Ultrasmall bullets of light--focusing few-cycle light pulses to the diffraction limit.

We demonstrate an essentially dispersion-free and diffraction-limited focusing of few-cycle laser pulses through all-reflective microscope objectives. By transmitting 6-fs-pulses from a Ti:sapphire oscillator through an all-reflective 0.5 NA objective, we reach a focus with a beam diameter of 1.0 µm, preserving the time structure of the pulses. The temporal and spatial pulse profile is recorded simultaneously using a novel tip-enhanced electron emission autocorrelator, indicating a focal volume of these pulses of only 1.8 µm3. We anticipate that the demonstrated technique is of considerable interest for inducing and probing optical nonlinearities of individual nanostructures.

Distinguishing between ultrafast optical harmonic generation and multi-photon-induced luminescence from ZnO thin films by frequency-resolved interferometric autocorrelation microscopy.

The nonlinear optical properties of thin ZnO film are studied using interferometric autocorrelation (IFRAC) microscopy. Ultrafast, below-bandgap excitation with 6-fs laser pulses at 800 nm focused to a spot size of 1 µm results in two emission bands in the blue and blue-green spectral region with distinctly different coherence properties. We show that an analysis of the wavelength-dependence of the interference fringes in the IFRAC signal allows for an unambiguous assignment of these bands as coherent second harmonic emission and incoherent, multiphoton-induced photoluminescence, respectively. More generally our analysis shows that IFRAC allows for a complete characterization of the coherence properties of the nonlinear optical emission from nanostructures in a single-beam experiment. Since this technique combines a very high temporal and spatial resolution we anticipate broad applications in nonlinear nano-optics.

Site specificity in femtosecond laser desorption of neutral H atoms from graphite(0001).

Femtosecond laser excitation and density functional theory reveal site and vibrational state specificity in neutral atomic hydrogen desorption from graphite induced by multiple electronic transitions. Multimodal velocity distributions witness the participation of ortho and para pair states of chemisorbed hydrogen in the desorption process. Very slow velocities of 700 and 400 ms^{-1} for H and D atoms are associated with the desorption out of the highest vibrational state of a barrierless potential.