Permanent electric dipole moments (EDMs) are signatures of time-reversal and parity violation and act as sensitive probes for physics beyond the Standard Model (BSM). The work in this thesis has been done as part of the NL-eEDM collaboration, which plans to measure the electron EDM using a beam of BaF molecules. The sensitivity of such a table-top precision experiment benefits from utilizing an intense, slow beam of molecules. We plan to achieve that through a combination of Stark deceleration and transverse laser cooling of a cryogenic beam of BaF. The work presented in this thesis has primarily been done to produce intense, slow molecular beams for an electron EDM measurement. We constructed a supersonic beam source of SrF and BaF molecules. The source produces high intensity beams with low translational and rotational temperatures. Time-resolved detection of laser-induced fluorescence from pulsed excitation of electronic states in BaF molecules was performed to determine the lifetimes of the A^{2}Pi_{1/2} and A^{2}Pi_{3/2} states. The lifetimes of these states were determined to be 57.1(3) ns and 47.9(7) ns, respectively. The transition between the A^{2}Pi_{1/2} and X^{2}Sigma^{+} states is the main laser cooling transition in BaF. We decelerated a beam of SrF molecules from a cryogenic source to a standstill inside a traveling-wave Stark decelerator, with the number of decelerated molecules on the order of 1000. BaF molecules will be decelerated with the same technique to perform an electron EDM measurement.
Permanent electric dipole moments (EDMs) are signatures of time-reversal and parity violation and act as sensitive probes for physics beyond the Standard Model (BSM). The work in this thesis has been done as part of the NL-eEDM collaboration, which plans to measure the electron EDM using a beam of BaF molecules. The sensitivity of such a table-top precision experiment benefits from utilizing an intense, slow beam of molecules. We plan to achieve that through a combination of Stark deceleration and transverse laser cooling of a cryogenic beam of BaF. The work presented in this thesis has primarily been done to produce intense, slow molecular beams for an electron EDM measurement. We constructed a supersonic beam source of SrF and BaF molecules. The source produces high intensity beams with low translational and rotational temperatures. Time-resolved detection of laser-induced fluorescence from pulsed excitation of electronic states in BaF molecules was performed to determine the lifetimes of the A^{2}Pi_{1/2} and A^{2}Pi_{3/2} states. The lifetimes of these states were determined to be 57.1(3) ns and 47.9(7) ns, respectively. The transition between the A^{2}Pi_{1/2} and X^{2}Sigma^{+} states is the main laser cooling transition in BaF. We decelerated a beam of SrF molecules from a cryogenic source to a standstill inside a traveling-wave Stark decelerator, with the number of decelerated molecules on the order of 1000. BaF molecules will be decelerated with the same technique to perform an electron EDM measurement.
To meet some demands for realizing precise measurements of an electric dipole moment of electron (eEDM) and examining cold collisions or cold chemical physics, we have proposed a novel, versatile electrostatic Stark decelerator with an array of true 3D electric potential wells, which are created by a series of horizontally-oriented, U-shaped electrodes with time-sequence controlling high voltages (± HV) and two guiding electrodes with a constant voltage. We have calculated the 2D electric field distribution, the Stark shifts of the four lowest rotational sub-levels of PbF molecules in the X1(2)Π1/2(v = 0) electronic and vibrational ground states as well as the population in the different rotational levels. We have discussed the 2D longitudinal and transverse phase-space acceptances of PbF molecules in our decelerator. Subsequently, we have simulated the dynamic processes of the decelerated PbF molecules using the 3D Monte-Carlo method, and have found that a supersonic PbF beam with a velocity of 300 m s(-1) can be efficiently slowed to about 5 m s(-1), which will greatly enhance the sensitivities to research a parity violation and measure an eEDM. In addition, we have investigated the dependences of the longitudinal velocity spread, longitudinal temperature and bunching efficiency on both the number of guiding stages and high voltages, and found that after bunching, a cold packet of PbF molecules in the J = 7/2, MΩ = -7/4 state with a longitudinal velocity spread of 0.69 m s(-1) (corresponding to a longitudinal temperature of 2.35 mK) will be produced by our high-efficient decelerator, which will generate a high energy-resolution molecular beam for studying cold collision physics. Finally, our novel decelerator can also be used to efficiently slow NO molecules with a tiny electric dipole moment (EDM) of 0.16 D from 315 m s(-1) to 28 m s(-1). It is clear that our proposed new decelerator has a good slowing performance and experimental feasibility as well as wide applications in the field of precise measurements and cold molecule physics.
