n^+ bond and its role for the vibrational spectra. In a first step, energetically low-lying isomer structures are identified through first-principles basin-hopping sampling runs and their vibrational spectra computed for a varying number of adsorbed Ar atoms. A comparison of these fingerprints with the experimental data enables in some cases a unique assignment of the cluster structure. Independent of the specific low-lying isomer, we obtain a pronounced increase of the Ar binding energy for the smallest cluster sizes, which correlates nicely with the observed increased influence of the Ar probe atoms on the IR spectra. Further analysis of the electronic structure motivates a simple electrostatic picture that not only explains this binding energy trend, but also why the influence of the rare-gas atom is much stronger than in the previously studied systems.

cond-mat.mtrl-sci↗