The main conclusion of our work is that it is unlikely that the storage density of DHA can be increased to a value above 0.5 kJ/g by substitution at positions 1-7 (at least without decreasing the barrier to back reaction). Yet, storage densities above 0.3 kJ/g of both molecules 9 and 10 may be sufficient for some applications when considering also their long storage times. There are, however, other drawbacks with these molecules. For example, their absorption profiles are not optimum. And maybe more problematic, these molecules have rather complicated substitution patterns. There are today synthetic protocols available for functionalizing selectively at positions 1, 2, 3, and 7 (and in part position 6) of DHA, but so far these protocols have only been used to introduce substituents efficiently at maximum three positions (see SI for further synthetic considerations). So new synthetic protocols need to be developed for introducing substituents around the entire DHA core, and some suitable protecting groups need to be installed, for example to allow both amino and aldehyde functionalities in the same molecule. To avoid intermolecular reactions between such groups, it could be attractive to simply make 9 and 10 part of the monomeric repeat units of a polymer scaffold via the amine functionality. Organization of DHA units along a polymer may in fact possibly also enhance the energy density further as observed for some azobenzene-based materials. A Other design strategies will also be pursued in future work, such as replacement of the cyano groups at position 1 or the introduction of non-carbon atoms in the DHA scaffold (heterocyclic structures).