Air-water Interface Research Articles

Elucidating the Mechanism of Helium Evaporation from Liquid Water.

We investigate the evaporation of trace amounts of helium solvated in liquid water using molecular dynamics simulations and theory. Consistent with experimental observations, we find a super-Maxwellian distribution of kinetic energies of evaporated helium. This excess of kinetic energy over typical thermal expectations is explained by an effective continuum theory of evaporation based on a Fokker-Planck equation, parametrized molecularly by a potential of mean force and position-dependent friction. Using this description, we find that helium evaporation is strongly influenced by the friction near the interface, which is anomalously small near the Gibbs dividing surface due to the ability of the liquid-vapor interface to deform around the gas particle. Our reduced description provides a mechanistic interpretation of trace gas evaporation as the motion of an underdamped particle in a potential subject to a viscous environment that varies rapidly across the air-water interface. From it we predict the temperature dependence of the excess kinetic energy of evaporation, which is yet to be measured.

Investigating the self-assembly of pH-sensitive switchable diamine surfactant using sum frequency generation spectroscopy and molecular dynamics simulations.

The responses of the N-alkyl diamine groups to variations in pH affect their conformations and surface activities, making them relevant to applications relying on interfacial interactions, such as controlled emulsification and mineral flotation. An in-depth understanding of interfacial self-assembly is crucial. Herein, a molecular-level study was performed to investigate the adsorption and self-assembly of N-dodecylpropane-1,3-diamine (DPDA) at the air-water (A/W) interface using sum frequency generation (SFG) spectroscopy and molecular dynamics (MD) simulations. The SFG spectra of DPDA, acquired under three pH conditions, suggest that the protonation of the DPDA diamine group influences the alkyl chain arrangement at a varying degree at the A/W interface. Analysis of the di-cationic DPDA SFG spectrum at a low pH showed fewer gauche defects at low concentration, as indicated by the relatively higher intensity ratio (ICH3SS/ICH2SS) of 18.1 ± 0.6. The density profiles from MD simulations at different surface areas per molecule and pH conditions, showing varying degrees of packing, support the observation of gauche defects in SFG. With MD simulation, the radial distribution factor for di-cationic species has the highest probability of forming hydrogen bonds compared to mono-cationic and non-ionic species. These g(r) probability results conform with observations obtained from SFG spectroscopy, where we observed a strong hydrogen bond interaction at low pH conditions with di-cationic species, forming tetrahedrally arranged water molecules at the A/W interface. Overall, comprehensive insights will facilitate the visualization of alkyl diamines and their potential derivatives at the A/W interface, enabling a better understanding of their behavior across various applications.

Revisiting the Thickness of the Air-Water Interface from Two Extremes of Interface Hydrogen Bond Dynamics.

The air-water interface plays a crucial role in many aspects of science because of its unique properties, such as a two-dimensional hydrogen bond (HB) network and completely different HB dynamics compared to bulk water. However, accurately determining the boundary of interfacial and bulk water, that is, the thickness of the air-water interface, still challenges experimentalists. Various simulation-based methods have been developed to estimate the thickness, converging on a range of approximately 3-10 (Å). In this study, we introduce a novel approach, grounded in density functional theory-based molecular dynamics and deep potential molecular dynamics simulations, to measure the air-water interface thickness, offering a different perspective based on prior research. To capture realistic HB dynamics in the air-water interface, two extreme scenarios of the interface HB dynamics are obtained: one underestimates the interface HB dynamics, while the other overestimates it. Surprisingly, our results suggest that the interface HB dynamics in both scenarios converges as the thickness of the air-water interface increases to 4 (Å). This convergence point, indicative of the realistic interface thickness, is also validated by our calculation of anisotropic decay of OH stretch and the free OH dynamics at the air-water interface.

