Controlling isomer population using a dual-oscillator infrared free-electron laser

We report on the control and characterization of the isomer population of ions inside superfluid helium nanodroplets, using two-color operation of a dual-oscillator infrared free-electron laser. The timing of both lasers is highly synchronized, and their frequencies (or “colors”) can be tuned independently over a wide range. Interaction of the singly deuterated proton-bound dimer of dihydrogen phosphate and formate inside helium nanodroplets with both colors enables the control over its isomer population and the recording of - one-color hidden - infrared spectra of individual isomers.