The emergence of macroscopic self-propelled oscillatory motion based on molecular design has attracted continual attention in relation to autonomous systems in living organisms. Herein, a series of perylenediimides (PDIs) with various imide side chains was prepared to explore the impact of molecular design and alignment on the self-propelled motion at the air-water interface. When placed on an aqueous solution containing a reductant, a solid disk of neutral PDI was reduced to form the water soluble, surface-active PDI dianion species, which induces a surface tension gradient in the vicinity of the disk for self-propelled motion. We found that centimeter-scale oscillatory motion could be elicited by controlling the supply rate of PDI dianion species through the reductant concentration and the structure of imide side chains. Furthermore, we found that the onset and speed of the self-propelled motion could be changed by the crystallinity of PDI at the water surface. This design principle using π-conjugated molecules and their self-assemblies could advance self-propelled, non-equilibrium systems powered by chemical energy.

Structural color, renowned for its enduring vibrancy, has been extensively developed and applied in the fields of display and anticounterfeiting. However, its limitations in brightness and saturation hinder further application in these areas. Herein, we propose a pendant evaporation self-assembly method to address these challenges simultaneously. By leveraging natural convection and Marangoni flow synchronization, the self-assembly process enhances the dynamics and duration of colloidal nanoparticles, thereby enhancing the orderliness of colloidal photonic crystals. On average, this technique boosts the brightness of structural color by 20% and its saturation by 35%. Moreover, pendant evaporation self-assembly is simple and convenient to operate, making it suitable for industrial production. We anticipate that its adoption will remarkably advance the industrialization of structural color, facilitating its engineering applications across various fields, such as display technology and anticounterfeiting identification.

Single-walled carbon nanotubes (SWCNTs) present excellent electronic and mechanical properties desired in wearable and flexible devices. The preparation of SWCNT films is the first step for fabricating various devices. This work developed a scalable and feasible method to assemble SWCNT thin films on water surfaces based on Marangoni flow induced by surface tension gradient. The films possess a large area of 40 cm × 30 cm (extensible), a tunable thickness of 15∼150 nm, a high transparency of up to 96%, and a decent conductivity. They are ready to be directly transferred to various substrates, including flexible ones. Flexible strain sensors were fabricated with the films on flexible substrates. These sensors worked with high sensitivity and repeatability. By realizing multi-functional human motion sensing, including responding to voices, monitoring artery pulses, and detecting knuckle and muscle actions, the assembled SWCNT films demonstrated the potential for application in smart devices.

OBJECTIVE: Electrostatically stabilised colloidal particles destabilise when brought into contact with cations causing the particles to aggregate in clusters. When a drop with stabilised colloidal partices is deposited on a liquid film containing cations the delicate balance between the fluid-mechanical and physicochemical properties of the system governs the spreading dynamics and formation of colloidal particle clusters.
METHODS: High-speed imaging and digital holographic microscopy were used to characterise the spreading process.
RESULTS: We reveal that a spreading colloidal drop evolves into a ring-shaped pattern after it is deposited on a thin saline water film. Clustered colloidal particles aggregate into larger trapezoidally-shaped \'supraclusters\'. Using a simple model we show that the trapezoidal shape of the supraclusters is determined by the transition from inertial spreading dynamics to Marangoni flow. These results may be of interest to applications such as wet-on-wet inkjet printing, where particle destabilisation and hydrodynamic flow coexist.

A commonly encountered challenge with freeze-dried drug products is glass vial fogging. Fogging is characterized by a thin layer of product deposited upon the inner surface of the vial above the lyophilized cake. While considered to be a routine cosmetic defect in many instances, fogging around the shoulder and neck of the vial may potentially impact container closure integrity and reject rates during inspection. In this work, the influence of processing conditions i.e. vial pre-treatment, lyophilization cycle modifications and filling conditions on fogging was evaluated. A battery of analytical techniques was employed to investigate factors affecting glass vial fogging. A fogging score was used to quantify its severity in freeze-dried products. Additionally, a dye-based method was used to study solution upcreep (Marangoni flow) following product filling. Our lab-scale results indicate measurable improvement in fogging following the addition of an annealing step in the lyophilization cycle. Pre-freeze isothermal holding of the vials (at 5°C on the lyophilizer shelf) for an extended duration indicated a reduction in fogging whereas an increase in the freezing time exhibited no effect on fogging. Vial pre-treatment conditions were critical determinants of fogging for Type 1 vials whereas they had no impact on fogging in TopLyo® vials. The headspace relative humidity (RH) investigation also indicated sufficient increase in the water vapor pressure inside the vial to be conducive to the formulation of a hydration film - the precursor to Marangoni flow.

