In this communication, we wish to report on the use of synchronously mode-locked picosecond lasers in a pump-probe configuration for TL spectroscopy. The peak power for these picosecond lasers is very high and, of course, the fundamental of the dye laser (red beam) can be efficiently (~10%) doubled in frequency (U.V. beam) by second harmonic generation in nonlinear crystals. We use this generated U.V. beam as a probe to monitor the very weak absorption of the red beam. An arrangement [4] of the beams involving different waist positions for the pump and probe is used. This arrangement results in an enhancement of sensitivity (at least a factor of three to seven). Also, a different dependence of the signal on the cell position compared to the single beam method is obtained. Finally, we have obtained the Δν = 5 CH-stretching overtone absorption spectrum of liquid toluene with this method (see Figure 1). Suggestions are made regarding new applications of this picosecond pulse thermal lensing technique
