Rahul P. Trivedi

Optical manipulation of colloids and defect structures in anisotropic liquid crystal fluids

Optical trapping in anisotropic fluids such as liquid crystals shows inherently different behavior compared to that in isotropic media. Anisotropic optical and visco-elastic properties of these materials result in direction-sensitive and polarization-dependent interaction of the focused laser beam with colloidal inclusions, defects and structures of long-range molecular order, providing new means of non-contact optical control. Optical trapping properties are further enriched by laser-induced realignment of the optical axis that can be observed in these liquid crystalline materials at relatively low trapping laser powers. Optical manipulation of particles and defects in these anisotropic fluids is of immense importance for their fundamental study and from the standpoint of technological applications such as light-directed colloidal self-assembly and generation of tunable photonic architectures in liquid crystals. We review the basic physical mechanisms related to optical trapping in anisotropic liquid crystalline fluids and demonstrate how it can be employed in quantitative studies of colloidal interactions and both topological and mechanical properties of defects.

Multimodal nonlinear optical polarizing microscopy of long-range molecular order in liquid crystals

We demonstrate orientation-sensitive multimodal nonlinear optical polarizing microscopy capable of probing orientational, polar, and biaxial features of mesomorphic ordering in soft matter. This technique achieves simultaneous imaging in broadband coherent anti-Stokes Raman scattering, multiphoton excitation fluorescence, and multiharmonic generation polarizing microscopy modes and is based on the use of a single femtosecond laser and a photonic crystal fiber as sources of the probing light. We show the viability of this technique for mapping of three-dimensional patterns of molecular orientations and show that images obtained in different microscopy modes are consistent with each other.

Three-dimensional parallel particle manipulation and tracking by integrating holographic optical tweezers and engineered point spread functions

We demonstrate an integrated holographic optical tweezers system with double-helix point spread function (DH-PSF) imaging for high precision three-dimensional multi-particle tracking. The tweezers system allows for the creation and control of multiple optical traps in three-dimensions, while the DH-PSF allows for high precision, 3D, multiple-particle tracking in a wide field. The integrated system is suitable for particles emitting/scattering either coherent or incoherent light and is easily adaptable to existing holographic tweezers systems. We demonstrate simultaneous tracking of multiple micro-manipulated particles and perform quantitative estimation of the lateral and axial forces in an optical trap by measuring the fluid drag force exerted on the particles. The system is thus capable of unveiling complex 3D force landscapes that make it suitable for quantitative studies of interactions in colloidal systems, biological materials, and a variety of soft matter systems.

Three dimensional optical manipulation and structural imaging of soft materials by use of laser tweezers and multimodal nonlinear microscopy

We develop an integrated system of holographic optical trapping and multimodal nonlinear microscopy and perform simultaneous three-dimensional optical manipulation and non-invasive structural imaging of composite soft-matter systems. We combine different nonlinear microscopy techniques such as coherent anti-Stokes Raman scattering, multi-photon excitation fluorescence and multi-harmonic generation, and use them for visualization of long-range molecular order in soft materials by means of their polarized excitation and detection. The combined system enables us to accomplish manipulation in composite soft materials such as colloidal inclusions in liquid crystals as well as imaging of each separate constituents of the composite material in different nonlinear optical modalities. We also demonstrate optical generation and control of topological defects and simultaneous reconstruction of their three-dimensional long-range molecular orientational patterns from the nonlinear optical images.

Reconfigurable interactions and three-dimensional patterning of colloidal particles and defects in lamellar soft media

Colloidal systems find important applications ranging from fabrication of photonic crystals to direct probing of phenomena typically encountered in atomic crystals and glasses. New applications—such as nanoantennas, plasmonic sensors, and nanocircuits—pose a challenge of achieving sparse colloidal assemblies with tunable interparticle separations that can be controlled at will. We demonstrate reconfigurable multiscale interactions and assembly of colloids mediated by defects in cholesteric liquid crystals that are probed by means of laser manipulation and three-dimensional imaging. We find that colloids attract via distance-independent elastic interactions when pinned to the ends of cholesteric oily streaks, line defects at which one or more layers are interrupted. However, dislocations and oily streaks can also be optically manipulated to induce kinks, allowing one to lock them into the desired configurations that are stabilized by elastic energy barriers for structural transformation of the particle-connecting defects. Under the influence of elastic energy landscape due to these defects, sublamellar-sized colloids self-assemble into structures mimicking the cores of dislocations and oily streaks. Interactions between these defect-embedded colloids can be varied from attractive to repulsive by optically introducing dislocation kinks. The reconfigurable nature of defect–particle interactions allows for patterning of defects by manipulation of colloids and, in turn, patterning of particles by these defects, thus achieving desired colloidal configurations on scales ranging from the size of defect core to the sample size. This defect-colloidal sculpturing may be extended to other lamellar media, providing the means for optically guided self-assembly of mesoscopic composites with predesigned properties.

