  Quantum spin dephasing is caused by inhomogeneous coupling to the
environment, with resulting limits to the measurement time and precision of
spin-based sensors. The effects of spin dephasing can be especially pernicious
for dense ensembles of electronic spins in the solid-state, such as for
nitrogen-vacancy (NV) color centers in diamond. We report the use of two
complementary techniques, spin bath control and double quantum coherence, to
enhance the inhomogeneous spin dephasing time ($T_2^*$) for NV ensembles by
more than an order of magnitude. In combination, these quantum control
techniques (i) eliminate the effects of the dominant NV spin ensemble dephasing
mechanisms, including crystal strain gradients and dipolar interactions with
paramagnetic bath spins, and (ii) increase the effective NV gyromagnetic ratio
by a factor of two. Applied independently, spin bath control and double quantum
coherence elucidate the sources of spin dephasing over a wide range of NV and
spin bath concentrations. These results demonstrate the longest reported
$T_2^*$ in a solid-state electronic spin ensemble at room temperature, and
outline a path towards NV-diamond magnetometers with broadband femtotesla
sensitivity.
