Comparison of the populations (b (i)) and coherences (b (ii)) of the S 0 (red) and S 1 (yellow) electronic states over time, with the pump (dashed lines) and pumpdump (solid lines) schemes shown, for 2-ps delay (b, corresponding to Fig. 3b). A coherence comparison is made between the pump and long 2-ps (b) pumpdump delays. The Wigner phasespace distributions of the S 0 ground state for all pulse schemes are shown in b (iii), with b (iii) showing minimal impact on the distribution, with a small generation of position ( q ) and no impulse momentum ( p ) transferred, but with population transfer after the dump interaction. The corresponding Wigner transformations for S 1 are shown in Supplementary Fig. 58 using surface representations. Calculations were performed using the parameters listed in Supplementary Table 11 , which are representative of the TR-SFX conditions and use the methodology described in Supplementary Section 13.