Real-Time Analysis and Digital Twin Modeling for CFD-Based Air Valve Control During Filling Procedures

Air exchange in pressurized water pipelines is an essential but complex aspect of pipeline modeling and operation. Implementing effective air management strategies can yield numerous benefits, enhancing the system’s energy efficiency, reliability, and safety. This paper comprehensively evaluates an irregular profile pipeline filling procedure involving air-release through an air valve. The analysis includes real-time data tests and numerical simulations using Computational Fluid Dynamics (CFD). A Digital Twin model was proposed and applied to filling maneuvers in water installations. In particular, this research considers an often-overlooked aspect, such as filling a pipe with an irregular profile rather than a simple straight pipe. CFD simulations have proven to capture the main features of the transient event, which are suitable for tracking the air-water interface, the unsteady water flow, and the evolution of the trapped air pocket. Thus, they provide thorough and reliable information for real-time operational processes in the industry, focusing on the filling pressure and geometry of the air-valve hydraulic system. Additionally, this study provides details regarding the application of an efficient Digital Twin CFD approach, demonstrating its feasibility in optimizing the filling procedure in pipes with irregular profiles.

Atomization by Acoustic Levitation Facilitates Contactless Microdroplet Reactions.

Microdroplet chemistry is now well-known to be able to remarkably accelerate otherwise slow reactions and trigger otherwise impossible reactions. The uniqueness of the microdroplet is attributable to either the air-water interface or solid-liquid interface, depending on the medium that the microdroplet is in contact with. To date, the importance of the solid-liquid interface might have been confirmed, but the contribution from the air-water interface seems to be elusive due to the lack of method for generating contactless microdroplets. In this study, we used a droplet atomization method with acoustic levitation. Upon manipulation of the acoustic field, the levitated parent droplet can be further atomized into progeny microdroplets. With this method, only the air-water interface was present, and a large variety of reactions were successfully tested. We anticipate that this study can be an advance toward the understanding of the air-water interfacial processes of microdroplet chemistry.

Role of zwitterionic lipid headgroups on monolayer formation and interfacial dilatational rheology in binary mixtures of phospholipids and cholesterol: A pendant drop tensiometer study

The complex composition of biological membranes, comprising a diverse array of lipids with unique moieties, has garnered increased attention due to the recognized roles of lipids in membrane stability and biological processes. Even subtle changes in phospholipid headgroups and fatty acyl tails profoundly affect the formation and interfacial dynamics of lipid monolayers at the air-water interface. However, the molecular-level understanding of their intermolecular forces and interactions during these processes, directly relating to the lipid chemical structures, is not well-explored. To better understand these complex physicochemical phenomena, simplified model monolayers with precise control over lipid types and compositions are utilized. In this study, we employ the pendant drop tensiometer technique to investigate the formation and interfacial rheology of 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) and 1,2-dipalmitoyl-sn-glycero-3-phosphoethanolamine (DPPE) monolayers, with varying amounts of cholesterol (CHOL) for the first time. These two phospholipids, with identical C16:0 acyl tails but different headgroups, exhibit marked differences in their interfacial interactions with CHOL and water molecules, consequently affecting monolayer formation and rheology. In the absence of CHOL, DPPE monolayers typically display a lower dilatational modulus than DPPC, attributed to increased headgroup hydration. However, introducing CHOL reverses this trend, resulting in stiffer DPPE-CHOL monolayers compared to DPPC-CHOL. With CHOL, we observe its well-known condensation effect on DPPC monolayers, yet for DPPE monolayers, both condensation and expansion effects are noted, contingent on CHOL amount. We anticipate this work will not only deepen our fundamental understanding of the structure-composition-property relationships in lipid molecules but also provide a robust foundation for comprehending more intricate biological systems.

Simulating PFAS transport in effluent-irrigated farmland using PRZM5, LEACHM, and HYDRUS-1D models.

