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We propose and experimentally demonstrate a scheme to generate optically controlled delays based on off-resonant Raman absorption. Dispersion in a transparency window between two neighboring, optically activated Raman absorption lines is used to reduce the group velocity of broadband 765 nm pulses. We implement this approach in a potassium titanyl phosphate (KTP) waveguide at room temperature, and demonstrate Raman-induced delays of up to 140 fs for a 650-fs duration, 1.8-THz bandwidth, pulse. Our approach should be applicable to single-photon signals, offers wavelength tunability, and is a step toward processing ultrafast photons.

Nonperturbative quantum control schemes in the intermediate field strength (nonionizing) regime are investigated. We restrict the matter-field interaction to the nonresonant dynamic Stark effect (NRDSE) as induced by infrared laser fields, which we argue is a new and general tool for quantum control of atomic and molecular dynamics. For the case of Raman coupled matter states, an effective Hamiltionian may be constructed, and quantum control via NRDSE may be thought of as reversibly modifying the effective Hamiltonian during system propagation, thus leading to control over dynamic processes. As an illustration, the creation of field-free “switched” wave packets through the adiabatic turn on and sudden turn off of the NRDSE is considered and experimentally demonstrated. Wave packets generated through the switched NRDSE interaction may be very different in form and content than wave packets generated via resonant transitions with Gaussian optical pulses. In order to provide an example, we discuss the specific case of rotational wave packet dynamics where the NRDSE manifests itself as molecular axis alignment. This technique is applied to the creation of field-free molecular axis alignment using an intense switched 1.064μm laser pulse. This switched laser pulse was generated via a plasma shuttering technique, giving a pulse with a rise time of 150ps and a fall time of 170fs. The temporal evolution of the molecular axis alignment is probed via the optical Kerr effect. Field-free alignment via the switched NRDSE is demonstrated for both linear (CO2, CS2) and symmetric top (1,2-propadiene) polyatomic molecules.