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We present an atom interferometer using large momentum transfer without $k$-reversal. More specifically, we use a microwave $\pi$/2 pulse to manipulate the spin state of $^{87}$Rb atoms before applying a Raman light $\pi$ pulse to achieve 4$\hbar k$ momentum transfer per Raman light pulse. A microwave $\pi$ pulse in the middle of the interferometer sequence reverses the spin states, which allows closing of the interferometer arms by the same Raman light $\pi$ pulses without $k$-reversal. We discuss the scalability of this large momentum transfer technique. Our results extend the scope of using large momentum transfer atom optics into atom interferometers where $k$-reversal optics are not available., Comment: 6 pages, 3 figures

Using a mid-infrared quantum cascade laser and wavelength modulation absorption spectroscopy, we measure the frequencies of ro-vibrational transitions of N$_2$O in the 17 $\mu$m region with uncertainties below 5 MHz. These lines, corresponding to the bending mode of the molecule, can be used for calibration of spectrometers in this spectral region. We present a model for the lineshapes of absorption features in wavelength modulation spectroscopy that takes into account Doppler broadening, collisional broadening, saturation of the absorption, and lineshape distortion due to frequency and intensity modulation. Combining our data with previous measurements, we provide a set of spectroscopic parameters for several vibrational states of N$_2$O. The lines measured here fall in the same spectral region as a mid-infrared frequency reference that we are currently developing using trapped, ultracold molecules. With such a frequency reference, the spectroscopic methods demonstrated here have the potential to improve frequency calibration in this part of the spectrum.

We study the properties of a cryogenic buffer gas source that uses a low temperature two-stage buffer gas cell to produce very slow beams of ytterbium monofluoride molecules. The molecules are produced by laser ablation inside the cell and extracted into a beam by a flow of cold helium. We measure the flux and velocity distribution of the beam as a function of ablation energy, helium flow rate, cell temperature, and the size of the gap between the first and second stages of the cell. We also compare the velocity distributions from one-stage and two-stage cells. The one-stage cell emits a beam with a speed of about 82 m s$^{-1}$ and a translational temperature of 0.63 K. The slowest beams are obtained using the two-stage cell at the lowest achievable cell temperature of 1.8 K. This beam has a peak velocity of 56 m s$^{-1}$ and a flux of $9 \times 10^9$ ground state molecules per steradian per pulse, with a substantial fraction at speeds below 40 m s$^{-1}$. These slow molecules can be decelerated further by radiation pressure slowing and then captured in a magneto-optical trap., Comment: 11 pages, 8 figures; Extra figure added and some improvements to the text throughout

We describe one of the largest radio-frequency RF atomic magnetometers presently operating. A total atomic volume of 128 $\mathrm{cm^3}$, with correspondingly large number of $^{87}$Rb atoms, can reduce atom noise. A total of 44 passes of the probe beam reduces photon-shot noise. The atomic vapor is divided between two chambers allowing for pumping of the cells individually; doing so with opposite-helicity light enables use as an intrinsic gradiometer. In this configuration, common-mode noise sources including light-shift noise can be reduced. Magnetic tuning fields can also be applied to the chambers individually, allowing simultaneous measurement of two frequencies. An application of this is in the search for contraband materials using Nuclear Quadrupole Resonance (NQR), for which simultaneous measurement can significantly reduce search times. We demonstrate dual-frequency measurement on an effective range of 423-531 kHz, corresponding to the NQR frequencies of ammonium nitrate NH$_4$NO$_3$ at the lowest value and potassium chlorate KClO$_3$ at the highest. We explore fundamental, as well as instrumental, noise contributions to the sensitivity in this system., Comment: 15 pages, 9 figures

The electron's electric dipole moment (eEDM) can be determined by polarizing the spin of an atom or a molecule and then measuring the spin precession frequency in an applied electric field. Radiation is used to polarize the spin and then analyze the precession angle, and the measurement is often sensitive to the polarization of this radiation. We show how systematic errors can arise when both the polarization of the radiation and the magnitude of the electric field are imperfectly controlled. We derive approximate analytical expressions for these errors, confirm their accuracy numerically, and show how they can be corrected empirically. We consider spin manipulation using single-photon pulses, Raman pulses, and Stimulated Raman Adiabatic Passage (STIRAP), and show that STIRAP provides better immunity to these systematic errors. An experimental study of these errors partly supports our findings but also reveals another potential error that is not captured by this analysis., Comment: 9 pages, 10 figures. Added new section presenting an experimental study of the effects described in the paper