Application of wastewater effluent to agricultural lands can serve as a sustainable approach to meet irrigation and nutrient needs for crop production. While nitrogen and phosphorous loadings can be effectively managed, concerns have been raised regarding the fate of emerging contaminants, including per- and polyfluoroalkyl substances (PFAS), which are widely detected in wastewater effluent. The objective of this paper was to evaluate the ability of three unsaturated flow and transport models, Pesticide Root Zone Model 5 (PRZM5), LEACHM, and HYDRUS-1D, to predict the distribution of PFAS in the soil profile at the Pennsylvania State University Living Filter site, which has received daily wastewater effluent applications for several decades. The models were modified to include adsorption at the air-water interface (AWI), which has been shown to be an important factor governing PFAS transport and phase distribution in the vadose zone. Simulations showed that PRZM5 did not accurately reproduce the observed perfluorooctanesulfonic acid (PFOS) behavior, which was attributed to the "tipping bucket" approach used for water flow that results in the disappearance of AWI during water flow. In contrast, both LEACHM and HYDRUS-1D captured the observed retention of PFOS and perfluorooctanoic acid (PFOA) over a 50-year simulation period. Due to differences in the approach used to calculate the AWI area, LEACHM predicted greater accumulation of PFOS and PFOA at the AWI compared to HYDRUS-1D. These findings indicate that mathematical models that directly account for unsaturated water flow and adsorption at the AWI are able to provide reasonable predictions of long-term PFAS leaching resulting from land application of wastewater effluent.

Distinguishing Surface and Bulk Reactivity: Concentration-Dependent Kinetics of Iodide Oxidation by Ozone in Microdroplets.

Iodine oxidation reactions play an important role in environmental, biological, and industrial contexts. The multiphase reaction between aqueous iodide and ozone is of particular interest due to its prevalence in the marine atmosphere and unique reactivity at the air-water interface. Here, we explore the concentration dependence of the I- + O3 reaction in levitated microdroplets under both acidic and basic conditions. To interpret the experimental kinetics, molecular simulations are used to benchmark a kinetic model, which enables insight into the reactivity of the interface, the nanometer-scale subsurface region, and the bulk interior of the droplet. For all experiments, a kinetic description of gas- and liquid-phase diffusion is critical to interpreting the results. We find that the surface dominates the iodide oxidation kinetics under concentrated and acidic conditions, with the reactive uptake coefficient approaching an upper limit of 10-2 at pH 3. In contrast, reactions in the subsurface dominate under more dilute and alkaline conditions, with inhibition of the surface reaction at pH 12 and an uptake coefficient that is 10× smaller. The origin of a changing surface mechanism with pH is explored and compared to previous ozone-dependent measurements.

Harnessing air-water interface to generate interfacial ROS for ultrafast environmental remediation

The air-water interface of microbubbles represents a crucial microenvironment that can dramatically accelerate reactive oxidative species (ROS) reactions. However, the dynamic nature of microbubbles presents challenges in probing ROS behaviors at the air-water interface, limiting a comprehensive understanding of their chemistry and application. Here we develop an approach to investigate the interfacial ROS via coupling microbubbles with a Fenton-like reaction. Amphiphilic single-Co-atom catalyst (Co@SCN) is employed to efficiently transport the oxidant peroxymonosulfate (PMS) from the bulk solution to the microbubble interface. This triggers an accelerated generation of interfacial sulfate radicals (SO4•−), with 20-fold higher concentration (4.48 × 10−11 M) than the bulk SO4•−. Notably, the generated SO4•− is preferentially situated at the air-water interface due to its lowest free energy and the strong hydrogen bonding interactions with H3O+. Moreover, it exhibits the highest oxidation reactivity toward gaseous pollutants like toluene, with a rate constant of 1010 M−1 s−1-over 100 times greater than bulk reactions. This work demonstrates a promising strategy to harness the air-water interface for accelerating ROS-induced reactions, highlighting the importance of interfacial ROS and its potential application.

