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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.

 

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.

 

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.

 

Constructing colloidal particles into functional nanostructures, materials, and devices is a promising yet challenging direction. Many optical techniques have been developed to trap, manipulate, assemble, and print colloidal particles from aqueous solutions into desired configurations on solid substrates. However, these techniques operated in liquid environments generally suffer from pattern collapses, Brownian motion, and challenges that come with reconfigurable assembly. Here, we develop an all-optical technique, termed optothermally-gated photon nudging (OPN), for the versatile manipulation and dynamic patterning of a variety of colloidal particles on a solid substrate at nanoscale accuracy. OPN takes advantage of a thin surfactant layer to optothermally modulate the particle-substrate interaction, which enables the manipulation of colloidal particles on solid substrates with optical scattering force. Along with in situ optical spectroscopy, our non-invasive and contactless nanomanipulation technique will find various applications in nanofabrication, nanophotonics, nanoelectronics, and colloidal sciences.

 

The assembly of nanoparticles on surfaces in defined patterns has long been achieved via template-assisted methods that involve long deposition and drying steps and the need for molds or masks to obtain the desired patterns. Control over deposition of materials on surfaces via laser-directed microbubbles is a nascent technique that holds promise for rapid fabrication of devices down to the micrometer scale. However, the influence of surface chemistry on the resulting assembly using such approaches has so far not been studied. Herein, the printing of layered silicate nanoclays using a laser-directed microbubble was established. Significant differences in the macroscale structure of the printed patterns were observed for hydrophilic, pristine layered silicates compared to hydrophobic, modified layered silicates, which provided the first example of how the surface chemistry of such nanoscale objects results in changes in assembly with this approach. Furthermore, the ability of layered silicates to adsorb molecules at the interface was retained, which allowed the fabrication of proof-of-concept sensors based on Förster resonance energy transfer (FRET) from quantum dots embedded in the assemblies to bound dye molecules. The detection limit for Rhodamine 800 sensing via FRET was found to be on the order of 10–12 M, suggesting signal enhancement due to favorable interactions between the dye and nanoclay. This work sets the stage for future advances in the control of hierarchical assembly of nanoparticles by modification of surface chemistry while also demonstrating a quick and versatile approach to achieve ultrasensitive molecular sensors.