This paper outlines the centralised design and production of the Ultra-High-Vacuum sidearm and Laser-Stabilisation systems for the AION Ultra-Cold Strontium Laboratories. Commissioning data on the residual gas and steady-state pressures in the sidearm chambers, on magnetic field quality, on laser stabilisation, and on the loading rate for the 3D Magneto-Optical Trap are presented. Streamlining the design and production of the sidearm and laser stabilisation systems enabled the AION Collaboration to build and equip in parallel five state-of-the-art Ultra-Cold Strontium Laboratories within 24 months by leveraging key expertise in the collaboration. This approach could serve as a model for the development and construction of other cold atom experiments, such as atomic clock experiments and neutral atom quantum computing systems, by establishing dedicated design and production units at national laboratories., Comment: 27 pages, 21 figures

We show, theoretically and experimentally, how the absolute orientation and polarization state of radio-frequency (RF) magnetic fields in a transverse 2D plane can be uniquely determined using two optically pumped atomic magnetometers. In addition, the output signals from these quantum sensors can be readily expressed as a magnetic Jones vector. This composite device can complement electric field detection in finding RF directions, or it can be used in applications where the electric field is negligible. The latter is found in a myriad of applications where the source can be modeled as radiating magnetic dipoles in the near-field limit. This new tool could be used to characterize a material's response to RF excitation or to distinguish signal from noise., Comment: 20 pages, 8 figures, submitted to Physical Review Applied

Theories that extend the Standard Model of particle physics often introduce new interactions that violate charge-parity (CP) symmetry. CP-violating effects within an atomic nucleus can be probed by measuring its nuclear magnetic quadrupole moment (MQM). The sensitivity of such a measurement is enhanced when using a heavy polar molecule containing a nucleus with quadrupole deformation. We determine how the energy levels of a molecule are shifted by the MQM and how those shifts can be measured. The measurement scheme requires molecules in a superposition of magnetic sub-levels that differ by many units of angular momentum. We develop a generic scheme for preparing these states. Finally, we consider the sensitivity that can be reached, showing that this method can reduce the current uncertainties on several CP-violating parameters., Comment: 13 pages, 7 figures. Section II has been re-organised and some details moved to an appendix. A few extra references have been added

The detection of variations of fundamental constants of the Standard Model would provide us with compelling evidence of new physics, and could lift the veil on the nature of dark matter and dark energy. In this work, we discuss how a network of atomic and molecular clocks can be used to look for such variations with unprecedented sensitivity over a wide range of time scales. This is precisely the goal of the recently launched QSNET project: A network of clocks for measuring the stability of fundamental constants. QSNET will include state-of-the-art atomic clocks, but will also develop next-generation molecular and highly charged ion clocks with enhanced sensitivity to variations of fundamental constants. We describe the technological and scientific aims of QSNET and evaluate its expected performance. We show that in the range of parameters probed by QSNET, either we will discover new physics, or we will impose new constraints on violations of fundamental symmetries and a range of theories beyond the Standard Model, including dark matter and dark energy models.

The QSNET consortium is building a UK network of next-generation atomic and molecular clocks that will achieve unprecedented sensitivity in testing variations of the fine structure constant, $\alpha$, and the electron-to-proton mass ratio, $\mu$. This in turn will provide more stringent constraints on a wide range of fundamental and phenomenological theories beyond the Standard Model and on dark matter models.

We study inelastic collisions between CaF molecules and $^{87}$Rb atoms in a dual-species magneto-optical trap. The presence of atoms increases the loss rate of molecules from the trap. By measuring the loss rates and density distributions, we determine a collisional loss rate coefficient $k_{2} = (1.43 \pm 0.29) \times 10^{-10}$ cm$^{3}$/s at a temperature of 2.4 mK. We show that this is not substantially changed by light-induced collisions or by varying the populations of excited-state atoms and molecules. The observed loss rate is close to the universal rate expected in the presence of fast loss at short range, and can be explained by rotation-changing collisions in the ground electronic state., Comment: 14 pages, 6 figures. Added a new figure and some further details about the methods; expanded our discussion of the results

We use two-dimensional transverse laser cooling to produce an ultracold beam of YbF molecules. Through experiments and numerical simulations, we study how the cooling is influenced by the polarization configuration, laser intensity, laser detuning and applied magnetic field. The ultracold part of the beam contains more than $2 \times 10^5$ molecules per shot and has a temperature below 200 $\mu$K, and the cooling yields a 300-fold increase in the brightness of the beam. The method can improve the precision of experiments that use molecules to test fundamental physics. In particular, the beam is suitable for measuring the electron electric dipole moment with a statistical precision better than $10^{-30}$ e cm., Comment: 25 pages, 14 figures. Trajectory simulations added and results compared to experiment; other minor revisions