Enhanced Diffusion and Non-Gaussian Displacements of Colloids in Quasi-2D Suspensions of Motile Bacteria

In the real world, active agents interact with surrounding passive objects, thus introducing additional degrees of complexity. The relative contributions of far-field hydrodynamic and near-field contact interactions to the anomalous diffusion of passive particles in suspensions of active swimmers remain a subject of ongoing debate. We constructed a quasi-two-dimensional microswimmer–colloid mixed system by taking advantage of Serratia marcescens’ tendency to become trapped at the air–water interface to investigate the origins of the enhanced diffusion and non-Gaussianity of the displacement distributions of passive colloidal tracers. Our findings reveal that the diffusion behavior of colloidal particles exhibits a strong dependence on bacterial density. At moderate densities, the collective dynamics of bacteria dominate the diffusion of tracer particles. In dilute bacterial suspensions, although there are multiple dynamic types present, near-field contact interactions such as collisions play a major role in the enhancement of colloidal transport and the emergence of non-Gaussian displacement distributions characterized by heavy exponential tails in short times. Despite the distinct types of microorganisms and their diverse self-propulsion mechanisms, a generality in the diffusion behavior of passive colloids and their underlying dynamics is observed.

Structure, orientation, and dynamics of per- and polyfluoroalkyl substance (PFAS) surfactants at the air-water interface: Molecular-level insights

HypothesisUnderstanding the intricate molecular-level details of toxic per- and polyfluoroalkyl substances (PFAS) partitioning to the air–water interface holds paramount importance in evaluating their fate and transport, as well as for finding safer alternatives for various applications, including aqueous film forming foams. The behavior of these substances at interfaces strongly depends on molecular architecture, chemistry, and concentration, which define molecular packing, self-assembly, interfacial diffusion, and the surface tension. SimulationsModeling of three PFAS surfactants, namely, longer-tail (perfluorooctanoate (PFOA)) and shorter-tail (perfluorobutanoate (PFBA) and 2,3,3,3-tetrafluoro-2-(heptafluoropropoxy) propanoate (GenX)) has been conducted using atomistic molecular dynamics simulations. A systematic comparison between these representative PFAS of different sizes and structure reveals factors influencing their association behavior, mechanism of surface tension reduction, and interfacial mobility as a function of surface coverage. FindingsShorter-chain PFAS surfactants (GenX or PFBA) require lower surface coverage compared to longer chain (PFOA) PFAS to achieve the same decrease in surface tension. However, a higher concentration of GenX and PFBA is necessary in the bulk aqueous solution to achieve the same surface coverage as PFOA, due to their higher solubility in water. The PFAS molecular orientation and mobility at the interface are found to be vastly influenced by the length and architecture of the hydrophobic fluorocarbon tail. A significant ordering of the water dipole moment near the anionic headgroup is apparent at high surface concentration. A direct correlation is established between the PFAS interfacial properties and PFAS-PFAS, PFAS-counterion, and PFAS-water interactions.

Modeling photomolecular effect using generalized boundary conditions for Maxwell equations

We recently demonstrated via experiments in hydrogels and at a single air-water interface the photomolecular effect: photons directly cleaving off water molecular clusters in the visible spectrum where bulk water has negligible absorption. To model single interface experiments, here we re-derive generalized boundary conditions for Maxwell equations by assuming a transition region of the electromagnetic fields across the interface, leading naturally to the Feibelman parameters used before to describe surface photoelectric and surface plasmon effects on metals. This generalization leads to modifications of the Fresnel coefficients and an expression for the surface absorptance that can reasonably explain trends in our single-interface experimental data on the angle and polarization dependence of the beam deflection. Our work provides further support for the existence of the photomolecular effect, suggests that surface absorption should exist in many materials, and lays a foundation for assessing the impacts of such surface absorption based on the Maxwell equations.

Optical anisotropy and surface phases of cholesterol derivative monolayer at air–water interface

