We examine the multiple exciton population dynamics in PbS quantum dots by
ultrafast spectrally-resolved supercontinuum transient absorption (SC-TA). We
simultaneously probe the first three excitonic transitions over a broad
spectral range. Transient spectra show the presence of first order bleach of
absorption for the 1S_h-1S_e transition and second order bleach along with
photoinduced absorption band for 1P_h-1P_e transition. We also report evidence
of the one-photon forbidden 1S_{h,e}-1P_{h,e} transition. We examine signatures
of carrier multiplication (multiexcitons for the single absorbed photon) from
analysis of the first and second order bleaches, in the limit of low absorbed
photon numbers (~ 10^-2), at pump energies from two to four times the
semiconductor band gap. The multiexciton generation efficiency is discussed
both in terms of a broadband global fit and the ratio between early- to
long-time transient absorption signals.. Analysis of population dynamics shows
that the bleach peak due to the biexciton population is red-shifted respect the
single exciton one, indicating a positive binding energy.Comment: 16 pages, 5 figure
