Deep-ultraviolet (DUV) nonlinear optical (NLO) crystal is indispensable in current DUV all-solid-state laser technology, which is the key device to generate DUV light by frequency conversion. Due to stringent criteria, DUV NLO crystals are scarce and their discovery faces a big challenge. Although KBe₂BO₃F₂ (KBBF) is already excellent for current uses, the development of DUV science requires the materials with shorter output wavelengths and larger NLO effects, so as to meet the needs of DUV lasers with higher precision and higher power. Therefore, how to efficiently design DUV NLO materials has always been the core issue in NLO materials science. Looking back on the development of NLO materials, it turns out that theoretical modeling and simulation is an effective and efficient method, not only for mechanism understandings, but also for experimental exploration. In this article, in order to accelerate the process of DUV materials discovery, we summarize and propose a powerful computeraided modeling system and design blueprint that can be used to evaluate the DUV NLO performance in a faster way than pure experiments. With this in hand, we enrich the understanding of NLO structure-property correlation, and systematically prospect the DUV NLO properties on the basis of many existing and designed structures according to different structural types and chemical compositions. Seven novel structures are predicted for the first time to exhibit potential DUV NLO capabilities. All the results enable us to believe that the computer-aided modeling blueprint will play an important role in the exploration of new DUV NLO crystals.

在当前的DUV全固态激光技术中，深紫外（DUV）非线性光学（NLO）晶体是必不可少的，这是通过频率转换产生DUV光的关键设备。由于严格的标准，DUV NLO晶体稀缺，其发现面临巨大挑战。虽然KBe ₂ BO ₃ F ₂（KBBF）已经非常适合当前使用，DUV科学的发展要求材料具有更短的输出波长和更大的NLO效应，以便满足具有更高精度和更高功率的DUV激光器的需求。因此，如何有效设计DUV NLO材料一直是NLO材料科学领域的核心问题。回顾NLO材料的发展，结果表明，理论建模和仿真不仅对机理的理解而且对实验的探索都是一种有效的方法。在本文中，为了加快DUV材料的发现过程，我们总结并提出了一个功能强大的计算机辅助建模系统和设计蓝图，可用于以比纯实验更快的方式评估DUV NLO性能。有了这个，我们丰富了对NLO结构性质相关性的理解，并根据许多现有和设计的结构，根据不同的结构类型和化学组成，系统地研究了DUV NLO性质。首次预测了七个新颖的结构，它们具有潜在的DUV NLO功能。所有结果使我们相信，计算机辅助建模蓝图将在探索新型DUV NLO晶体中发挥重要作用。