We report on the dynamics of the dielectric function of single-wall carbon nanotubes in the 10-30 THz frequency range after ultrafast laser excitation. The absence of a distinct free-carrier response is attributed to the photogeneration of strongly bound excitons in the tubes with large energy gaps. We find a feature of enhanced transmission caused by the blocking of optical transitions in small-gap tubes. The rapid decay of a featureless background with pronounced dichroism is associated with the increased absorption of spatially localized charge carriers before thermalization is completed.

Ultrafast charge carrier dynamics in graphite are investigated by time-resolved THz spectroscopy. Our data show that: (i) more than 90% of the initially deposited excitation energy is transferred to few strongly coupled lattice vibrations within 500 fs; and (ii) these optical phonons substantially contribute to the striking increase of the Drude relaxation rate.

Ultrafast charge carrier dynamics in graphite has been investigated by time-resolved terahertz spectroscopy. Analysis of the transient dielectric function and model calculations show that more than 90% of the initially deposited excitation energy is transferred to a few strongly coupled lattice vibrations within 500 fs. These hot optical phonons also substantially contribute to the striking increase of the Drude relaxation rate observed during the first picosecond after photoexcitation. The subsequent cooling of the hot phonons yields a lifetime estimate of 7 ps for these modes.

We demonstrate broad-field, non-scanning, two-photon excitation fluorescence (2PEF) close to a glass/cell interface by total internal reflection of a femtosecond-pulsed infrared laser beam. We exploit the quadratic intensity dependence of 2PEF to provide nonlinear evanescent wave (EW) excitation in a well-defined sample volume and to eliminate scattered background excitation. A simple model is shown to describe the resulting 2PEF intensity and to predict the effective excitation volume in terms of easily measurable beam, objective and interface properties. We demonstrate nonlinear evanescent wave excitation at 860 nm of acridine orange-labelled secretory granules in live chromaffin cells, and excitation at 900 nm of TRITC-phalloidinactin/GPI-GFP double-labelled fibroblasts. The confined excitation volume and the possibility of simultaneous multi-colour excitation of several fluorophores make EW 2PEF particularly advantageous for quantitative microscopy, imaging biochemistry inside live cells, or biosensing and screening applications in miniature high-density multi-well plates.

Total internal reflection fluorescence (TIRF), a general term that embraces any spectroscopic or microscopic technique based on the evanescent field created by TIR of light, is further establishing itself as an important tool for studying near-surface phenomena. Impingement of a femtosecond-pulsed infrared beam on a reflecting interface creates the conditions for 'macroscopic' evanescent-field two-photon fluorescence excitation. The two-photon fluorescence excitation volume is confined by both the non-linearity of the multi-photon process and the spatial inhomogeneity of the evanescent field. The absence of scattered excitation resulting in a low background and the possibility of simultaneous multi-colour fluorescence excitation should make non-linear evanescent-field excitation particularly attractive for quantitative single-molecule observation and ultra-sensitive screening assays. In this topical review, we survey the requirements, present the current results and explore the potential of this novel non-linear microscopy.