We present a thorough analysis of one- and two-color transient absorption measurements performed on single- and double-walled semiconducting carbon nanotubes. By combining the currently existing models describing exciton-exciton annihilation-the coherent and the diffusion-limited ones-we are able to simultaneously reproduce excitation kinetics following both E11 and E22 pump conditions. Our simulations revealed the fundamental photophysical behavior of one-dimensional coherent excitons and non-trivial excitation relaxation pathways. In particular, we found that after non-linear annihilation a doubly-excited exciton relaxes directly to its E11 state bypassing the intermediate E22 manifold, so that after excitation resonant with the E11 transition, the E22 state remains unpopulated. A quantitative explanation for the observed much faster excitation kinetics probed at E22 manifold, comparing to those probed at the E11 band, is also provided.

Quantum superposition of molecular electronic states is very fragile because of thermal energy fluctuations and the static conformational disorder induced by the intimate surrounding of constituent molecules of the system. However, the nature of the long-lived quantum beats, observed in time-resolved spectra of molecular aggregates at physiological conditions, is still being debated. We present our study of the conditions when long-lived electronic quantum coherences originating from recently proposed inhomogeneous broadening mechanism are enhanced and reflected in the two-dimensional electronic spectra of the excitonically coupled molecular dimer. We show that depending on the amount of inhomogeneous broadening, the excitonically coupled molecular system can establish long-lived electronic coherences, caused by a disordered subensemble, for which the dephasing due to static energy disorder becomes significantly reduced. On the basis of these considerations, we present explanations for why the electronic or vibrational coherences were or were not observed in a range of recent experiments.

Methylammonium lead iodide (CH3NH3PbI3) hybrid perovskite in the tetragonal and orthorhombic phases have different exciton binding energies and demonstrate different excitation kinetics. Here, we explore the role that crystal structure plays in the kinetics via fluence dependent transient absorption spectroscopy. We observe stronger saturation of the free carrier concentration under high pump energy density in the orthorhombic phase relative to the tetragonal phase. We attribute this phenomenon to small dielectric constant, large exciton binding energy, and weak Coulomb screening, which results in difficult exciton dissociation under high light intensity in the orthorhombic phase. At higher excitation intensities, we observe a coherent phonon with an oscillation frequency of 23.4 cm(-1) at 77 K, whose amplitude tracks the increase of the first-order lifetime.