Cryogenic buffer gas cells have been a workhorse for the cooling of molecules in the last few decades. The straightforward sympathetic cooling principle makes them applicable to a huge variety of different species. Notwithstanding this success, detailed simulations of buffer gas cells are rare, and have never been compared to experimental data in the regime of low to intermediate buffer gas densities. Here, we present a numerical approach based on a trajectory analysis, with molecules performing a random walk in the cell due to collisions with a homogeneous buffer gas. This method can reproduce experimental flux and velocity distributions of molecules emerging from the buffer gas cell for varying buffer gas densities. This includes the strong decrease in molecule output from the cell for increasing buffer gas density and the so-called boosting effect, when molecules are accelerated by buffer-gas atoms after leaving the cell. The simulations provide various insights which could substantially improve buffer-gas cell design.
Cryogenic buffer gas cells have been a workhorse for the cooling of molecules in the last few decades. The straightforward sympathetic cooling principle makes them applicable to a huge variety of different species. Notwithstanding this success, detailed simulations of buffer gas cells are rare, and have never been compared to experimental data in the regime of low to intermediate buffer gas densities. Here, we present a numerical approach based on a trajectory analysis, with molecules performing a random walk in the cell due to collisions with a homogeneous buffer gas. This method can reproduce experimental flux and velocity distributions of molecules emerging from the buffer gas cell for varying buffer gas densities. This includes the strong decrease in molecule output from the cell for increasing buffer gas density and the so-called boosting effect, when molecules are accelerated by buffer-gas atoms after leaving the cell. The simulations provide various insights which could substantially improve buffer-gas cell design.
Abstract Cryogenic buffer gas cells have been a workhorse for the cooling of molecules in the last few decades. The straightforward sympathetic cooling principle makes them applicable to a huge variety of different species. Notwithstanding this success, detailed simulations of buffer gas cells are rare, and have never been compared to experimental data in the regime of low to intermediate buffer gas densities. Here, we present a numerical approach based on a trajectory analysis, with molecules performing a random walk in the cell due to collisions with a homogeneous buffer gas. This method can reproduce experimental flux and velocity distributions of molecules emerging from the buffer gas cell for varying buffer gas densities. This includes the strong decrease in molecule output from the cell for increasing buffer gas density and the so-called boosting effect, when molecules are accelerated by buffer-gas atoms after leaving the cell. The simulations provide various insights which could substantially improve buffer-gas cell design.
Abstract Cryogenic buffer gas beam(CBGB) sources have become an essential tool for experiments requiring cold molecular beams with low forward velocities. Although recent experimental advances have led to significant progress in source optimization, numerical studies remain limited due to the challenges posed by the large parameter ranges required to describe both the dense buffer gas and the dilute seed molecules. In this work, we report a numerical evaluation of CBGB cells operating in the hydrodynamic extraction regime. While most prior studies focused on box-like or cylindrical cells, we investigated hydrodynamic effects including vortex formation in a dome-shaped cell and assessed whether these could be utilized to enhance the performance in molecule cooling and extraction. To achieve this, we performed steady-state slip-flow simulations for helium buffer gas and employed a direct-simulation Monte Carlo diffusion routine to track particle trajectories. We compared the performance of the source across different buffer gas throughputs and injection angles and identified parameter regimes where vortex formation enhances molecule extraction. From the simulations, we extracted experimental observables, which allow these effects to be verified through velocity or time-of-flight measurements on the molecular beam.
The cryogenic buffer gas beam (CBGB) is an important tool in the study of cold and ultracold molecules.While there are known techniques to enhance desired beam properties of a CBGB, such as high flux, low velocity, or reduced divergence, they have generally not undergone detailed numerical optimization.Numerical simulation of buffer gas beams is challenging, because the relevant dynamics occur in regions where the density varies by orders of magnitude, rendering typical numerical methods unreliable or intractable.Here we simulate CBGBs with a hybrid approach that combines gas dynamics methods with particle tracing.The simulations capture important properties, such as velocitiy and divergence, across an assortment of designs, including two-stage slowing cells and de Laval nozzles.This approach should therefore be a useful tool for optimizing CBGB designs across a wide range of applications.
A comprehensive characterisation of cold molecular beams from a cryogenic buffer-gas cell, providing insight into the physics of buffer-gas cooling, is presented. Cold molecular beams are extracted from a cryogenic cell by electrostatic guiding, which is also used to measure their velocity distribution. The rotational-state distribution of the molecules is probed by radio-frequency resonant depletion spectroscopy. With the help of complete trajectory simulations, yielding the guiding efficiency for all of the thermally populated states, it is possible to determine both the rotational and the translational temperature of the molecules at the output of the buffer-gas cell. This thermometry method is demonstrated for various regimes of buffer-gas cooling and beam formation as well as for molecular species of different sizes (CH3 F and CF3 CCH). Comparison of the rotational and translational temperatures provides evidence of faster rotational thermalisation for the CH3 F/He system in the limit of low He density. In addition, the relaxation rates for different rotational states appear to be different.
Cold gases of atoms and molecules provide a system for the exploration of a diverse set of physical phenomena. For example, cold gasses of magnetically and electrically polar atoms and molecules are ideal systems for quantum simulation and quantum computation experiments, and cold gasses of large polar molecules allow for novel spectroscopic techniques. Buffer-gas cooling is a robust and widely applicable method for cooling atoms and molecules to temperatures of approximately 1 Kelvin. In this thesis, I present novel applications of buffer-gas cooling to obtaining gases of trapped, ultracold atoms and diatomic molecules, as well as the study of the cooling of large organic molecules. In the first experiment of this thesis, a buffer-gas beam source of atoms is used to directly load a magneto-optical trap. Due to the versatility of the buffer-gas beam source, we obtain trapped, sub-milliKelvin gases of four different lanthanide species using the same experimental apparatus. In the second experiment of this thesis, a buffer-gas beam is used as the initial stage of an experiment to directly laser cool and magneto-optically trap the diatomic molecule CaF. In the third experiment of this thesis, buffer-gas cooling is used to study the cooling of the conformational state of large organic molecules. We directly observe conformational relaxation of gas-phase 1,2-propanediol due to cold collisions with helium gas. Lastly, I present preliminary results on a variety of novel applications of buffer-gas cooling, such as mixture analysis, separation of chiral mixtures, the measurement of parity-violation in chiral molecules, and the cooling and spectroscopy of highly unstable reaction intermediates.
We characterize a continuous buffer gas cooled source using CO molecules. We show results about the source performance considering different parameters, like gas flow rate, nozzle size, and internal cell volume. The beam contains 2.5 × 10 14 molecules/(s sr) at about 160 m/s. Moreover, for two rotational states we observe an unexpected population distribution that we tentatively attribute to a lower temperature inside the cell. Considering the importance of buffer-gas cooling for experiments on ultracold molecules prepared with direct laser cooling, we believe that our work will improve this key first-stage cooling, accelerating the adoption of molecules in the framework of quantum technologies.