Due to the high computational costs of the Eulerian multiphase model, which solves the conservation equations for each considered phase, a two-phase mixture model is proposed to reduce these costs in the current study. Only one single equation for each the momentum and enthalpy equations has to be solved for the mixture phase. The Navier-Stokes and energy equations were solved using the 3D finite volume method. The model was used to simulate the liquid-solid phase transformation of a Fe-0.82wt%C steel alloy under the effect of both thermocapillary and buoyancy convections. The alloy was cooled in a rectangular ingot (100 × 100 × 10 mm3) from the bottom cold surface to the top hot free surface by applying a heat transfer coefficient of h = 600 W/m2/K, which allows for heat exchange with the outer medium. The purpose of this work is to study the effect of the surface tension on the flow and segregation patterns. The results before solidification show that Marangoni flow was formed at the free surface of the molten alloy, extending into the liquid depth and creating polygonized hexagonal patterns. The size and the number of these hexagons were found to be dependent on the Marangoni number, where the number of convective cells increases with the increase in the Marangoni number. During solidification, the solid front grew in a concave morphology, as the centers of the cells were hotter; a macro-segregation pattern with hexagonal cells was formed, which was analogous to the hexagonal flow cells generated by the Marangoni effect. After full solidification, the segregation was found to be in perfect hexagonal shapes with a strong compositional variation at the free surface. This study illuminates the crucial role of surface-tension-driven Marangoni flow in producing hexagonal patterns before and during the solidification process and provides valuable insights into the complex interplay between the Marangoni flow, buoyancy convection, and solidification phenomena.

Ion-selective membrane has broad application in various fields, while the present solution-processed techniques can only prepare uniform membrane with microscale thickness. Herein, a high-quality polymer membrane with nanoscale thickness and uniformity is precisely prepared by controlling solution spreading and solvent evaporation stability/rate. With the arrayed capillaries, the stable spreading of polymer solution with volume of microliter induces the formation of solution film with micrometers thickness. Moreover, the fast increase of solution dynamic viscosity during solvent evaporation inhibits nonuniform Marangoni flow and capillary flow in solution film. Consequently, the uniform Nafion-Li membranes with ∼200 nm thickness are prepared, while their Li+ conductivity is 2 orders of magnitude higher than that of commercially Nafion-117 membrane. Taking lithium-sulfur battery as a model device, the cells (capacities of 8-10 mAh cm-2) can stably operate for 150 cycles at a S loading of 12 mg cm-2 and an electrolyte/sulfur ratio of ∼7.

Despite the rapid development in the performances of organic solar cells (OSCs), high-performance OSC modules based on green printing are still limited. The severe Coffee-ring effect (CRE) is considered to be the primary reason for the nonuniform distribution of active layer films. To solve this key printing problem, the cosolvent strategy is presented to deposit the active layer films. The guest solvent Mesitylene with a higher boiling point and a lower surface tension is incorporated into the host solvent o-XY to optimize the rheological properties, such as surface tension and viscosity of the active layer solutions. And the synergistic effect of inward Marangoni flow generation and solution thickening caused by the cosolvent strategy can effectively restrain CRE, resulting in highly homogeneous large-area active layer films. In addition, the optimized crystallization and phase separation of active layer films effectively accelerate the charge transport and exciton dissociation of devices. Consequently, based on PM6:BTP-eC9 system, the device prepared with the co-solvent strategy shows the a power conversion efficiency of 17.80%. Moreover, as the effective area scales to 1 and 16.94 cm2, the recorded performances are altered to 16.71% and 14.58%. This study provides a universal pathway for the development of green-printed high-efficiency organic photovoltaics.

OBJECTIVE: The coalescence of droplets with liquid-gas interfaces of different surface tensions is common in nature and industrial applications, where the Marangoni-driven film spreading is an essential process. Unlike immiscible fluids governed by triple contact line dynamics, the mixing between two miscible fluids strongly couples with the film spreading process, which are expected to manifest distinct power-law relations for the temporal increase in the film radius.
METHODS: We experimentally investigate the Marangoni-driven film spreading phenomenon for a droplet with lower surface tension dropping onto a miscible, thin liquid layer. The temporal growth of the film radius was detected by using a novel deep convolutional neural network, the U2-net method. Scaling analysis was performed to interpret the spreading dynamics of the film.
RESULTS: We find that the film radius exhibits a three-stage power-law relation over time, with the exponent varying from 1/2 to 1/8, and back to 1/2. The diffusion-affected Marangoni stresses in these three stages were derived, and two estimations of viscous stress were considered. Through estimating and balancing the viscous stress with the Marangoni stress, the three-stage power-law relation was derived and validated.

Laser processing in metals is versatile yet limited by its reliance on phase transformation through heating rather than electronic excitation due to their low absorptivity, attributing from highly ordered structures. Metastable states (i.e., surfaces, glasses, undercooled liquids), however, present a unique platform, both energetically and structurally to enable energy landscape tuning through selective stimuli. Herein, this ansatz is demonstrated by exploiting thin passivating oxides to stabilize an undercooled state, followed by photo-perturbation of the near surface order to induce convective Marangoni flows, edge-coalescence and phase transition into a larger metastable solid bearing asymmetric composition between the near surface and core of the formed structure. The self-terminating nature of the process creates a perfectly contained system which can maintain a high relaxation energy barrier hence deep metastable states for extended periods of time.