Opto-thermal manipulation with a 3†µm mid-infrared Er:ZBLAN fiber laser.

Water has significantly high absorption around 3 µm wavelength region, originated by its fundamental OH vibrational modes. Here, we successfully demonstrate an opto-thermal manipulation of particles utilizing a 3 µm mid-infrared Er:ZBLAN fiber laser (adjustable from 2700 to 2826 nm) that can efficiently elevate the temperature at a laser focus with a low laser power. The 3 µm laser indeed accelerates the formation of the particle assembly by simply irradiating the laser into water. By altering the laser wavelengths, the assembling speed and size, instantaneous particle velocity, particle distribution, trapping stiffness and temperature elevation are evaluated systematically. We propose that the dynamics of particle assembly can be understood through thermo-osmotic slip flows, taking into account the effects of volume heating within the focal cone and point heating at the focus.

Gaining control on optical force by the stimulated-emission resonance effect.

The resonance between an electronic transition of a micro/nanoscale object and an incident photon flux can modify the radiation force exerted on that object, especially at an interface. It has been theoretically proposed that a non-linear stimulated emission process can also induce an optical force, however its direction will be opposite to conventional photon scattering/absorption processes. In this work, we experimentally and theoretically demonstrate that a stimulated emission process can induce a repulsive pulling optical force on a single trapped dye-doped particle. Moreover, we successfully integrate both attractive pushing (excited state absorption) and repulsive pulling (stimulated emission) resonance forces to control the overall exerted optical force on an object, validating the proposed non-linear optical resonance theory. Indeed, the results presented here will enable the optical manipulation of the exerted optical force with exquisite control and ultimately enable single particle manipulation.

Mid-Infrared Optical Force Chromatography of Microspheres Containing Siloxane Bonds.

Recent interest in particle sorting using optical forces has grown due to its ability to separate micro- and nanomaterials based on their optical properties. Here, we present a mid-infrared optical force manipulation technique that enables precise sorting of microspheres based on their molecular vibrational properties using a mid-infrared quantum cascade laser. Utilizing the optical pushing force driven by a 9.3 µm mid-infrared evanescent field generated on a prism through total internal reflection, a variety of microspheres, including those composed of Si-O-Si bonds, can be separated in accordance with their absorbance values at 9.3 µm. The experimental results are in good agreement with the optical force calculations using finite-difference time-domain simulation. Thus, each microsphere's displacement and velocity can be predicted from the absorbance value; conversely, the optical properties (e.g., absorbance and complex refractive index in the mid-infrared region) of individual microspheres can be estimated by monitoring their velocity.

Unravelling 3D Dynamics and Hydrodynamics during Incorporation of Dielectric Particles to an Optical Trapping Site.

Mapping of the spatial and temporal motion of particles inside an optical field is critical for understanding and further improvement of the 3D spatio-temporal control over their optical trapping dynamics. However, it is not trivial to capture the 3D motion, and most imaging systems only capture a 2D projection of the 3D motion, in which the information about the axial movement is not directly available. In this work, we resolve the 3D incorporation trajectories of 200 nm fluorescent polystyrene particles in an optical trapping site under different optical experimental conditions using a recently developed widefield multiplane microscope (imaging volume of 50 × 50 × 4 µm3). The particles are gathered at the focus following some preferential 3D channels that show a shallow cone distribution. We demonstrate that the radial and the axial flow speed components depend on the axial distance from the focus, which is directly related to the scattering/gradient optical forces. While particle velocities and trajectories are mainly determined by the trapping laser profile, they cannot be completely explained without considering collective effects resulting from hydrodynamic forces.

The primeval optical evolving matter by optical binding inside and outside the photon beam.

Optical binding has recently gained considerable attention because it enables the light-induced assembly of many-body systems; however, this phenomenon has only been described between directly irradiated particles. Here, we demonstrate that optical binding can occur outside the focal spot of a single tightly focused laser beam. By trapping at an interface, we assemble up to three gold nanoparticles with a linear arrangement which fully-occupies the laser focus. The trapping laser is efficiently scattered by this linear alignment and interacts with particles outside the focus area, generating several discrete arc-shape potential wells with a half-wavelength periodicity. Those external nanoparticles inside the arcs show a correlated motion not only with the linear aligned particles, but also between themselves even both are not directly illuminated. We propose that the particles are optically bound outside the focal spot by the back-scattered light and multi-channel light scattering, forming a dynamic optical binding network.

Opto-thermophoretic trapping of micro and nanoparticles with a 2 µm Tm-doped fiber laser.

We propose a method for opto-thermophoretic trapping with a 2 µm Tm-doped fiber laser. The infrared continuous-wave laser beam is directly and strongly absorbed by water solution, and some local temperature gradient is generated around a focus. The particles are migrated along the temperature gradient, and form a hexagonal close-packed structure at a bottom-glass solution interface. On the other hand, the particles are not trapped in heavy water which does not absorb 2 µm light. The fact indicates that the local temperature elevation is the origin of this phenomenon. We have investigated the dependence of the phenomenon on the material, particle size, and laser power. To the best of our knowledge, 2 µm is the longest wavelength used for the opto-thermophoretic trapping.

