Three-Dimensional Optothermal Manipulation of Light-Absorbing Particles in Phase-Change Gel Media.

Rational manipulation and assembly of discrete colloidal particles into architected superstructures have enabled several applications in materials science and nanotechnology. Optical manipulation techniques, typically operated in fluid media, facilitate the precise arrangement of colloidal particles into superstructures by using focused laser beams. However, as the optical energy is turned off, the inherent Brownian motion of the particles in fluid media impedes the retention and reconfiguration of such superstructures. Overcoming this fundamental limitation, we present on-demand, three-dimensional (3D) optical manipulation of colloidal particles in a phase-change solid medium made of surfactant bilayers. Unlike liquid crystal media, the lack of fluid flow within the bilayer media enables the assembly and retention of colloids for diverse spatial configurations. By utilizing the optically controlled temperature-dependent interactions between the particles and their surrounding media, we experimentally exhibit the holonomic microscale control of diverse particles for repeatable, reconfigurable, and controlled colloidal arrangements in 3D. Finally, we demonstrate tunable light-matter interactions between the particles and 2D materials by successfully manipulating and retaining these particles at fixed distances from the 2D material layers. Our experimental results demonstrate that the particles can be retained for over 120 days without any change in their relative positions or degradation in the bilayers. With the capability of arranging particles in 3D configurations with long-term stability, our platform pushes the frontiers of optical manipulation for distinct applications such as metamaterial fabrication, information storage, and security.

Synchronous and Fully Steerable Active Particle Systems for Enhanced Mimicking of Collective Motion in Nature.

The collective motion observed in living active matter, such as fish schools and bird flocks, is characterized by its dynamic and complex nature, involving various moving states and transitions. By tailoring physical interactions or incorporating information exchange capabilities, inanimate active particles can exhibit similar behavior. However, the lack of synchronous and arbitrary control over individual particles hinders their use as a test system for the study of more intricate collective motions in living species. Herein, a novel optical feedback control system that enables the mimicry of collective motion observed in living objects using active particles is proposed. This system allows for the experimental investigation of the velocity alignment, a seminal model of collective motion (known as the Vicsek model), in a microscale perturbed environment with controllable and realistic conditions. The spontaneous formation of different moving states and dynamic transitions between these states is observed. Additionally, the high robustness of the active-particle group at the critical density under the influence of different perturbations is quantitatively validated. These findings support the effectiveness of velocity alignment in real perturbed environments, thereby providing a versatile platform for fundamental studies on collective motion and the development of innovative swarm microrobotics.

Hypothermal opto-thermophoretic tweezers.

Optical tweezers have profound importance across fields ranging from manufacturing to biotechnology. However, the requirement of refractive index contrast and high laser power results in potential photon and thermal damage to the trapped objects, such as nanoparticles and biological cells. Optothermal tweezers have been developed to trap particles and biological cells via opto-thermophoresis with much lower laser powers. However, the intense laser heating and stringent requirement of the solution environment prevent their use for general biological applications. Here, we propose hypothermal opto-thermophoretic tweezers (HOTTs) to achieve low-power trapping of diverse colloids and biological cells in their native fluids. HOTTs exploit an environmental cooling strategy to simultaneously enhance the thermophoretic trapping force at sub-ambient temperatures and suppress the thermal damage to target objects. We further apply HOTTs to demonstrate the three-dimensional manipulation of functional plasmonic vesicles for controlled cargo delivery. With their noninvasiveness and versatile capabilities, HOTTs present a promising tool for fundamental studies and practical applications in materials science and biotechnology.

Multimodal Optothermal Manipulations along Various Surfaces.