Cholesterol and its derivatives play crucial roles in regulating processes of biological membranes. Langmuir monolayer can mimic a bio-membrane which can be used to investigate the molecular interaction governing the important physical phenomena. The cholesterol derivative exhibiting mesophases (CHLC molecules) was synthesized and spread at the air–water (A/W) interface to investigate the surface behavior. The monolayer exhibited a variety of surface phases such as gas, liquid expanded (LE), low density liquid like (L1) and liquid condensed (L2) phases. Treating the CHLC molecules to be rod-like, the average tilt of the molecules with respect to the surface normal in these phases are found to be different. The tilt angle decreases systematically from LE to L2 phase. The optical anisotropy of the ultrathin Langmuir-Blodgett (LB) films of CHLC molecules in these phases was measured using the surface plasmon resonance (SPR) spectroscopy. The high tilted molecules in the ultrathin LB film displayed a high value of optical anisotropy. The ultrathin film of CHLC molecules at different interfaces was investigated using Brewster angle microscopy, X-ray reflectivity (XRR), SPR spectroscopy and atomic force microscopy. This study is useful for the systems where the physical phenomena are governed by tilt of the molecules.

Quantifying the effects of spectral and directional distribution of radiation on its propagation in saline water

The interactions of radiation with saline water facilitate various energy-related applications, such as radiative evaporation at the air–water interface, radiation-driven underwater vapor generation, and underwater photovoltaic systems. However, these applications require a comprehensive understanding of radiation propagation through saline water, considering both its spectral and directional characteristics, which are often inadequately explored. This study introduces a three-dimensional Monte Carlo radiative transfer model equipped with fine spectral resolution and detailed angular considerations. The model simulates the transfer of radiation from the air to the air–water interface and throughout the saline water body to thoroughly examine the effects of spectral and directional properties of incident radiation on its propagation across different depths of saline water. The findings reveal that within the solar spectrum, radiation entering the water at a 62.7-degree angle of incidence and completely diffuse radiation exhibit similar absorption effects in water layers less than 2 meters deep. In addition, the incident angle has little impact on the absorption rate of both the water surface and the water body when the angle is below 62.7°. Spectrally, radiation wavelengths longer than 1.4μm, 1.14μm, and 1μm are fully absorbed within the first 1, 8, and 50 centimeters of saline water, respectively, representing approximately 20%, 30%, and 50% of incident solar radiation. Additionally, radiation from blackbody sources below 1300 Kelvin is absorbed entirely within the top 1 centimeter of saline water. Empirical correlations are then developed to easily estimate the absorption rate based on the depth of the water and the temperature of the blackbody heat source. The findings elucidate the influence of the spectral and directional characteristics of incident radiation on its underwater propagation, offering essential guidance for the design and performance evaluation of various energy-centric applications.

Two-Step Noncatalyzed Hydrolysis Mechanism of Imines at the Air-Water Interface.

The hydrolysis of imines has long been assumed to be their main atmospheric fate, based on early studies in the field of organic chemistry. However, the hydrolysis mechanism and kinetics of atmospheric imines remain unclear. Here, an advanced Born-Oppenheimer molecular dynamics method was employed to investigate the noncatalyzed hydrolysis mechanism and kinetics at the air-water interface by selecting CH2NH as a model molecule. The results indicate that CH2NH exhibits a pronounced surface preference. The noncatalyzed hydrolysis of CH2NH follows a unique two-step reaction mechanism involving first proton transfer and then OH- transfer through the water bridge at the air-water interface, in contrast to the traditional one-step mechanism. The calculated reaction rate for the rate-determining step is 3.32 × 105 s-1, which is 2 orders of magnitude greater than that of the bulk phase. In addition, the involvement of the interfacial electric field further enhances the reaction rate by approximately 3 orders of magnitude. The noncatalyzed hydrolysis rate at both the air-water interface and the bulk phase is higher than that of the possible acid-catalyzed one, clarifying noncatalyzed hydrolysis as the dominant mechanism for CH2NH. This study elucidates that the noncatalyzed hydrolysis of atmospheric imines is feasible at the air-water interface and that the revealed unique two-step hydrolysis mechanism has significant implications in atmospheric and water environmental chemistry.

Propensity of hydroxide and hydronium ions for the air-water and graphene-water interfaces from abinitio and force field simulations.

