arXiv subjects

Gerard Meijer

Publications and source records attributed to Gerard Meijer.

At least 19 recordsLinked to original sources

arXiv2026

A two-color dual-oscillator infrared free-electron laser

We report on the design and performance of a two-color dual-oscillator infrared free-electron laser (FEL). The mid-infrared (MIR) FEL at the Fritz Haber Institute (FHI FEL) has been upgraded to include a second oscillator FEL beamline that permits lasing in the far-infrared (FIR) regime from 4.5 {\mu}m to 175 {\mu}m. In addition, a 500 MHz kicker cavity has been installed downstream of the electron accelerator. It allows to deflect electron bunches of up to 50 MeV energy alternately left and right by an angle of {\pm}2{\deg}. It can, thus, split the high-repetition-rate (1 GHz) electron bunch train from the accelerator into two bunch trains of 500 MHz repetition rate each; one is steered to the MIR FEL and the other one to the new FIR FEL. In this two-color mode of simultaneous, synchronized operation the wavelengths in both FELs can be tuned independently over wide ranges of up to a factor of four each by undulator-gap variation. In addition, two-color operation is also available at reduced repetition rates (e.g. 55.6 MHz of both MIR and FIR pulses), as needed for some applications. This unique two-color mode opens up a wealth of novel user applications such as, MIR-FIR pump-probe experiments.

physics.acc-ph↗

arXiv2026

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↗

arXiv2026

Controlling isomer population using a dual-oscillator infrared free-electron laser

We report on the control and characterization of the isomer population of ions inside superfluid helium nanodroplets, using two-color operation of a dual-oscillator infrared free-electron laser. The timing of both lasers is highly synchronized, and their frequencies (or "colors") can be tuned independently over a wide range. Interaction of the singly deuterated proton-bound dimer of dihydrogen phosphate and formate inside helium nanodroplets with both colors enables the control over its isomer population and the recording of - one-color hidden - infrared spectra of individual isomers.

physics.chem-ph↗

arXiv2025

Magnetic atoms with a large electric dipole moment

We experimentally show that an electric dipole moment of more than 1 Debye can be induced in the dysprosium (Dy) atom, in a long-lived state that is about 17513 cm$^{-1}$ above the ground state. This metastable state is part of a strongly coupled opposite-parity doublet. Using optically detected microwave spectroscopy in an atomic beam, we determine the approximately 1.12 cm$^{-1}$ doublet spacing for the five stable bosonic isotopes of Dy with kHz-level accuracy. From the shift of the microwave transition frequency in low electric fields (below 150 V/cm) and from optical spectra in high electric fields (up to 150 kV/cm), a reduced transition dipole moment of 7.65 $\pm$ 0.05 Debye between the doublet states is extracted. In high electric fields the doublet interacts with a third state at 17727 cm$^{-1}$, that connects to the ground state via an electric-dipole transition. The three-state Stark interaction enables preparation of Dy atoms in the metastable state via single-photon excitation from the ground state.

physics.atom-ph↗

arXiv2025

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↗

arXiv2024

Photoelectron Circular Dichroism of Aqueous-Phase Alanine

Amino acids and other small chiral molecules play key roles in biochemistry. However, in order to understand how these molecules behave in vivo, it is necessary to study them under aqueous-phase conditions. Photoelectron circular dichroism (PECD) has emerged as an extremely sensitive probe of chiral molecules, but its suitability for application to aqueous solutions had not yet been proven. Here, we report on our PECD measurements of aqueous-phase alanine, the simplest chiral amino acid. We demonstrate that the PECD response of alanine in water is different for each of alanine's carbon atoms, and is sensitive to molecular structure changes (protonation states) related to the solution pH. For C~1s photoionization of alanine's carboxylic acid group, we report PECD of comparable magnitude to that observed in valence-band photoelectron spectroscopy of gas-phase alanine. We identify key differences between PECD experiments from liquids and gases, discuss how PECD may provide information regarding solution-specific phenomena -- for example the nature and chirality of the solvation shell surrounding chiral molecules in water -- and highlight liquid-phase PECD as a powerful new tool for the study of aqueous-phase chiral molecules of biological relevance.