We prepare mixtures of ultracold CaF molecules and Rb atoms in a magnetic trap and study their inelastic collisions. When the atoms are prepared in the spin-stretched state and the molecules in the spin-stretched component of the first rotationally excited state, they collide inelastically with a rate coefficient of $k_2 = (6.6 \pm 1.5) \times 10^{-11}$ cm$^{3}$/s at temperatures near 100~$\mu$K. We attribute this to rotation-changing collisions. When the molecules are in the ground rotational state we see no inelastic loss and set an upper bound on the spin relaxation rate coefficient of $k_2 < 5.8 \times 10^{-12}$ cm$^{3}$/s with 95% confidence. We compare these measurements to the results of a single-channel loss model based on quantum defect theory. The comparison suggests a short-range loss parameter close to unity for rotationally excited molecules, but below 0.04 for molecules in the rotational ground state., Comment: 9 pages, 6 figures. Minor changes following review

Measurements of the electron's electric dipole moment (eEDM) are demanding tests of physics beyond the Standard Model. We describe how ultracold YbF molecules could be used to improve the precision of eEDM measurements by two to three orders of magnitude. Using numerical simulations, we show how the combination of magnetic focussing, two-dimensional transverse laser cooling, and frequency-chirped laser slowing, can produce an intense, slow, highly-collimated molecular beam. We show how to make a magneto-optical trap of YbF molecules and how the molecules could be loaded into an optical lattice. eEDM measurements could be made using the slow molecular beam or using molecules trapped in the lattice. We estimate the statistical sensitivity that could be reached in each case and consider how sources of noise can be reduced so that the shot-noise limit of sensitivity can be reached. We also consider systematic effects due to magnetic fields and vector light shifts and how they could be controlled.

The electric dipole moment of the electron (eEDM) can be measured with high precision using heavy polar molecules. In this paper, we report on a series of new techniques that have improved the statistical sensitivity of the YbF eEDM experiment. We increase the number of molecules participating in the experiment by an order of magnitude using a carefully designed optical pumping scheme. We also increase the detection efficiency of these molecules by another order of magnitude using an optical cycling scheme. In addition, we show how to destabilise dark states and reduce backgrounds that otherwise limit the efficiency of these techniques. Together, these improvements allow us to demonstrate a statistical sensitivity of $1.8 \times 10^{-28}$ e cm after one day of measurement, which is 1.2 times the shot-noise limit. The techniques presented here are applicable to other high-precision measurements using molecules., Comment: 22 pages, 11 figures

We present a brief review of our progress towards measuring parity violation in heavy-metal chiral complexes using mid-infrared Ramsey interferometry. We discuss our progress addressing the main challenges, including the development of buffer-gas sources of slow, cold polyatomic molecules, and the frequency-stabilisation of quantum cascade lasers calibrated using primary frequency standards. We report investigations on achiral test species of which promising chiral derivatives have been synthesized.

We outline the experimental concept and key scientific capabilities of AION (Atom Interferometer Observatory and Network), a proposed UK-based experimental programme using cold strontium atoms to search for ultra-light dark matter, to explore gravitational waves in the mid-frequency range between the peak sensitivities of the LISA and LIGO/Virgo/ KAGRA/INDIGO/Einstein Telescope/Cosmic Explorer experiments, and to probe other frontiers in fundamental physics. AION would complement other planned searches for dark matter, as well as probe mergers involving intermediate mass black holes and explore early universe cosmology. AION would share many technical features with the MAGIS experimental programme in the US, and synergies would flow from operating AION in a network with this experiment, as well as with other atom interferometer experiments such as MIGA, ZAIGA and ELGAR. Operating AION in a network with other gravitational wave detectors such as LIGO, Virgo and LISA would also offer many synergies., Comment: v3: Update to match published version in JCAP

Polar molecules in superpositions of rotational states exhibit long-range dipolar interactions, but maintaining their coherence in a trapped sample is a challenge. We present calculations that show many laser-coolable molecules have convenient rotational transitions that are exceptionally insensitive to magnetic fields. We verify this experimentally for CaF where we find a transition with sensitivity below 5 Hz G$^{-1}$ and use it to demonstrate a rotational coherence time of 6.4(8) ms in a magnetic trap. Simulations suggest it is feasible to extend this to more than 1 s using a smaller cloud in a biased magnetic trap.

