Brennendes Wasser, did you try isolating the Harmaline by recrystallization in EtOH or EtOAc? 

The database entry you created for Harmine/Harmaline lumps the two together as having the same solubility properties, and distinct from THH.

Harmine forms 1cm long off nearly clear shard like crystals after 2x re crystallization from EtOH. However, attempts at recrystallization of Harmaline from EtOH (same procedure as Harmine) result in a fine tan crystalline powder - evidently not nearly as pure.

Since Harmaline seems more soluble in EtOH as compared to Harmine, perhaps this could be another way to isolate the Harmine from Harmaline.