The production of dense samples of atoms whose translational velocity can be parameterized\nby temperatures in the microkelvin range has revolutionized the fields of spectroscopy,\nmetrology, quantum computing and sensitive tests of quantum mechanics.\nSuch ultracold temperatures may be reached by Doppler cooling which uses a velocitysensitive\nscattering force. This technique relies upon atoms which have closed electronic\ntransitions between two states so that the atoms may continuously absorb photon momenta\nand do not spontaneous decay into a dark state. Very few atoms fulfil this condition\nand attempts to cool molecules are inhibited by their extra degrees of freedom,\nvia rotation and vibration, which add manifolds of extra states.\n\nThis thesis describes the early experimental stages of investigation into coherent laseratom\ninteractions which may be used as a general all-optical method to impart momentum\nto atoms and molecules and thus manipulate their velocity. The thesis covers the\nconstruction and operation of stable diode lasers, a magneto-optical trap to produce cold\nsamples of the test species Rubidium and a high-power, phase and intensity, controllable\nlaser to induce Raman transitions. Studies into the spectroscopy of Rubidium and the\nnature of coherent Raman interactions in multilevel atoms is also covered. Experimental\nresults shows that coherent Raman transitions between the 5S1/2 ground states has been\nachieved in the form of sinc-squared lineshapes and Rabi-flopping.
The production of dense samples of atoms whose translational velocity can be parameterized\nby temperatures in the microkelvin range has revolutionized the fields of spectroscopy,\nmetrology, quantum computing and sensitive tests of quantum mechanics.\nSuch ultracold temperatures may be reached by Doppler cooling which uses a velocitysensitive\nscattering force. This technique relies upon atoms which have closed electronic\ntransitions between two states so that the atoms may continuously absorb photon momenta\nand do not spontaneous decay into a dark state. Very few atoms fulfil this condition\nand attempts to cool molecules are inhibited by their extra degrees of freedom,\nvia rotation and vibration, which add manifolds of extra states.\n\nThis thesis describes the early experimental stages of investigation into coherent laseratom\ninteractions which may be used as a general all-optical method to impart momentum\nto atoms and molecules and thus manipulate their velocity. The thesis covers the\nconstruction and operation of stable diode lasers, a magneto-optical trap to produce cold\nsamples of the test species Rubidium and a high-power, phase and intensity, controllable\nlaser to induce Raman transitions. Studies into the spectroscopy of Rubidium and the\nnature of coherent Raman interactions in multilevel atoms is also covered. Experimental\nresults shows that coherent Raman transitions between the 5S1/2 ground states has been\nachieved in the form of sinc-squared lineshapes and Rabi-flopping.
Cold atom samples, at temperatures of the order 100 uK, are useful for a wide reaching array of new and exciting technological and scientific endeavours. Atoms are conventionally cooled by Doppler cooling, which relies on the continuous absorption and reemission of photons in a closed optical cycle. This requirement is diffcult to achieve when there are many allowed decay paths for the excited atom, making Doppler cooling only feasible for a handful atoms with simple energy level structures. More exotic energy level structures, such as those found in molecules, are notoriously diffcult to cool. Coherent cooling schemes in comparison, offer advantages such as insensitivity to frequency detuning or a higher number of photon momenta which can be imparted for each spontaneous emission event making them promising candidates for the optical cooling of particles with more general energy level structures. In order to demonstrate these schemes, we have explored the coherent manipulation of an atomic cloud of Rubidium cooled using a two photon Raman resonance. Despite the long spontaneous decay times of such systems, we find a significant decay in the fidelity of the coherent manipulations, which we have characterised using the techniques of Raman spectroscopy, Rabi oscillations, Ramsey interferometry and spin echo. We have found the minimum time constant for the decay in the decoherence to be 2.1fi0:2 ms, which is a result of non-radiative and partially non-stochastic dephasing mechanisms. Due to a high level of decoherence during the spin-echo experiments further investigation is required to determine the exact ratio of stochastic to non-stochastic dephasing
Ultracold samples of laser-cooled atoms are quantum systems over which modern atomic physicists can exert exquisite control. Largely decoupled from their environment, they can act as near-ideal test masses for inertial sensors based on atom interferometry and are well suited to experiments in coherent control of quantum systems that probe the fundamental nature of quantum mechanics and pave the way for practical quantum simulation and computation. This thesis details a series of experimental results that arise from the coherent control of rubidium atoms with laser light, focusing on the interplay between these interactions and atomic velocities; the laser frequency an atom ‘sees’ is Doppler shifted according to its velocity, while conservation of momentum dictates that, in exchanging photons with a laser, an atom’s velocity is altered. Coherent light–atom interactions can thus be tailored either to measure or to narrow the spread of velocities in an ultracold atomic gas. Alternatively, it can be desirable to design interactions that are homogeneous across a large spread of atomic velocities. All of these aspects are explored in this thesis. The velocity-sensitive interactions that lie at the heart of atom-interferometric inertial sensors are reexamined in a manner that yields considerable insight into the underlying processes and culminates in a novel, precise and elegant technique for measuring the velocity of ultracold atoms that is used to reveal the Gaussian nature of the velocity spread in a cloud with an effective temperature of 18.7(6) µK, undistorted by artefacts that plague other methods. Furthermore, optimal control techniques are applied to the problem of coherently and uniformly manipulating the quantum states of atoms in an ensemble with a large spread of velocities, even subject to variations in laser intensity. A broadband inversion pulse is demonstrated to change the internal state of 99.8(3) % of atoms in a ∼35 µK ensemble and — for the first time — this technique is used to optimise an entire atom interferometry sequence, yielding a threefold enhancement in the measurement contrast. Finally, a version of grey molasses cooling — in which atoms accumulate in velocity-dependent ‘dark’ states, narrowing their momentum spread and increasing their phase space density — is demonstrated with phase-coherent cooling beams; dark states that exist in this system prove to be particularly resilient to the spatially varying light shifts that are present in an optical dipole trap, and this is used both to enhance the number of atoms loaded into such a trap — by a factor of 7 compared to loading from a conventional optical molasses — and to further cool them once they are loaded in a technique that has promising prospects for the rapid production of ultracold, trapped, atoms.
