In this note, we introduce one basic concept in nonlinear optical spectroscopy: time-dependent Hamiltonian. Then we give one example of application of the time evolution operator.
The concept of complete positivity fixes in considerable detail the mathematical structure of quantum Markovian master equations which describe the combined reversible-irreversible dynamics of open systems for the case of time-independent Hamilton operators. For many applications such as, for instance, problems of time-resolved spectroscopy, similar results would be of great value but involve time-varying external fields with a corresponding time-dependent Hamiltonian. For this reason, we propose a suitable extension of the Kossakowski generator to the time-dependent case by maintaining complete positivity and using arguments suggested by experimental facts. As an example, generalized Bloch-like equations can be obtained with three different relaxation times and a nonlinear dependence upon field strength.
We introduce a new approach for describing nonstationary quantum systems with a discrete energy spectrum. The essence of this approach is that we describe the evolution of a quantum system in a time-dependent basis. In a sense, this approach is similar to the description of the system in the interaction representation. However, the time dependence of the basic states of the representation is determined not by the evolution operator with a time-independent Hamiltonian but by the eigenstates of the time-dependent Hamiltonian defined at the current time. The time dependence of the basic states of the representation leads to the appearance of an additional term in the Schrödinger equation, which in the case of slowly changing parameters of the Hamiltonian can be considered as a small perturbation. The adiabatic representation is suitable in cases where it is impossible to apply the standard interaction representation. The application of the adiabatic representation is illustrated by the example of two spins connected by a magnetic dipole–dipole interaction in a slowly varying external magnetic field.
Magnus expansion (ME) provides a general way to expand the real-time propagator of a time-dependent Hamiltonian within the exponential such that the unitarity is satisfied at any order. We use this property and explicit integration of Lagrange interpolation formulas for the time-dependent Hamiltonian within each time interval and derive approximations that preserve unitarity for the differential time evolution operators of general time-dependent Hamiltonians. The resulting second-order approximation is the same as using the average of Hamiltonians for two end points of time. We identify three fourth-order approximations involving commutators of Hamiltonians at different times and also derive a sixth-order expression. A test of these approximations along with other available expressions for a two-state time-dependent Hamiltonian with sinusoidal time dependences provides information on the relative performance of these approximations and suggests that the derived expressions can serve as useful numerical tools for time evolution in time-resolved spectroscopy, quantum control, quantum sensing, real-time ab initio quantum dynamics, and open system quantum dynamics.