The question, however, remains whether this behavior is driven by a charge transfer mechanism or by the heating effect. To answer this question, we further performed a control experiment by adsorbing the nanostructures on a smart micro heating substrate (Interherence GmbH), which allows a precise heating of the nanoparticles. We first reproduced our previous findings at room temperature while irradiating the sample continuously. As shown in Figure , the two peaks at 1391 and 1438 cm -1 are completely vanished after 10 minutes, while the other SERS peaks are relatively stable. This confirms the formation of a carbon nanomembrane a top of the black gold film. Further irradiation (1.5 h) of the sample disturbs this layer and leads to the formation of amorphous carbon layer, as evidenced by the appearance of the D-band at 1384 cm -1 . For the comparison with the temperature induced reaction, we conducted the reaction under heating in the dark, while the laser was only used to probe the reaction (less than 100 µW of laser power at the focal point). As seen in Figure , increasing the temperature from RT (~22 °C) to 122 °C leads to the loss of SERS signals gradually, without observation of any distinct Raman bands. This behavior is commonly associated with the thermal-driven desorption/degradation of the adsorbed molecules. At the same time, we observe that the initial vibration peaks are present throughout the study but losing intensity. Thus, these results confirm that the crosslinking reaction of the diazonium molecules into a carbon nanomembrane is mainly driven by the hotelectron transfer mechanism, Figure8c. While the pure thermal mechanism (by heating the sample in dark) leads to desorption and degradation of the reactant molecules.