We first measured the Raman spectrum of a pentacene crystal to identify the intermolecular and intramolecular modes, with particular focus on the low frequency region (Fig. ). We recorded five modes below 200 cm -1 , consistent with previously reported phonon spectra for pentacene crystals grown via physical vapor transport. We collected femtosecond stimulated Raman (FSR) spectra at two spatially offset regions and one fully overlapped position to monitor phonon impacts on exciton transport in both the fast and slow axes. We perform six SOFSRS scans, using a single pulse excitation in addition to five double pulse excitations corresponding to each measured phonon mode. Each excited state FSR spectrum is subtracted from the ground state spectrum to remove residual ground state contributions. In Figure , we show selected time points from the ground state subtracted spectra for the single pulse excitation (2A-C) and the 91 cm -1 double pulse excitation (2D-F). We present selected time points from the ground state subtracted spectra for all other double pulse pairs in Figures . Figures and depict FSR spectra with the actinic pulse fully overlapped with the probing region, indicated by the shaded pixel in the inset. Figures and show FSR spectra when the actinic is offset by 2.7 µm from the probe along the crystallographic a axis, and Figures and correspond to an actinic offset 2.7 µm along the b axis. In all photoexcitation locations Raman Shift (cm -1 )