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The Liouville-space pathways with time-ordering "pump-probe-pump" give rise to coherent coupling. Here, the first two field interactions generate a spatial grating, which scatters pump light from the third field interaction into the direction of the probe light. Hence, the coherent coupling signal varies with pump frequency and causes a small tilt of the negative v = O → 1 bleach and stimulated emission contribution, even when no inhomogeneity is present. This signal decays on a time scale given by the pump pulse duration and should not be misinterpreted as inhomogeneous broadening. However, model calculations show that this tilt is significantly smaller than that found in the data (Fig. 1) and, more importantly, that the tilt of the v = 1 → 2 excited state absorption, which is not resonant with the pump light, is not at all affected by coherent coupling.
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