A generalized Suzuki–Trotter type method in optimal control of coupled Schrödinger equations

Abstract

A generalized Suzuki–Trotter (GST) method for the solution of an optimal control problem for quantum molecular systems is presented in this work. The control of such systems gives rise to a minimization problem with constraints given by a system of coupled Schrödinger equations. The computational bottleneck of the corresponding minimization methods is the solution of time-dependent Schrödinger equations. To solve the Schrödinger equations we use the GST framework to obtain an explicit polynomial approximation of the matrix exponential function. The GST method almost exclusively uses the action of the Hamiltonian and is therefore efficient and easy to implement for a variety of quantum systems. Following a first discretize, then optimize approach we derive the correct discrete representation of the gradient and the Hessian. The derivatives can naturally be expressed in the GST framework and can therefore be efficiently computed. By recomputing the solutions of the Schrödinger equations instead of saving the whole time evolution, we are able to significantly reduce the memory requirements of the method at the cost of additional computations. This makes first and second order optimization methods viable for large scale problems. In numerical experiments we compare the performance of different first and second order optimization methods using the GST method. We observe fast local convergence of second order methods.