The magnitude of T-jumps in partially hydrated zeolite systems were measured through the use of temperaturerelated changes in the positioning of the ν(SiOD) silanol mode. This allows us to determine that our approach is able to produce T-jumps of ≥ 50 °C from a pump energy input of 70 μJ in the bare zeolite. Even larger temperature changes are achievable at temperatures where the sample contains adsorbed water, increasing absorption of the pump laser light. Use of multiplepulse pumping allows temperature jumps to be extended to achieve arbitrarily large increases in temperature while still providing nanosecond-resolution information on the sample at each temperature. The rate of cooling of the sample is unaffected by starting temperature in cases where the sample contains ≤ 1 water molecule per acid site and results in the sample remaining at least 10 °C above base temperature for > 1 ms in all cases. Owing to the increased presence of water clusters, low starting temperatures show decreased T-jump magnitude and slower recovery. One particular feature of interest not explained in this paper is the weaker than expected appearance of free Brønsted site in the transient infrared data upon loss of hydrogen bonded Brønsted site. Further tests will be required to determine whether this is due to laser induced deprotonation of the Brønsted site.