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

Ultrafast control of donor-bound electron spins with single detuned optical pulses