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.