Search

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 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 insight into the interplay between quantum statistics and coherent driving is a promising development for future applications involving fermionic systems., (© 2022. The Author(s).)

We report on the electrostatic trapping of neutral SrF molecules. The molecules are captured from a cryogenic buffer-gas beam source into the moving traps of a 4.5-m-long traveling-wave Stark decelerator. The SrF molecules in X^{2}Σ^{+}(v=0,N=1) state are brought to rest as the velocity of the moving traps is gradually reduced from 190  m/s to zero. The molecules are held for up to 50 ms in multiple electric traps of the decelerator. The trapped packets have a volume (FWHM) of 1  mm^{3} and a velocity spread of 5(1)  m/s, which corresponds to a temperature of 60(20) mK. Our result demonstrates a factor 3 increase in the molecular mass that has been Stark decelerated and trapped. Heavy molecules (mass>100  amu) offer a highly increased sensitivity to probe physics beyond the standard model. This work significantly extends the species of neutral molecules of which slow beams can be created for collision studies, precision measurement, and trapping experiments.

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-eEDM collaboration is preparing an experiment to measure the eEDM and S-PS interaction in a slow beam of cold BaF molecules [P. Aggarwal et al., 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 ±0.12×10 24 Hzecm for W d and 8.29 ± 0.12 kHz for W s .

A supersonic beam source for SrF and BaF molecules is constructed by combining the expansion of carrier gas (a mixture of 2% SF 6 and 98% argon) from an Even-Lavie valve with laser ablation of a barium/strontium metal target at a repetition rate of 10 Hz. Molecular beams with a narrow translational velocity spread are produced at relative values of Δv/v = 0.053(11) and 0.054(9) for SrF and BaF, respectively. The relative velocity spread of the beams produced in our source is lower in comparison with the results from other metal fluoride beams produced in supersonic laser ablation sources. The rotational temperature of BaF is measured to be 3.5 K. The source produces 6 × 10 8 and 10 7 molecules per steradian per pulse in the X 2 Σ + (ν = 0, N = 1) state of BaF and SrF molecules, respectively, a state amenable to Stark deceleration and 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 [NL-eEDM Collaboration, Eur. Phys. J. D 72, 197 (2018)]. Knowledge of the molecular properties of BaF is thus needed to plan the measurements and, in particular, to determine the optimal laser-cooling scheme. Accurate and reliable theoretical predictions of these properties require the incorporation of both high-order correlation and relativistic effects in the calculations. In this work, theoretical investigations of the ground and lowest excited states of BaF and its lighter homologs, CaF and SrF, are carried out in the framework of the relativistic Fock-space coupled cluster and multireference configuration interaction methods. Using the calculated molecular properties, we determine the Franck-Condon factors (FCFs) for the A 2 Π 1/2 →X 2 Σ 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 2 Σ 1/2 + →X 2 Σ 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 nondiagonal nature of the FCFs in this system. Special attention is given to the properties of the A' 2 Δ 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 excited states of the three molecules and the transition dipole moments (TDMs) between the different states. Finally, using the calculated FCFs and TDMs, we determine that the A 2 Π 1/2 →X 2 Σ 1/2 + transition is suitable for transverse cooling in BaF.

The ionization energy of ortho-H_{2} has been determined to be E_{I}^{o}(H_{2})/(hc)=124 357.238 062(25)  cm^{-1} from measurements of the GK(1,1)-X(0,1) interval by Doppler-free, two-photon spectroscopy using a narrow band 179-nm laser source and the ionization energy of the GK(1,1) state by continuous-wave, near-infrared laser spectroscopy. E_{I}^{o}(H_{2}) was used to derive the dissociation energy of H_{2}, D_{0}^{N=1}(H_{2}), at 35 999.582 894(25)  cm^{-1} with a precision that is more than one order of magnitude better than all previous results. The new result challenges calculations of this quantity and represents a benchmark value for future relativistic and QED calculations of molecular energies.

We study collisions between neutral, deuterated ammonia molecules (ND_{3}) stored in a 50 cm diameter synchrotron and argon atoms in copropagating 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 ND_{3}+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.

