Grant: Discovery Grants Program - Individual

Nano and micro-confining environments, such as droplets in any medium and biological assemblies, crevices in corroding metals as well as interfaces are subject to distinct chemistry in contrast to their bulk solution counterparts.  The overarching goal of my research program is to push the boundaries of chemistry by enhancing our understanding of chemical mechanisms within small-scale volumes, particularly in systems with linear dimensions at the nano- and micro-scale levels and at interfaces. We aim to uncover universal principles and patterns governing chemistry within these confined spaces and intricate geometries. To achieve that we have developed a suite of computational methods that includes multi-scale, atomistic and mathematical modelling, and numerical solutions of electrostatic equations. An immediate outcome of our research is to explain physical and chemical phenomena, offer guidelines for experimental protocols and insights in data interpretation. This would, in turn, increase the capabilities of analytical chemistry techniques, namely mass spectrometry, ensuring reliable detection of surface composition in atmospheric aerosols, surface reactivity, and biological assemblies. Searching for the underlying principles that govern chemistry in confining environments, in this proposal, we examine the chemistry in aerosols and interfaces. The ice-sea water interface in the Arctic has always intrigued many NSE disciplines because of its key role in the thermohaline circulation and life on Earth. Here, we use advanced computational chemistry methods to resolve intricate mechanisms of the formation of the brine layer below the ice sheet in the Arctic. We put forward a new hypothesis for the mechanism of its formation from the common belief. The methods and the open-source software that we will develop in the course of this study will find applicability into a variety of problems beyond the ones examined here. The proton transfer reactions are ubiquitous in nature. For example, they constantly take place in water between two water molecules, enzymatic action, and neutralization reactions to mention but a few examples.  Here, we investigate the rate of proton transfer reactions in gaseous phase protein complexes to answer key questions on the conformation-charge relation and derive general laws.  Applications of the study are found in broadly used analytical chemistry methods, namely mass spectrometry, used for the analysis of biological samples.  Finally, several questions are investigate on the growth, hygroscopicity and transport properties within atmospheric aerosols that play a key role in the air quality. The topics covered in this proposal serve EDI principles in that they may include in their development not only theoretical chemists but also trainees and collaborators with interests in atmospheric and environmental chemistry, mass spectrometry and biochemistry with science or engineering background.