Ultraflat Langmuir-Blodgett assembled graphene oxide saturable-absorber films for pulsed near-infrared laser generation

Large-scale production of ultraflat broadband saturable-absorber films is highly desired for passive mode-locked solid-state lasers. However, the current vapour deposition and spin coating routes for fabricating saturable absorbers (SAs) are suffering from the limited flexibility in substrate choice and complexity of mass production processes. Here, we demonstrate an ultraflat carboxyl-functionalized graphene oxide (GO-COOH) SA film via Langmuir-Blodgett (LB) assembly for solid state laser mode-locking. Hydrophilic carboxyl groups from GO sheets weaken the aggregation effect thus contribute to the uniform and stable dispersion of GO sheets in water. Such GO suspensions are made into an ultrathin large-area graphene-based SA film by a LB assembly process ensuring high surface uniformity. The room-temperature and highly repeated operation for GO LB films avoids the thermal damage of GO sheets and improves the membrane repeatability. Consequently, the ultrathin GO-COOH SA shows the modulation depth (2.3%) and low saturation intensity (24.7 KW cm-2) under 1064 nm laser irradiation. By inserting the GO SA into a Nd:GdVO4 laser, both passive Q-switched (QS) and passive Q-switched mode-locked (QML) operations are also attained. The slope efficiency of QS laser is up to 35.6% and the maximum single pulse energy is 1.48 μJ. In particular, the QML pulses can be achieved stably and repeatedly with an average output power of 1.33 W and a pulse energy of 13.2 nJ. Our strategy provides a new concept for improving the modulation stability of graphene-based SAs and promoting their industrial application in pulsed solid-state lasers.