Ag[SC(NH₂)₂]₂F: A Laser Damage-Tolerant Infrared Nonlinear Optical Material

Abstract

Mild hydrothermal reactions of π-conjugated SC(NH2)2, Ag(NO3), and NaF afforded a new prospective infrared (IR) nonlinear optical (NLO) crystal, namely, Ag[SC(NH2)2]2F. It shows a 3D open framework consisting of corner-sharing AgS4 tetrahedra with six-member ring tunnels that are filled by organic groups of the SC(NH2)2 molecules. Ag[SC(NH2)2]2F maintains 80% transmittance in the spectral region of 0.32–5.91 μm and features large second harmonic generation (SHG) responses with phase-matching at both 1064 nm (15.8 × KH2PO4) and 2.05 μm (0.7 × AgGaS2). It also exhibits a large band gap of 4.19 eV, resulting in a high laser-induced damage threshold (LIDT) of 9.3 times that of AgGaS2. Theoretical calculation revealed that SC(NH2)2, AgS4 tetrahedra, and F– anions all give the positive contribution to SHG effects. Ag[SC(NH2)2]2F overcomes the small band gap and low LIDT of tetrahedral-based chalcogenides while maintaining a large SHG response. This work gives a promising facile design strategy for IR NLO materials.

Ultraviolet Crystal with Strong Optical Nonlinearity by Creating Halogen-Centered Secondary Building Blocks

“…The ultraviolet (UV) nonlinear optical (NLO) crystal is the core and urgently required device in the all-solid-state laser industry, which is capable of converting the finite incident light source to a shorter wavelength spectral range based on the multistage nonlinear process. − Although numerous efforts have been done for decades, only a few UV NLO crystals have been proven feasible in practical application since three crucial but mutually restrictive optical indexes that are determined by different microstructures are needed to be met simultaneously, − that is, large second-harmonic generation (SHG) response (>1 × KDP) with a noncentrosymmetric crystal structure as a prerequisite, short cutoff edge (<200 nm), and appropriate birefringence to realize phase matching.…”

Na2CeF6: A Highly Laser Damage‐Tolerant Double Perovskite Type Ce(IV) Fluoride Exhibiting Strong Second‐Harmonic Generation Effect

“…[14][15] The NLO halides with wide bandgaps have aroused much attention. [16][17][18][19][20] In the last period, several NLO halides including Ag 2 HgI 4 , [21] RbHgI 3 , [22] KHgI 3 •H 2 O, [24] CsHgBr 3 , [23,27] Cs 2 HgI 2 Cl 2 , [25] HgBr 2 , [22] Rb 2 CdBr 2 I 2 , [26] NH 4 HgBr 3 •H 2 O, [28] CsGeCl 3 , [29] Rb 2 CdBrI 3 , [30] KBi 4 F 13 , [31] Pb 7 F 12 Cl 2 , [32] and NaSb 3 F 10 [33] have been discovered, and some of them exhibit large LIDTs (over 20 times that of AGS) and strong SHG effects, such as NH 4 HgBr 3 •H 2 O, Rb 2 CdBrI 3 , and NaSb 3 F 10 . Considering the better stability and larger band gaps for fluorides among halides, the introduction of the F element appears feasible to explore materials with large LIDTs and excellent NLO effects.…”

The Electronic Properties of Cadmium Naphthalene Diimide Coordination Complex

“…Transition-metal complexes based on these materials have taken a prominent position due to their improved electrical and structural properties, as well as polarizability coefficient [11,12]. Due to desirable properties such as ease of synthesis, transparency, strength, and increased thermal stability, π-conjugated metal-organic compounds along amidic group-based electro-opto materials with significant first or second hyperpolarizabilities had piqued researchers' interest [13,14]. To obtain ultrarapid high hyperpolarizability response, a wide range of conventional techniques have been used, including donoracceptor bridge system [15,16], diradical character [17], octupolar molecules [18], and excess electron model.…”