In this example of autonomous monitoring of Curtius rearrangement using NMR spectroscopy, the experimental protocol includes detailed documentation of monitoring techniques. Notably, the timing of reagent addition was determined by referencing the number of spectra collected. The complexity of the sampling technique may pose a barrier to proof-of-concept experimentations without autonomous monitoring tools. However, by prompting for calculation of actual reagent addition time using the sampling time interval, GPT-4 can comprehensively interpret the protocol and effectively generate a stepwise procedure as well as an iControl XML script with estimated reaction time (Fig. ). The iControl design was executed, and the reaction was monitored with online-HPLC (Fig. , zoomed initial 7-hour data in ESI † Fig. ).