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Construction and Operation of a Cryogenic Source for Cold Polar Molecules

Christian Sommer

Published Jan 1, 2011• 0 citations
OpenAlex

Abstract

This thesis reports on the combination of buffer-gas cooling with electric velocity filtering to produce a high-density guided beam of slow and internally cold polar molecules. In the continuous source, warm molecules are first cooled by collisions with a cryogenic helium buffer gas. Cold molecules are then extracted by means of an electric quadrupole guide. For formaldehyde the population of individual rotational states in the guide is monitored by depletion spectroscopy, resulting in single-state populations up to 82 %. This thesis also reports on a technique to produce pulses of slow guided molecules. The pulses exhibit a narrow velocity distribution around a tunable velocity.

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Electrostatic Extraction of Cold Molecules from a Cryogenic Reservoir

L. D. van Buuren, Christian Sommer, M. Motsch +5 more

We present a method which delivers a continuous, high-density beam of slow and internally cold polar molecules. In our source, warm molecules are first cooled by collisions with a cryogenic helium buffer gas. Cold molecules are then extracted by means of an electrostatic quadrupole guide. For ${\mathrm{ND}}_{3}$ the source produces fluxes up to $(7{\ifmmode\pm\else\textpm\fi{}}_{4}^{7})\ifmmode\times\else\texttimes\fi{}{10}^{10}\text{ }\text{ }\mathrm{\text{molecules}}/\mathrm{s}$ with peak densities up to $(1.0{\ifmmode\pm\else\textpm\fi{}}_{0.6}^{1.0})\ifmmode\times\else\texttimes\fi{}{10}^{9}\text{ }\text{ }\mathrm{\text{molecules}}/{\mathrm{cm}}^{3}$. For ${\mathrm{H}}_{2}\mathrm{CO}$ the population of rovibrational states is monitored by depletion spectroscopy, resulting in single-state populations up to $(82\ifmmode\pm\else\textpm\fi{}10)%$.

arXiv:0806.2523•Physical Review Letters•Jan 21, 2009•93 citations

Continuous guided beams of slow and internally cold polar molecules

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We describe the combination of buffer-gas cooling with electrostatic velocity filtering to produce a high-flux continuous guided beam of internally cold and slow polar molecules. In a previous paper (L.D. van Buuren et al., Phys. Rev. Lett., 2009, 102, 033001) we presented results on density and state purity for guided beams of ammonia and formaldehyde using an optimized set-up. Here we describe in more detail the technical aspects of the cryogenic source, its operation, and the optimization experiments that we performed to obtain the best performance. The versatility of the source is demonstrated by the production of guided beams of different molecular species.

arXiv:0812.1923•Faraday Discussions•Jan 1, 2009•44 citations

Cold guided beams of polar molecules

M. Motsch

Slow molecules are efficiently extracted from a thermal reservoir by exploiting the interaction between polar molecules and the field provided by an electrostatic quadrupole guide. Electrostatic velocity filtering is widely applicable, which is demonstrated by producing guided beams of ammonia ND3, formaldehyde H2CO, and the water isotopologs H2O, D2O, and HDO. Ultraviolet depletion spectroscopy in a cold guided beam of formaldehyde makes the population in individual rotational states visible and testifies their key role in velocity filtering. Enhanced Rayleigh scattering into an optical cavity is investigated as an alternative non-destructive detection method for cold molecules. For various room-temperature gases, the observed enhancement is well described by interference of electromagnetic fields scattered into the resonator by a classical driven dipole oscillator.

