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A laser, maybe, but definitely not LEDs. Vapor/gas lamps produce the narrowest frequency bands possible, because it comes from very well defined atomic transitions (Hz range). LEDs produce frequency bands with widths in the GHz/THz range, while semiconductor lasers can maybe reach KHz if they are really good. So, unfortunately, for this type of applications, vapor lamps would probably still be needed.
Source: I work with lasers and spectroscopy.
Edit: very good idea about using non-visible light!