Two-dimensional electronic spectroscopy with double modulation lock-in detection: enhancement of sensitivity and noise resistance

In many potential applications of two-dimensional (2D) electronic spectroscopy the excitation energies per pulse are strictly limited, while the samples are strongly scattering. We demonstrate a technique, based on double-modulation of incident laser beams with mechanical choppers, which can be implemented in almost any non-collinear four wave mixing scheme including 2D spectroscopy setup. The technique virtually eliminates artifacts or "ghost" signals in 2D spectra, which arise due to scattering and accumulation of long-lived species. To illustrate the advantages of the technique, we show a comparison of porphyrin J-aggregate 2D spectra obtained with different methods following by discussion. (C) 2011 Optical Society of America