Optical pump terahertz probe spectroscopy (OPTP) is a versatile non-contact technique that measures transient photoconductance decays with femtosecond temporal resolution. However, its maximum temporal range is limited to only a few nanoseconds by the mechanical delay lines used. We extended the temporal range of OPTP to milliseconds and longer while retaining sub-nanosecond resolution. A separate pump laser was electrically synchronized to the probe pulses, allowing the pump–probe delay to be controlled with an electronic delay generator. We demonstrated the capabilities of this technique by examining the photoconductance decays of semiconductors with lifetimes ranging over six orders of magnitude: III-Vs, metal halide perovskites, germanium, and silicon. A direct comparison of results on silicon from OPTP and inductively coupled photoconductance decay highlighted the higher spatial and temporal resolution of OPTP, which allowed in-plane and out-of-plane carrier diffusion to be studied.

The perturbed free induction decay (PFID) observed in ultrafast infrared spectroscopy was used to unveil the rates at which different vibrational modes of the same atomic-scale defect can interact with their environment. The N₃VH⁰ defect in diamond provided a model system, allowing a comparison of stretch and bend vibrational modes within different crystal lattice environments. The observed bend mode (first overtone) exhibited dephasing times T₂=2.8(1)  ps, while the fundamental stretch mode had surprisingly faster dynamics T₂<1.7  ps driven by its more direct perturbation of the crystal lattice, with increased phonon coupling. Further, at high defect concentrations the stretch mode’s dephasing rate was enhanced. The ability to reliably measure T₂ via PFID provides vital insights into how vibrational systems interact with their local environment.