SummaryNear-field optical second harmonic microscopy has been applied to imaging of the c/a/c/a polydomain structure of epitaxial PbZr x Ti 1±x O 3 thin films in the 0 , x , 0.4 range.Comparison of the near-field optical images and the results of atomic force microscopy and X-ray diffraction studies show that an optical resolution of the order of 100 nm is achieved. Symmetry properties of the near-field second harmonic signal allow us to obtain good optical contrast between the local second harmonic generation in c-and a-domains. Experimentally measured near-field second harmonic images have been compared with the results of theoretical calculations. Good agreement between theory and experiment is demonstrated.
Experimental resultsOptical second harmonic generation (SHG) is a sensitive technique for characterization and investigation of the symmetry properties of different samples (Shen, 1984). It is known to be affected by crystal structure, magnetic and ferroelectric order, mechanical strain, etc. Very recently we have introduced an apertureless near-field optical technique for second harmonic imaging using a bare tapered optical fibre tip externally illuminated with femtosecond laser pulses (Smolyaninov et al., 2000). We have presented initial evidence of high spatial resolution of this technique (of the order of 80 nm), and indicated its sensitivity to local crystal symmetry. In this paper, we apply our technique to the imaging of polydomain c/a/c/a structures (consisting of alternating c-domains with the tetragonal axis perpendicular to the film±substrate interface, and a-domains with the c axis of the tetragonal film along either [100] or [010] directions of the substrate) that are commonly observed in thin epitaxial PbZr x Ti 1±x O 3 films in the 0 , x , 0.4 range, and in many other ferroelectric films such as BaTiO 3 , PbTiO 3 , KNbO 3 , etc. (Alpay et al., 1999). We also perform theoretical analysis of our images based on the symmetry properties of the near-field SH signal for different orientations of the poling direction of a poled single crystal of BaTiO 3 . Although simple and qualitative, such an analysis allows us to obtain impressive agreement with the data of experimental measurements. Using this theory, we also analyse the transition from the near-field to the far-field mode of operation of our microscope. This study provides necessary justification for the developed procedure of local poling direction recovery of individual ferroelectric domains in polycrystalline thin ferroelectric films.Our experimental set-up is shown in Fig. 1. Weakly focused light (illuminated spot diameter on the order of 50 mm) from a Ti: sapphire laser system consisting of an oscillator and a regenerative amplifier operating at 810 nm (repetition rate up to 250 kHz, 100 fs pulse duration, and up to 10 mJ pulse energy) was directed at an angle of incidence around 508 onto the sample surface. Excitation power at the sample surface was kept well below the ablation threshold. The local SHG was collected using an uncoate...