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In exploring the genesis of life, liquid–liquid phase-separated coacervate droplets have been proposed as primitive protocells. Within the hydrothermal hypothesis, these droplets would emerge from molecule-rich hot fluids and thus be subjected to temperature gradients. Investigating their thermophoretic behavior can provide insights into protocell footprints in thermal landscapes, advancing our understanding of life’s origins. Here, we report the thermophilic behavior of heat-dissociative droplets, contrary to the intuition that heat-associative condensates would prefer hotter areas. This aspect implies the preferential presence of heat-dissociative primordial condensates near hydrothermal environments, facilitating molecular incorporation and biochemical syntheses. Additionally, our investigations reveal similarities between thermophoretic and electrophoretic motions, dictated by molecular redistribution within droplets due to their fluid nature, which necessitates revising current electrophoresis frameworks for surface charge characterization. Our study elucidates how coacervate droplets navigate thermal and electric fields, reveals their thermal-landscape-dependent molecular characteristics, and bridges foundational theories of early life: the hydrothermal and condensate-as-protocell hypotheses. 

Liquid–liquid interfaces hold the potential to serve as versatile platforms for dynamic processes, due to their inherent fluidity and capacity to accommodate surface-active materials. This study explores laser-driven actuation of liquid–liquid interfaces with and without loading of gold nanoparticles and further exploits the laser-actuated interfaces with nanoparticles for tunable photonics. Upon laser exposure, gold nanoparticles were rearranged along the interface, enabling the reconfigurable, small-aperture modulation of light transmission and the tunable lensing effect. Adapting the principles of optical and optothermal tweezers, we interpreted the underlying mechanisms of actuation and modulation as a synergy of optomechanical and optothermal effects. Our findings provide an analytical framework for understanding microscopic interfacial behaviors, contributing to potential applications in tunable photonics and interfacial material engineering. 

It is beneficial for collective structures to simultaneously have high persistence to environmental noise and high responsivity to nontrivial external stimuli. However, without the ability to differentiate useful information from noise, there is always a tradeoff between persistence and responsivity within the collective structures. To address this, we propose adaptive time delay inspired by the adaptive behavior observed in the school of fish. This strategy is tested using particles powered by optothermal fields coupled with an optical feedback-control system. By applying the adaptive time delay with a proper threshold, we experimentally observe the responsivity of the collective structures enhanced by approximately 1.6 times without sacrificing persistence. Furthermore, we integrate adaptive time delay with long-distance transportation and obstacle-avoidance capabilities to prototype adaptive swarm microrobots. This research demonstrates the potential of adaptive time delay to address the persistence-responsivity tradeoff and lays the foundation for intelligent swarm micro/nanorobots operating in complex environments. 

Microscale temperature sensing and control are essential in various applications. Thermistors are widely utilized for temperature sensing owing to their simple design and high sensitivity. The future of thermistors lies in miniaturization and integration in highly customizable and sustainable electronics. Moreover, the ever-reducing size of the transistors requires the thermistors to scale down proportionally, without any compromise to its functionality. However, fabricating microscale thermistors exhibiting high accuracy and repeatable measurements has been challenging for state-of-the-art device miniaturization. Here, we develop versatile printing of microscale thermistors from silver fluoride solution by exploiting laser-induced opto-thermal microbubbles. The microscale temperature gradients on the bubble surface create an enhanced concentration of silver ions around the bubble to enable high-resolution printing of submicrometer structures with low-concentration precursors and low wastage. We demonstrate the bubble printing of thermistor arrays with both positive and negative thermal coefficients by exploiting the size effect on the electrical conductivity. We further investigate the sensing performance and long-term stability of the printed thermistors and conclude that the bubble-printed thermistors exhibit high-resolution sensing capabilities with long-term stability, promising enhanced performance in medical and semiconductor applications. 

Optically resonant particles are key building blocks of many nanophotonic devices such as optical antennas and metasurfaces. Because the functionalities of such devices are largely determined by the optical properties of individual resonators, extending the attainable responses from a given particle is highly desirable. Practically, this is usually achieved by introducing an asymmetric dielectric environment. However, commonly used simple substrates have limited influences on the optical properties of the particles atop. Here, we show that the multipolar scattering of silicon microspheres can be effectively modified by placing the particles on a dielectric-covered mirror, which tunes the coupling between the Mie resonances of microspheres and the standing waves and waveguide modes in the dielectric spacer. This tunability allows selective excitation, enhancement, suppression, and even elimination of the multipolar resonances and enables scattering at extended wavelengths, providing transformative opportunities in controlling light–matter interactions for various applications. We further demonstrate with experiments the detection of molecular fingerprints by single-particle mid-infrared spectroscopy and with simulations strong optical repulsive forces that could elevate the particles from a substrate. 

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.