Development of a broadband picosecond infrared spectrometer and its incorporation into an existing ultrafast time-resolved resonance raman, UV/visible, and fluorescence spectroscopic apparatus

We have constructed a broadband ultra fast time-resolved infrared (TRIR) spectrometer and incorporated it into onr existing time-resolved spectroscopy apparatus, thus creating a single instrument capable of performing the complementary techniques of femto-/pi-cosecond time-resolved resonance Raman (TR₃), fluorescence, and UV/visible/infrared transient absorption spectroscopy. The TRIR spectrometer employs broadband (150 fs, ~150 cm^-1 FWHM) mid-infrared probe and reference pulses (generated by difference frequency mixing of near-infrared poises in type I AgCaS₂), which are dispersed over two 64-element linear infrared array detectors (HgCdTe). These are coupled via custom-built data acquisition electronics to a personal computer for data processing. This data acquisition system performs signal handling on a shot-by-shot basis at the 1 kHz repetition rate of the pulsed laser system. The combination of real-time signal processing and the ability to normalize each probe and reference pnlse has enabled os to achieve a high sensitivity on the order of AOD ~ 10^-4-10^-5 with 1 min of acqui-ition time. We present preliminary picosecond TRIR studies using Jiis spectrometer and also demonstrate how a combination of TRIR and TR³ spectroscopy can provide key information for the full elucidation of a photochemical process.