That the universe contains a disproportionate amount of matter compared to antimatter cannot be explained by the standard model of particle physics; this is because it contains too little charge-parity (CP) symmetry violation. Low energy experiments with atoms and molecules can be extremely sensitive probes for many types of new physics. An active area of research is the search for electric dipole moments (EDMs) of fundamental particles or nuclei; a nonzero EDM would be evidence for new sources of CP violation. Ytterbium monofluoride (YbF) molecules in a supersonic beam are currently being used to measure the electric dipole moment of the electron (eEDM). This thesis presents progress towards a new, more sensitive eEDM experiment that will use a slower YbF beam source and transverse laser cooling to collimate this beam. We have demonstrated laser cooling of YbF in one transverse dimension to less than 100 μK, which is below the Doppler cooling limit. This was done using a Sisyphus-type mechanism called magnetic field induced laser cooling. We also demonstrate polarisation gradient cooling of YbF. After rebuilding and upgrading much of the experiment, we cooled the beam in both transverse dimensions. By scanning experimental parameters, we have gained insight into the cooling mechanisms, and the optimum conditions for laser cooling. We placed an upper limit of a few mK on the transverse temperature of the molecules, although I argue that the true temperature must be very much lower. The number of ultracold molecules was carefully quantified and found to be 2.0(4)x10^5 per pulse. These experiments lay the foundations for an eEDM sensitivity improvement by up to a factor of 100.
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.
Bright beams of cold molecules provide valuable quantum sensors for measuring permanent electric dipole moments that violate fundamental symmetries, which enables these tabletop experiments to probe energy scales exceeding those available with current or near-future particle colliders. The precision of such experiments generally scales with the number of molecules that are detected per unit time, typically a few meters downstream of the place where the molecular beam is created. So, improving the precision -and thereby probing new physics at higher and higher energy scales- requires increasing the downstream flux of molecules. This can be achieved by collimating the molecular beam to maintain a high number density. These molecular experiments can borrow techniques for control and manipulation from the extremely well-developed field of atomic physics. One such technique is laser cooling, which is a powerful method to achieve this boost in brightness, whose implementation however remains challenging due to the complex energy level structure of molecules. In this work, we demonstrate and analyze laser cooling of a focused cryogenic beam of BaF molecules. We conclude that with some follow-up steps this method will increase the beam brightness by a factor 100, a crucial milestone towards a high precision measurement of the electron electric dipole moment (eEDM).
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.
Physicists have observed all the elementary particles predicted by the Standard Model. These particles, however, account for only 5% of the total mass-energy of the Universe. In the quest to solve the mystery of missing matter and to extend our knowledge about nature, a large number of experimental research programs are devoted to find a glimpse of New Physics. Table-top high precision measurements on molecules can contribute to these efforts in a manner complementary to high-energy experiments at colliders. In this thesis, we describe the operation of a traveling-wave Stark decelerator. This device is designed and constructed in order to slow down heavy polar molecules for various future explorations. Deceleration is achieved by manipulation of the molecules in controllable electric fields. We demonstrate in an experiment the successful operation of the Stark decelerator by slowing down a beam of SrF molecules to one-third of their initial velocity, thus removing almost 90% of the initial kinetic energy. We also reveal limiting conditions for this process. These results are of importance for many exciting experiments using heavy molecules in the near future. One relevant and promising example of such experiments is the search for a permanent electric dipole moment of the electron.