Balanced Second-Order Nonlinear Optical Properties of Adducts CHI₃·(S₈)₃ and AsI₃·(S₈)₃: A Systematic Survey

Abstract

Two isostructural adducts CHI 3 •(S 8 ) 3 (1) and AsI 3 •(S 8 ) 3 (2) are synthesized by a simple solution method. Both of them crystallize in noncentrosymmetric R3m, featuring van der Waals interaction linked CHI 3 tetrahedra or SbI 3 trigonal pyramids with crown-like S 8 molecules. Both 1 and 2 show strong SHG responses and phase matchability under either 1.064 or 2.1 μm. The results of DFT calculations indicate that the electron transfer happens from S-3p to I-5p orbitals, and both of them demonstrate indirect band gaps. The NLO effects of 1 and 2 are almost fully contributed from the CHI 3 or AsI 3 units. Compared with AgGaS 2 , their powder laser damage thresholds are ca. 15 and 51 times higher.

(Na0.60Ba0.70)Ga2Se4: An Infrared Nonlinear Optical Crystal Designed using AgGaSe2 as the Template

“…19 To better understand the potential of 1, the LIDT for the powder samples of 1 and AGS comprised of 75−100 μm particles was measured under 1064 nm. 21 The results indicate an LIDT of 6.13 MW/cm 2 for 1, ∼2.4 times that of AGS (2.55 MW/cm 2 ). It must be mentioned that, especially for IR NLO materials, their LIDT values are not just determined by their band gaps.…”

“…On the other hand, the substitution of Na by the other heavier alkali metals may have a positive effect . To better understand the potential of 1 , the LIDT for the powder samples of 1 and AGS comprised of 75–100 μm particles was measured under 1064 nm . The results indicate an LIDT of 6.13 MW/cm 2 for 1 , ∼2.4 times that of AGS (2.55 MW/cm 2 ).…”

Density Functional Theory Investigation of Nonlinear Optical Properties of T-Graphene Quantum Dots

“…Designing novel materials with excellent nonlinear optical (NLO) properties has been a hot topic from several years in view of their potential application in various optical and electro-optical devices. − Among these materials, carbon-based nanomaterials, such as fullerenes, carbon nanotubes, graphene, graphyne, graphdiyne, etc. are widely used to design nonlinear optical material due to the presence of delocalized π-electron in it. − Progress in the field of NLO material depends on characterization and synthesis of chromophore, which has large first or higher-order hyperpolarizabilities .…”

Bulk polarity of 3,5,7-trinitro-1-azaadamantane mediated by asymmetric NO2(lone pair)...NO2(π-hole) supramolecular bonding

“…For comparison, the polar structures of pyroelectric and piezoelectric material -LiIO 3 (Svensson et al, 1983), a lowtemperature polymorph of CHI 3 (Bertolotti & Gervasio, 2013) and high-pressure phases of CHCl 3 and CHBr 3 (Dziubek & Katrusiak, 2008) incorporate C 3v -symmetric pyramidal moieties, which combine an acentric structure and the ability to generate polar shape-complementary stacks. Adducts of SbX 3 (X = Cl or Br) with 1,3,5-trithiane (Lindemann et al, 1977) and the NLO-active (NLO is nonlinear optical) materials CHI 3 Á3(S 8 ) and AsI 3 Á3(S 8 ) (Lu et al, 2019) are examples of bulk polarity generated when different kinds of polar stacks are combined in the structure of a cocrystal. In this view, trigonal crystal structures composed of three different polar stacks could be especially interesting due to a further break of symmetry.…”