物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2013年
5期
920-928
,共9页
周和根%温兴伟%方振兴%李奕%丁开宁%黄昕%章永凡*
週和根%溫興偉%方振興%李奕%丁開寧%黃昕%章永凡*
주화근%온흥위%방진흥%리혁%정개저%황흔%장영범*
AgGaS2-AgGaSe2固溶体%密度泛函理论%电子结构%二阶倍频效应%光学性质
AgGaS2-AgGaSe2固溶體%密度汎函理論%電子結構%二階倍頻效應%光學性質
AgGaS2-AgGaSe2고용체%밀도범함이론%전자결구%이계배빈효응%광학성질
AgGaS2-AgGaSe2 solid solution%Density functional theory%Electronic structure%Second harmonic generation%Optical property
采用基于赝势平面波基组的密度泛函理论方法,对一系列具有黄铜矿结构的AgGa(S1-xSex)2固溶体的构型、电子结构、线性和二阶非线性光学性质进行了系统研究.结果表明,各固溶体具有类似的能带结构,体系带隙随x值增加而逐渐减小.当所引入的Hartree-Fock交换项贡献为22.56%时,对应的杂化PBE泛函得到的带隙值与实验结果相近.固溶体的各种光学性质,包括折射率、双折射率、反射率、吸收系数和二阶倍频系数等均随着组成的改变呈现出有规律的变化趋势,变化范围介于AgGaS2和AgGaSe2二者之间.因此,利用固溶体光学性质的变化规律,可从中寻找出具有特定光学性能的晶体材料.
採用基于贗勢平麵波基組的密度汎函理論方法,對一繫列具有黃銅礦結構的AgGa(S1-xSex)2固溶體的構型、電子結構、線性和二階非線性光學性質進行瞭繫統研究.結果錶明,各固溶體具有類似的能帶結構,體繫帶隙隨x值增加而逐漸減小.噹所引入的Hartree-Fock交換項貢獻為22.56%時,對應的雜化PBE汎函得到的帶隙值與實驗結果相近.固溶體的各種光學性質,包括摺射率、雙摺射率、反射率、吸收繫數和二階倍頻繫數等均隨著組成的改變呈現齣有規律的變化趨勢,變化範圍介于AgGaS2和AgGaSe2二者之間.因此,利用固溶體光學性質的變化規律,可從中尋找齣具有特定光學性能的晶體材料.
채용기우안세평면파기조적밀도범함이론방법,대일계렬구유황동광결구적AgGa(S1-xSex)2고용체적구형、전자결구、선성화이계비선성광학성질진행료계통연구.결과표명,각고용체구유유사적능대결구,체계대극수x치증가이축점감소.당소인입적Hartree-Fock교환항공헌위22.56%시,대응적잡화PBE범함득도적대극치여실험결과상근.고용체적각충광학성질,포괄절사솔、쌍절사솔、반사솔、흡수계수화이계배빈계수등균수착조성적개변정현출유규률적변화추세,변화범위개우AgGaS2화AgGaSe2이자지간.인차,이용고용체광학성질적변화규률,가종중심조출구유특정광학성능적정체재료.
Density functional theory (DFT) based on the plane wave basis set was used to investigate the geometries, electronic structures, and linear and second-order nonlinear optical properties of a series of AgGa(S1-xSex)2 solid solutions with chalcopyrite structures. The compounds showed similar band structures, and band gaps decreased with increasing x value. When 22.56%Hartree-Fock exchange was employed, the solid solution band gaps predicted by hybrid PBE functionals were consistent with experimental values. The optical properties of AgGa(S1-xSex)2 solid solutions, including refractive index, birefringence, reflectivity, adsorption coefficient, and second harmonic generation coefficient, changed regularly with composition. The range of variation was between that for AgGaS2 and AgGaSe2. The results indicated that crystals with specialized optical performances could be designed.