Optical tweezers have provided tremendous opportunities for fundamental studies and applications in the life sciences, chemistry, and physics by offering contact-free manipulation of small objects. However, it requires sophisticated real-time imaging and feedback systems for conventional optical tweezers to achieve controlled motion of micro/nanoparticles along textured surfaces, which are required for such applications as high-resolution near-field characterizations of cell membranes with nanoparticles as probes. In addition, most optical tweezers systems are limited to single manipulation modes, restricting their broader applications. Herein, we develop an optothermal platform that enables the multimodal manipulation of micro/nanoparticles along various surfaces. Specifically, we achieve the manipulation of micro/nanoparticles through the synergy between the optical and thermal forces, which arise due to the temperature gradient self-generated by the particles absorbing the light. With a simple control of the laser beam, we achieve five switchable working modes [i.e., tweezing, rotating, rolling (toward), rolling (away), and shooting] for the versatile manipulation of both synthesized particles and biological cells along various substrates. More interestingly, we realize the manipulation of micro/nanoparticles on rough surfaces of live worms and their embryos for localized control of biological functions. By enabling the three-dimensional control of micro/nano-objects along various surfaces, including topologically uneven biological tissues, our multimodal optothermal platform will become a powerful tool in life sciences, nanotechnology, and colloidal sciences.

Optical Manipulation Heats up: Present and Future of Optothermal Manipulation.

Optothermal manipulation is a versatile technique that combines optical and thermal forces to control synthetic micro-/nanoparticles and biological entities. This emerging technique overcomes the limitations of traditional optical tweezers, including high laser power, photon and thermal damage to fragile objects, and the requirement of refractive-index contrast between target objects and the surrounding solvents. In this perspective, we discuss how the rich opto-thermo-fluidic multiphysics leads to a variety of working mechanisms and modes of optothermal manipulation in both liquid and solid media, underpinning a broad range of applications in biology, nanotechnology, and robotics. Moreover, we highlight current experimental and modeling challenges in the pursuit of optothermal manipulation and propose future directions and solutions to the challenges.

Hypothermal opto-thermophoretic tweezers.

Optical tweezers have profound importance across fields ranging from manufacturing to biotechnology. However, the requirement of refractive index contrast and high laser power results in potential photon and thermal damage to the trapped objects, such as nanoparticles and biological cells. Optothermal tweezers have been developed to trap particles and biological cells via opto-thermophoresis with much lower laser powers. However, the intense laser heating and stringent requirement of the solution environment prevent their use for general biological applications. Here, we propose hypothermal opto-thermophoretic tweezers (HOTTs) to achieve low-power trapping of diverse colloids and biological cells in their native fluids. HOTTs exploit an environmental cooling strategy to simultaneously enhance the thermophoretic trapping force at sub-ambient temperatures and suppress the thermal damage to target objects. We further apply HOTTs to demonstrate the three-dimensional manipulation of functional plasmonic vesicles for controlled cargo delivery. With their noninvasiveness and versatile capabilities, HOTTs present a promising tool for fundamental studies and practical applications in materials science and biotechnology.

Tunable Strong Coupling in Transition Metal Dichalcogenide Nanowires.

Subwavelength optical resonators with spatiotemporal control of light are essential to the miniaturization of optical devices. In this work, chemically synthesized transition metal dichalcogenide (TMDC) nanowires are exploited as a new type of dielectric nanoresonators to simultaneously support pronounced excitonic and Mie resonances. Strong light-matter couplings and tunable exciton polaritons in individual nanowires are demonstrated. In addition, the excitonic responses can be reversibly modulated with excellent reproducibility, offering the potential for developing tunable optical nanodevices. Being in the mobile colloidal state with highly tunable optical properties, the TMDC nanoresonators will find promising applications in integrated active optical devices, including all-optical switches and sensors.

Programmable Multimodal Optothermal Manipulation of Synthetic Particles and Biological Cells.

Optical manipulation of tiny objects has benefited many research areas ranging from physics to biology to micro/nanorobotics. However, limited manipulation modes, intense lasers with complex optics, and applicability to limited materials and geometries of objects restrict the broader uses of conventional optical tweezers. Herein, we develop an optothermal platform that enables the versatile manipulation of synthetic micro/nanoparticles and live cells using an ultralow-power laser beam and a simple optical setup. Five working modes (i.e., printing, tweezing, rotating, rolling, and shooting) have been achieved and can be switched on demand through computer programming. By incorporating a feedback control system into the platform, we realize programmable multimodal control of micro/nanoparticles, enabling autonomous micro/nanorobots in complex environments. Moreover, we demonstrate in situ three-dimensional single-cell surface characterizations through the multimodal optothermal manipulation of live cells. This programmable multimodal optothermal platform will contribute to diverse fundamental studies and applications in cellular biology, nanotechnology, robotics, and photonics.

