A millimeter-scale dense liquid droplet of glycine is prepared by focusing a CW near-infrared laser beam at the glass/solution interface of a thin film of its supersaturated heavy water solution. The formation process is investigated by direct observation with CCD and by measuring temporal change of the surface height with a displacement meter. The droplet becomes much larger than a focal spot size, a few mm width and ∼150 μm height, and observable with the naked eye. Interestingly, the droplet remains for a few tens of seconds even after switching off the laser beam. Whereas the droplet is kept during laser irradiation, the crystallization is immediately attained by shifting the laser beam to the air/droplet surface. It is considered that the droplet is possibly the early stage of the multistep crystallization process and plays an important role in photon pressure-induced crystallization of glycine.SECTION Nanoparticles and Nanostructures P hoton pressure, which is a gradient force toward a focal spot generated by a focused CW laser beam, has been widely employed as an optical tweezers technique to trap and to manipulate micrometer-sized objects in many fields of physics, optics, and biology. 1-3 Over the past decades, the study on photon pressure in solution has progressed with the size reduction of target materials from microscale to nanoscale, 4-6 and actually, we have extended a series of experiments on the dynamics of photon pressure-induced association of nanoparticles, polymers, micelles, and J-aggregates in their solutions at room temperature. [7][8][9][10][11] As an example, polystyrene latex nanoparticles with 24 nm diameter were trapped and gathered by photon pressure, leading to their assemblies in a focal spot. 11 In single-molecule level, Osborne et al. and Chirico et al. separately reported that the diffusion of Rhodamine 6G molecules in the focal spot were suppressed under photon pressure, although no stable trapping was achieved. 12,13 These results imply that photon pressure efficiently works even on small clusters or molecules, which have the sizes much smaller than the wavelength of the trapping laser.In 2007, we applied photon pressure of a focused CW nearinfrared laser beam to a supersaturated heavy water solution of glycine, and for the first time succeeded in inducing the crystallization, which we call "laser trapping crystallization". 14 This novel phenomenon was explained by assuming that glycine molecules form aggregates under a supersaturated condition before irradiation because the optical gradient force in our experiment is too small to trap the single molecule.Indeed, the presence of small liquid-like clusters of glycine under a supersaturated condition has been experimentally demonstrated. 15 Such clusters, which are associated with each other through weak hydrogen bonds without forming nucleus, should be gathered in the focal spot and reorganized into ordered structures by photon pressure. In 2005, Myerson et al. reported the direct confirmation on the cluster structure...