The laser cooling of atoms to ultracold temperatures has propelled many groundbreaking advances in fundamental research and precision measurement, through such applications as quantum simulators and interferometric sensors. Laser cooling remains, however, highly species-selective, and techniques for its application to molecules are still in their infancy. This thesis broadly concerns the development of laser cooling schemes, based on sequences of coherent optical pulses, which can in principle be applied to a wide range of species. We describe a cooling scheme, in which a velocity-selective impulse analogous to that in Doppler cooling is generated by a light-pulse Ramsey interferometer, and present a proof-of-concept demonstration of the scheme using ultracold rubidium-85 atoms as a test-bed. We realise an interferometer for the atoms, as they are in free-fall after release from a magneto-optical trap, by inducing stimulated Raman transitions between their ground hyperfine states. We provide a comprehensive characterisation of these Raman light-pulse interferometer optics, where particular attention is paid to light shift effects. Raman pulses, and indeed coherent operations in any quantum control system, unavoidably suffer from systematic errors in the control field intensity and frequency, and these lead to reductions in pulse fidelity and readout contrast. In parallel to the work on interferometric cooling in this thesis, we report our preliminary investigations into composite pulses, whereby 'naive' single pulses are replaced by sequences of rotations with tailored durations and phases, for improving pulse fidelity in the presence of inhomogeneities. We find that composite pulses can indeed be highly effective in our cold atom system, and propose that their application in such devices as interferometric sensors is a promising prospect.
Cold atom samples, at temperatures of the order 100 uK, are useful for a wide reaching array of new and exciting technological and scientific endeavours. Atoms are conventionally cooled by Doppler cooling, which relies on the continuous absorption and reemission of photons in a closed optical cycle. This requirement is diffcult to achieve when there are many allowed decay paths for the excited atom, making Doppler cooling only feasible for a handful atoms with simple energy level structures. More exotic energy level structures, such as those found in molecules, are notoriously diffcult to cool. Coherent cooling schemes in comparison, offer advantages such as insensitivity to frequency detuning or a higher number of photon momenta which can be imparted for each spontaneous emission event making them promising candidates for the optical cooling of particles with more general energy level structures. In order to demonstrate these schemes, we have explored the coherent manipulation of an atomic cloud of Rubidium cooled using a two photon Raman resonance. Despite the long spontaneous decay times of such systems, we find a significant decay in the fidelity of the coherent manipulations, which we have characterised using the techniques of Raman spectroscopy, Rabi oscillations, Ramsey interferometry and spin echo. We have found the minimum time constant for the decay in the decoherence to be 2.1fi0:2 ms, which is a result of non-radiative and partially non-stochastic dephasing mechanisms. Due to a high level of decoherence during the spin-echo experiments further investigation is required to determine the exact ratio of stochastic to non-stochastic dephasing
The range of atoms which can be cooled by lasers is limited to those which have a closed two level structure. Several schemes have been proposed which aim to extend this range by using coherent control of the particle momenta, but none have yet been demonstrated. We hope to implement these and other coherent manipulation schemes, and we begin with a system which is well understood and over which we can exert precise control. This thesis covers the design and construction of an experiment to demonstrate coherent manipulation of cold rubidium atoms collected in a magneto-optical trap. The lower hyperfine levels of these cold atoms very closely mimic the ideal two-level atom, and we use carefully crafted laser pulses to prepare, manipulate, and read their quantum state. The hyperfine levels are coupled using two fields whose frequency difference is equal to the hyperfine splitting. The way in which these Raman coupled levels can be used to emulate a two-level atom is explored, and the experimental apparatus used to create and control the driving fields is described in detail. The amplitude, frequency and phase of these fields is programmable, and complex manipulation schemes can be implemented merely by programming a computer. We have observed Raman transitions in the cold rubidium atoms, and the experimental methods used to detect these features amidst large experimental noise are discussed. Although we have not yet seen Rabi oscillations, we are confident that we can now have sufficient control to begin to implement simple interferometric sequences. However, there remain significant challenges if we are to coherently manipulate the momentum, and the prospects for such manipulation are discussed.
The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3