The latter two forms of asymmetric catalysts have been seen as very promising alternatives to transition metal catalysts, due to their reduced costs and toxicity. In fact, the potential impact of these alternatives was recently recognized when the Nobel Prize in Chemistry was awarded to Frances Arnold (2018, directed evolution of enzymes), then Benjamin List and David MacMillan (2020, asymmetric organocatalysis), after Barry Sharpless, Ryoji Noyori and William Knowles shared the Nobel Prize in 2001 for asymmetric transition metal catalyzed reactions. Developing new catalysts. The relatively simple mechanisms of organocatalyzed reactions are a significant advantage for their development and optimization. However, the use of these catalysts has been hampered by their lower stereoselectivities and the need for higher loading. Alternatively, development of transition metal catalysts is facing complex mechanisms often involving multiple possible transition states (TSs), metal coordinations, additives, and ligands. As a result, the very tedious "trial-and-error" approach is still commonly used. To address environmental concerns, catalysts based on greener and cheaper metals (bismuth, iron, copper) have been developed, yet the most used transition metal catalysts are built around palladium, rhodium, and other toxic and expensive metals. Thus, despite tremendous progress in the field of small molecule catalysis, development of new chiral catalysts remains quite challenging and often calls for stepwise optimization. This is often a time-consuming, labour-intensive process. It requires the synthesis and evaluation of multiple novel ligands/catalysts, in an iterative process that is often pursued in an empirical fashion with little guidance other than simple models and intuition. Computational methods guiding the design of new catalysts are sought after and should address this major issue.