The complex multiscale physics of nano-particle laden functional droplets in a reacting environment is of fundamental and applied significance for a wide variety of applications ranging from thermal sprays to pharmaceutics to modern day combustors using new brands of bio-fuels. Formation of homogenous nucleated bubbles at the superheat limit inside vaporizing droplets (with or without nanoparticles) represents an unstable system. Here we show that self-induced boiling in burning functional pendant droplets can produce severe volumetric shape oscillations. Internal pressure build-up due to ebullition activity ejects bubbles from the droplet domain causing undulations on the droplet surface and oscillations in bulk. Through experiments, we establish that the degree of droplet deformation depends on the frequency and intensity of these bubble expulsion events. In a distinct regime of single isolated bubble residing in the droplet, however, pre-ejection transient time is identified by Darrieus-Landau evaporative instability, where bubble-droplet system behaves as a synchronized driver-driven system with bulk bubble-shape oscillations being imposed on the droplet. The agglomeration of nanophase additives modulates the flow structures within the droplet and also influences the bubble inception and growth leading to different levels of instabilities.

Understanding the transients of buckling in drying colloidal suspensions is pivotal for producing new functional microstructures with tunable morphologies. Here, we report first observations and elucidate the buckling instability induced morphological transition (sphere to ring structure) in an acoustically levitated, heated nanosuspension droplet using dynamic energy balance. Droplet deformation featuring the formation of symmetric cavities is initiated by capillary pressure that is two to three orders of magnitude greater than the acoustic radiation pressure, thus indicating that the standing pressure field has no influence on the buckling front kinetics. With an increase in heat flux, the growth rate of surface cavities and their post-buckled volume increase while the buckling time period reduces, thereby altering the buckling pathway and resulting in distinct precipitate structures. However, irrespective of the heating rate, the volumetric droplet deformation exhibits a linear time dependence and the droplet vaporization is observed to deviate from the classical D²-law.

Understanding the combustion characteristics of fuel droplets laden with energetic nanoparticles (NP) is pivotal for lowering ignition delay, reducing pollutant emissions and increasing the combustion efficiency in next generation combustors. In this study, first we elucidate the feedback coupling between two key interacting mechanisms, namely, secondary atomization and particle agglomeration; that govern the effective mass fraction of NPs within the droplet. Second, we show how the initial NP concentration modulates their relative dominance leading to a master-slave configuration. Secondary atomization of novel nanofuels is a crucial process since it enables an effective transport of dispersed NPs to the flame (a pre-requisite condition for NPs to burn). Contrarily, NP agglomeration at the droplet surface leads to shell formation thereby retaining NPs inside the droplet. In particular, we show that at dense concentrations shell formation (master process) dominates over secondary atomization (slave) while at dilute particle loading it is the high frequency bubble ejections (master) that disrupt shell formation (slave) through its rupture and continuous outflux of NPs. This results in distinct combustion residues at dilute and dense concentrations, thereby providing a method of manufacturing flame synthesized microstructures with distinct morphologies.

The evaporation of a nanocolloidal sessile droplet exhibits preferential particle assembly, nanoporous shell formation and buckling to form cavities with unique morphological features. Here, we have established many universal trends that explain the buckling dynamics under one umbrella irrespective of hydrophobicity, evaporation mode and particle loading. We provide a regime map explaining the droplet morphology and buckling characteristics for droplet evaporation on various substrates. Specifically, we find that the final droplet volume and the radius of curvature at the buckling onset are universal functions of particle concentration. Furthermore, we establish that post-buckling cavity growth is evaporation driven regardless of the substrate.