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The simulation of open quantum systems coupled to a reservoir throughmultiple channels remains a substantial challenge. This kind of open quantumsystem arises when considering the radiationless decay of excited states thatare coupled to molecular vibrations, for example. We use the chain mappingstrategy in the interaction picture to study systems linearly coupled to aharmonic bath through multiple interaction channels. In the interactionpicture, the bare bath Hamiltonian is removed by a unitary transformation (thesystem-bath interactions remain), and a chain mapping transforms the bath modesto a new basis. The transformed Hamiltonian contains time-dependent localsystem-bath couplings. The open quantum system is coupled to a limited numberof (transformed) bath modes in the new basis. As such, the entanglementgenerated by the system-bath interactions is local, making efficient dynamicalsimulations possible with matrix product states. We use this approach tosimulate singlet fission, using a generalized spin-boson Hamiltonian. Theelectronic states are coupled to a vibrational bath both diagonally andoff-diagonally. This approach generalizes the chain mapping scheme to the caseof multi-channel system-bath couplings, enabling the efficient simulation ofthis class of open quantum systems using matrix product states.

Efficient simulation of open quantum systems coupled to a reservoir through multiple channels