physics.chem-ph↗

arXiv2024

Metal monoxide abundances as a function of the C/O ratio

The diatomic metal monoxides whose optical spectra define the classification of stars on the asymptotic giant branch (AGB), that is, TiO, YO, ZrO, and LaO, have the unusual property that their ionization energy is below their dissociation limit. The cations of these metal monoxides can be efficiently produced via associative ionization of their constituent ground state atoms and are long-lived. We present a simple model that can explain the observed relative abundance of these metal oxides as a function of the C/O ratio.

astro-ph.SR↗

arXiv2024

Cold molecular ions via autoionization below the dissociation limit

Several diatomic transition metal oxides, rare-earth metal oxides and fluorides have the unusual property that their bond dissociation energy is larger than their ionization energy. In these molecules, bound levels above the ionization energy can be populated via strong, resonant transitions from the ground state. The only relevant decay channel of these levels is autoionization; predissociation is energetically not possible and radiative decay is many orders of magnitude slower. Starting from translationally cold neutral molecules, translationally cold molecular ions can thus be produced with very high efficiency. By populating bound levels just above the ionization energy, internally cold molecular ions, exclusively occupying the lowest rotational level, are produced. This is experimentally shown here for the dysprosium monoxide molecule, DyO, for which the lowest bond dissociation energy is determined to be 0.0831(6) eV above the ionization energy.

physics.atm-clus↗

arXiv2024

Full quantum state control of chiral molecules

Controlling the internal quantum states of chiral molecules for a selected enantiomer has a wide range of fundamental applications. Using tailored microwave fields, a chosen rotational state can be enriched for a selected enantiomer, even starting from a racemic mixture. This enables rapid switching between samples of different enantiomers in a given state, holding great promise, for instance, for measuring parity violation in chiral molecules. Achieving full enantiomer-specific state transfer is a key requirement for this and many other applications. Although theoretically feasible, achieving the required experimental conditions seemed unrealistic. Here, we realize near-ideal conditions, overcoming both the limitations of thermal population and spatial degeneracy in rotational states. Our results show that 96% state-specific enantiomeric purity can be obtained from a racemic mixture, in an approach that is universally applicable to all chiral molecules of C1 symmetry.

physics.chem-ph↗

arXiv2023

The influence of microwave pulse conditions on enantiomer-specific state transfer

We report a combined experimental and theoretical study on the influence of microwave pulse durations on enantiomer-specific state transfer. Two triads of rotational states within a chiral molecule (1-indanol) are selected to address the possible scenarios. In the triad connected to the absolute ground state, the simplest triad that exists for all chiral molecules, the enantiomer-specific state transfer process simplifies into a sequence of two-level transitions. The second triad, including higher rotational states, represents a more generic scenario that involves multiple Rabi frequencies for each transition. Our study reveals that the conventional $\fracπ{2}-π-\fracπ{2}$ pulse sequence is not the optimal choice, except for the ideal case when in the simplest triad only the lowest level is initially populated. We find that employing a shorter duration for the first and last pulse of the sequence leads to significantly higher state-specific enantiomeric enrichment, albeit at the expense of overall population in the target state. Our experimental results are in very good agreement with theory, substantiating the quantitative understanding of enantiomer-specific state transfer.