Understanding acids and bases at interfaces is relevant for a range of applications from environmental chemistry to energy storage. We present combined abinitio and force-field molecular dynamics simulations of hydrochloric acid and sodium hydroxide highly concentrated electrolytes at the interface with air and graphene. In agreement with surface tension measurements at the air-water interface, we find that HCl presents an ionic surface excess, while NaOH displays an ionic surface depletion, for both interfaces. We further show that graphene becomes less hydrophilic as the water ions concentration increases, with a transition to being hydrophobic for highly basic solutions. For HCl, we observe that hydronium adsorbs to both interfaces and orients strongly toward the water phase, due to the hydrogen bonding behavior of hydronium ions, which donate three hydrogen bonds to bulk water molecules when adsorbed at the interface. For NaOH, we observe density peaks of strongly oriented hydroxide ions at the interface with air and graphene. To extrapolate our results from concentrated electrolytes to dilute solutions, we perform single ion-pair abinitio simulations, as well as develop force-field parameters for ions and graphene that reproduce the density profiles at high concentrations. We find the behavior of hydronium ions to be rather independent of concentration. For NaOH electrolytes, the force-field simulations of dilute NaOH solutions suggest no hydroxide adsorption but some adsorption at high concentrations. For both interfaces, we predict that the surface potential is positive for HCl and close to neutral for NaOH.

Spatiotemporal distribution of pCO2 and CO2 flux and the regulatory factors: From the perspective of a subtropical canyon-shaped reservoir, southwest China

Reservoir carbon cycling is a critical component of the global carbon cycle, particularly in subtropical canyon-shaped reservoirs where unique geomorphological features and hydrological regulation under monsoon climate provide a distinct perspective for carbon cycle research. This study takes the Zipingpu Reservoir (ZPPR) in southwestern China as an example and reveals significant seasonal variations in partial pressure of carbon dioxide (pCO2) and carbon dioxide flux at the water-air interface (FCO2) through annual monitoring. The average pCO2 in ZPPR is 486 μatm, and the average FCO2 is 0.093 g C m-2d-1, with approximately 42.4 % of FCO2 measurements being negative, indicating the reservoir's role can act as a carbon sink. The study also estimated the gas transfer coefficient (K), with an average value of 1.888 md-1. Peak FCO2 during spring and summer is three times higher than in other seasons, consistent with the main influencing factors of inflow dynamics, metabolic processes, and reservoir operation strategies. Inflow and operational activities, particularly during spring and summer, drive CO2 emissions in the downstream reach and upstream tributary, while biological activity facilitates CO2 uptake in the lacustrine area and forebay tributary, with enhanced absorption occurring in the autumn. Concurrently, high-intensity FCO2 emissions from the upstream river section during summer underscore the importance of carbon emission monitoring and management during critical periods. The findings not only enhance the understanding of FCO2 assessment accuracy but also provide a framework for evaluating and optimizing carbon dynamics management strategies in canyon-shaped reservoirs, contributing valuable insights to global carbon cycle research.

Stearic Acid as Polymerization Medium, Dopant and Hydrophobizer: Chemical Oxidative Polymerization of Pyrrole.

In recent years, fatty acids have garnered significant attention as a natural phase-change material and a hydrophobizer due to their biocompatibility and biodegradability. In this study, the utilization of fatty acid is proposed as a polymerization medium for the first time. As a specific reaction, chemical oxidative polymerizations of pyrrole is conducted using ferric chloride as an oxidant in a stearic acid medium. The polymerizations resulted in the production of micrometer-sized polypyrrole (PPy) grains, which are aggregates of atypical primary particles with submicrometer size. The PPy grains are doped with stearic acid, suggesting that the stearic acid functioned as a dopant and a hydrophobizing agent as well as a polymerization medium. The dried PPy grains can adsorb at the air-water interface and function as a liquid marble stabilizer with light-to-heat photothermal properties. The liquid marble can move on a planar air-water interface by Marangoni flow induced by NIR laser light irradiation.

Reduction‐Induced Self‐Propelled Oscillatory Motion of Perylenediimides on Water

AbstractThe 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 the 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.

Reduction-Induced Self-Propelled Oscillatory Motion of Perylenediimides on Water.

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 the 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.