Our concept for a quantum computational system is based on qubits encoded in vibrational normal modes of polyatomic molecules. The quantum gates are implemented by shaped femtosecond laser pulses. We adopt this concept to the new species manganese pentacarbonyl bromide [MnBr(CO)(5)] and show that it is a promising candidate in the mid-infrared (IR) frequency range to connect theory and experiment. As direct reference for the ab initio calculations we evaluated experimentally the absorption bands of MnBr(CO)(5) in the mid-IR as well as the related transition dipole moments. The two-dimensional potential-energy surface spanned by the two strongest IR active modes and the dipole vector surfaces are calculated with density-functional theory. The vibrational eigenstates representing the qubit system are determined. Laser pulses are optimized by multitarget optimal control theory to form a set of global quantum gates: NOT, CNOT, Pi, and Hadamard. For all of them simply structured pulses with low pulse energies around 1 mu J could be obtained. Exemplarily for the CNOT gate we investigated the possible transfer to experimental shaping, based on the mask function for pulse shaping in the frequency regime as well as decomposition into a train of subpulses. (c) 2005 American Institute of Physics.
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