•Jan 1, 2010•1 citation

Slow, cold beams of polar molecules for precision measurements

N. E. Bulleid

This thesis reports on the use of buffer gas cooling to produce slow and intense molecular beams, with the aim of creating a source of molecules that can be used to measure the electron electric dipole moment. A beam of Yb is extracted from a buffer gas cell by entrainment in a flow of helium. The beam is characterised and simulations are performed of the helium flow through the cell to better understand the effect this has on the beam characteristics. The velocity of the beam is found to vary between 65 m/s[superscript -1] and 204 m/s[superscript -1] depending on the helium flow through the cell, in agreement with the predictions of the simulations. The temperature of the beam is 2.4 K and the minimum divergence is 12°. The percentage of Yb that is extracted from the cell is ~10%. Sources which use a pulsed valve to produce a supersonic jet are also characterised at cryogenic temperatures. The addition of a thermalisation cell is found to produce beams that are slower, colder and more intense. The peak beam intensity is 4.5×10[superscript 10] molecules per seradian per pulse, the velocity (206 ± 5) m/s and the translational temperature is (12.3 ± 0.5) K. An electric decelerator is used to decelerate a pulse of YbF molecules from 300 m/s[superscript -1] to 276 m/s[superscript -1] by confining them to a travelling trap. Simulations of the molecules in the decelerator show that its acceptance is greater than those demonstrated previously. A detailed understanding of this deceleration is developed. The Franck-Condon factors for the A[superscript 2]Π[subscript 1/2] (v = 0) − X[superscript 2]Σ[superscript +] (v - 0, 1, 2) transition of YbF are measured. The results show that, using three lasers, the molecule could be laser-cooled.

•Aug 1, 2013•2 citations

Buffer gas cooling of YbF molecules

Sarah M. Skoff

This thesis reports on the production and characterisation of the first slow and cold beam of YbF molecules using buffer gas cooling. These molecules are being used to measure the electron’s electric dipole moment, and an intense source of slow-moving molecules is desirable for this experiment. The molecules are loaded into a buffer gas cell via laser ablation where they thermalise with cold helium buffer gas. They are then detected inside the cell using laser absorption imaging and spectroscopy on the X2Σ+→A2II1/2 transition. The formation, diffusion and thermalisation dynamics of the molecules inside the cell are studied. Measurements of laser absorption versus intensity reveal that saturation of the absorption is due to a competition between optical pumping into dark states and repopulation of the addressed level by inelastic and velocity-changing collisions. A beam of YbF molecules is extracted through an aperture in the buffer gas cell and characterised using laser induced fluorescence detection. Peak fluxes of 1010 molecules per steradian per pulse, in the rotational and vibrational ground state, are obtained. The translational and rotational temperatures are in equilibrium with the cell temperature of 4 K. The forward velocity of the pulses can be varied between 130 m/s and 200 m/s by changing the buffer gas pressure. This source is an order of magnitude brighter and more than three times slower than a supersonic source of YbF molecules and provides an excellent starting point for improving the measurement of the electron’s electric dipole moment and for deceleration and trapping experiments. In order to reduce the helium load on the vacuum system and to shorten the molecular pulses, a second set-up, delivering the buffer gas into an open copper cylinder in pulses rather than in a continuous flow,is characterised and shows promising first results.

•Sep 1, 2011•2 citations

Thermometry of Guided Molecular Beams from a Cryogenic Buffer-Gas Cell

Wu, X., Gantner, T., Zeppenfeld, M. +2 more

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.

