Solid-state electron spin qubits, like the nitrogen-vacancy center in
diamond, rely on control sequences of population inversion to enhance
sensitivity and improve device coherence. But even for this paradigmatic
system, the fundamental limits of population inversion and potential impacts on
applications like quantum sensing have not been assessed quantitatively. Here,
we perform high accuracy simulations beyond the rotating wave approximation,
including explicit unitary simulation of neighboring nuclear spins. Using
quantum optimal control, we identify analytical pulses for the control of a
qubit subspace within the spin-1 ground state and quantify the relationship
between pulse complexity, control duration, and fidelity. We find exponentially
increasing amplitude and bandwidth requirements with reduced control duration
and further quantify the emergence of non-Markovian effects for multipulse
sequences using sub-nanosecond population inversion. From this, we determine
that the reduced fidelity and non-Markovianity is due to coherent interactions
of the electron spin with the nuclear spin environment. Ultimately, we identify
a potentially realizable regime of nanosecond control duration for
high-fidelity multipulse sequences. These results provide key insights into the
fundamental limits of quantum information processing using electron spin
defects in diamond.Comment: 9 pages, 5 figure