  The ability to control spins in semiconductors is important in a variety of
fields including spintronics and quantum information processing. Due to the
potentially fast dephasing times of spins in the solid state [1-3], spin
control operating on the picosecond or faster timescale may be necessary. Such
speeds, which are not possible to attain with standard electron spin resonance
(ESR) techniques based on microwave sources, can be attained with broadband
optical pulses. One promising ultrafast technique utilizes single broadband
pulses detuned from resonance in a three-level Lambda system [4]. This
attractive technique is robust against optical pulse imperfections and does not
require a fixed optical reference phase. Here we demonstrate the principle of
coherent manipulation of spins theoretically and experimentally. Using this
technique, donor-bound electron spin rotations with single-pulse areas
exceeding pi/4 and two-pulses areas exceeding pi/2 are demonstrated. We believe
the maximum pulse areas attained do not reflect a fundamental limit of the
technique and larger pulse areas could be achieved in other material systems.
This technique has applications from basic solid-state ESR spectroscopy to
arbitrary single-qubit rotations [4, 5] and bang-bang control[6] for quantum
computation.
