Journal of the Korean Chemical Society (대한화학회지)

Korean Chemical Society (대한화학회)
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The ab Initio Quantum Mechanical Investigation for the Weakly Bound $H^+_{2n+1}$(n=1-6) Complexes

약한 결합을 갖는 $H^+_{2n+1}$(n=1-6) complex들에 대한 순 이론 양자역학적 연구

  • 인은정 (한남대학교 이과대학 화학과) ;
  • 서현일 (한남대학교 이과대학 화학과) ;
  • 김승준 (한남대학교 이과대학 화학과)
  • Published : 20011000
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Abstract

The geometrical parameters, vibrational frequencies, and dissociation energies for $H_{2n+1}^+$ (n=1~6) clusters have been investigated using high level ab initio quantum mechanical techniques with large basis sets. The equilibrium geometries have been optimized at the self-consistent field (SCF), the single and double excitation configuration interaction (CISD), the coupled cluster with single and double excitation (CCSD), and the CCSD with connected triple excitations [CCSD(T)] levels of theory. The highest levels of theory employed in this study are TZ2P+d CCSD(T) up to $H^+_g$ and TZ2P CCSD(T) for $H_{11}^+$ and $H_{13}^+$. Harmonic vibrational frequencies are also determined at the SCF level of theory with various basis sets and confirm that all the optimized geometries are true minima. The dissociation energies, $D_e$, for $H_{2n+1}^+$ (n=26) have been predicted using energy differences at each optimized geometry and zero-point vibrational energies(ZPVEs) have been considered to compare with experimental dissociation energies, $D_0$.

$H_{2n+1}^+$ (n=1~6) cluster들에 대하여 높은 수준의 순 이론적(ab initio) 양자역학적 방법을 사용하여 분자 구조, 진동 주파수(vibrational frequency), 그리고 해리 에너지 등을 계산하였다. 분자구조는 $H^+_g$까지는 TZ2P+ d CCSD(T) 수준에서 그리고 $H_{11}^+$과 $H_{13}^+$에 대해서는 TZ2P CCSD(T) 수준까지 최적화하였다. 진동 주파수는 여러 basis set에서 SCF 방법으로 계산하였으며, 본 연구에서 최적화된 모든 분자구조들이 local minimum 구조임을 확인하였다. $H_{2n+1}^+$로부터 $H_2$ 의 해리 에너지($D_e$)는 각각의 최적화된 분자구조에서의 에너지 차로부터 계산하였으며, 영점 진동에너지(ZPVE)를 고려하여, 지금까지의 이론 및 실험결과($D_0$)와 비교하였다.

Keywords

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