Quantitative measurement of the near-field enhancement of nanostructures by two-photon polymerization.

The quantitative determination of the strength of the near-field enhancement in and around nanostructures is essential for optimizing and using these structures for applications. We combine the gaussian intensity distribution of a laser profile and two-photon-polymerization of SU-8 to a suitable tool for the quantitative experimental measurement of the near-field enhancement of a nanostructure. Our results give a feedback to the results obtained by finite-difference time-domain (FDTD) simulations. The structures under investigation are gold nanotriangles on a glass substrate with 85 nm side length and a thickness of 40 nm. We compare the threshold fluence for polymerization for areas of the gaussian intensity profile with and without the near-field enhancement of the nanostructures. The experimentally obtained value of the near-field intensity enhancement is 600 ± 140, independent of the laser power, irradiation time, and spot size. The FDTD simulation shows a pointlike maximum of 2600 at the tip. In a more extended area with an approximate size close to the smallest polymerized structure of 25 nm in diameter, we find a value between 800 and 600. Using our novel approach, we determine the threshold fluence for polymerization of the commercially available photopolymerizable resin SU-8 by a femtosecond laser working at a wavelength of 795 nm and a repetition rate of 82 MHz to be 0.25 J/cm(2) almost independent of the irradiation time and the laser power used. This finding is important for future applications of the method because it enables one to use varying laser systems.

Pulse duration dependent nonlinear propagation of a focused femtosecond laser pulse in fused silica.

The nonlinear propagation of a single focused femtosecond laser pulse in fused silica has been investigated both experimentally and by numerical simulations. In particular, the filamentation behavior was systematically studied by varying pulse duration. At low pulse energy, the peak plasma density inside the filament first increases to a maximum value with increasing pulse duration and then begins to decrease. At relatively high pulse energy, denser plasma can be induced around the geometrical focus with a certain longer pulse duration, where the peak power is already below the self-focusing critical power and no filament is formed. This pulse duration dependent behavior can be explained by different ionization mechanisms.

Optical vortices from liquid crystal droplets.

We report on the generation of mono- and polychromatic optical phase singularities from micron-sized birefringent droplets. This is done experimentally by using liquid crystal droplets whose three dimensional architecture of the optical axis is controlled within the bulk by surfactant agents. Because of its microscopic size these optical vortex generators are optically trapped and manipulated at will, thus realizing a robust self-aligned micro-optical device for orbital angular momentum conversion. Experimental observations are supported by a simple model of optical spin-orbit coupling in uniaxial dielectrics that emphasizes the prominent role of the transverse optical anisotropy with respect to the beam propagation direction.

Statics and dynamics of radial nematic liquid-crystal droplets manipulated by laser tweezers.

Laser manipulation of trapped radial 4'-n-pentyl-4-cyanobiphenyl (5CB) nematic liquid-crystal droplets induced by molecular reordering is presented. We show experimentally that optical tweezers having linear, elliptical, or circular polarization can break the radial symmetry of the initial molecular organization inside a radial nematic droplet. Static distorted or twisted deformation modes and steady or unsteady nonlinear rotational dynamics are observed. Statics results are analyzed in terms of light-induced radial or left-right symmetry breaking effects associated with optical reorientation. The dynamical observations are compared with simulations from a slab analog model, for which orientational processes driven by optical nonlinearities can be accurately described. This study confirms that light-induced bulk reordering is an essential ingredient towards the understanding of the behavior of radial nematic liquid-crystal droplets in laser tweezers, as suggested by previous studies.

Coupled laser molecular trapping, cluster assembly, and deposition fed by laser-induced Marangoni convection.

A coupled mechanism for molecular aggregation in a thin water solution film by laser-tweezers is suggested based on (i) simulation of light intensity distribution and (ii) order of magnitude analysis of heat and mass transport induced by Marangoni convection. The analysis suggests that the laser induced temperature distribution develops within 1 ms and Marangoni convection flow commences within 0.01-1 s, which increases by 1-2 orders of magnitude the mass transfer of dissolved molecules into the laser focus where they are trapped and aggregate by attractive van der Waals forces. This mechanism, considered for the particular case of polymer assembly, suggests that it can also be successfully applied for assembling other types of clusters and molecular aggregates from solutions.

Laser trapping of deformable objects.

We report the trapping and manipulation of bubbles in viscous glass melts through the use of a laser. This phenomenon is observed in bubbles tens of micrometers in diameter under illumination by low numerical aperture (NA = 0.55). Once the bubble was centered on the optical axis, it was trapped and followed a lateral relocation of the laser beam. This phenomenon is explained by modifications of the bubble's shape induced by axial heating and a decrease in surface tension. It is shown that formation of a concave dimple on the bubble's front surface explains the observed laser trapping and manipulation. This mechanism of laser trapping is expected to take place in other deformable materials and can also be used to remove bubbles from melts or liquids. For this technique to be effective, the alteration of the bubble's shape should be faster than its expulsion out of the laser's point of focus.

Laser manipulation based on a light-induced molecular reordering.

We report on a novel principle of actuation of micrometer-sized liquid crystal droplets. It is based on a light-induced reordering of liquid crystal molecules inside the droplets. Polariscope imaging allowed to evaluate the birefringence change inside the micro-droplets. Directional actuation of the trapped droplet was achieved by cycling laser power with the direction defined by the polarization of the tweezing beam. Micro-actuation resulted from optically-induced birefringence; i.e., a nonlinear optical effect was utilized for mechanical manipulation of the micro-droplet. This principle of actuation can be used to induce molecular flows in sub-micrometer volumes.

Control of the molecular alignment inside liquid-crystal droplets by use of laser tweezers.

Here, we demonstrate how the light-induced birefringence due to the dipole molecular realignment and anisotropic polarizability of a nematic liquid crystal inside a droplet changes the droplet's radial (and thus optically isotropic) structure into a birefringent one. This intensity-dependent change of birefringence can be understood in terms of the anisotropic polarizability and orientational optical nonlinear effect. Birefringence induced by laser tweezers changes the momentum of the passing light. In turn, for the circularly polarized tweezers, this change generates an angular momentum change large enough to spin micrometer-sized droplets. For the linearly polarized tweezers, the molecular ordering generates momentum, which laterally displaces the droplet. It is shown that the optical nonlinearity can be "large" enough to have mechanical (ponderomotive) implications, that is, it allows control of the movement and position of micro-objects with submicrometer resolution. The optically induced molecular alignment controlled by the polarization and power of the laser tweezers allows one to actuate, rotate, and translate objects which are up to 10(3)-10(4) times larger than the constituent molecules themselves.