A generalized eigenequation is derived for the optimal pairs of phase-
unlocked pump-dump fields in the control of pure state molecular syste
ms in the weak response regime. The associated eigenvalues are further
correlated to the yields of pump-dump control, thus the globally opti
mal pair of phase-unlocked pump-dump fields is identified unambiguousl
y. Presented is also a hierarchy of reduction from the general Liouvil
le-space density matrix control formulation in the strong response reg
ime to various linearized control equations in the weak response regim
e. Application to the control of a molecular ro-vibronic level in the
ground electronic surface reveals a novel symmetry relation between th
e optimal pump field and its counterpart of the optimal dump field. (C
) 1997 American Institute of Physics.