Going forward, the development of tools for systematical quantification of helicality in MOs is a prerequisite to investigate how helical MOs correlate with, or can be used to predict, molecular properties. This might, for example, allow us to control molecular properties based on our knowledge of how to chemically manipulate helical MOs. As we become increasingly aware of molecules where helical ⇡-systems appear, the need grows for better tools to make quantitative assessments of helicality. In this work we have used MAD as the quantitative descriptor of orbital helicality, because it both summarizes how well the data follows a given model and allows for comparison across data sets. While there may be more elaborate measures that could be envisaged, it is a simple, intuitive, and well-known assessment approach. The use of MAD as the test for cylindrical helicality answers the following question: Is the MO a perfect helix or not? While the case of a cylindrical helix is well-defined and corresponds to a MAD of 1, the "or not"-situation is less well-defined as there will be more situations that deviate a cylindrical helix. In practice, this is not a problem in the present study. However, future work may aim for a more distinct definition of the edge-cases, especially if MO helicality turns out to be decisive for molecular properties.