The physical chemistry laboratory is sometimes constrained to one semester, resulting in pedagogical deficiencies for the students taking the course. The use of a multidimensional laboratory exercise offers students the opportunity to encounter multiple experimental techniques and physical chemistry concepts while not sacrificing a significant amount of time. Here, we show that the classic binary liquid-vapor phase diagram experiment can be modified to incorporate both molecular spectroscopy and quantum chemistry. Using Raman spectroscopy as a means of detection and quantum chemistry to investigate the resulting vibrational spectra, students can explore three important subject areas in one laboratory exercise. (Contains 5 figures.)