Pimsleur’s strength is at the beginner level; after that, it would be better to have something a bit more sophisticated. Anyhow, the next step might be Michelle Thomas (you might find some samples on Youtube). Rutledge has books (their “Colloquial” series) with the audio available online for free at their site. I’ve heard good things about Assimil, but have never tried it. Spanish and French are both extremely well covered, and have phonetic spelling systems, so once your pronunciation is OK, you can start using immersion-method language textbooks and graded readers (as Loki suggests). You should also start looking for listening material, preferably level-appropriate (podcasts, Deutsche-Welle is excellent for German) perhaps starting with songs you like.