Universal optothermal micro/nanoscale rotors.

Rotation of micro/nano-objects is important for micro/nanorobotics, three-dimensional imaging, and lab-on-a-chip systems. Optical rotation techniques are especially attractive because of their fuel-free and remote operation. However, current techniques require laser beams with designed intensity profile and polarization or objects with sophisticated shapes or optical birefringence. These requirements make it challenging to use simple optical setups for light-driven rotation of many highly symmetric or isotropic objects, including biological cells. Here, we report a universal approach to the out-of-plane rotation of various objects, including spherically symmetric and isotropic particles, using an arbitrary low-power laser beam. Moreover, the laser beam is positioned away from the objects to reduce optical damage from direct illumination. The rotation mechanism based on opto-thermoelectrical coupling is elucidated by rigorous experiments combined with multiscale simulations. With its general applicability and excellent biocompatibility, our universal light-driven rotation platform is instrumental for various scientific research and engineering applications.

Opto-Thermocapillary Nanomotors on Solid Substrates.

Motors that can convert different forms of energy into mechanical work are of profound importance to the development of human societies. The evolution of micromotors has stimulated many advances in drug delivery and microrobotics for futuristic applications in biomedical engineering and nanotechnology. However, further miniaturization of motors toward the nanoscale is still challenging because of the strong Brownian motion of nanomotors in liquid environments. Here, we develop light-driven opto-thermocapillary nanomotors (OTNM) operated on solid substrates where the interference of Brownian motion is effectively suppressed. Specifically, by optically controlling particle-substrate interactions and thermocapillary actuation, we demonstrate the robust orbital rotation of 80 nm gold nanoparticles around a laser beam on a solid substrate. With on-chip operation capability in an ambient environment, our OTNM can serve as light-driven engines to power functional devices at the nanoscale.

Bubble-pen lithography: Fundamentals and applications: Nanoscience: Special Issue Dedicated to Professor Paul S. Weiss.

Developing on-chip functional devices requires reliable fabrication methods with high resolution for miniaturization, desired components for enhanced performance, and high throughput for fast prototyping and mass production. Recently, laser-based bubble-pen lithography (BPL) has been developed to enable sub-micron linewidths, in situ synthesis of custom materials, and on-demand patterning for various functional components and devices. BPL exploits Marangoni convection induced by a laser-controlled microbubble to attract, accumulate, and immobilize particles, ions, and molecules onto different substrates. Recent years have witnessed tremendous progress in theory, engineering, and application of BPL, which motivated us to write this review. First, an overview of experimental demonstrations and theoretical understandings of BPL is presented. Next, we discuss the advantages of BPL and its diverse applications in quantum dot displays, biological and chemical sensing, clinical diagnosis, nanoalloy synthesis, and microrobotics. We conclude this review with our perspective on the challenges and future directions of BPL.

Opto-refrigerative tweezers.

Optical tweezers offer revolutionary opportunities for both fundamental and applied research in materials science, biology, and medical engineering. However, the requirement of a strongly focused and high-intensity laser beam results in potential photon-induced and thermal damages to target objects, including nanoparticles, cells, and biomolecules. Here, we report a new type of light-based tweezers, termed opto-refrigerative tweezers, which exploit solid-state optical refrigeration and thermophoresis to trap particles and molecules at the laser-generated cold region. While laser refrigeration can avoid photothermal heating, the use of a weakly focused laser beam can further reduce the photodamages to the target object. This novel and noninvasive optical tweezing technique will bring new possibilities in the optical control of nanomaterials and biomolecules for essential applications in nanotechnology, photonics, and life science.

Label-Free Ultrasensitive Detection of Abnormal Chiral Metabolites in Diabetes.