Nanoparticle Assembling Dynamics Induced by Pulsed Optical Force.

Femtosecond (fs) laser trapping dynamics is summarized for silica, hydrophobically modified silica, and polystyrene nanoparticles (NPs) in aqueous solution, highlighting their distinct optical trapping dynamics under CW laser. Mutually repulsive silica nanoparticles are tightly confined under fs laser compared to CW laser trapping and, upon increasing laser power, they are ejected from the focus as an assembly. Hydrophobically modified silica and polystyrene (PS) NPs are sequentially ejected just like a stream or ablated, giving bubbles. The ejection and bubbling take place with the direction perpendicular to laser polarization and its direction is randomly switched from one to the other. These characteristic features are interpreted from the viewpoint of single assembly formation of NPs at an asymmetric position in the optical potential. Temporal change in optical forces map is prepared for a single PS NP by calculating scattering, gradient, and temporal forces. The relative contribution of the forces changes with the volume increase of the assembly and, when the pushing force along the trapping pulse propagation overcome the gradient in the focal plane, the assembly undergoes the ejection. Further fs multiphoton absorption is induced for the larger assembly leading to bubble generation. The assembling, ejection, and bubbling dynamics of NPs are characteristic features of pulsed optical force and are considered as a new platform for developing new material fabrication method.

Anomalously Large Assembly Formation of Polystyrene Nanoparticles by Optical Trapping at the Solution Surface.

We demonstrated the optical trapping-induced formation of a single large disc-like assembly (∼50 µm in diameter) of polystyrene (PS) nanoparticles (NPs) (100 nm in diameter) at a solution surface. Different from the conventional trapping behavior in solution, the assembly grows from the focus to the outside along the surface and contains needle structures expanding radially in all directions. Upon switching off the trapping laser, the assembly disperses and needle structures disappear, while the highly concentrated domain of the NPs is left for a while. The single assembly is quickly restored by switching on the laser again, where the needle structures are also reproduced but in a different way. When a single 10 µm PS microparticle (MP) is trapped in the NP solution, a single disc-like assembly containing needle structures is similarly prepared outside the MP. Based on backscattering imaging and tracking analyses of the MP at the solution surface, it is proposed that scattering and propagation of the trapping laser from the central part of the NP assembly or the MP lead to this new phenomenon.

Surface plasmon resonance effect on laser trapping and swarming of gold nanoparticles at an interface.

Laser trapping at an interface is a unique platform for aligning and assembling nanomaterials outside the focal spot. In our previous studies, Au nanoparticles form a dynamically evolved assembly outside the focus, leading to the formation of an antenna-like structure with their fluctuating swarms. Herein, we unravel the role of surface plasmon resonance on the swarming phenomena by tuning the trapping laser wavelength concerning the dipole mode for Au nanoparticles of different sizes. We clearly show that the swarm is formed when the laser wavelength is near to the resonance peak of the dipole mode together with an increase in the swarming area. The interpretation is well supported by the scattering spectra and the spatial light scattering profiles from single nanoparticle simulations. These findings indicate that whether the first trapped particle is resonant with trapping laser or not essentially determines the evolution of the swarming.

Large Submillimeter Assembly of Microparticles with Necklace-like Patterns Formed by Laser Trapping at Solution Surface.

In colloidal solution, nanoparticles can be optically trapped by a tightly focused laser beam, and they are assembled in a focal spot whose diameter is typically about one micrometer. We herein report that a large submillimeter sized assembly of polystyrene microparticles with necklace-like patterns are prepared by laser trapping at a solution surface. The light propagation outside the focal spot is directly confirmed by 1064 nm backscattering images, and finite difference time domain simulation well supports the idea that an optical potential is expanded outside the focal spot based on light propagation through whispering gallery mode. This demonstration opens a new method for fabrication of a millimeter-order huge assembly by a single tightly focused laser beam.

A Single Large Assembly with Dynamically Fluctuating Swarms of Gold Nanoparticles Formed by Trapping Laser.

Laser trapping has been utilized as tweezers to three-dimensionally trap nanoscale objects and has provided significant impacts in nanoscience and nanotechnology. The objects are immobilized at the position where the tightly focused laser beam is irradiated. Here, we report the swarming of gold nanoparticles in which component nanoparticles dynamically interact with each other, keeping their long interparticle distance around the trapping laser focus at a glass/solution interface. A pair of swarms are directionally extended outside the focal spot perpendicular to the linear polarization like a radiation pattern of dipole scattering, while a doughnut-shaped swarm is prepared by circularly polarized trapping laser. The light field is expanded as scattered light through trapped nanoparticles; this modified light field further traps the nanoparticles, and scattering and trapping cooperatively develop. Due to these nonlinear dynamic processes, the dynamically fluctuating swarms are evolved up to tens of micrometers. This finding will open the way to create various swarms of nanoscale objects that interact and bind through the scattered light depending on the properties of the laser beam and the nanomaterials.

