Hey there
so what do you exactly try to do?
Peganum Harmala has some alkaloids inside - mostly people are after the classic 'Harmalas' which is Harmin + Harmalin.
So in any regular case people are trying to extract just those. There are many TEKs out there to get these 2 alkaloids specificially. Most easily just check for the megathread: *Verification on the VDS protocols*.
That will exactly tell how to extract the alkaloids inside the seeds of that plant. They are responsible for any effect that people are trying to accomplish when administering extracts from that plant.
Is that what you are searching for?
You are specificially asking for crystals. As harmala alkaloids are normally just meant to enhance the psychedelic experience of monoamines like DMT there would be no benefit to get your harmala alkaloids exceptionally in crystalline form.
So just extract them *the regular way* and you are good. If you are really seeking for a crystalline form (which is rather cosmetically) you can extract them and dissolve them in a minimal amount of dimethyl sulfoxide. Then just wait over 4-5 days and then they will precipitate in a crystalline form. But a lot of stuff will stay back in solution. So apart from being truly crystalline you will not have many benefits.