We propose in this White Paper a concept for a space experiment using cold atoms to search for ultra-light dark matter, and to detect gravitational waves in the frequency range between the most sensitive ranges of LISA and the terrestrial LIGO/Virgo/KAGRA/INDIGO experiments. This interdisciplinary experiment, called Atomic Experiment for Dark Matter and Gravity Exploration (AEDGE), will also complement other planned searches for dark matter, and exploit synergies with other gravitational wave detectors. We give examples of the extended range of sensitivity to ultra-light dark matter offered by AEDGE, and how its gravitational-wave measurements could explore the assembly of super-massive black holes, first-order phase transitions in the early universe and cosmic strings. AEDGE will be based upon technologies now being developed for terrestrial experiments using cold atoms, and will benefit from the space experience obtained with, e.g., LISA and cold atom experiments in microgravity. This paper is based on a submission (v1) in response to the Call for White Papers for the Voyage 2050 long-term plan in the ESA Science Programme. ESA limited the number of White Paper authors to 30. However, in this version (v2) we have welcomed as supporting authors participants in the Workshop on Atomic Experiments for Dark Matter and Gravity Exploration held at CERN: ({\tt https://indico.cern.ch/event/830432/}), as well as other interested scientists, and have incorporated additional material., Comment: V2 -- added support authors

We introduce a scheme for deep laser cooling of molecules based on robust dark states at zero velocity. By simulating this scheme, we show it to be a widely applicable method that can reach the recoil limit or below. We demonstrate and characterise the method experimentally, reaching a temperature of 5.4(7) $\mu$K. We solve a general problem of measuring low temperatures for large clouds by rotating the phase-space distribution and then directly imaging the complete velocity distribution. Using the same phase-space rotation method, we rapidly compress the cloud. Applying the cooling method a second time, we compress both the position and velocity distributions., Comment: 9 pages, 7 figures

We study several new magneto-optical trapping configurations in $^{87}$Rb. These unconventional MOTs all use type-II transitions, where the angular momentum of the ground state is greater than or equal to that of the excited state, and they may use either red-detuned or blue-detuned light. We describe the conditions under which each new MOT forms. The various MOTs exhibit an enormous range of lifetimes, temperatures and density distributions. At the detunings where they are maximized, the lifetimes of the various MOTs vary from 0.1 to 15 s. One MOT forms large ring-like structures with no density at the centre. The temperature in the red-detuned MOTs can be three orders of magnitude higher than in the blue-detuned MOTs. We present measurements of the capture velocity of a blue-detuned MOT, and we study how the loss rate due to ultracold collisions depends on laser intensity and detuning., Comment: 8 pages, 7 figures

We explore the uses of ultracold molecules as a platform for future experiments in the field of quantum simulation, focusing on two molecular species, $^{40}$Ca$^{19}$F and $^{87}$Rb$^{133}$Cs. We report the development of coherent quantum state control using microwave fields in both molecular species; this is a crucial ingredient for many quantum simulation applications. We demonstrate proof-of-principle Ramsey interferometry measurements with fringe spacings of $\sim 1~\rm kHz$ and investigate the dephasing time of a superposition of $N=0$ and $N=1$ rotational states when the molecules are confined. For both molecules, we show that a judicious choice of molecular hyperfine states minimises the impact of spatially varying transition-frequency shifts across the trap. For magnetically trapped $^{40}$Ca$^{19}$F we use a magnetically insensitive transition and observe a coherence time of 0.61(3) ms. For optically trapped $^{87}$Rb$^{133}$Cs we exploit an avoided crossing in the AC Stark shift and observe a maximum coherence time of 0.75(6) ms., Comment: Accepted for publication in Quantum Science and Technology

We present the properties and advantages of a new magneto-optical trap (MOT) where blue-detuned light drives `type-II' transitions that have dark ground states. Using $^{87}$Rb, we reach a radiation-pressure-limited density exceeding $10^{11}$cm$^{-3}$ and a temperature below 30$\mu$K. The phase-space density is higher than in normal atomic MOTs, and a million times higher than comparable red-detuned type-II MOTs, making it particularly attractive for molecular MOTs which rely on type-II transitions. The loss of atoms from the trap is dominated by ultracold collisions between Rb atoms. For typical trapping conditions, we measure a loss rate of $1.8(4)\times10^{-10}$cm$^{3}$s$^{-1}$.