We have recently demonstrated a general and sensitive method to study low energy collisions that exploits the unique properties of a molecular synchrotron (Van der Poel et al., Phys Rev Lett 120:033402, 2018). In that work, the total cross section for ND3 + Ar collisions was determined from the rate at which ammonia molecules were lost from the synchrotron due to collisions with argon atoms in supersonic beams. This paper provides further details on the experiment. In particular, we derive the model that was used to extract the relative cross section from the loss rate, and present measurements to characterize the spatial and velocity distributions of the stored ammonia molecules and the supersonic argon beams., Competing Interests: The authors declare that they have no competing interests.Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

The resolution of any spectroscopic or interferometric experiment is ultimately limited by the total time a particle is interrogated. Here we 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  μK and a longitudinal temperature of <1  μK) 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 ms, making it possible, in principle, to perform sub-Hz measurements in molecular systems and paving the way for stringent tests of fundamental physics theories.

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 × 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× 10(9) years and to ∣Δμ∕μ∣ < 10(-7) for look-back times of 7× 10(9) years. The last result, obtained from high-redshift observation of methanol, translates into μ̇/μ=(1.4±1.4)×10(-17)/yr if a linear rate of change is assumed.

A limit on a possible cosmological variation of the proton-to-electron mass ratio μ is derived from methanol (CH3OH) 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 CH3OH covering a wide range of sensitivity coefficients K(μ) are used to derive a purely statistical 1σ constraint of Δμ/μ=(1.5±1.5)×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 multidimensional linear regression analysis leads to a robust constraint of Δμ/μ=(-1.0±0.8(stat)±1.0(sys))×10(-7).

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 (HV) 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 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.

The standard model of physics is built on the fundamental constants of nature, but it does not provide an explanation for their values, nor require their constancy over space and time. Here we set a limit on a possible cosmological variation of the proton-to-electron mass ratio μ by comparing transitions in methanol observed in the early universe with those measured in the laboratory. From radio-astronomical observations of PKS1830-211, we deduced a constraint of Δμ/μ = (0.0 ± 1.0) × 10(-7) at redshift z = 0.89, corresponding to a look-back time of 7 billion years. This is consistent with a null result.

Velocity map imaging inside an electrostatic quadrupole guide is demonstrated. By switching the voltages that are applied to the rods, the quadrupole can be used for guiding Stark decelerated molecules and for extracting the ions. The extraction field is homogeneous along the axis of the quadrupole, while it defocuses the ions in the direction perpendicular to both the axis of the quadrupole and the axis of the ion optics. To compensate for this astigmatism, a series of planar electrodes with horizontal and vertical slits is used. A velocity resolution of 35 m s(-1) is obtained. It is shown that signal due to thermal background can be eliminated, resulting in the detection of slow molecules with an increased signal-to-noise ratio. As an illustration of the resolving power we have used the velocity map imaging system to characterize the phase-space distribution of a Stark decelerated ammonia beam.

In this paper, we analyze electric deflection fields for polar molecules in terms of a multipole expansion and derive a simple but rather insightful expression for the force on the molecules. Ideally, a deflection field exerts a strong, constant force in one direction, while the force in the other directions is zero. We show how, by a proper choice of the expansion coefficients, this ideal can be best approximated. We present a design for a practical electrode geometry based on this analysis. By bending such a deflection field into a circle, a simple storage ring can be created; the direct analog of a weak-focusing cyclotron for charged particles. We show that for realistic parameters a weak-focusing ring is only stable for molecules with a very low velocity. A strong-focusing (alternating-gradient) storage ring can be created by arranging many straight deflection fields in a circle and by alternating the sign of the hexapole term between adjacent deflection fields. The acceptance of this ring is numerically calculated for realistic parameters. Such a storage ring might prove useful in experiments looking for an EDM of elementary particles.

The 6.7 and 12.2 GHz masers, corresponding to the 5(1) → 6(0)A+ and 2(0) → 3(-1)E transitions in methanol (CH3OH), respectively, are among the brightest radio objects in the sky. We present calculations for the sensitivity of these and other transitions in the ground state of methanol to a variation of the proton-to-electron mass ratio. We show that the sensitivity is greatly enhanced due to a cancellation of energies associated with the hindered internal rotation and the overall rotation of the molecule. We find sensitivities of K(μ) = -42 and K(μ) = -33, for the 5(1) → 6(0)A+ and 2(0) → 3(-1)E transitions, respectively. The sensitivities of other transitions in the different isotopologues of methanol range from -88 to 330. This makes methanol a sensitive probe for spatial and temporal variations of the proton-to-electron mass ratio.

