arXiv subjects

Hendrick L. Bethlem

Publications and source records attributed to Hendrick L. Bethlem.

At least 19 recordsLinked to original sources

arXiv2025

A cold beam of BaOH molecules using a water-vapour seeded neon gas

In this paper we report on the production and characterization of a cold beam of BaOH molecules using a cryogenic buffer-gas beam source. BaOH is a highly suitable molecule for studies of the violation of fundamental symmetries, such as the search for the electron's electric dipole moment. BaOH molecules are synthesised inside the cold source through laser ablation of a barium metal target while water vapor is seeded into the neon buffer gas. The BaOH flux is significantly enhanced ($\sim$11 times) when laser-exciting the barium atoms inside the buffer-gas cell on the $^1\mathrm S_0 - ^3\mathrm P_1$ transition. A similar enhancement has been reported for other alkaline-earth(-like) monohydroxides. For typical source conditions, the molecular beam has an average velocity of $\approx180$ m/s and an intensity of $\sim 10^{9}$ molecules s$^{-1}$ in $N=1$, which is comparable to that of cryogenic BaF beams.

physics.atom-ph↗

arXiv2025

2D transverse laser cooling of a hexapole focused beam of cold BaF molecules

A cryogenic buffer gas beam, an electrostatic hexapole lens, and 2D transverse Doppler laser cooling are combined to produce a bright beam of barium monofluoride ($^{138}$Ba$^{19}$F) molecules. Experimental results and trajectory simulations are used to study the laser cooling effect as a function of laser detuning, laser power, laser alignment, and interaction time. A scattering rate of 6.1(1.4) $\times 10^{5}$ s$^{-1}$ on the laser cooling transition is obtained; this is $14 \%$ of the expected maximum, which is attributed to limited control of the magnetic field used to remix dark states. Using 3 tuneable lasers with appropriate sidebands and detuning, each molecule scatters approximately 400 photons during 2D laser cooling, limited by the interaction time and scattering rate. Leaks to dark states are less than 10$\%$. The experimental results are used to benchmark the trajectory simulations to predict the achievable flux 3.5 m downstream for a planned $e$EDM experiment.

physics.atom-ph↗

arXiv2024

Manipulating a beam of barium fluoride molecules using an electrostatic hexapole

An electrostatic hexapole lens is used to manipulate the transverse properties of a beam of barium fluoride molecules from a cryogenic buffer gas source. The spatial distribution of the beam is measured by recording state-selective laser-induced fluorescence on an emccd camera, providing insight into the intensity and transverse position spread of the molecular beam. Although the high mass and unfavorable Stark shift of barium fluoride pose a considerable challenge, the number of molecules in the low-field seeking component of the N=1 state that pass a 4 mm diameter aperture 712 mm behind the source is increased by a factor of 12. Furthermore, it is demonstrated that the molecular beam can be displaced by up to +/-5 mm by moving the hexapole lens. Our measurements agree well with numerical trajectory simulations. We discuss how electrostatic lenses may be used to increase the sensitivity of beam experiments such as the search for the electric dipole moment of the electron.

physics.atom-ph↗

arXiv2024

A novel method to determine the phase-space distribution of a pulsed molecular beam

We demonstrate a novel method to determine the longitudinal phase-space distribution of a cryogenic buffer gas beam of barium-fluoride molecules based on a two-step laser excitation scheme. The spatial resolution is achieved by a transversely aligned laser beam that drives molecules from the ground state $X^2Σ^+$ to the $A^2Π_{1/2}$ state around 860 nm, while the velocity resolution is obtained by a laser beam that is aligned counter-propagating with respect to the molecular beam and that drives the Doppler shifted $A^2Π_{1/2}$ to $D^2Σ^+$ transition around 797 nm. Molecules in the $D$-state are detected virtually background-free by recording the fluorescence from the $D-X$ transition at 413 nm. As molecules in the ground state do not absorb light at 797 nm, problems due to due to optical pumping are avoided. Furthermore, as the first step uses a narrow transition, this method can also be applied to molecules with hyperfine structure. The measured phase-space distributions, reconstructed at the source exit, show that the average velocity and velocity spread vary significantly over the duration of the molecular beam pulse. Our method gives valuable insight into the dynamics in the source and helps to reduce the velocity and increase the intensity of cryogenic buffer gas beams. In addition, transition frequencies are reported for the $X-A$ and $X-D$ transitions in barium fluoride with an absolute accuracy below 0.3 MHz.

