A nonlinear optical phenomenon, relativistic cross-phase modulation, is reported. A relativistically intense light beam ͑I = 1.3ϫ 10 18 W cm −2 , = 1.05 m͒ is experimentally observed to cause phase modulation of a lower intensity, copropagating light beam in a plasma. The latter beam is generated when the former undergoes the stimulated Raman forward scattering instability. The bandwidth of the Raman satellite is found to be broadened from 3.8-100 nm when the pump laser power is increased from

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... .45-2.4 TW. A signature of relativistic cross-phase modulation, namely, asymmetric spectral broadening of the Raman signal, is observed at a pump power of 2.4 TW. The experimental cross-phase modulated spectra compared well with theoretical calculations. Applications to generation of high-power single-cycle pulses are also discussed.