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.

The recently demonstrated methods to cool and manipulate neutral molecules offer new possibilities for precision tests of fundamental physics theories. We here discuss the possibility of testing the time-invariance of fundamental constants using near degeneracies between rotational levels in the fine structure ladders of molecular radicals. We show that such a degeneracy occurs between the J = 6, Q2 1 and the J = 8, Q = 0 levels of the various natural isotopomers of carbon monoxide in its a 3pi state. As a result, the 2-photon transition that connects these states is 300 times more sensitive to a variation of m(p)/m(e) than a pure rotational transition. We present a molecular beam apparatus that might be used to measure these transitions with a fractional accuracy of 10(-12). Ultimately, the precision of an experiment on metastable CO will be limited by the lifetime of the a 3pi state. We will discuss other possible molecules that have a suitable level structure and can be cooled using one of the existing methods.

A microstructured array of over 1200 electrodes on a substrate has been configured to generate an array of local minima of electric field strength with a periodicity of 120 microm about 25 microm 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. This is experimentally demonstrated by transporting metastable CO molecules in 30 mK deep wells that move at constant velocities above the substrate.

A linear AC trap for polar molecules in high-field seeking states has been devised and implemented, and its characteristics have been investigated both experimentally and theoretically. The trap is loaded with slow 15ND3 molecules in their ground state (para-ammonia) from a Stark decelerator. The trap's geometry offers optimal access as well as improved loading. We present measurements of the dependence of the trap's performance on the switching frequency, which exhibit a characteristic structure due to nonlinear resonance effects. The molecules are found to oscillate in the trap under the influence of the trapping forces, which were analyzed using 3D numerical simulations. On the basis of expansion measurements, molecules with a velocity and a position spread of 2.1 m/s and 0.4 mm, respectively, are still accepted by the trap. This corresponds to a temperature of 2.0 mK. From numerical simulations, we find the phase-space volume that can be confined by the trap (the acceptance) to be 50 mm3 (m/s)3.

The merging of molecular beam methods with those of accelerator physics has yielded new tools to manipulate the motion of molecules. Over the last few years, decelerators, lenses, bunchers, traps, and storage rings for neutral molecules have been demonstrated. Molecular beams with a tunable velocity and with a tunable width of the velocity distribution can now be produced, and are expected to become a valuable tool in a variety of physical chemistry and chemical physics experiments. Here we present a compact molecular beam machine, capable of producing 3D spatially focused packets of state-selected accelerated or decelerated molecules.

We here report on the realization of an electrodynamic trap, capable of trapping neutral atoms and molecules in both low-field and high-field seeking states. Confinement in three dimensions is achieved by switching between two electric field configurations that have a saddle point at the center of the trap, i.e., by alternating a focusing and a defocusing force in each direction. The ac trapping of 15ND(3) molecules is experimentally demonstrated, and the stability of the trap is studied as a function of the switching frequency. A 1 mK sample of 15ND(3) molecules in the high-field seeking component of the |J,K=|1,1 level, the ground state of para-ammonia, is trapped in a volume of about 1 mm(3).

By miniaturizing electrode geometries high electric fields can be produced using modest voltages. A planar array of 20 microm wide gold electrodes, spaced 20 microm apart, is made on a sapphire substrate. A voltage difference of up to 350 V is applied to adjacent electrodes, generating an electric field that decreases exponentially with distance from the substrate. This microstructured array can be used as a mirror for polar molecules and can be rapidly switched on and off. This is demonstrated by retro-reflecting a beam of state-selected ammonia molecules with a forward velocity of about 30 m/s.

We have decelerated a supersonic beam of 174YbF molecules using a switched sequence of electrostatic field gradients. These molecules are 7 times heavier than any previously decelerated. An alternating gradient structure allows us to decelerate and focus the molecules in their ground state. We show that the decelerator exhibits the axial and transverse stability required to bring the molecules to rest. Our work significantly extends the range of molecules amenable to this powerful method of cooling and trapping.

