【摘 要】
：
In electride molecules with multi-excess electrons,unusual manipulative effects of spin multiplicity and excess electron number on structure and static first hyperpolarizability(β0)are revealed for th
【机 构】
：
State Key Laboratory of Theoretical and Computational Chemistry Institute of Theoretical Chemistry,J
论文部分内容阅读
In electride molecules with multi-excess electrons,unusual manipulative effects of spin multiplicity and excess electron number on structure and static first hyperpolarizability(β0)are revealed for the first time.(1)The low spin multiplicity(ground state)for linear structures(1L2 and 2L3)brings molecular bend.(2)The low spin structure 2L3 with considerable β0 of 4540 ×104 au is larger by 4100 times than that of 1.1×104 au with high spin structure 4L3.(3)The β0 value acceleratedly increases with increasing of excess electron number.A further clue for understanding the spin multiplicity effect on β0 is revealed that low spin multiplicity-forming double occupied orbital-changing properties of electron transition(or electron density distribution)-enhancing the static first hyperpolarizability.This work will also enlighten new electronic perspective on new NLO molecule investigation field including the manipulations of spin multiplicity and excess electron number for electride molecules.
其他文献
采用ONIOM2(B3LYP/6-31G(d,p)：HF/3-21)计算方法研究了全氟辛酸气相热解消除HF的反应历程.计算结果表明,全氟辛酸(C7F15COOH)在气相中的热解反应可以通过六元环反应机理(通道1、2)、五元环反应机理(通道3、4)、直接脱CO、CO2反应机理(通道5、6)平行进行得到产物；其中以五元环反应机理进行反应生成CO和CF3(CF2)5CFO的活化势垒最低,为主反应通道(通
Based on our previous work,[1,2,3,4] the computational study on the detailed mechanism of NHC-catalyzed enantioselective [4+2] annulation of oxidized enals and azodicarboxylates[5](Scheme 1)has been p
The mechanisms of the palladium-catalyzed hydrothiolation of aliphatic and aromatic alkynes with aliphatic and aromatic thiols have been investigated using density functional theory calculations done
Tsuji and co-workers first reported the Cu-catalyzed silacarboxylation of internal alkynes utilizing CO2 and silylborane affording two isomeric silalactone products P1 and P2 with high regioselectivit
Corroles,as the ring-contracted analogues of porphyrins have attracted considerable attentions recently owing to their novel electronic,catalytic,and photoelectronic properties.Herein we systematicall
H2S 约占煤气中含硫气体的90％,这些气体不仅造成环境污染,而且导致后续煤化工过程中催化剂中毒和设备腐蚀,因此煤气中H2S 的脱除引起了广泛关注.氧化铈被誉为第二代高温脱硫剂,且在多次脱硫再生循环中保持良好的脱硫活性[1,2].为了了解氧化铈脱除H2S 的本质,本研究采用量子化学密度泛函理论方法(DFT+U)系统研究了H2S、SH、S 和H 原子在完美和O 空缺CeO2(110)表面的吸附和解离
The water-mediated neutral hydrolysis mechanisms of carbonyl sulfide(OCS)and carbon disulfide(CS2)has been re-examined by using the hybrid supramolecule/continuum models with n = 2-8 explicit water cl
自从1972年日本的藤岛昭教授发现了氧化钛单结晶在光照射的情况下可以把水分解为氧气和氢气[1]以来，光催化技术在有机物的降解、水污染的处理、空气的净化等方面都去得了重大的进展[2].但是，光催化剂在应用方面主要会遇到以下几个问题：1.大多数光催化剂所需的催化条件是紫外光，这在很大程度上限制了光催化剂的应用范围；2.光电子的迁移率比较低，即光催化剂的催化效率较低；3.能否有效的抑制光生电子-空穴对的
Zeolites are crystalline porous materials,which have widespread applications in industry.The synthesis methods,structure and acid properties of zeolites are important factors,which influences the appl
Solar energy,a renewable energy source,is generally considered as the most promising way tosolve the global energy crisis.Since O Regan and Gra tzel announced a high solar energyconversion efficiency(