We demonstrate one-dimensional sub-Doppler laser cooling of a beam of YbF molecules to 100 $\mu$K. This is a key step towards a measurement of the electron's electric dipole moment using ultracold molecules. We compare the effectiveness of magnetically-assisted and polarization-gradient sub-Doppler cooling mechanisms. We model the experiment and find good agreement with our data.

We demonstrate coherent microwave control of the rotational, hyperfine and Zeeman states of ultracold CaF molecules, and the magnetic trapping of these molecules in a single, selectable quantum state. We trap about $5\times 10^{3}$ molecules for 2 s at a temperature of 65(11) $\mu$K and a density of $1.2 \times 10^{5}$ cm$^{-3}$. We measure the state-specific loss rate due to collisions with background helium., Comment: 6 pages, 4 figures

Experiments with cold molecules usually begin with a molecular source. We describe the construction and characteristics of a cryogenic buffer gas source of CaF molecules. The source emits pulses with a typical duration of 240 $\mu$s, a mean speed of about 150 m/s, and a flux of $5\times 10^{10}$ molecules per steradian per pulse in a single rotational state., Comment: 13 pages, 5 figures

We present the properties of a magneto-optical trap (MOT) of CaF molecules. We study the process of loading the MOT from a decelerated buffer-gas-cooled beam, and how best to slow this molecular beam in order to capture the most molecules. We determine how the number of molecules, the photon scattering rate, the oscillation frequency, damping constant, temperature, cloud size and lifetime depend on the key parameters of the MOT, especially the intensity and detuning of the main cooling laser. We compare our results to analytical and numerical models, to the properties of standard atomic MOTs, and to MOTs of SrF molecules. We load up to $2 \times 10^4$ molecules, and measure a maximum scattering rate of $2.5 \times 10^6$ s$^{-1}$ per molecule, a maximum oscillation frequency of 100 Hz, a maximum damping constant of 500 s$^{-1}$, and a minimum MOT rms radius of 1.5 mm. A minimum temperature of 730 $\mu$K is obtained by ramping down the laser intensity to low values. The lifetime, typically about 100 ms, is consistent with a leak out of the cooling cycle with a branching ratio of about $6 \times 10^{-6}$. The MOT has a capture velocity of about 11 m/s., Comment: 27 pages, 16 figures

The ability to cool atoms below the Doppler limit -- the minimum temperature reachable by Doppler cooling -- has been essential to most experiments with quantum degenerate gases, optical lattices and atomic fountains, among many other applications. A broad set of new applications await ultracold molecules, and the extension of laser cooling to molecules has begun. A molecular magneto-optical trap has been demonstrated, where molecules approached the Doppler limit. However, the sub-Doppler temperatures required for most applications have not yet been reached. Here we cool molecules to 50 uK, well below the Doppler limit, using a three-dimensional optical molasses. These ultracold molecules could be loaded into optical tweezers to trap arbitrary arrays for quantum simulation, launched into a molecular fountain for testing fundamental physics, and used to study ultracold collisions and ultracold chemistry., Comment: 8 pages, 6 figures

We describe a parallel pair of high voltage electric field plates designed and constructed to minimise magnetic Johnson noise. They are formed by laminating glass substrates with commercially available polyimide (Kapton) tape, covered with a thin gold film. Tested in vacuum, the outgassing rate is less than $5\times10^{-5}$ mbar.l/s. The plates have been operated at electric fields up to 8.3 kV/cm, when the leakage current is at most a few hundred pA. The design is discussed in the context of a molecular spin precession experiment to measure the permanent electric dipole moment of the electron., Comment: 9 pages, 3 figures

Using frequency-chirped radiation pressure slowing, we precisely control the velocity of a pulsed CaF molecular beam down to a few m/s, compressing its velocity spread by a factor of 10 while retaining high intensity: at a velocity of 15~m/s the flux, measured 1.3~m from the source, is 7$\times$10$^{5}$ molecules per cm$^{2}$ per shot in a single rovibrational state. The beam is suitable for loading a magneto-optical trap or, when combined with transverse laser cooling, improving the precision of spectroscopic measurements that test fundamental physics. We compare the frequency-chirped slowing method with the more commonly used frequency-broadened slowing method., Comment: 19 pages, 8 figures. Extension of earlier version to include detailed comparison of slowing methods

