All-Organic Composite Films for High Flexibility and Giant Nonlinear Optical Limiting Responses

Given the substantial pi-electron delocalization observed in 4-N,N-dimethylamino-4'-N'-methyl-stilbazolium tosylate (DAST), a high third-order nonlinear optical response can be expected that might manifest itself in various ways for potential applications. To probe the possibility and assess its potential, all-organic DAST-polymethyl methacrylate (PMMA) composite films were prepared by a simple solution casting method, and their nonlinear absorption performances were measured by an open aperture Z-scan system. The results reveal that under irradiation by a 380 fs laser pulse at 520 nm or a 6 ns laser pulse at 532 nm, the DAST-PMMA composite films with a DAST concentration of 0.125 wt % exhibit similar giant optical limiting (OL) responses with OL threshold of 7.84 or 0.37 GW cm-2, both superior to those of most organic and inorganic OL materials measured under similar conditions. These all-organic composite films show high flexibility, and interestingly, their OL responses can remain stable even after exposure to air for 3 months. The superior OL behaviors of such materials in the femtosecond and nanosecond regimes are attributed to the two-photon absorption and the combination of two-photon absorption and excited-state absorption, respectively. The simple preparation, high flexibility, giant OL responses, and excellent environmental stability suggest that such novel all-organic composite films hold great potential for applications in flexible OL devices.