We report the observation of a three-photon resonant transition of charge-carrier spins in an organic light-emitting diode using electrically detected magnetic resonance (EDMR) spectroscopy at room temperature. Under strong magnetic-resonant drive (drive field $B_1\sim$ static magnetic field $B_0$), a $B_0$-field swept EDMR line emerges when $B_0$ is approximately three times the one-photon resonance center. Ratios of drive-induced shifts of this line to the shifts of two- and one-photon lines agree with analytical expressions derived from the Floquet Hamiltonian and confirm the nature of these three-photon transitions, enabling access of spin physics to a hitherto inaccessible domain of quantum mechanics.

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• Carrier generation & recombination
• Multiphoton or tunneling ionization & excitation
• Spin dynamics
• Floquet systems
• Organic LEDs
• Electron paramagnetic resonance
• Electron spin resonance