Abstract

Here, we present a detailed investigation on the synthesis and nonlinear multiphoton absorption properties of the colloidal solution of Au nanoclusters (AuNCs) which contains the atomic clusters, with the number of atoms per cluster (NAC) of only one (Au1NC) and two (Au2NC). These AuNCs are synthesized by an easy single step one-pot simple chemical process and by using dimethylformamide (DMF) both as reducer and stabilizer. The presence of both Au1NC and Au2NC are found in the sample by their distinct signature in the UV–Vis. absorption spectrum as well as in the high-resolution mass spectrum. The synthesized material has been found to exhibits a strong and stable blue-luminescence with a moderately high quantum yield (QY) of 12.4% when excited with UV light. The nonlinear optical two-photon absorption (2PA) properties of Au1, Au2NC solutions are being reported here by Z-scan studies, for the first time, by using both 10 ns and 100 fs pulse laser radiations having wavelength of 532 nm. It is significantly noted here that the synthesized AuNCs are found to exhibit reverse saturable absorption (RSA) when excited either by ns or by fs laser pulses. A high third-order nonlinear susceptibility (ꭓ(3)) of the order of 10−13 (esu) of the synthesized materials are obtained under fs laser excitation and it is attributed to the 2PA through electronic band to band transition. In contrast, the variation of the 2PA coefficient (β) with input intensity (I0) represents the footprint of free carrier involvement in the enhanced nonlinear absorption in the case of ns excitation. Furthermore, through the non-saturable nonlinear multiphoton absorption, the synthesized AuNCs exhibit excellent optical power limiting phenomenon with the limiting threshold (Fth) of 9.1 mJ/cm2 (fs excitation) and 2.02 J/cm2 (ns excitation) owing to their enhanced 2PA coefficient. Therefore, we believe that our synthesized ultra-small colloidal AuNCs can be used as the promising candidate material for advanced photonics application in the future.

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