Non-Technical Summary<br/>When you wait to check out in a supermarket, do you ever wonder how the staff can scan everything so fast? 'Ding', one done. 'Ding', another done! You need barcodes printed on items and an infrared laser scanner! This is not the only example of infrared lasers used in our daily life! In addition to our daily life, infrared lasers have various important applications such as instrumental spectroscopy, optical sensing, optical imaging, and long-distance communications. To generate infrared lasers, one crucial and applicable way is via the nonlinear harmonic generation process, where two or more photons are merged together. The nonlinear harmonic generation process is incorporated into solid-state laser systems, which are compact, highly efficient, and reliable. The heart of the nonlinear harmonic generation process is the infrared nonlinear optical (IR NLO) material. With support through an MPS-LEAPS award, which is in part funded by the Established Program to Stimulate Competitive Research (EPSCoR), the principal investigator from Wichita State University employs the design, synthesis, discovery, optimization, and crystal growth of emerging inorganic compounds for IR NLO applications. Thus newly discovered materials are expected to be useful to generate IR lasers. The educational efforts of the award are to incorporate research into inorganic chemistry teaching and outreach activities via the development of a crystal museum, diverse hiring, development of a new class, and outreach activities to elementary schools. The PI builds a diverse team by hiring women researchers, African-American students, first generation college students, and other groups underrepresented in scientific fields.<br/><br/>Technical Summary<br/>Middle Infrared nonlinear optical materials (MIR NLO) have sparked growing interest due to their capability to extend infrared laser frequencies via the second harmonic generation process. This research project, supported by an MPS-LEAPS award, emphasizes employing various synthetic methods, achieving balanced NLO properties via different strategies, understanding electronic structures and bonding characteristics via TB-LMTO-ASA simulations, and growing large crystals. The proposed research advances the understanding of the structure-property relationships of inorganic compounds such as thiophosphates and uncovers promising MIR NLO materials. Thiophosphates are a class of materials combining sulfur and phosphorus. The PI and his research group tackle the exploration of thiophosphates as MIR NLO materials, which are aimed to replace current MIR NLO materials. Current MIR NLO materials have low laser damage thresholds and modest conversion efficiencies. The developed new materials are utilized to produce new frequencies of mid-IR lasers, which enables a wide range of spectroscopic studies in chemistry, biology, and physics, etc. The employed methodology of understanding crystal growth processes via in-situ powder X-ray coupled with differential scanning calorimetry tests shortens the “trial and error” process of crystal growth of new phases. Understanding how the electronic structure influences optical properties, and how geometry, topology, and defects affect electronic structure, helps build promising functional materials such as quantum materials, thermoelectric materials, etc. The long-term educational goal for the PI and his research group is to incorporate research into inorganic chemistry teaching, increase the diversity and inclusion of the PI’s research team, increase public engagement of chemistry, train next generation chemists, and support students from minority groups underrepresented in STEM.<br/><br/>This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.