We performed SOFSRS measurements on a lab-built system previously described. The three beams are generated from a 1kHz Ti:Sapphire laser (Coherent Libra) with an 800 nm, 4 W output. We used a custom etalon (TecOptics) to generate a 4 picosecond 805 nm Raman pump pulse. We generated the Raman probe in a 2 mm thick sapphire crystal and compressed it using a fused silica prism pair. We used a home built non-collinear optical parametric amplifier to generate the 569 nm actinic pump and compressed it using an acousto-optical programmable dispersive filter (Fastlite Dazzler). The actinic beam traveled through an automated time delay stage (ThorLabs DDS220) before passing through a set of 2D scanning galvo mirrors (ThorLabs GVS012), which spatially offset the actinic beam from the Raman pump and probe. We focused 42 µW of probe power, 415 µW Raman pump power and 123-137 µW of actinic power onto the sample with a 20X objective (NA= 0.40, Olympus PLN 20X) on an inverted microscope (Olympus IX73). All beams were p-polarized with respect to the b crystallographic axis of the pentacene crystal. We spatially offset the actinic beam by 2.7 µm, measured from the center of the Raman probe to the center of the actinic pump and performed FSRS with three spatial positions of the actinic beam. By only looking at three excitation locations, we probe exciton transport in both the fast and slow exciton transport axes while minimizing experiment time. We measured the beam diameters using the scanning knife edge method on a three-axis piezo positioning stage (Mad City Labs, Nano-LPQ) and determined the diameter of each beam by using the distance from 90% to 10 % of intensity (Fig. ). The probe diameter is 3.2 µm, the actinic diameter is 6.5 µm and the Raman pump diameter is 14.5 µm. We determined the temporal cross-correlation of the Raman probe and actinic pump by measuring the optical Kerr effect in a 40 µm thick diamond. The cross correlation for the single pulse excitation was 169 ± 4 fs (Fig. ). We collected the signal with a 25 mm focal length lens in transmission geometry and focused it into a spectrometer (10-320, Instruments SA) with a 600 gr/mm grating blazed at 750 nm. We recorded with a CCD detector (PIXIS 100F). We averaged each spectrum for 2.5 seconds and recorded with LabView code described elsewhere. For the double pulse SOFSRS measurements, we shaped the actinic pulse and tuned the time delay between the photoexcitation pulses using the acousto-optical programmable dispersive filter (Fastlite Dazzler) as previously described. The time delay between the two actinic pulses is given by one oscillation period of the phonon mode (Table ). We measured the optical Kerr effect cross-correlation of each double pulse and defined time zero as the delay stage position when the second pulse interacts with the probe (Fig. ). All double and single pulse SOFSRS measurements were performed sequentially without moving the sample.