physics.chem-ph↗

arXiv2023

How to measure work functions from aqueous solutions

The recent application of concepts from condensed-matter physics to photoelectron spectroscopy (PES) of volatile, liquid-phase systems has enabled the measurement of electronic energetics of liquids on an absolute scale. Particularly, vertical ionization energies, VIEs, of liquid water and aqueous solutions, both in the bulk and at associated interfaces, can now be routinely determined. These IEs are referenced to the local vacuum level, which is the appropriate quantity for condensed matter with associated surfaces, including liquids. Here, we connect this newly accessible energy level to another important surface property, namely, the solution work function, e$Φ_{liq}$. We lay out the prerequisites for and unique challenges of determining e$Φ$ of aqueous solutions and liquids in general. We demonstrate - for a model aqueous solution with a tetra-n-butylammonium iodide (TBAI) surfactant solute - that concentration-dependent work functions, associated with the surface dipoles generated by the segregated interfacial layer of TBA$^+$ and I$^-$ions, can be accurately measured under controlled conditions. We detail the nature of surface potentials, uniquely tied to the nature of the flowing-liquid sample, which must be eliminated or quantified to enable such measurements. This allows us to refer measured spectra of aqueous solutions to the Fermi level and quantitatively assign surfactant concentration-dependent spectral shifts to competing work function and electronic-structure effects, the latter determining, e.g., (electro)chemical reactivity. We describe the extension of liquid-jet PES to quantitatively access concentration-dependent surface descriptors that have so far been restricted to solid-phase measurements. These studies thus mark the beginning of a new era in the characterization of the interfacial electronic structure of aqueous solutions and liquids more generally.

cond-mat.soft↗

arXiv2023

Hyperfine structure and isotope shifts of the $^1P_1 \leftarrow{} ^{1}S_0$ transition in atomic zinc

We report absolute frequency, isotope shift, radiative lifetime and hyperfine structure measurements of the $^1P_1 \leftarrow{} ^{1}S_0$ (213.8 nm) transition in Zn I using a cryogenic buffer gas beam. Laser-induced fluorescence is collected with two orthogonally oriented detectors to take advantage of differences in the emission pattern of the isotopes. This enables clear distinction between isotopes whose resonances are otherwise unresolved, and a measurement of the fermion hyperfine structure parameters, $A(^{67}$Zn)$=20(2)$ MHz and $B(^{67}$Zn)$=10(5)$ MHz. We reference our frequency measurements to an ultralow expansion cavity and achieve an uncertainty at the level of 1 MHz, about 1 percent of the natural linewidth of the transition.

physics.atom-ph↗

arXiv2023

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↗

arXiv2022

Cryogenic Buffer Gas beams of AlF, CaF, MgF, YbF, Al, Ca, Yb and NO -- a comparison

Cryogenic buffer gas beams are central to many cold molecule experiments. Here, we use absorption and fluorescence spectroscopy to directly compare molecular beams of AlF, CaF, MgF, and YbF molecules, produced by chemical reaction of laser ablated atoms with fluorine rich reagents. The beam brightness for AlF is measured as $2\times 10^{12}$ molecules per steradian per pulse in a single rotational state, comparable to an Al atomic beam produced in the same setup. The CaF, MgF and YbF beams show an order of magnitude lower brightness than AlF, and far below the brightness of Ca and Yb beams. The addition of either NF$_3$ or SF$_6$ to the cell extinguishes the Al atomic beam, but has a minimal effect on the Ca and Yb beams. NF$_3$ reacts more efficiently than SF$_6$, as a significantly lower flow rate is required to maximise the molecule production, which is particularly beneficial for long-term stability of the AlF beam. We use NO as a proxy for the reactant gas as it can be optically detected. We demonstrate that a cold, rotationally pure NO beam can be generated by laser desorption, thereby gaining insight into the dynamics of the reactant gas inside the buffer gas cell.

physics.atom-ph↗

arXiv2022

High-resolution isotope-shift spectroscopy of Cd I

We present absolute frequency measurements of the ${}^{1}\text{P}_1 \leftarrow {}^{1}\text{S}_0$ ($229$nm) and ${}^{3}\text{P}_1 \leftarrow {}^{1}\text{S}_0$ ($326$nm) transitions for all naturally occurring isotopes of cadmium. The isotope shifts and hyperfine intervals of the fermionic isotopes are determined with an accuracy of 3.3MHz. We find that quantum interference in the laser-induced fluorescence spectra of the ${}^{1}\text{P}_1 \leftarrow {}^{1}\text{S}_0$ transition causes an error of up to 29(5)MHz in determining the hyperfine splitting, when not accounted for with an appropriate model. Using a King-plot analysis, we extract the field- and mass-shift parameters and determine nuclear charge radius differences for the fermions. The lifetime of the $^1\text{P}_1$ state is determined to be 1.60(5)ns by measuring the natural linewidth of the ${}^{1}\text{P}_1 \leftarrow {}^{1}\text{S}_0$ transition. These results resolve significant discrepancies among previous measurements.

