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Increasing atmospheric concentrations of greenhouse gases due to industrial activity have led to concerning levels of global warming. Reducing carbon dioxide (CO 2 ) emissions, one of the main contributors to the greenhouse effect, is key to mitigating further warming and its negative effects on the planet. CO 2 capture solvent systems are currently the only available technology deployable at scales commensurate with industrial processes. Nonetheless, designing these solvents for a given application is a daunting task requiring the optimization of both thermodynamic and transport properties. Here, we discuss the use of atomic scale modeling for computing reaction energetics and transport properties of these chemically complex solvents. Theoretical studies have shown that in many cases, one is dealing with a rich ensemble of chemical species in a coupled equilibrium that is often difficult to characterize and quantify by experiment alone. As a result, solvent design is a balancing act between multiple parameters which have optimal zones of effectiveness depending on the operating conditions of the application. Simulation of reaction mechanisms has shown that CO 2 binding and proton transfer reactions create chemical equilibrium between multiple species and that the agglomeration of resulting ions and zwitterions can have profound effects on bulk solvent properties such as viscosity. This is balanced against the solvent systems needing to perform different functions (e.g., CO 2 uptake and release) depending on the thermodynamic conditions (e.g., temperature and pressure swings). The latter constraint imposes a "Goldilocks" range of effective parameters, such as binding enthalpy and p K a , which need to be tuned at the molecular level. The resulting picture is that solvent development requires an integrated approach where theory and simulation can provide the necessary ingredients to balance competing factors., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)