We derive new bounds on the total squared correlation (TSC) of quaternary (quadriphase) signature/sequence sets for all lengths L and set sizes K. Then, for all K, L, we design minimum-TSC optimal sets that meet the new bounds with equality. Direct numerical comparison with the TSC value of the recently obtained optimal binary sets shows under what K, L realizations gains are materialized by moving from the binary to the quaternary code-division multiplexing alphabet. On the other hand, comparison with the Welch TSC value for real/complexfield sets shows that, arguably, not much is to be gained by raising the alphabet size above four for any K, L.