Recently, there has been substantial interest in the large-scale synthesis of hierarchically architectured transition metal dichalcogenides and designing electrodes for energy conversion and storage applications such as electrocatalysis, rechargeable batteries, and supercapacitors. Here we report a novel hybrid laser-assisted micro/nanopatterning and sulfurization method for rapid manufacturing of hierarchically architectured molybdenum disulfide (MoS₂) layers directly on molybdenum sheets. This laser surface structuring not only provides the ability to design specific micro/nanostructured patterns but also significantly enhances the crystal growth kinetics. Micro and nanoscale characterization methods are employed to study the morphological, structural, and atomistic characteristics of the formed crystals at various laser processing and crystal growth conditions. To compare the performance characteristics of the laser-structured and unstructured samples, Li-ion battery cells are fabricated and their energy storage capacity is measured. The hierarchically architectured MoS₂ crystals show higher performance with specific capacities of about 10 mAh cm⁻², at a current rate of 0.1 mA cm⁻². This rapid laser patterning and growth of 2D materials directly on conductive sheets may enable the future large-scale and roll-to-roll manufacturing of energy and sensing devices.

Direct growth and patterning of atomically thin two-dimensional (2D) materials on various substrates are essential steps towards enabling their potential for use in the next generation of electronic and optoelectronic devices. The conventional gas-phase growth techniques, however, are not compatible with direct patterning processes. Similarly, the condensed-phase methods, based on metal oxide deposition and chalcogenization processes, require lengthy processing times and high temperatures. Here, a novel self-limiting laser crystallization process for direct crystallization and patterning of 2D materials is demonstrated. It takes advantage of significant differences between the optical properties of the amorphous and crystalline phases. Pulsed laser deposition is used to deposit a thin layer of stoichiometric amorphous molybdenum disulfide (MoS₂) film (~3 nm) onto the fused silica substrates. A tunable nanosecond infrared (IR) laser (1064 nm) is then employed to couple a precise amount of power and number of pulses into the amorphous materials for controlled crystallization and direct writing processes. The IR laser interaction with the amorphous layer results in fast heating, crystallization, and/or evaporation of the materials within a narrow processing window. However, reduction of the midgap and defect states in the as crystallized layers decreases the laser coupling efficiency leading to higher tolerance to process parameters. The deliberate design of such laser 2D material interactions allows the self-limiting crystallization phenomena to occur with increased quality and a much broader processing window. This unique laser processing approach allows high-quality crystallization, direct writing, patterning, and the integration of various 2D materials into future functional devices.