Homochirality is necessary for normal biochemical processes in humans. Abnormal amounts of chiral molecules in biofluids have been found in patients with diabetes. However, the detailed analysis of diabetes-related abnormal chirality in biofluids and its potential use for clinical applications have been hindered by the difficulty in detecting and monitoring the chiral changes in biofluids, due to their low molar mass and trace concentrations. Herein, we demonstrate the label-free detection of chiral molecules using only 10 µL with 107-fold enhancement in sensitivity compared with traditional plasmonic chiral metamaterials. The ultrahigh sensitivity and low sample consumption were enabled by microbubble-induced rapid accumulation of biomolecules on plasmonic chiral sensors. We have applied our technique on mouse and human urine samples, uncovering the previously undetectable diabetes-induced abnormal dextrorotatory shift in chirality of urine metabolites. Furthermore, the accumulation-assisted plasmonic chiral sensing achieved a diagnostic accuracy of 84% on clinical urine samples from human patients. With the ultrahigh sensitivity, ultralow sample consumption, and fast response, our technique will benefit diabetes research and could be developed as point-of-care devices for first-line noninvasive screening and prognosis of prediabetes or diabetes and its complications.

Light-Driven Magnetic Encoding for Hybrid Magnetic Micromachines.

Remote manipulation of a micromachine under an external magnetic field is significant in a variety of applications. However, magnetic manipulation requires that either the target objects or the fluids should be ferromagnetic or superparamagnetic. To extend the applicability, we propose a versatile optical printing technique termed femtosecond laser-directed bubble microprinting (FsLDBM) for on-demand magnetic encoding. Harnessing Marangoni convection, evaporation flow, and capillary force for long-distance delivery, near-field attraction, and printing, respectively, FsLDBM is capable of printing nanomaterials on the solid-state substrate made of arbitrary materials. As a proof-of-concept, we actuate a 3D polymer microturbine under a rotating magnetic field by implementing γ-Fe2O3 nanomagnets on its blade. Moreover, we demonstrate the magnetic encoding on a living daphnia and versatile manipulation of the hybrid daphnia. With its general applicability, the FsLDBM approach provides opportunities for magnetic control of general microstructures in a variety of applications, such as smart microbots and biological microsurgery.

Liquid Optothermoelectrics: Fundamentals and Applications.

Liquid thermoelectricity describes the redistribution of ions in an electrolytic solution under the influence of temperature gradients, which leads to the formation of electric fields. The thermoelectric field is effective in driving the thermophoretic migration of charged colloidal particles for versatile manipulation. However, traditional macroscopic thermoelectric fields are not suitable for particle manipulations at high spatial resolution. Inspired by optical tweezers and relevant optical manipulation techniques, we employ laser interaction with light-absorbing nanostructures to achieve subtle heat management on the micro- and nanoscales. The resulting thermoelectric fields are exploited to develop new optical technologies, leading to a research field known as liquid optothermoelectrics. This Invited Feature Article highlights our recent works on advancing fundamentals, technologies, and applications of optothermoelectrics in colloidal solutions. The effects of light irradiation, substrates, electrolytes, and particles on the optothermoelectric manipulations of colloidal particles along with their theoretical limitations are discussed in detail. Our optothermoelectric technologies with the versatile capabilities of trapping, manipulating, and pulling colloidal particles at low optical power are finding applications in microswimmers and nanoscience. With its intricate interfacial processes and tremendous technological promise, optothermoelectrics in colloidal solutions will remain relevant for the foreseeable future.

Atomistic modeling and rational design of optothermal tweezers for targeted applications.

Optical manipulation of micro/nanoscale objects is of importance in life sciences, colloidal science, and nanotechnology. Optothermal tweezers exhibit superior manipulation capability at low optical intensity. However, our implicit understanding of the working mechanism has limited the further applications and innovations of optothermal tweezers. Herein, we present an atomistic view of opto-thermo-electro-mechanic coupling in optothermal tweezers, which enables us to rationally design the tweezers for optimum performance in targeted applications. Specifically, we have revealed that the non-uniform temperature distribution induces water polarization and charge separation, which creates the thermoelectric field dominating the optothermal trapping. We further design experiments to systematically verify our atomistic simulations. Guided by our new model, we develop new types of optothermal tweezers of high performance using low-concentrated electrolytes. Moreover, we demonstrate the use of new tweezers in opto-thermophoretic separation of colloidal particles of the same size based on the difference in their surface charge, which has been challenging for conventional optical tweezers. With the atomistic understanding that enables the performance optimization and function expansion, optothermal tweezers will further their impacts.

