Quantum computation with vibrationally excited polyatomic molecules: effects of rotation, level structure, and field gradients

Accurate rotation-vibration energy levels and transition dipoles of the molecule thiophosgene are used to model the execution of quantum gates with shaped laser pulses. Qubits are encoded in 2n vibrational computing states on the ground electronic surface of the molecule. Computations are carried out by cycling amplitude between these computing states and a gateway state with a shaped laser pulse. The shaped pulse that performs the computation in the computing states is represented by a physical model of a 128-1024 channel pulse shaper. Pulse shapes are optimized with a standard genetic algorithm, yielding experimentally realizable computing pulses. We study the robustness of optimization as a function of the vibrational states selected, rotational level structure, additional vibrational levels not assigned to the computation, and compensation for laser power variation across a molecular ensemble.