Laser direct writing is an attractive method for patterning 2D materials without contamination. Literature shows that the ultrafast ablation threshold of graphene across substrates varies by an order of magnitude. Some attribute it to the thermal coupling to the substrates, but it remains by and large an open question. For the first time the effect of substrates on the femtosecond ablation of 2D materials is studied using MoS2 as an example. We show unambiguously that femtosecond ablation of MoS2 is an adiabatic process with negligible heat transfer to the substrates. The observed threshold variation is due to the etalon effect which was not identified before for the laser ablation of 2D materials. Subsequently, an intrinsic ablation threshold is proposed as a true threshold parameter for 2D materials. Additionally, we demonstrate for the first time femtosecond laser patterning of monolayer MoS2 with sub-micron resolution and mm/s speed. Moreover, engineered substrates are shown to enhance the ablation efficiency, enabling patterning with low-power ultrafast oscillators. Finally, a zero-thickness approximation is introduced to predict the field enhancement with simple analytical expressions. Our work clarifies the role of substrates on ablation and firmly establishes ultrafast laser ablation as a viable route to pattern 2D materials.
Transition metal dichalcogenides are known to possess large optical nonlinearities, and driving these materials at high intensities is desirable for many applications. Understanding their optical responses under repetitive intense excitation is essential to improve the performance limit of these strong-field devices and to achieve efficient laser patterning. Here, we report the incubation study of monolayer MoS2 and WS2 induced by 160 fs, 800 nm pulses in air to examine how their ablation threshold scales with the number of admitted laser pulses. Both materials were shown to outperform graphene and most bulk materials; specifically, MoS2 is as resistant to radiation degradation as the best of the bulk thin films with a record fast saturation. Our modeling provides convincing evidence that the small reduction in threshold and fast saturation of MoS2 originate from its excellent bonding integrity against radiation-induced softening. Sub-ablation damages, in the form of vacancies, strain, lattice disorder, and nanovoids, were revealed by transmission electron microscopy, photoluminescence, Raman, and second harmonic generation studies, which were attributed to the observed incubation in 2D materials. For the first time, a sub-ablation damage threshold is identified for monolayer MoS2 to be 78% of the single-shot ablation threshold, below which MoS2 remains intact for many laser pulses. Our results firmly establish MoS2 as a robust material for strong-field devices and for high-throughput laser patterning.
We report the first experiment on single-shot femtosecond laser ablation of monolayer hexagonal boron nitride (hBN). The observed intrinsic ablation threshold fluence is nearly 660 mJ/cm2, which is at least 10× higher than all other two-dimensional materials. Our work indicates the feasibility of hBN for femtosecond laser patterning.
Two pulse ablation experiments were conducted on monolayer MoS2 with various substrates. The hole size variation is explained via bandgap renormalization and carrier relaxation for different pulse separations.
Multi-shot ablation studies of monolayer MoS2 and WS2 reveal the record optical robustness of these materials where optical damage results in laser-induced vacancies that greatly affect their optical properties.
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