In recent decades, the Lyapunov-based method has been used in quantum systems control because of its simple design and without iterations. Research on the Lyapunov-based method has been in two stages. The first stage involved its applications in physics and chemistry, where it is called local optimal control (Sugawara, 2002(Sugawara, , 2003. The method has been successfully used to solve regulation problems such as pump-dump reaction control, isomerization, and splitting reaction controls. The control goals of these problems focused on the effective excitation of eigenstate population distribution, path transfer, and wave packet shaping of quantum systems by means of experiments or simulations. The research focused on the external control field design, but the desired control goal usually cannot be guaranteed due to the lack of theoretical analysis for the final state and the control effect. In fact, in simulation experiments it is easy to see that the Lyapunov-based control law doesn't always guarantee the realization of the control goal. This is because the stable Lyapunov-based control method may not be convergent. To achieve this convergence, the second stage is used. Scientists in the fields of control systems and mathematics led the research on quantum control based on the Lyapunov method (. They focused on analyzing theoretically the convergence of state evolution, which provides the theoretical foundation for the reachability of the Lyapunov method applied to the fields of physics and chemistry. For the Lyapunov functions selected, assumed the eigenstate to be the target state for a pure state model. By means of the invariance principle, they proved the equivalence between the asymptotic stability of the target state and the controllability of the linear system of eigenstates. They also proposed adiabatic evolution to asymptotically track the target eigenstate in a unreachable linearized system. For a closed-loop system model with the density operator as its variable, Altafini and Schirmer Control of Quantum Systems: Theory and Methods, First Edition. Shuang Cong.