Manipulative effects of spin multiplicity and excess electron number on the structure and nonlinear optical response
【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 the first time.(1)The low spin multiplicity(ground state)for linear structures(1L2 and2L3)brings molecular bend.(2)The low spin structure 2L3 with considerableβ0 of 4540×104 au is larger by 4100 times than that of 1.1×104 au with high spin structure 4L3.(3)Theβ0 value acceleratedly increases with increasing of excess electron number.A further clue for understanding the spin multiplicity effect onβ0 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.