physics.atom-ph↗

arXiv2022

Electric dipole moments and the search for new physics

Static electric dipole moments of nondegenerate systems probe mass scales for physics beyond the Standard Model well beyond those reached directly at high energy colliders. Discrimination between different physics models, however, requires complementary searches in atomic-molecular-and-optical, nuclear and particle physics. In this report, we discuss the current status and prospects in the near future for a compelling suite of such experiments, along with developments needed in the encompassing theoretical framework.

hep-ph↗

arXiv2022

Pauli blocking of stimulated emission in a degenerate Fermi gas

The Pauli exclusion principle in quantum mechanics has a profound influence on the structure of matter and on interactions between fermions. Almost 30 years ago it was predicted that the Pauli exclusion principle could lead to a suppression of spontaneous emission, and only recently several experiments confirmed this phenomenon. Here we report that this so-called Pauli blockade not only affects incoherent processes but also, more generally, coherently driven systems. It manifests itself as an intriguing sub-Doppler narrowing of a doubly-forbidden transition profile in an optically trapped Fermi gas of $^3\mathrm{He}$. By actively pumping atoms out of the excited state, we break the coherence of the excitation and lift the narrowing effect, confirming the influence of Pauli blockade on the transition profile. This new insight into the interplay between quantum statistics and coherent driving is a promising development for future applications involving fermionic systems.

physics.atom-ph↗

arXiv2022

Benchmarking of the Fock space coupled cluster method and uncertainty estimation: Magnetic hyperfine interaction in the excited state of BaF

We present an investigation of the performance of the relativistic multi-reference Fock-space coupled cluster (FSCC) method for predicting molecular hyperfine structure (HFS) constants, including a thorough computational study to estimate the associated uncertainties. In particular, we considered the $^{19}$F HFS constant in the ground and excited states of BaF. Due to a larger basis set dependence, the uncertainties on the excited state results (16-85%) were found to be significantly larger than those on the ground state constants ($\sim$2%). The ab initio values were compared to the recent experimental results, and good overall agreement within the theoretical uncertainties was found. This work demonstrates the predictive power of the FSCC method and the reliability of the established uncertainty estimates, which can be crucial in cases where the calculated property cannot be directly compared to experiment.

physics.atom-ph↗

arXiv2021

Systematic study and uncertainty evaluation of $P,T$-odd molecular enhancement factors in BaF

A measurement of the magnitude of the electric dipole moment of the electron (eEDM) larger than that predicted by the Standard Model (SM) of particle physics is expected to have a huge impact on the search for physics beyond the SM. Polar diatomic molecules containing heavy elements experience enhanced sensitivity to parity ($P$) and time-reversal ($T$)-violating phenomena, such as the eEDM and the scalar-pseudoscalar (S-PS) interaction between the nucleons and the electrons, and are thus promising candidates for measurements. The NL-\textit{e}EDM collaboration is preparing an experiment to measure the eEDM and S-PS interaction in a slow beam of cold BaF molecules [Eur. Phys. J. D, 72, 197 (2018)]. Accurate knowledge of the electronic structure parameters, $W_d$ and $W_s$, connecting the eEDM and the S-PS interaction to the measurable energy shifts is crucial for the interpretation of these measurements. In this work we use the finite field relativistic coupled cluster approach to calculate the $W_d$ and $W_s$ parameters in the ground state of the BaF molecule. Special attention was paid to providing a reliable theoretical uncertainty estimate based on investigations of the basis set, electron correlation, relativistic effects and geometry. Our recommended values of the two parameters, including conservative uncertainty estimates, are 3.13 $\pm$ $0.12 \times 10^{24}\frac{\text{Hz}}{e\cdot \text{cm}}$ for $W_d$ and 8.29 $\pm$ 0.12 kHz for $W_s$.

physics.atom-ph↗

arXiv2019

High accuracy theoretical investigations of CaF, SrF, and BaF and implications for laser-cooling

