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Nonlinear optical (NLO) crystals are very important optoelectronic functional materials and their developments have significantly contributed to the progress of laser science and technology for decades. In order to explore new NLO crystals with superior performances, it is greatly desirable to understand the intrinsic relationship between the macroscopic optical properties and microscopic structural features in crystals. In this paper, the applications of density functional theory (DFT) method to the elucidation of the structure-property relationship and to the exploration on novel NLO materials in the ultraviolet and infrared spectrum regions are reviewed. The great success in the linear and NLO property predictions has been achieved using the first-principles computational simulations, and the mechanism understanding obtained by various analysis tools can give substantial guidance to the search and design of new NLO crystals. [ABSTRACT FROM AUTHOR]

With the development of laser technology and related scientific fields, understanding of the structure–property relationships in nonlinear optical (NLO) crystals is becoming more and more important. In this article, first-principles studies based on density functional theory, and their applications to elucidate the microscopic origins of the linear and NLO properties in NLO crystals, are reviewed. The ab initio approaches have the ability to accurately predict the optical properties in NLO crystals, and the developed analysis tools are vital to investigating their intrinsic mechanism. This microscopic understanding has further guided molecular engineering design for NLO crystals with novel structures and properties. It is anticipated that first-principle material approaches will greatly improve the search efficiency and greatly help experiments to save resources in the exploration of new NLO crystals with good performance. [ABSTRACT FROM AUTHOR]