Phase-resolved two-dimensional spectroscopy based on collinear n-wave mixing in the ultrafast time domain.

We present a novel approach for femtosecond two-dimensional (2D) spectroscopy in the midinfrared combining a collinear beam geometry and phase-resolved detection. Two phase-locked pulses of variable time delay tau interact with the sample. The transmitted electric fields are measured in real time t by electro-optic sampling. 2D spectra are generated by Fourier transforming the signal along the two time axes tau and t. In the 2D spectra, nonlinear signals originating from different orders n in the electric field are separated. Such decomposition of the overall response is demonstrated by mapping the nonlinear response of intersubband transitions in GaAs/AlGaAs multiple quantum wells.