Resonance optical trapping of individual dye-doped polystyrene particles with blue- and red-detuned lasers.

We demonstrate resonance optical trapping of individual dye-doped polystyrene particles with blue- and red-detuned lasers whose energy are higher and lower compared to electronic transition of the dye molecules, respectively. Through the measurement on how long individual particles are trapped at the focus, we here show that immobilization time of dye-doped particles becomes longer than that of bare ones. We directly confirm that the immobilization time of dye-doped particles trapped by the blue-detuned laser becomes longer than that by the red-detuned one. These findings are well interpreted by our previous theoretical proposal based on nonlinear optical response under intense laser field. It is discussed that the present result is an important step toward efficient and selective manipulation of molecules, quantum dots, nanoparticles, and various nanomaterials based on their quantum mechanical properties.

Optically Evolved Assembly Formation in Laser Trapping of Polystyrene Nanoparticles at Solution Surface.

Assembling dynamics of polystyrene nanoparticles by optical trapping is studied with utilizing transmission/reflection microscopy and reflection microspectroscopy. A single nanoparticle assembly with periodic structure is formed upon the focused laser irradiation at solution surface layer and continuously grows up to a steady state within few minutes. By controlling nanoparticle and salt concentrations in the colloidal solution, the assembling behavior is obviously changed. In the high concentration of nanoparticles, the assembly formation exhibits fast growth, gives large saturation size, and leads to dense packing structure. In the presence of salt, one assembly with the elongated aggregates was generated from the focal spot and 1064 nm trapping light was scattered outwardly with directions, while a small circular assembly and symmetrical expansion of the 1064 nm light were found without salt. The present nanoparticle assembling in optical trapping is driven through multiple scattering in gathered nanoparticles and directional scattering along the elongated aggregates derived from optical association of nanoparticles, which dynamic phenomenon is called optically evolved assembling. Repetitive trapping and release processes of nanoparticles between the assembly and the surrounding solution always proceed, and the steady state at the circular assembly formed by laser trapping is determined under optical and chemical equilibrium.

Optical Trapping-Formed Colloidal Assembly with Horns Extended to the Outside of a Focus through Light Propagation.

We report optical trapping and assembling of colloidal particles at a glass/solution interface with a tightly focused laser beam of high intensity. It is generally believed that the particles are gathered only in an irradiated area where optical force is exerted on the particles by laser beam. Here we demonstrate that, the propagation of trapping laser from the focus to the outside of the formed assembly leads to expansion of the assembly much larger than the irradiated area with sticking out rows of linearly aligned particles like horns. The shape of the assembly, its structure, and the number of horns can be controlled by laser polarization. Optical trapping study utilizing the light propagation will open a new avenue for assembling and crystallizing quantum dots, metal nanoparticles, molecular clusters, proteins, and DNA.

Resonance optical manipulation of nano-objects based on nonlinear optical response.

Optical manipulation is a technique to control the mechanical motion of small objects by using electromagnetic radiation force. Optical tweezers are the most popular tool to trap and move microparticles suspended in a medium. Recent interest has been shifting to manipulating nano-objects considerably smaller than the wavelength of light. Since the radiation force exerted on nano-objects is extremely small, an innovative method is necessary to make this concept feasible. Utilizing the resonant optical response of the objects to electronic transitions is one of the promising ways to approach nanoscale optical manipulation, and several advances in this direction have been made recently. Despite experimental studies on resonance optical tweezers showing favorable results, conventional theories have been unable to explain the results though demonstrations of resonant manipulations for traveling and standing waves have shown favorable results. In the present article, we provide a perspective view of resonance optical manipulation based on nonlinear optical response that we have recently proposed. This idea coherently elucidates recently reported puzzling phenomena appearing in studies concerning resonance optical tweezers that contradict the conventional understanding of resonance optical trapping. Further, this concept opens up the possibility to develop potentially powerful manipulation techniques because the nonlinear optical response involves processes with considerably greater degrees of freedom than those of the linear optical response. As examples, we propose a method for trapping single organic molecules that is more effective than ever before, selectively pulling the molecules with a particular transition energy, and our proposed method allows for high-spatial-resolution optical manipulation beyond the diffraction limit.

Proposed nonlinear resonance laser technique for manipulating nanoparticles.

We propose nonlinear resonant laser manipulation, a technique that drastically enhances the number of degrees of freedom when manipulating nano-objects. Considering the high laser intensity required to trap single molecules, we calculate the radiation force exerted on a molecule in a focused laser beam by solving the density matrix equations using the nonperturbative method. The results coherently elucidate certain recently reported puzzling phenomena that contradict the conventional understanding of laser trapping. Further, we demonstrate unconventional forms of laser manipulations using "stimulated recoil force" and "subwavelength laser manipulation."