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OrphanWilde comments on Rationalist Lent - Less Wrong Discussion
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Tried it; the most awesome part about not taking caffeine anymore, for me, was the fact that one cup of coffee would then do as much as five previously.
The downside is that I did not, in fact, feel less groggy generally, even after adjusting. Even with my high tolerances a caffeinated life is more energetic than a non-caffeinated life. I'm sticking with caffeine.
What I do is being liberal with caffeine on weekdays but almost completely abstaining from it at weekends.