  Three-dimensional topological insulators (TIs) are characterized by
spin-polarized Dirac-cone surface states that are protected from backscattering
by time-reversal symmetry. Control of the spin polarization of topological
surface states (TSSs) using femtosecond light pulses opens novel perspectives
for the generation and manipulation of dissipationless surface spin currents on
ultrafast timescales. Using time-, spin-, and angle-resolved spectroscopy, we
directly monitor for the first time the ultrafast response of the spin
polarization of photoexcited TSSs to circularly-polarized femtosecond pulses of
infrared light. We achieve all-optical switching of the transient out-of-plane
spin polarization, which relaxes in about 1.2 ps. Our observations establish
the feasibility of ultrafast optical control of spin-polarized Dirac fermions
in TIs and pave the way for novel optospintronic applications at ultimate
speeds.
