Thermo-Electro-Mechanics at Individual Particles in Complex Colloidal Systems

It has been well established that thermoelectric (TE) field can arise from different Soret coefficients of salt ions in aqueous solution under constant temperature gradient. Despite their high relevance to cellular biology and particle manipulations, understanding and controlling of TE field in complex colloidal systems that involve micro/nanoparticles, salt ions, and molecules have remained challenging. In such colloidal systems, challenge arises from the thermal interactions with charged micro/nanoparticles that distort the TE field around the particles. Herein, we provide a framework for TE field in colloidal suspensions with various ions and surfactants at the single-nanoparticle level. In particular, we reveal the spatial variation of TE field around a dielectric particle under temperature gradient to determine the thermoelectric trapping force on the particle. Our theoretical results on the trapping stiffness predicted from the TE force profile match well with the experimental optothermoelectric trapping stiffness of particles in the solutions where the temperature gradient was well controlled by a laser beam. With insights into the TE field and force in complex systems, our framework and methodology can be extended to engineer the TE field for versatile optothermoelectric manipulations of arbitrarily shaped particles with nonuniform surface morphology and to advance the scientific research in cellular biology

Opto-Thermophoretic Manipulation and Construction of Colloidal Superstructures in Photocurable Hydrogels

Light-based manipulation of colloidal particles holds great promise in fabrication of functional devices. Construction of complex colloidal superstructures using traditional optical tweezers is limited by high operation power and strong heating effect. Herein, we demonstrate low-power opto-thermophoretic manipulation and construction of colloidal superstructures in photocurable hydrogels. By introducing cationic surfactants into a hydrogel solution under a light-directed temperature field, we create both thermoelectric fields and depletion attraction forces to control the suspended colloidal particles. The particles of various sizes and compositions are thus trapped and organized into various superstructures. Furthermore, the colloidal superstructures are immobilized and patterned onto solid-state substrates through UV-induced photopolymerization of the hydrogel. Our opto-thermophoretic technique will open up avenues for bottom-up assembly of colloidal materials and devices

Opto-Thermophoretic Manipulation and Construction of Colloidal Superstructures in Photocurable Hydrogels

Light-based manipulation of colloidal particles holds great promise in fabrication of functional devices. Construction of complex colloidal superstructures using traditional optical tweezers is limited by high operation power and strong heating effect. Herein, we demonstrate low-power opto-thermophoretic manipulation and construction of colloidal superstructures in photocurable hydrogels. By introducing cationic surfactants into a hydrogel solution under a light-directed temperature field, we create both thermoelectric fields and depletion attraction forces to control the suspended colloidal particles. The particles of various sizes and compositions are thus trapped and organized into various superstructures. Furthermore, the colloidal superstructures are immobilized and patterned onto solid-state substrates through UV-induced photopolymerization of the hydrogel. Our opto-thermophoretic technique will open up avenues for bottom-up assembly of colloidal materials and devices

Opto-Thermophoretic Attraction, Trapping, and Dynamic Manipulation of Lipid Vesicles

Lipid vesicles are important biological assemblies, which are critical to biological transport processes, and vesicles prepared in the lab are a workhorse for studies of drug delivery, protein unfolding, biomolecular interactions, compartmentalized chemistry, and stimuli-responsive sensing. The current method of using optical tweezers for holding lipid vesicles in place for single-vesicle studies suffers from limitations such as high optical power, rigorous optics, and small difference in the refractive indices of vesicles and water. Herein, we report the use of plasmonic heating to trap vesicles in a temperature gradient, allowing long-range attraction, parallel trapping, and dynamic manipulation. The capabilities and limitations with respect to thermal effects on vesicle structure and optical spectroscopy are discussed. This simple approach allows vesicle manipulation using down to 3 orders of magnitude lower optical power and at least an order of magnitude higher trapping stiffness per unit power than traditional optical tweezers while using a simple optical setup. In addition to the benefit provided by the relaxation of these technical constraints, this technique can complement optical tweezers to allow detailed studies on thermophoresis of optically trapped vesicles and effects of locally generated thermal gradients on the physical properties of lipid vesicles. Finally, the technique itself and the large-scale collection of vesicles have huge potential for future studies of vesicles relevant to detection of exosomes, lipid-raft formation, and other areas relevant to the life sciences

Opto-Thermophoretic Manipulation and Construction of Colloidal Superstructures in Photocurable Hydrogels