The NL-eEDM collaboration is building an experimental setup to search for the permanent electric dipole moment of the electron in a slow beam of cold barium fluoride molecules [Eur. Phys. J. D, 72, 197 (2018)]. Knowledge of molecular properties of BaF is thus needed to plan the measurements and in particular to determine an optimal laser-cooling scheme. Accurate and reliable theoretical predictions of these properties require incorporation of both high-order correlation and relativistic effects in the calculations. In this work theoretical investigations of the ground and the lowest excited states of BaF and its lighter homologues, CaF and SrF, are carried out in the framework of the relativistic Fock-space coupled cluster (FSCC) and multireference configuration interaction (MRCI) methods. Using the calculated molecular properties, we determine the Franck-Condon factors (FCFs) for the $A^2Π_{1/2} \rightarrow X^2Σ^{+}_{1/2}$ transition, which was successfully used for cooling CaF and SrF and is now considered for BaF. For all three species, the FCFs are found to be highly diagonal. Calculations are also performed for the $B^2Σ^{+}_{1/2} \rightarrow X^2Σ^{+}_{1/2}$ transition recently exploited for laser-cooling of CaF; it is shown that this transition is not suitable for laser-cooling of BaF, due to the non-diagonal nature of the FCFs in this system. Special attention is given to the properties of the $A'^2Δ$ state, which in the case of BaF causes a leak channel, in contrast to CaF and SrF species where this state is energetically above the excited states used in laser-cooling. We also present the dipole moments of the ground and the excited states of the three molecules and the transition dipole moments (TDMs) between the different states.

physics.atom-ph↗

arXiv2018

Measuring the electric dipole moment of the electron in BaF

We investigate the merits of a measurement of the permanent electric dipole moment of the electron ($e$EDM) with barium monofluoride molecules, thereby searching for phenomena of CP violation beyond those incorporated in the Standard Model of particle physics. Although the BaF molecule has a smaller enhancement factor in terms of the effective electric field than other molecules used in current studies (YbF, ThO and ThF$^+$), we show that a competitive measurement is possible by combining Stark-deceleration, laser-cooling and an intense primary cold source of BaF molecules. With the long coherent interaction times obtainable in a cold beam of BaF, a sensitivity of $5\times10^{-30}$ e$\cdot$cm for an $e$EDM is feasible. We describe the rationale, the challenges and the experimental methods envisioned to achieve this target.

physics.atom-ph↗

arXiv2017

Cold collisions in a molecular synchrotron

We study collisions between neutral, deuterated ammonia molecules (ND$_3$) stored in a 50 cm diameter synchrotron and argon atoms in co-propagating supersonic beams. The advantages of using a synchrotron in collision studies are twofold: (i) By storing ammonia molecules many round-trips, the sensitivity to collisions is greatly enhanced; (ii) The collision partners move in the same direction as the stored molecules, resulting in low collision energies. We tune the collision energy in three different ways: by varying the velocity of the stored ammonia packets, by varying the temperature of the pulsed valve that releases the argon atoms, and by varying the timing between the supersonic argon beam and the stored ammonia packets. These give consistent results. We determine the relative, total, integrated cross-section for $\mathrm{ND}_3+\mathrm{Ar}$ collisions in the energy range of 40-140 cm$^{-1}$, with a resolution of 5-10 cm$^{-1}$ and an uncertainty of 7-15%. Our measurements are in good agreement with theoretical scattering calculations.

physics.chem-ph↗

arXiv2016

A molecular fountain

The resolution of any spectroscopic or interferometric experiment is ultimately limited by the total time a particle is interrogated. We here demonstrate the first molecular fountain, a development which permits hitherto unattainably long interrogation times with molecules. In our experiments, ammonia molecules are decelerated and cooled using electric fields, launched upwards with a velocity between 1.4 and 1.9\,m/s and observed as they fall back under gravity. A combination of quadrupole lenses and bunching elements is used to shape the beam such that it has a large position spread and a small velocity spread (corresponding to a transverse temperature of $<$10\,$μ$K and a longitudinal temperature of $<$1\,$μ$K) when the molecules are in free fall, while being strongly focused at the detection region. The molecules are in free fall for up to 266\,milliseconds, making it possible to perform sub-Hz measurements in molecular systems and paving the way for stringent tests of fundamental physics theories.

physics.chem-ph↗

arXiv2014

Preparation of an ultra-cold sample of ammonia molecules for precision measurements

We present experiments in which an ultra-cold sample of ammonia molecules is released from an electrostatic trap and recaptured after a variable time. It is shown that, by performing adiabatic cooling before releasing the molecules and adiabatic re-compression after they are recaptured, we are able to observe molecules even after more than 10 ms of free expansion. A coherent measurement performed during this time will have a statistical uncertainty that decreases approximately as the inverse of the square root of the expansion time. This offers interesting prospects for high-resolution spectroscopy and precision tests of fundamental physics theories.