Three-dimensional imaging of liquid crystal structures and defects by means of holographic manipulation of colloidal nanowires with faceted sidewalls

We use nanowires with faceted sidewalls for mapping of the patterns of three-dimensional orientational order and defect structures. In chiral nematics, the nanowires follow the local average orientation of rod-shaped molecules. When spatially translated by use of holographic optical tweezers in three dimensions, they mediate direct nondestructive visualization of the helicoidal ground-state structures, edge and screw dislocations, and kinks, as well as enable non-contact manipulation of these defects. We probe interactions of faceted nanowires with different defects and demonstrate their spontaneous self-alignment along the cores of singular defect lines.

Unconventional structure-assisted optical manipulation of high-index nanowires in liquid crystals

Stable optical trapping and manipulation of high-index particles in low-index host media is often impossible due to the dominance of scattering forces over gradient forces. Here we explore optical manipulation in liquid crystalline structured hosts and show that robust optical manipulation of high-index particles, such as GaN nanowires, is enabled by laser-induced distortions in long-range molecular alignment, via coupling of translational and rotational motions due to helicoidal molecular arrangement, or due to elastic repulsive interactions with confining substrates. Anisotropy of the viscoelastic liquid crystal medium and particle shape give rise to a number of robust unconventional trapping capabilities, which we use to characterize defect structures and study rheological properties of various thermotropic liquid crystals.

Non-contact optical control of multiple particles and defects using holographic optical trapping with phase-only liquid crystal spatial light modulator

In this work, three-dimensional manipulation of multiple defects and structures is performed in the framework of holographic optical trapping approach using a spatial light modulator. A holographic optical tweezers system is constructed using a liquid crystal spatial light modulator to generate multiple optical traps. We optimize the tweezers setup to perform polarization-sensitive holographic optical trapping and then explore properties of optical trapping in thermotropic liquid crystals and compare them to the case of isotropic fluids. One of the major challenges complicating the quantitative measurements in these fluids is the anisotropic nature of the liquid crystal medium, which makes the tight focusing of the laser beam difficult and considerably weakens optical trapping forces. Using liquid crystals with low birefringence allows us to mitigate these artefacts. Optical trapping forces and the trap stiffness are first calibrated for different laser powers using viscous drag forces. This is then used to probe inter-particle and defect-particle interaction forces as well as to characterize tension of line defects in the bulk of liquid crystals.

Nonsingular defects and self-assembly of colloidal particles in cholesteric liquid crystals

Cholesteric liquid crystals can potentially provide a means for tunable self-organization of colloidal particles. However, the structures of particle-induced defects and the ensuing elasticity-mediated colloidal interactions in these media remain much less explored and understood as compared to their nematic liquid crystal counterparts. Here we demonstrate how colloidal microspheres of varying diameter relative to the helicoidal pitch can induce dipolelike director field configurations in cholesteric liquid crystals, where these particles are accompanied by point defects and a diverse variety of nonsingular line defects forming closed loops. Using laser tweezers and nonlinear optical microscopy, we characterize the ensuing medium-mediated elastic interactions and three-dimensional colloidal assemblies. Experimental findings show a good agreement with numerical modeling based on minimization of the Landau-de Gennes free energy and promise both practical applications in the realization of colloidal composite materials and a means of controlling nonsingular topological defects that attract a great deal of fundamental interest.

Engineered point spread functions for 3D parallel particle tracking of optically trapped particles

We integrate a holographic optical tweezer system with a double-helix point spread function imaging for high precision three-dimensional (3D) multi-particle tracking. We perform precise quantitative estimates of the 3D forces in an optical trap.