We optically excite the electronic state $3s3p~^3P_{0}$ in $^{24}$Mg atoms, laser-cooled and trapped in a magic-wavelength lattice. An applied magnetic field enhances the coupling of the light to the otherwise strictly forbidden transition. We determine the magic wavelength, the quadratic magnetic Zeeman shift and the transition frequency to be 468.463(207)$\,$nm, -206.6(2.0)$\,$MHz/T$^2$ and 655 058 646 691(101)$\,$kHz, respectively. These are compared with theoretical predictions and results from complementary experiments. We also developed a high-precision relativistic structure model for magnesium, give an improved theoretical value for the blackbody radiation shift and discuss a clock based on bosonic magnesium., Comment: 5 pages, 3 figures

We characterize a Fabry-Perot microwave cavity designed for trapping atoms and molecules at the antinode of a microwave field. The cavity is fed from a waveguide through a small coupling hole. Focussing on the compact resonant modes of the cavity, we measure how the electric field profile, the cavity quality factor, and the coupling efficiency, depend on the radius of the coupling hole. We measure how the quality factor depends on the temperature of the mirrors in the range from 77 to 293K. The presence of the coupling hole slightly changes the profile of the mode, leading to increased diffraction losses around the edges of the mirrors and a small reduction in quality factor. We find the hole size that maximizes the intra-cavity electric field. We develop an analytical theory of the aperture-coupled cavity that agrees well with our measurements, with small deviations due to enhanced diffraction losses. We find excellent agreement between our measurements and finite-difference time-domain simulations of the cavity., Comment: 16 pages, 8 figures

The simple structure of the BH molecule makes it an excellent candidate for direct laser cooling. We measure the branching ratios for the decay of the ${\rm A}^{1}\Pi (v'=0)$ state to vibrational levels of the ground state, ${\rm X}^{1}\Sigma^{+}$, and find that they are exceedingly favourable for laser cooling. We verify that the branching ratio for the spin-forbidden transition to the intermediate ${\rm a}^{3}\Pi$ state is inconsequentially small. We measure the frequency of the lowest rotational transition of the X state, and the hyperfine structure in the relevant levels of both the X and A states, and determine the nuclear electric quadrupole and magnetic dipole coupling constants. Our results show that, with a relatively simple laser cooling scheme, a Zeeman slower and magneto-optical trap can be used to cool, slow and trap BH molecules., Comment: 7 pages, 5 figures. Updated analysis of A state hyperfine structure and other minor revisions

We demonstrate slowing and longitudinal cooling of a supersonic beam of CaF molecules using counter-propagating laser light resonant with a closed rotational and almost closed vibrational transition. A group of molecules are decelerated by about 20 m/s by applying light of a fixed frequency for 1.8 ms. Their velocity spread is reduced, corresponding to a final temperature of about 300 mK. The velocity is further reduced by chirping the frequency of the light to keep it in resonance as the molecules slow down., Comment: 6 pages, 6 figures

We present a combined experimental and theoretical study of beam formation from a cryogenic buffer gas cell. Atoms and molecules are loaded into the cell by laser ablation of a target, and are cooled and swept out of the cell by a flow of cold helium. We study the thermalization and flow dynamics inside the cell and measure how the speed, temperature, divergence and extraction efficiency of the beam are influenced by the helium flow. We use a finite element model to simulate the flow dynamics and use the predictions of this model to interpret our experimental results., Comment: 10 pages, 14 figures

We propose an experiment to measure the electric dipole moment of the electron using ultracold YbF molecules. The molecules are produced as a thermal beam by a cryogenic buffer gas source, and brought to rest in an optical molasses that cools them to the Doppler limit or below. The molecular cloud is then thrown upward to form a fountain in which the electric dipole moment of the electron is measured., Comment: 18 pages, 8 figures, 53 references

We recently reported a new measurement of the electron's electric dipole moment using YbF molecules [Nature 473, 493 (2011)]. Here, we give a more detailed description of the methods used to make this measurement, along with a fuller analysis of the data. We show how our methods isolate the electric dipole moment from imperfections in the experiment that might mimic it. We describe the systematic errors that we discovered, and the small corrections that we made to account for these. By making a set of additional measurements with greatly exaggerated experimental imperfections, we find upper bounds on possible uncorrected systematic errors which we use to determine the systematic uncertainty in the measurement. We also calculate the size of some systematic effects that have been important in previous electric dipole moment measurements, such as the motional magnetic field effect and the geometric phase, and show them to be negligibly small in the present experiment. Our result is consistent with an electric dipole moment of zero, so we provide upper bounds to its size at various confidence levels. Finally, we review the prospects for future improvements in the precision of the experiment., Comment: 35 pages, 15 figures

