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Water is a unique solvent with strong, yet highly dynamic, intermolecular interactions. Many insights into this distinctive liquid have been obtained using ultrafast vibrational spectroscopy of water’s O-H stretch vibration. However, it has been challenging to separate the different contributions to the dynamics of the O-H stretch vibration in H_{2}O. Here, we present a novel nonequilibrium molecular dynamics (NEMD) algorithm that allows for a detailed picture of water vibrational dynamics by generating nonequilibrium vibrationally excited states at targeted vibrational frequencies. Our ab initio NEMD simulations reproduce the experimentally observed time scales of vibrational dynamics in H_{2}O. The approach presented in this work uniquely disentangles the effects on the vibrational dynamics of four contributions: the delocalization of the O-H stretch mode, structural dynamics of the hydrogen bonded network, intramolecular coupling within water molecules, and intermolecular coupling between water molecules (near-resonant energy transfer between O-H groups). Our results illustrate that intermolecular energy transfer and the delocalization of the O-H stretch mode are particularly important for the spectral diffusion in H_{2}O.