A neutral polar molecule experiences a force in an inhomogeneous electric field. This electric field can be designed such that a beam of polar molecules is exposed to a harmonic potential in the forward direction. In this potential the longitudinal phase-space distribution of the ensemble of molecules is rotated uniformly. This property is used to longitudinally focus a pulsed beam of ammonia molecules and to produce a beam with a longitudinal velocity spread of 0.76 m/s, corresponding to a temperature of 250 mu K.

Neutral dipolar molecules can be decelerated and trapped using time-varying inhomogeneous electric fields. This has been demonstrated only for molecules in low-field seeking states, but can, in principle, be performed on molecules in high-field seeking states as well. Transverse stability is then much more difficult to obtain, however, since molecules in high-field seeking states always experience a force towards the electrodes. Here we demonstrate that an array of dipole lenses in alternate gradient configuration can be used to maintain transverse stability. A pulsed beam of metastable CO in high-field seeking states is accelerated from 275 to 289 m/s as well as decelerated from 275 to 260 m/s.

The ability to cool and manipulate atoms with light has yielded atom interferometry, precision spectroscopy, Bose-Einstein condensates and atom lasers. The extension of controlled manipulation to molecules is expected to be similarly rewarding, but molecules are not as amenable to manipulation by light owing to a far more complex energy-level spectrum. However, time-varying electric and magnetic fields have been successfully used to control the position and velocity of ions, suggesting that these schemes can also be used to manipulate neutral particles having an electric or magnetic dipole moment. Although the forces exerted on neutral species are many orders of magnitude smaller than those exerted on ions, beams of neutral dipolar molecules have been successfully slowed down in a series of pulsed electric fields and subsequently loaded into an electrostatic trap. Here we extend the scheme to include a prototype electrostatic storage ring made of a hexapole torus with a circumference of 80 cm. After injection, decelerated bunches of deuterated ammonia molecules, each containing about 106 molecules in a single quantum state and with a translational temperature of 10 mK, travel up to six times around the ring. Stochastic cooling might provide a means to increase the phase-space density of the stored molecules in the storage ring, and we expect this to open up new opportunities for molecular spectroscopy and studies of cold molecular collisions.

Orientational effects in rotationally elastic collisions of OH with Ar were studied in a crossed molecular beam setup. A static electric field was applied to orient the molecules before the collision. After the collision the orientation was measured by using a narrow-band laser system to probe the Stark-split states corresponding to different orientations. Differential and integral cross sections for reorientation of the molecular axis have been determined as a function of the initial orientation. The cross section for reorientation by one quantum is 25 A2 with a preference for O-end collisions.

The ability to cool and slow atoms with light for subsequent trapping allows investigations of the properties and interactions of the trapped atoms in unprecedented detail. By contrast, the complex structure of molecules prohibits this type of manipulation, but magnetic trapping of calcium hydride molecules thermalized in ultra-cold buffer gas and optical trapping of caesium dimers generated from ultra-cold caesium atoms have been reported. However, these methods depend on the target molecules being paramagnetic or able to form through the association of atoms amenable to laser cooling, respectively, thus restricting the range of species that can be studied. Here we describe the slowing of an adiabatically cooled beam of deuterated ammonia molecules by time-varying inhomogeneous electric fields and subsequent loading into an electrostatic trap. We are able to trap state-selected ammonia molecules with a density of 10(6) cm(-3) in a volume of 0.25 cm3 at temperatures below 0.35 K. We observe pronounced density oscillations caused by the rapid switching of the electric fields during loading of the trap. Our findings illustrate that polar molecules can be efficiently cooled and trapped, thus providing an opportunity to study collisions and collective quantum effects in a wide range of ultra-cold molecular systems.

A series of pulsed electric fields can be arranged such that it creates a traveling potential well in which neutral dipolar molecules can be confined. This provides a method to transport, to decelerate, and to cool a sample of neutral molecules while maintaining the initial phase-space density. This method is described using the concept of phase stability. The oscillating motion of molecules in the traveling potential well, reaching a minimum velocity spread corresponding to a translational temperature of 4 mK, is experimentally observed.