•Jan 1, 2016•11 citations
This thesis reports on the combination of buffer-gas cooling with electric velocity filtering to produce a high-density guided beam of slow and internally cold polar molecules. In the continuous source, warm molecules are first cooled by collisions with a cryogenic helium buffer gas. Cold molecules are then extracted by means of an electric quadrupole guide. For formaldehyde the population of individual rotational states in the guide is monitored by depletion spectroscopy, resulting in single-state populations up to 82 %. This thesis also reports on a technique to produce pulses of slow guided molecules. The pulses exhibit a narrow velocity distribution around a tunable velocity.
We present a method which delivers a continuous, high-density beam of slow and internally cold polar molecules. In our source, warm molecules are first cooled by collisions with a cryogenic helium buffer gas. Cold molecules are then extracted by means of an electrostatic quadrupole guide. For ND3{\mathrm{ND}}_{3}ND3​ the source produces fluxes up to $(7{\ifmmode\pm\else\textpm\fi{}}_{4}^{7})\ifmmode\times\else\texttimes\fi{}{10}^{10}\text{ }\text{ }\mathrm{\text{molecules}}/\mathrm{s}$ with peak densities up to $(1.0{\ifmmode\pm\else\textpm\fi{}}_{0.6}^{1.0})\ifmmode\times\else\texttimes\fi{}{10}^{9}\text{ }\text{ }\mathrm{\text{molecules}}/{\mathrm{cm}}^{3}$. For H2CO{\mathrm{H}}_{2}\mathrm{CO}H2​CO the population of rovibrational states is monitored by depletion spectroscopy, resulting in single-state populations up to $(82\ifmmode\pm\else\textpm\fi{}10)%$.
We describe the combination of buffer-gas cooling with electrostatic velocity filtering to produce a high-flux continuous guided beam of internally cold and slow polar molecules. In a previous paper (L.D. van Buuren et al., Phys. Rev. Lett., 2009, 102, 033001) we presented results on density and state purity for guided beams of ammonia and formaldehyde using an optimized set-up. Here we describe in more detail the technical aspects of the cryogenic source, its operation, and the optimization experiments that we performed to obtain the best performance. The versatility of the source is demonstrated by the production of guided beams of different molecular species.
Slow molecules are efficiently extracted from a thermal reservoir by exploiting the interaction between polar molecules and the field provided by an electrostatic quadrupole guide. Electrostatic velocity filtering is widely applicable, which is demonstrated by producing guided beams of ammonia ND3, formaldehyde H2CO, and the water isotopologs H2O, D2O, and HDO. Ultraviolet depletion spectroscopy in a cold guided beam of formaldehyde makes the population in individual rotational states visible and testifies their key role in velocity filtering. Enhanced Rayleigh scattering into an optical cavity is investigated as an alternative non-destructive detection method for cold molecules. For various room-temperature gases, the observed enhancement is well described by interference of electromagnetic fields scattered into the resonator by a classical driven dipole oscillator.
This thesis reports on the use of buffer gas cooling to produce slow and intense molecular beams, with the aim of creating a source of molecules that can be used to measure the electron electric dipole moment. A beam of Yb is extracted from a buffer gas cell by entrainment in a flow of helium. The beam is characterised and simulations are performed of the helium flow through the cell to better understand the effect this has on the beam characteristics. The velocity of the beam is found to vary between 65 m/s[superscript -1] and 204 m/s[superscript -1] depending on the helium flow through the cell, in agreement with the predictions of the simulations. The temperature of the beam is 2.4 K and the minimum divergence is 12°. The percentage of Yb that is extracted from the cell is ~10%. Sources which use a pulsed valve to produce a supersonic jet are also characterised at cryogenic temperatures. The addition of a thermalisation cell is found to produce beams that are slower, colder and more intense. The peak beam intensity is 4.5×10[superscript 10] molecules per seradian per pulse, the velocity (206 ± 5) m/s and the translational temperature is (12.3 ± 0.5) K. An electric decelerator is used to decelerate a pulse of YbF molecules from 300 m/s[superscript -1] to 276 m/s[superscript -1] by confining them to a travelling trap. Simulations of the molecules in the decelerator show that its acceptance is greater than those demonstrated previously. A detailed understanding of this deceleration is developed. The Franck-Condon factors for the A[superscript 2]Π[subscript 1/2] (v = 0) − X[superscript 2]Σ[superscript +] (v - 0, 1, 2) transition of YbF are measured. The results show that, using three lasers, the molecule could be laser-cooled.
This thesis reports on the production and characterisation of the first slow and cold beam of YbF molecules using buffer gas cooling. These molecules are being used to measure the electron’s electric dipole moment, and an intense source of slow-moving molecules is desirable for this experiment. The molecules are loaded into a buffer gas cell via laser ablation where they thermalise with cold helium buffer gas. They are then detected inside the cell using laser absorption imaging and spectroscopy on the X2Σ+→A2II1/2 transition. The formation, diffusion and thermalisation dynamics of the molecules inside the cell are studied. Measurements of laser absorption versus intensity reveal that saturation of the absorption is due to a competition between optical pumping into dark states and repopulation of the addressed level by inelastic and velocity-changing collisions. A beam of YbF molecules is extracted through an aperture in the buffer gas cell and characterised using laser induced fluorescence detection. Peak fluxes of 1010 molecules per steradian per pulse, in the rotational and vibrational ground state, are obtained. The translational and rotational temperatures are in equilibrium with the cell temperature of 4 K. The forward velocity of the pulses can be varied between 130 m/s and 200 m/s by changing the buffer gas pressure. This source is an order of magnitude brighter and more than three times slower than a supersonic source of YbF molecules and provides an excellent starting point for improving the measurement of the electron’s electric dipole moment and for deceleration and trapping experiments. In order to reduce the helium load on the vacuum system and to shorten the molecular pulses, a second set-up, delivering the buffer gas into an open copper cylinder in pulses rather than in a continuous flow,is characterised and shows promising first results.
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.