I tend to pick them when there is a noticeable yellow blush to them (maybe half yellow). Perhaps, though, that's just because that's when I notice them. With limequats, and kumquats and their hybrids in general, I think you have significant latitude in timing your harvest (moreso than some mandarins, e.g.) - especially, in the case of limequats, if you are using them for juice. For eating, you might wait until they have fully turned.