Tunable femtosecond pump-near IR probe measurements on InAs/CdSe/ZnSe core/shell1/shell2 nanocrystal quantum dots were conducted to quantify spontaneous carrier multiplication previously reported in this system. Experimental conditions were chosen to eliminate the need for determining absolute wavelength dependent cross sections of the nanocrystals and allow direct comparison of band edge absorption bleach kinetics for different excitation energies up to 3.7 times the band gap. Results for two sample sizes show no signs of carrier multiplication within that range. This result is discussed in light of reports describing occurrence of this novel phenomenon in quantum dots based on this as well as numerous other semiconductor materials.

Understanding a chemical reaction ultimately requires the knowledge of how each atom in the reactants moves during product formation. Such knowledge is seldom complete and is often limited to an oversimplified reaction coordinate that neglects global motions across the molecular framework. To overcome this limit, we recorded transient impulsive Raman spectra during ultrafast photoisomerization of cis-stilbene in solution. The results demonstrate a gradual frequency shift of a low-frequency spectator vibration, reflecting changes in the restoring force along this coordinate throughout the isomerization. A high-level quantum-chemical calculation reproduces this feature and associates it with a continuous structural change leading to the twisted configuration. This combined spectroscopic and computational approach should be amenable to detailed reaction visualization in other photoisomerizing systems as well.