Light-based manipulation of colloidal particles holds great promise in fabrication of functional devices. Construction of complex colloidal superstructures using traditional optical tweezers is limited by high operation power and strong heating effect. Herein, we demonstrate low-power opto-thermophoretic manipulation and construction of colloidal superstructures in photocurable hydrogels. By introducing cationic surfactants into a hydrogel solution under a light-directed temperature field, we create both thermoelectric fields and depletion attraction forces to control the suspended colloidal particles. The particles of various sizes and compositions are thus trapped and organized into various superstructures. Furthermore, the colloidal superstructures are immobilized and patterned onto solid-state substrates through UV-induced photopolymerization of the hydrogel. Our opto-thermophoretic technique will open up avenues for bottom-up assembly of colloidal materials and devices

Photoswitchable Rabi Splitting in Hybrid Plasmon–Waveguide Modes

Rabi splitting that arises from strong plasmon–molecule coupling has attracted tremendous interests. However, it has remained elusive to integrate Rabi splitting into the hybrid plasmon–waveguide modes (HPWMs), which have advantages of both subwavelength light confinement of surface plasmons and long-range propagation of guided modes in dielectric waveguides. Herein, we explore a new type of HPWMs based on hybrid systems of Al nanodisk arrays covered by PMMA thin films that are doped with photochromic molecules and demonstrate the photoswitchable Rabi splitting with a maximum splitting energy of 572 meV in the HPWMs by controlling the photoisomerization of the molecules. Through our experimental measurements combined with finite-difference time-domain (FDTD) simulations, we reveal that the photoswitchable Rabi splitting arises from the switchable coupling between the HPWMs and molecular excitons. By harnessing the photoswitchable Rabi splitting, we develop all-optical light modulators and rewritable waveguides. The demonstration of Rabi splitting in the HPWMs will further advance scientific research and device applications of hybrid plasmon–molecule systems

Thermophoretic Tweezers for Low-Power and Versatile Manipulation of Biological Cells

Optical manipulation of biological cells and nanoparticles is significantly important in life sciences, early disease diagnosis, and nanomanufacturing. However, low-power and versatile all-optical manipulation has remained elusive. Herein, we have achieved light-directed versatile thermophoretic manipulation of biological cells at an optical power 100–1000 times lower than that of optical tweezers. By harnessing the permittivity gradient in the electric double layer of the charged surface of the cell membrane, we succeed at the low-power trapping of suspended biological cells within a light-controlled temperature gradient field. Furthermore, through dynamic control of optothermal potentials using a digital micromirror device, we have achieved arbitrary spatial arrangements of cells at a resolution of ∼100 nm and precise rotation of both single and assemblies of cells. Our thermophoretic tweezers will find applications in cellular biology, nanomedicine, and tissue engineering

Optothermophoretic Manipulation of Colloidal Particles in Nonionic Liquids

The response of colloidal particles to a light-controlled external temperature field can be harnessed for optothermophoretic manipulation of the particles. The thermoelectric effect is regarded as the driving force for thermophoretic trapping of particles at the light-irradiated hot region, which is thus limited to ionic liquids. Herein, we achieve optothermophoretic manipulation of colloidal particles in various nonionic liquids, including water, ethanol, isopropyl alcohol, and 1-butanol, and establish the physical mechanism of the manipulation at the molecular level. We reveal that the nonionic driving force originates from a layered structure of solvent molecules at the particle–solvent interface, which is supported by molecular dynamics simulations. Furthermore, the effects of hydrophilicity, solvent type, and ionic strength on the layered interfacial structures and thus the trapping stability of particles are investigated, providing molecular-level insight into thermophoresis and guidance on interfacial engineering for optothermal manipulation

Optothermophoretic Manipulation of Colloidal Particles in Nonionic Liquids

The response of colloidal particles to a light-controlled external temperature field can be harnessed for optothermophoretic manipulation of the particles. The thermoelectric effect is regarded as the driving force for thermophoretic trapping of particles at the light-irradiated hot region, which is thus limited to ionic liquids. Herein, we achieve optothermophoretic manipulation of colloidal particles in various nonionic liquids, including water, ethanol, isopropyl alcohol, and 1-butanol, and establish the physical mechanism of the manipulation at the molecular level. We reveal that the nonionic driving force originates from a layered structure of solvent molecules at the particle–solvent interface, which is supported by molecular dynamics simulations. Furthermore, the effects of hydrophilicity, solvent type, and ionic strength on the layered interfacial structures and thus the trapping stability of particles are investigated, providing molecular-level insight into thermophoresis and guidance on interfacial engineering for optothermal manipulation