physics.chem-ph↗

arXiv2013

Robust Constraint on a Drifting Proton-to-Electron Mass Ratio at z=0.89 from Methanol Observation at Three Radio Telescopes

A limit on a possible cosmological variation of the proton-to-electron mass ratio $μ$ is derived from methanol (CH$_3$OH) absorption lines in the benchmark PKS1830$-$211 lensing galaxy at redshift $z = 0.89$ observed with the Effelsberg 100-m radio telescope, the Institute de Radio Astronomie Millimétrique 30-m telescope, and the Atacama Large Millimeter/submillimeter Array. Ten different absorption lines of CH$_3$OH covering a wide range of sensitivity coefficients $K_μ$ are used to derive a purely statistical 1-$σ$ constraint of $Δμ/μ= (1.5 \pm 1.5) \times 10^{-7}$ for a lookback time of 7.5 billion years. Systematic effects of chemical segregation, excitation temperature, frequency dependence and time variability of the background source are quantified. A multi-dimensional linear regression analysis leads to a robust constraint of $Δμ/μ= (-1.0 \pm 0.8_{\rm stat} \pm 1.0_{\rm sys}) \times 10^{-7}$.

astro-ph.CO↗

arXiv2013

Perspective: Tipping the scales - search for drifting constants from molecular spectra

Transitions in atoms and molecules provide an ideal test ground for constraining or detecting a possible variation of the fundamental constants of nature. In this Perspective, we review molecular species that are of specific interest in the search for a drifting proton-to-electron mass ratio $μ$. In particular, we outline the procedures that are used to calculate the sensitivity coefficients for transitions in these molecules and discuss current searches. These methods have led to a rate of change in $μ$ bounded to $6 \times 10^{-14}$/yr from a laboratory experiment performed in the present epoch. On a cosmological time scale the variation is limited to $|Δμ/μ| < 10^{-5}$ for look-back times of 10-12 billion years and to $|Δμ/μ| < 10^{-7}$ for look-back times of 7 billion years. The last result, obtained from high-redshift observation of methanol, translates into $\dotμ/μ= (1.4 \pm 1.4) \times 10^{-17}$/yr if a linear rate of change is assumed.

physics.chem-ph↗

arXiv2013

Deceleration and trapping of ammonia molecules in a traveling wave decelerator

We have recently demonstrated static trapping of ammonia isotopologues in a decelerator that consists of a series of ring-shaped electrodes to which oscillating high voltages are applied [Quintero-Pérez et al., Phys. Rev. Lett. 110, 133003 (2013)]. In this paper we provide further details on this traveling wave decelerator and present new experimental data that illustrate the control over molecules that it offers. We analyze the performance of our setup under different deceleration conditions and demonstrate phase-space manipulation of the trapped molecular sample.

physics.atom-ph↗

arXiv2013

Methyl mercaptan (CH3SH) as a probe for $μ$ variation

Torsion-rotation transitions in molecules exhibiting hindered internal rotation possess enhanced sensitivities to a variation of the proton-to-electron mass ratio. This enhancement occurs due to a cancellation of energies associated with the torsional and rotational degrees of freedom of the molecule. This effect occurs generally in every internal rotor molecule, but is exceptionally large in methanol. In this paper we calculate the sensitivity coefficients of methyl mercaptan, the thiol analogue of methanol. The obtained sensitivity coefficients in this molecule range from $K_μ=-14.8$ to $+12.2$ for transitions with a lower-level excitation energy below 10\,cm$^{-1}$.

physics.atom-ph↗

arXiv2013

Static trapping of polar molecules in a traveling wave decelerator

We present experiments on decelerating and trapping ammonia molecules using a combination of a Stark decelerator and a traveling wave decelerator. In the traveling wave decelerator a moving potential is created by a series of ring-shaped electrodes to which oscillating high voltages are applied. By lowering the frequency of the applied voltages, the molecules confined in the moving trap are decelerated and brought to a standstill. As the molecules are confined in a true 3D well, this new kind of deceleration has practically no losses, resulting in a great improvement on the usual Stark deceleration techniques. The necessary voltages are generated by amplifying the output of an arbitrary wave generator using fast HV-amplifiers, giving us great control over the trapped molecules. We illustrate this by experiments in which we adiabatically cool trapped NH3 and ND3 molecules and resonantly excite their motion.

physics.atom-ph↗