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Article Abstract
Crystallographically, noncentrosymmetricity (NCS) is an essential precondition and foundation of achieving nonlinear optical (NLO), pyroelectric, ferroelectric, and piezoelectric materials. Herein, structurally, octahedral [SmCl] is substituted by the acentric tetrahedral polyanion [CdBr], which is employed as a templating agent to induce centrosymmetric (CS)-to-NCS transformation based on the new CS supramolecule [CdP][SmCl]Cl (1), thereby providing the NCS supramolecule [CdP][CdBr] (2). Meanwhile, this replacement further results in the host 2D [CdP] layers converting to yield the twisted 3D [CdP] framework, which promotes the growth of bulk crystals. Additionally, phase 2 possesses well-balanced NLO properties, enabling considerable second-harmonic generation (SHG) responses (0.8-2.7 × AgGaS) in broadband spectra, the thermal expansion anisotropy (2.30) together with suitable band gap (2.37 eV) primarily leading to the favorable laser-induced damage threshold (3.33 × AgGaS), broad transparent window, and sufficient calculated birefringence (0.0433) for phase-matching ability. Furthermore, the first polyanion substitution of the supramolecule plays the role of templating agent to realize the CS-to-NCS transformation, which offers an effective method to rationally design promising NCS-based functional materials.
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| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10685307 | PMC |
| http://dx.doi.org/10.1039/d3sc04818g | DOI Listing |
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