Tailoring the band alignment of van der Waals (vdW) heterostructures is essential for regulating the electronic and optoelectronic performance of devices with superior functions. However, current band alignment engineering methods suffer from complexity, inflexibility, and limited tuning range, which hinders further applications. In this study, we demonstrate a novel strategy for tailoring the band alignment of BP/MoS₂ heterostructures using femtosecond (fs) laser-controlled band alignment engineering. Although this approach compromises the rectification ratio of heterostructures, it dramatically expands the tuning range of the band alignment and improves optoelectronic response by localized doping and healing effect at heterojunctions. We also present a new physical model to describe carrier transport behavior for m-n-p structures and investigate the effect of fs laser irradiation. Finally, two conceptual devices are demonstrated to show the advanced applications of this post-processing technique. In optoelectronic applications, we utilized this strategy to improve photoresponsivity (> 8 times), detectivity (∼1.48 ×10¹¹ Jones), and fill the response gap in the NIR region of photodetectors. In multivalued logic applications, site-specific engineering was used to transform the inverter operating mode from binary to ternary with a wide output swing (∼90%) by creating a unique NDT region. Our study demonstrates the potential of fs laser irradiation as a high-spatial-accuracy, air-stable, and versatile band alignment engineering method for electronic and optoelectronic applications in the future.

定制范德华 (vdW) 异质结构的能带排列对于调节具有卓越功能的器件的电子和光电性能至关重要。然而，当前的频带对齐工程方法存在复杂性、不灵活性和有限的调谐范围等问题，阻碍了进一步的应用。_{在这项研究中，我们展示了一种用于定制 BP/MoS 2}带对齐的新策略使用飞秒 (fs) 激光控制带对准工程的异质结构。尽管这种方法损害了异质结构的整流比，但它极大地扩大了带对准的调谐范围，并通过异质结处的局部掺杂和愈合效应改善了光电响应。我们还提出了一种新的物理模型来描述 mnp 结构的载流子传输行为并研究 fs 激光照射的影响。最后，演示了两个概念设备以展示此后处理技术的高级应用。在光电应用中，我们利用这种策略提高了光响应性（> 8 倍）、探测率（∼1.48 ×10 ¹¹琼斯），并填补了光电探测器近红外区域的响应间隙。在多值逻辑应用中，站点特定工程用于通过创建独特的 NDT 区域将逆变器操作模式从二进制转换为具有宽输出摆幅 (~90%) 的三元。我们的研究证明了 fs 激光照射作为未来电子和光电应用的高空间精度、空气稳定和多功能带对准工程方法的潜力。