physics.atom-ph↗

arXiv2022

Quantitative study of enantiomer-specific state transfer

We here report on a quantitative study of Enantiomer-Specific State Transfer (ESST), performed in a pulsed, supersonic molecular beam. The chiral molecule 1-indanol is cooled to low rotational temperatures (1-2 K) and a selected rotational level in the electronic and vibrational ground state of the most abundant conformer is depleted via optical pumping on the $S_{1} \leftarrow S_{0}$ transition. Further downstream, three consecutive microwave pulses with mutually perpendicular polarizations and with a well-defined duration and phase are applied. The population in the originally depleted rotational level is subsequently monitored via laser induced fluorescence (LIF) detection. This scheme enables a quantitative comparison of experiment and theory for the transfer efficiency in what is the simplest ESST triangle for any chiral molecule, that is, the one involving the absolute ground state level, $\left|J_{K_{a}K_{c}}\right\rangle = \left|0_{00}\right\rangle$. Moreover, this scheme improves the enantiomer enrichment by over an order of magnitude compared to previous works. Starting with a racemic mixture, a straightforward extension of this scheme allows to create a molecular beam with an enantiomer-pure rotational level, holding great prospects for future spectroscopic and scattering studies.

physics.chem-ph↗

arXiv2022

Photoelectron circular dichroism in angle-resolved photoemission from liquid fenchone

We present an experimental X-ray photoelectron circular dichroism (PECD) study of liquid fenchone at the C 1s edge. A novel setup to enable PECD measurements on a liquid microjet [Malerz et al., Rev. Sci. Instrum., 2022, 93, 015101] was used. For the C 1s line assigned to fenchone's carbonyl carbon, a non-vanishing asymmetry is found in the intensity of photoelectron spectra acquired under a fixed angle in the backward-scattering plane. This experiment paves the way towards a novel probe of the chirality of organic/biological molecules in aqueous solution.

physics.chem-ph↗

arXiv2022

Spectroscopic characterization of the a$^3Π$ state of aluminum monofluoride

Spectroscopic studies of aluminum monofluoride (AlF) have revealed its highly favorable properties for direct laser cooling. All $Q$ lines of the strong A$^1Π$ $\leftarrow$ X$^1Σ^+$ transition around 227~nm are rotationally closed and thereby suitable for the main cooling cycle. The same holds for the narrow, spin-forbidden a$^3Π$ $\leftarrow$ X$^1Σ^+$ transition around 367 nm which has a recoil limit in the micro Kelvin range. We here report on the spectroscopic characterization of the lowest rotational levels in the a$^3Π$ state of AlF for $v=0-8$ using a jet-cooled, pulsed molecular beam. An accidental AC Stark shift is observed on the a$^3Π_0, v=4$ $\leftarrow$ X$^1Σ^+, v=4$ band. By using time-delayed ionization for state-selective detection of the molecules in the metastable a$^3Π$ state at different points along the molecular beam, the radiative lifetime of the a$^3Π_1, v=0, J=1$ level is experimentally determined as $τ=1.89 \pm 0.15$~ms. A laser/radio-frequency multiple resonance ionization scheme is employed to determine the hyperfine splittings in the a$^3Π_1, v=5$ level. The experimentally derived hyperfine parameters are compared to the outcome of quantum chemistry calculations. A spectral line with a width of 1.27 kHz is recorded between hyperfine levels in the a$^3Π, v=0$ state. These measurements benchmark the electronic potential of the a$^3Π$ state and yield accurate values for the photon scattering rate and for the elements of the Franck-Condon matrix of the a$^3Π$ $-$ X$^1Σ^+$ system.

physics.chem-ph↗