Opto-thermoelectric microswimmers.

Inspired by the "run-and-tumble" behaviours of Escherichia coli (E. coli) cells, we develop opto-thermoelectric microswimmers. The microswimmers are based on dielectric-Au Janus particles driven by a self-sustained electrical field that arises from the asymmetric optothermal response of the particles. Upon illumination by a defocused laser beam, the Janus particles exhibit an optically generated temperature gradient along the particle surfaces, leading to an opto-thermoelectrical field that propels the particles. We further discover that the swimming direction is determined by the particle orientation. To enable navigation of the swimmers, we propose a new optomechanical approach to drive the in-plane rotation of Janus particles under a temperature-gradient-induced electrical field using a focused laser beam. Timing the rotation laser beam allows us to position the particles at any desired orientation and thus to actively control the swimming direction with high efficiency. By incorporating dark-field optical imaging and a feedback control algorithm, we achieve automated propelling and navigation of the microswimmers. Our opto-thermoelectric microswimmers could find applications in the study of opto-thermoelectrical coupling in dynamic colloidal systems, active matter, biomedical sensing, and targeted drug delivery.

Opto-thermoelectric pulling of light-absorbing particles.

Optomechanics arises from the photon momentum and its exchange with low-dimensional objects. It is well known that optical radiation exerts pressure on objects, pushing them along the light path. However, optical pulling of an object against the light path is still a counter-intuitive phenomenon. Herein, we present a general concept of optical pulling-opto-thermoelectric pulling (OTEP)-where the optical heating of a light-absorbing particle using a simple plane wave can pull the particle itself against the light path. This irradiation orientation-directed pulling force imparts self-restoring behaviour to the particles, and three-dimensional (3D) trapping of single particles is achieved at an extremely low optical intensity of 10-2 mW µm-2. Moreover, the OTEP force can overcome the short trapping range of conventional optical tweezers and optically drive the particle flow up to a macroscopic distance. The concept of self-induced opto-thermomechanical coupling is paving the way towards freeform optofluidic technology and lab-on-a-chip devices.

Optical Patterning of Two-Dimensional Materials.

Recent advances in the field of two-dimensional (2D) materials have led to new electronic and photonic devices enabled by their unique properties at atomic thickness. Structuring 2D materials into desired patterns on substrates is often an essential and foremost step for the optimum performance of the functional devices. In this regard, optical patterning of 2D materials has received enormous interest due to its advantages of high-throughput, site-specific, and on-demand fabrication. Recent years have witnessed scientific reports of a variety of optical techniques applicable to patterning 2D materials. In this minireview, we present the state-of-the-art optical patterning of 2D materials, including laser thinning, doping, phase transition, oxidation, and ablation. Several applications based on optically patterned 2D materials will be discussed as well. With further developments, optical patterning is expected to hold the key in pushing the frontiers of manufacturing and applications of 2D materials.

Opto-thermoelectric speckle tweezers.

Opto-thermoelectric tweezers present a new paradigm for optical trapping and manipulation of particles using low-power and simple optics. New real-life applications of opto-thermoelectric tweezers in areas such as biophysics, microfluidics, and nanomanufacturing will require them to have large-scale and high-throughput manipulation capabilities in complex environments. Here, we present opto-thermoelectric speckle tweezers, which use speckle field consisting of many randomly distributed thermal hotspots that arise from an optical speckle pattern to trap multiple particles over large areas. By further integrating the speckle tweezers with a microfluidic system, we experimentally demonstrate their application for size-based nanoparticle filtration. With their low-power operation, simplicity, and versatility, opto-thermoelectric speckle tweezers will broaden the applications of optical manipulation techniques.