Optical Properties of Few-Layer Ti₃CN MXene: From Experimental Observations to Theoretical Calculations

Despite the emerging interest in research and development of Ti₃CN MXene nanosheet (NS)-based optoelectronic devices, there is still a lack of in-depth studies of the underlying photophysical processes, like carrier relaxation dynamics and nonlinear photon absorption, operating in such devices, hindering their further and precise design. In this paper, we attempt to remedy the situation by fabricating few-layer Ti₃CN NSs <i>via</i> combining selective etching and molecular intercalation and by investigating the carrier relaxation possesses and broadband nonlinear optical responses <i>via</i> transient absorption and Z-scan techniques. These results are complemented by first-principle theoretical analyses of the optical properties. Both saturable absorption and reverse saturable absorption phenomena are observed due to multiphoton absorption effects. The analysis of these results adds to the understanding of the basic photophysical processes, which is anticipated to be beneficial for the further design of MXene-based devices.