Under negative feedback, the quality factor Q of a radio-frequency magnetometer can be decreased by more than two orders of magnitude, so that any initial perturbation of the polarized spin system can be rapidly damped, preparing the magnetometer for detection of the desired signal. We find that noise is also suppressed under such spin-damping, with a characteristic spectral response corresponding to the type of noise; therefore magnetic, photon-shot, and spin-projection noise can be measured distinctly. While the suppression of resonant photon-shot noise implies the closed-loop production of polarization-squeezed light, the suppression of resonant spin-projection noise does not imply spin-squeezing, rather simply the broadening of the noise spectrum with Q. Furthermore, the application of spin-damping during phase-sensitive detection suppresses both signal and noise in such a way as to increase the sensitivity bandwidth. We demonstrate a three-fold increase in the magnetometer's bandwidth while maintaining 0.3 fT/\surdHz sensitivity., Comment: 24 pages, 7 figures

The fluorescence spectrum resulting from laser excitation of the A^{2}\Pi_{1/2} - X^{2}\Sigma^{+} (0,0) band of ytterbium monofluoride, YbF, has been recorded and analyzed to determine the Franck-Condon factors. The measured values are compared with those predicted from Rydberg-Klein-Rees (RKR) potential energy curves. From the fluorescence decay curve the radiative lifetime of the A^{2}\Pi_{1/2} state is measured to be 28\pm2 ns, and the corresponding transition dipole moment is 4.39\pm0.16 D. The implications for laser cooling YbF are discussed., Comment: 5 pages, 5 figures

We report the Stark deceleration of CaF molecules in the strong-field seeking ground state and in a weak-field seeking component of a rotationally-excited state. We use two types of decelerator, a conventional Stark decelerator for the weak-field seekers, and an alternating gradient decelerator for the strong-field seekers, and we compare their relative merits. We also consider the application of laser cooling to increase the phase-space density of decelerated molecules., Comment: 10 pages, 8 figures

We discuss an experiment underway at Imperial College London to measure the permanent electric dipole moment (EDM) of the electron using a molecular beam of YbF. We describe the measurement method, which uses a combination of laser and radiofrequency resonance techniques to detect the spin precession of the YbF molecule in a strong electric field. We pay particular attention to the analysis scheme and explore some of the possible systematic effects which might mimic the EDM signal. Finally, we describe technical improvements which should increase the sensitivity by more than an order of magnitude over the current experimental limit., Comment: 6 pages, 2 figures

We produce YbF molecules with a density of 10^18 m^-3 using laser ablation inside a cryogenically-cooled cell filled with a helium buffer gas. Using absorption imaging and absorption spectroscopy we study the formation, diffusion, thermalization and optical pumping of the molecules. The absorption images show an initial rapid expansion of molecules away from the ablation target followed by a much slower diffusion to the cell walls. We study how the time constant for diffusion depends on the helium density and temperature, and obtain values for the YbF-He diffusion cross-section at two different temperatures. We measure the translational and rotational temperatures of the molecules as a function of time since formation, obtain the characteristic time constant for the molecules to thermalize with the cell walls, and elucidate the process responsible for limiting this thermalization rate. Finally, we make a detailed study of how the absorption of the probe laser saturates as its intensity increases, showing that the saturation intensity is proportional to the helium density. We use this to estimate collision rates and the density of molecules in the cell., Comment: 20 pages, 11 figures, minor revisions following referee suggestions

We demonstrate Doppler-free saturated absorption spectroscopy of cold molecular radicals formed by laser ablation inside a cryogenic buffer gas cell. By lowering the temperature, congested regions of the spectrum can be simplified, and by using different temperatures for different regions of the spectrum a wide range of rotational states can be studied optimally. We use the technique to study the optical spectrum of YbF radicals with a resolution of 30 MHz, measuring the magnetic hyperfine parameters of the electronic ground state. The method is suitable for high resolution spectroscopy of a great variety of molecules at controlled temperature and pressure, and is particularly well-suited to those that are difficult to produce in the gas phase., Comment: 11 pages, 4 figures

An alternating gradient electric guide provides a way to transport a wide variety of polar molecules, including those in high-field seeking states. We investigate the motion of polar molecules in such a guide by measuring the transmission of CaF molecules in their high-field seeking ground state, with the guide operating at a variety of switching frequencies and voltages. We model the guide using analytical and numerical techniques and compare the predictions of these models to the experimental results and to one another. The analytical results are approximate, but provide simple and useful estimates for the maximum phase-space acceptance of the guide and for the switching frequency required. The numerical methods provide more accurate results over the full range of switching frequencies. Our investigation shows that, even when the fields are static, some high-field seeking molecules are able to pass through the guide on metastable trajectories. We show that the maximum possible transmission requires accurate alignment within the guide and between the guide and detector., Comment: 10 pages, 5 figures; revised following referee suggestions

