Optimal control of the external electromagnetic field input for the maximization of the quantum triplet-singlet yield of the radical pairs in biochemical reactions modeled by Schrödinger system with spin Hamiltonians given by the sum of Zeeman interaction and hyperfine coupling interaction terms are analyzed. Fréchet differentiability and Pontryagin Maximum Principle in Hilbert space is proved and the bang-bang structure of the optimal control is established. A closed optimality system of nonlinear differential equations for the identification of the bang-bang optimal control is revealed. Numerical methods for the identification of the bang-bang optimal control based on the Pontryagin maximum principle are developed. Numerical simulations are pursued, and the convergence and stability of the numerical methods are demonstrated. The results contribute towards understanding the structure-function relationship of the putative magnetoreceptor to manipulate and enhance quantum coherences at room temperature and leveraging biofidelic function to inspire novel quantum devices.