Hybrid organic-inorganic structures trigger the formation of primitive cell-like compartments.

Alkaline hydrothermal vents have become a candidate setting for the origins of life on Earth and beyond. This is due to several key features including the presence of gradients of temperature, redox potential, pH, the availability of inorganic minerals, and the existence of a network of inorganic pore spaces that could have served as primitive compartments. Chemical gardens have long been used as experimental proxies for hydrothermal vents. This paper investigates-10pc]Please note that the spelling of the following author name in the manuscript differs from the spelling provided in the article metadata: Richard J. G. Löffler. The spelling provided in the manuscript has been retained; please confirm. a set of prebiotic interactions between such inorganic structures and fatty alcohols. The integration of a medium-chain fatty alcohol, decanol, within these inorganic minerals, produced a range of emergent 3 dimensions structures at both macroscopic and microscopic scales. Fatty alcohols can be considered plausible prebiotic amphiphiles that might have assisted the formation of protocellular structures such as vesicles. The experiments presented herein show that neither chemical gardens nor decanol alone promote vesicle formation, but chemical gardens grown in the presence of decanol, which is then integrated into inorganic mineral structures, support vesicle formation. These observations suggest that the interaction of fatty alcohols and inorganic mineral structures could have played an important role in the emergence of protocells, yielding support for the evolution of living cells.

Survival strategies of artificial active agents.

Artificial cells can be engineered to display dynamics sharing remarkable features in common with the survival behavior of living organisms. In particular, such active systems can respond to stimuli provided by the environment and undertake specific displacements to remain out of equilibrium, e.g. by moving towards regions with higher fuel concentration. In spite of the intense experimental activity aiming at investigating this fascinating behavior, a rigorous definition and characterization of such "survival strategies" from a statistical physics perspective is still missing. In this work, we take a first step in this direction by adapting and applying to active systems the theoretical framework of Transition Path Theory, which was originally introduced to investigate rare thermally activated transitions in passive systems. We perform experiments on camphor disks navigating Petri dishes and perform simulations in the paradigmatic active Brownian particle model to show how the notions of transition probability density and committor function provide the pivotal concepts to identify survival strategies, improve modeling, and obtain and validate experimentally testable predictions. The definition of survival in these artificial systems paves the way to move beyond simple observation and to formally characterize, design and predict complex life-like behaviors.

New types of complex motion of a simple camphor boat.

We discuss the motion of a rectangular camphor boat, considering the position of a camphor pill in relation to the boat's stern as the control parameter. The boat moves because the pill releases surface active molecules that decrease the surface tension and support the motion. We introduce a new experimental system in which the boat rotates on a long arm around the axis located at the centre of a Petri dish; thus, the motion is restricted to a circle and can be studied under stationary conditions for a long time. The experiments confirmed two previously reported modes of motion: continuous motion when the pill was located at the boat edge and pulsating (intermittent) motion if it was close to the boat centre (Suematsu et al., J. Phys. Chem. C, 2010, 114(21), 9876-9882). For intermediate pill locations, we observed a new, unreported type of motion characterised by oscillating speed (i.e. oscillating motion). Different modes of motion can be observed for the same pill location. The experimental results are qualitatively confirmed using a simple reaction-diffusion model of the boat evolution used in the above-mentioned paper.

Complexity and bifurcations in the motion of a self-propelled rectangle confined in a circular water chamber.

We consider the motion of a self-propelled object of rectangular shape inside a circular water chamber. The mathematical model of self-motion includes equations for the orientation and location of the rectangle and reaction-diffusion equation with an effective diffusion coefficient for the time evolution of the surface concentration of active molecules. Numerical simulations of motion were performed for different values of the ratio between the supply rate S and the evaporation rate a of active molecules. Treating S0 = S/a as a control parameter, we found the critical behavior in variables characterizing the trajectory and identified different types of motion. If the value of S0 is small, the rectangle rests at the chamber center. For larger S0, a reciprocal motion during which the rectangle passes through the center is observed. At yet higher supply rates, the star-polygonal motion appears, and the trajectory remains at a distance from the chamber center. In the experiments with a rectangle made of camphor-camphene-polypropylene plastic moving in a Petri dish, we observed the transition from the star-polygonal motion to the reciprocal motion in time. This transition can be understood on the basis of the developed model if we assume that the supply rate decreases in time.

Dynamic ordering caused by a source-sink relation between two droplets.

Two droplets composed of different chemicals, 1-decanol and liquid paraffin, floating on the water surface show characteristic co-responsive behavior. The presence of two different types of droplets in the system imposes an asymmetry that would not be possible with single droplets alone. The self-propulsion and interactions between droplets appear because surface active 1-decanol molecules provided by the source are absorbed by the paraffin sink thus generating an asymmetric surface tension gradient. This source-sink relation between droplets stabilizes and enhances the self-propulsion, and leads to a variety of dynamic structures including oscillations in the inter-droplet distance. We found that the character of time evolution also depends on the concentration of dye, Sudan Black B, initially used just to stain the decanol droplet. A simple mathematical model explains the transition between the stationary state and the oscillations as a Hopf bifurcation.

A camphene-camphor-polymer composite material for the production of superhydrophobic absorbent microporous foams.

In a recently published paper (doi.org/10.3390/molecules26113116) on self-propelled motion of objects on the water surface, we described a novel surface-active plastic material obtained by dissolution of camphor and polypropylene in camphene at 250 [Formula: see text]C. The material has wax-like mechanical properties, can be easily formed to any moldable shape, and allows for longer and more stable self-propelled motion if compared with pure camphor or pure camphene or of a camphene-camphor wax. Here we use scanning electron microscopy to visualize and characterize the microporous structure of the solid polypropylene foam formed in the plastic for different polypropylene contents. The topology of foams remaining in the material after camphor and camphene molecules have been removed through evaporation or dissolution is similar to polypropylene foams obtained using thermally-induced phase separation. We show that the foams have a superhydrophobic surface but strongly absorb non-polar liquids, and suggest an array of potential scientific and industrial applications.

A Perfect Plastic Material for Studies on Self-Propelled Motion on the Water Surface.

We describe a novel plastic material composed of camphene, camphor, and polypropylene that seems perfectly suited for studies on self-propelled objects on the water surface. Self-motion is one of the attributes of life, and chemically propelled objects show numerous similarities with animated motion. One of important questions is the relationship between the object shape and its motility. In our previous paper, {R. Löffler et al. PCCP, 2019, 21, 24852-24856}, we presented a novel hybrid material, obtained from the solution of camphor in camphene, that allowed making objects of various shapes. This hybrid material has wax-like mechanical properties, but it has a very high tackiness. Here, we report that a small amount of polypropylene removed this undesirable feature. We investigated the properties of camphor-camphene-polypropylene plastic by performing the statistical analysis of a pill trajectory inside a Petri dish and compared them with those of camphor-camphene wax. The plastic showed the stable character of motion for over an hour-long experiment. The surface activity of objects made of plastic did not significantly depend on the weight ratios of the compounds. Such a significant increase in usefulness came from the polypropylene, which controlled the dissipation of camphor and camphene molecules.

A hybrid camphor-camphene wax material for studies on self-propelled motion.

A new material that combines the self-propelling properties of camphor with the malleability of camphene is reported. It has wax-like mechanical properties at room temperature and can be formed into required shapes. The speed of the self-propelled objects and the trajectory depend on the shape and camphor-camphene weight ratio.