Abstract: The invention provides surface plasmon resonance-mass spectroscopy for the rapid, sensitive and accurate investigation of molecular interactions coupled with the identification and quantification of the same. Methods of the invention include capturing an analyte present within a sample by an interactive surface layer on a real-time interaction analysis sensor, analyzing the analyte by surface plasmon resonance while the analyte is captured by the interactive surface layer, and identifying the captured analyte by desorbing/ionizing the analyte from the interactive surface layer while under vacuum within a mass spectrometer. Devices of the invention include a transparent material, a conductive material capable of supporting surface plasmon resonance affixed to the transparent material, an interactive surface affixed to the conductive material, and a means for exposing the interactive surface to the interior of a mass spectrometer without breaking the vacuum therein.