Citation: LIU Chong, DU Rui, ZHAO Yan-Ying, WANG Hui-Gang, ZHENG Xu-Ming. Resonance Raman Spectroscopy of the Excited State Structural Dynamics of 6-N,N-Dimethyladenine[J]. Acta Physico-Chimica Sinica, ;2011, 27(01): 17-24. doi: 10.3866/PKU.WHXB20110132 shu

Resonance Raman Spectroscopy of the Excited State Structural Dynamics of 6-N,N-Dimethyladenine

1.
Key Laboratory of Advanced Textiles Materials and Manufacture Technology, and Engineering Research Center for Eco-dyeing and Finishing of Textiles, Ministry of Education, Department of Chemistry, Zhejiang Science and Technology University, Hangzhou 310018, P. R. China

Received Date: 13 August 2010
Available Online: 13 December 2010
Fund Project: 国家重点基础研究发展规划(973) (2007CB815203) (973) (2007CB815203) 国家自然科学基金(21033002, 20573097) (21033002, 20573097)浙江省自然科学基金(R405465)资助项目 (R405465)

The A- and B-band electronic excitations and the excited state structural dynamics of 6-N,N-dimethyladenine (DMA) were studied by resonance Raman spectroscopy and density functional theory calculations. The π_H→π_L^* transition is the main part of the A-band absorption and its calculated oscillator strength occupies 79% of the A-band absorption. n→Ryd and π_H→Ryd transitions where Ryd denotes the diffuse Rydberg orbital play important roles in the B-band electronic transitions and their calculated oscillator strengths occupy about 62% of the B-band absorption. The oscillator strength for the π_H→π_L^* transition, which dominates the A-band electronic transition only occupies about 33% of the B-band absorption. The foundamental vibrations of the purine ring deformation stretch plus the C8H/N9H bend mode ν₂₃ and the 5 member ring deformation stretch plus the C8H bend mode ν₁₃, and their overtones and combination bands occupy most of the A-band resonance Raman intensities. Therefore, the ¹π_Hπ_L^* excited state structural dynamics of DMA is mainly along the ν₂₃ and ν₁₃ reaction coordinates. The majority of the B-band resonance Raman intensities are dominated by the fundamental vibrations of ν₁₀, ν₂₉, ν₂₁, ν₂₆, ν₄₀, and their overtones and combination bands. This suggests the B-band excited state structural dynamics of DMA is mostly along the purine ring deformation, the C6N10 stretch, the N9H/C8H/C2H bend and the N(CH₃)₂ antisymmetric stretch. The appearance of ν₂₆ and ν₁₂ in the A-band resonance Raman spectrum is correlated to the Franck-Condon region ¹nπ^*/¹ππ^* conical intersection. The activation of ν₂₁ in the B-band resonance Raman spectrum is correlated to the Franck-Condon region ¹ππ^*/¹πσ_N9H^* conical intersection.
- 6-N,N-dimethyladenine,
- Excited state structural dynamics,
- Resonance Raman spectrum,
- Electronic transition
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沈阳化工大学材料科学与工程学院沈阳 110142