Synchro-Excited Free-Running Single Photon Counting: A Novel Method for Measuring Short-Wave Infrared Emission Kinetics.

Time-resolved measurements of short-wave infrared (SWIR) photoluminescence on the submicrosecond to millisecond scale are needed for physical and chemical studies involving singlet oxygen, single-walled carbon nanotubes, and other samples with weak, slow emission. We present here an alternative to the common method of time-correlated single photon counting (TCSPC) that is well suited to indium gallium arsenide avalanche photodiode (APD) detectors operated in Geiger mode. In the new method, termed synchro-excited free-running single photon counting (SEFR-SPC), excitation pulses from inexpensive laser diodes (providing a variety of wavelengths) are synchronized to detection events from a free-running detector covering the 900 to 1700 nm range. In contrast to traditional TCSPC, data from this method can be rigorously corrected for pile-up distortions, allowing operation with high excitation powers and low repetition rates. A technique is described to extend the system's dynamic range to approximately 108. We also show that SEFR-SPC provides state-of-the-art sensitivity in the SWIR spectral region and that spectrally filtered kinetic data can offer additional insights. A six-step correction protocol has been developed and implemented as a LabVIEW program for very accurate acquisition of kinetic shapes. The SEFR-SPC method will be a valuable tool for studies of weak, long-lived emission sources.