We report on ultracold atomic collision experiments utilizing frequency-chirped laser light. A rapid chirp below the atomic resonance results in adiabatic excitation to an attractive molecular potential over a wide range of internuclear separation. This leads to a transient inelastic collision rate which is large compared to that obtained with fixed-frequency excitation. The combination of high efficiency and temporal control demonstrates the benefit of applying the techniques of coherent control to the ultracold domain. DOI: 10.1103/PhysRevLett.95.063001 PACS numbers: 32.80.Pj, 32.80.Qk, 34.50.Rk The ability to control the dynamics of microscopic systems has been a major motivation in physics and chemistry in recent years [1]. The development of ultrafast lasers and pulse-shaping techniques has allowed selective bond breaking and coherent control of chemical reactions [2]. At the other temporal extreme, slow collisions between ultracold atoms [3,4] can be controlled by long-range laser excitation because the colliding atoms have minimal kinetic energy and their trajectories are easily manipulated. In the present work, we adapt the techniques of coherent control to the nanosecond time scale and use frequencychirped light to control inelastic collisions between ultracold atoms. The combination of adiabatic excitation and the large number of atom pairs addressed by the chirp leads to a large transient collision rate. Such extensions of coherent control to the ultracold domain may significantly benefit processes such as ultracold molecule formation [5,6]. As an example, chirped two-photon Raman photoassociation [7,8] may provide an attractive alternative to magnetic Feshbach resonances for the coherent conversion of an atomic Bose-Einstein condensate into a molecular one. Because light can be controlled much faster than magnetic fields, the chirped excitation techniques developed here may allow the probing of quantum gases on much shorter time scales than previously achieved [9].There have been a number of experiments exploring the temporal dynamics of ultracold collisions. A long-lived ground-state shape resonance has been probed by timedependent photoassociation [10,11], and laser-induced collisions have been followed in real time [12,13]. Motivated by earlier predictions [14], photoassociative ionization dynamics on the nanosecond time scale have been probed with picosecond pulses [15]. In ultracold highly excited Rydberg atoms, the microsecond-scale evolution of resonant energy transfer has been observed via field ionization [16,17]. Our use of rapidly frequency-chirped laser light brings a new dimension to these studies. The temporal evolution of the light can lead to an efficient and robust adiabatic transfer of population to the excited state. Also, the wide range of frequencies spanned by the chirp leads to excitation of atom pairs over a wide range of internuclear separations. The advantages of chirped excitation have been discussed in the context of ultracold atom photoassociation with picosecond puls...