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Hierarchical Contribution of Anions to Second Harmonic Generation in A2HgI4 (A = Na, Ag, Cu) Regulated Dramatically by Metal Cations
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2020-09-16 , DOI: 10.1021/acs.cgd.0c01134
Le Gao 1 , Tinghao Tong 1 , Kewang Zhang 1 , Jun Zhang 1
Affiliation  

Screening infrared (IR) nonlinear optical (NLO) materials remains an urgent concern, owing to the lack of efficient IR frequency-conversion materials with good NLO response. The deepened cognition of how cations regulate the contribution of anions to the SHG response is necessary to guide the exploration of IR NLO materials. In this work, the typical NLO materials A2HgI4 (A = Ag, Cu) were studied systematically by the first-principles method. It is shown that they exhibit excellent SHG responses d14 = 23.09 pm/V for Ag2HgI4 and d14 = 29.50 pm/V for Cu2HgI4, which are about two times the IR benchmark AgGaS2. A2HgI4 (A = Ag, Cu) also possess moderate band gaps of 2.38 and 2.04 eV. To analyze the regulation of A-site cation to the anions, two hypothetical compounds, α-Na2HgI4 and β-Na2HgI4, were designed via atom substitution, which maintain strong NLO response about d14 = 11.68 pm/V and d14 = 14.43 pm/V and larger band gaps (3.36 eV for α-Na2HgI4, 3.13 eV for β-Na2HgI4), respectively. Interestingly, these four compounds show hierarchical properties for differences in the A-site cation. The real-space atom-cutting (RSAC) method and SHG-density method reveal that the difference is not obtained directly from the change of A-site metals. Via the analysis of the electronic density method and SHG-density method, the iodine anions display hierarchical contributions to SHG response under the unexpected regulation by the A-site metals. Our findings offer a strategy to explore new NLO materials with desirable performances.

中文翻译:

阴离子对A 2 HgI 4(A = Na,Ag,Cu)中第二谐波产生的层次贡献受金属阳离子显着调节

由于缺少具有良好NLO响应的高效IR频率转换材料,筛选红外(IR)非线性光学(NLO)材料仍然是迫切需要解决的问题。对阳离子如何调节阴离子对SHG反应的贡献的加深认识对于指导IR NLO材料的探索是必要的。在这项工作中,通过第一原理方法系统地研究了典型的NLO材料A 2 HgI 4(A = Ag,Cu)。结果表明,它们对Ag 2 HgI 4的d 14 = 23.09 pm / V和对Cu 2 HgI 4的d 14 = 29.50 pm / V表现出优异的SHG响应约为IR基准AgGaS的两倍。2。A 2 HgI 4(A = Ag,Cu)也具有2.38和2.04 eV的中等带隙。为了分析A位阳离子的调节到阴离子,两个假设的化合物,α-的Na 2 HGI 4和β-的Na 2 HGI 4,分别经由原子取代,其中维持约强NLO响应设计d 14 = 11.68分/ V和d 14 = 14.43分/ V和较大的带隙(为3.36eV​​α-的Na 2 HGI 4,3.13 eV的β-的Na 2 HGI 4), 分别。有趣的是,这四种化合物对于A位阳离子的差异显示出层次特性。实空间原子切割(RSAC)方法和SHG密度方法表明,差异不是直接从A位金属的变化获得的。通过对电子密度法和SHG密度法的分析,在A位金属出乎意料的调节下,碘阴离子显示出对SHG反应的分层贡献。我们的发现为探索具有理想性能的新型NLO材料提供了一种策略。
更新日期:2020-11-04
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