“…[2][3][4][5][6][7][8][9] Specifically, this class of compounds are known to exhibit very large hyperpolarizability tensor β ijk components (i.e., first-order NLO responses) along the direction of charge transfer, [10][11][12][13][14] and their applications include, e.g., frequency doubling of low power diode lasers, electrooptic modulation, optical signal processing, imaging enhancements, and frequency upconversion lasing. 15 But despite all the interest and research around NLO, the design of materials with tailor-made optical properties remains challenging.…”