We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the spectral cut position to the asymptotic transition frequency of the rubidium D1 or D2 lines, respectively. Measurements of the molecular photoassociation signal as a function of the pulse energy reveal a non-linear dependence and indicate a non-perturbative excitation process. Chirping the association laser pulse allowed us to change the phase of the coherent transients. Furthermore, a signature for molecules in the electronic ground state is found, which is attributed to molecule formation by femtosecond photoassociation followed by spontaneous decay. In a subsequent article [A. Merli et al., submitted] quantum mechanical calculations are presented, which compare well with the experimental data and reveal further details about the observed coherent transient dynamics.

Heavy polar molecules can be used to measure the electric dipole moment of the electron, which is a sensitive probe of physics beyond the Standard Model. The value is determined by measuring the precession of the molecule's spin in a plane perpendicular to an applied electric field. The longer this precession evolves coherently, the higher the precision of the measurement. For molecules in a trap, this coherence time could be very long indeed. We evaluate the sensitivity of an experiment where neutral molecules are trapped electrically, and compare this to an equivalent measurement in a molecular beam. We consider the use of a Stark decelerator to load the trap from a supersonic source, and calculate the deceleration efficiency for YbF molecules in both strong-field seeking and weak-field seeking states. With a 1s holding time in the trap, the statistical sensitivity could be ten times higher than it is in the beam experiment, and this could improve by a further factor of five if the trap can be loaded from a source of larger emittance. We study some effects due to field inhomogeneity in the trap and find that rotation of the electric field direction, leading to an inhomogeneous geometric phase shift, is the primary obstacle to a sensitive trap-based measurement., Comment: 22 pages, 7 figures, prepared for Faraday Discussion 142

We describe a method for determining the radiative decay properties of a molecule by studying the saturation of laser-induced fluorescence and the associated power broadening of spectral lines. The fluorescence saturates because the molecules decay to states that are not resonant with the laser. The amplitudes and widths of two hyperfine components of a spectral line are measured over a range of laser intensities and the results compared to a model of the laser-molecule interaction. Using this method we measure the lifetime of the A(v'=0) state of CaF to be tau=19.2 \pm 0.7 ns, and the Franck-Condon factor for the transition to the X(v=0) state to be Z=0.987 (+0.013 || -0.019). In addition, our analysis provides a measure of the hyperfine interval in the lowest-lying state of A(v'=0), Delta_e=4.8 \pm 1.1 MHz., Comment: 10 pages, 6 figures. Minor revisions following referee suggestions

This paper is a chapter from an upcoming book on cold molecule physics. In it we describe techniques for the preparation and manipulation of cold molecules. We further describe techniques for applying said cold molecules to tests of fundamental physics., Comment: 22 pages, 18 figures

We describe a technique for mapping the spatial variation of static electric, static magnetic, and rf magnetic fields using a pulsed atomic or molecular beam. The method is demonstrated using a beam designed to measure the electric dipole moment of the electron. We present maps of the interaction region, showing sensitivity to (i) electric field variation of 1.5 V/cm at 3.3 kV/cm with a spatial resolution of 15 mm; (ii) magnetic field variation of 5 nT with 25 mm resolution; (iii) radio-frequency magnetic field amplitude with 15 mm resolution. This new diagnostic technique is very powerful in the context of high-precision atomic and molecular physics experiments, where pulsed beams have not hitherto found widespread application., Comment: 6 pages, 12 figures. Figures heavily compressed to comply with arxiv's antediluvian file-size policy

We have developed a source of cold LiH molecules for Stark deceleration and trapping experiments. Lithium metal is ablated from a solid target into a supersonically expanding carrier gas. The translational, rotational and vibrational temperatures are 0.9(0.1) K, 5.9(0.5) K and 468(17) K respectively. Although they have not reached thermal equilibrium with the carrier gas, we estimate that 90% of the LiH molecules are in the ground state, X^{1} \Sigma^{+} (v=0, J=0). With a single 7 ns ablation pulse, the number of molecules in the ground state is 4.5(1.8)*10^{7} molecules per steradian. A second, delayed, ablation pulse produces another LiH beam in a different part of the same gas pulse, thereby almost doubling the signal. A long pulse, lasting 150 microseconds, can make the beam up to 15 times more intense., Comment: 8 pages, 6 figures