Citation: Sha Guo-He, Zhang Cun-Hao. Quantum Interference Effect in Collision－induced Intramolecular Energy Transfer within Singlet-triplet Mixed States[J]. Acta Physico-Chimica Sinica, ;2004, 20(08S): 1010-1016. doi: 10.3866/PKU.WHXB200408zk18 shu

Quantum Interference Effect in Collision－induced Intramolecular Energy Transfer within Singlet-triplet Mixed States

1.
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023

Received Date: 23 March 2004
Available Online: 15 August 2004

The principle of wave-particle duality of quantum mechanics ascertains that any microscopic particle must also exhibit wave properties. The matter wave, or de Broglie wave, was first evidenced by Davisson and Germer in 1927 in the electron diffraction by crystals. In recent years, numerous fascinating examples of the quantum interference effect (QIE) have been discovered in the molecular systems in their excitation, dissociation and ionization by photons as well as in collision processes. Our group was the first to obtain the experimental evidence of QIE in a collision, specifically for the singlet-triplet mixed state of a diatomic species, and to derive an explicit expression for its energy transfer cross-section. In this expression, the interference phase angle (θST) that describes the phase angle difference between singlet and triplet energy transfer channels is defined and experimentally measured for CO(A 1Π,v=0/e 3Σ－,v =1)-M collision system with M= rare gases (He, Ne, Ar), homonuclear diatomics (H2, N2, O2) and heteronuclear diatomics (HCl) via the optical-optical double resonance multiphoton ionization (OODR-MPI) technique. We have also observed QIE in Na2(A 1Σu＋, v=8/b 3Π0u, v =14)-Na collision. More recently, we have carried out quantum scattering calculations of the interference angle based on the first order Born approximation of time dependent perturbation theory. For atom-diatom collision,the anisotropic Lennard-Jones interaction potential was adopted, and for polar diatom-diatom collision, the long-range dipole-dipole interaction proportional to R－3 was shown to be a proper potential for the calculation. All the calculated θST at T=77,253 and 470 K for CO(A 1Π,v=0/e 3Σ－, v =1)-M, for M=He(θST=58°～65°), Ne(66°～69°), Ar(72°～90°) and HCl(101°～110°), are in od agreement with the experiments. Our calculated differential θST are in the range of 48°～70° for CO-He and 93°～112° for CO-HCl collision for all v and b values that are physically significant. These values are close to those experimental θST′s obtained in the gas cell, implying that the “average effect” is not serious. The calculation also gives an effective collision time of 0.3 ps for CO－He and 1.5 ps for CO－HCl collision, which explains why the experimental θST for the former is much smaller than that of the latter. These results show that θST should provide important information on the singlet-triplet mixed state intermolecular potential, which is difficult to obtain by other experimental or theoretical methods.
- Singlet-triplet mixed state;Collisional energy transfer;Quantum interference;Double resonance multiphoton ionization
1. [1]
  Zihan Cheng , Kai Jiang , Jun Jiang , Henggang Wang , Hengwei Lin . Achieving thermal-stimulus-responsive dynamic afterglow from carbon dots by singlet-triplet energy gap engineering through covalent fixation. Acta Physico-Chimica Sinica, 2026, 42(2): 100169-0. doi: 10.1016/j.actphy.2025.100169
2. [2]
  Linhan Tian , Changsheng Lu . Discussion on Sextuple Bonding in Diatomic Motifs of Chromium Family Elements. University Chemistry, 2024, 39(8): 395-402. doi: 10.3866/PKU.DXHX202401056
3. [3]
  Cuijuan Xuan , Jie Wang , Li Yin , Xiuling Xu , Fengyu Du , Lubin Xu , Liangyu Gong . Construction and practice of a “dual-perspective three-dimensional” experimental teaching model enabled by AI-quantum chemistry synergy in the context of new agricultural science. University Chemistry, 2026, 41(7): 67-75. doi: 10.12461/PKU.DXHX202506031
4. [4]
  Chao Zheng , Chengxi Sun , Runfeng Chen . Theoretical calculations of triplet state lifetimes and phosphorescence radiative rates in organic long-persistent luminescence molecules: Introducing a comprehensive computational chemistry experiment. University Chemistry, 2026, 41(6): 374-384. doi: 10.12461/PKU.DXHX202507082
5. [5]
  Li'na ZHONG , Jingling CHEN , Qinghua ZHAO . Synthesis of multi-responsive carbon quantum dots from green carbon sources for detection of iron ions and L-ascorbic acid. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 709-718. doi: 10.11862/CJIC.20240280
6. [6]
  Qi Wu , Changhua Wang , Yingying Li , Xintong Zhang . Enhanced photocatalytic synthesis of H₂O₂ by triplet electron transfer at g-C₃N₄@BN van der Waals heterojunction interface. Acta Physico-Chimica Sinica, 2025, 41(9): 100107-0. doi: 10.1016/j.actphy.2025.100107
7. [7]
  Longxiang LUO , Xiaoguo CAO , Yannan QIAN . Interface engineering with NH₄PF₆ for CsPbI₂Br quantum dots for enhancing the performance of carbon-based all-inorganic perovskite solar cells. Chinese Journal of Inorganic Chemistry, 2026, 42(2): 227-236. doi: 10.11862/CJIC.20250279
8. [8]
  Peifeng Su , Xin Lu . Development of Undergraduate Quantum Mechanics Module in Chemistry Department under the “Double First Class” Initiative. University Chemistry, 2024, 39(8): 99-103. doi: 10.3866/PKU.DXHX202401087
9. [9]
  Ke Zhao , Zhen Liu , Luyao Liu , Changyuan Yu , Jingshun Pan , Xuguang Huang . Functionalized Reflective Structure Fiber-Optic Interferometric Sensor for Trace Detection of Lead Ions. Acta Physico-Chimica Sinica, 2024, 40(4): 2304029-0. doi: 10.3866/PKU.WHXB202304029
10. [10]
  Lianghong Ye , Junqing Ni , Zhongyi Yan , Zhanming Zhang , Can Zhu , Mo Sun . Chemical Fuel-Driven Non-Equilibrium Color Change. University Chemistry, 2025, 40(3): 349-354. doi: 10.12461/PKU.DXHX202406109
11. [11]
  Weijie Yang , Mansheng Chen , Chen Xu , Fujian Xu . Hydroxyl-Rich Polycations: Innovative Materials Empowering Life and Health. University Chemistry, 2025, 40(9): 332-343. doi: 10.12461/PKU.DXHX202410072
12. [12]
  Yecang Tang , Shan Ling , Zhen Fang . Exploration of a Hierarchical and Integration-Oriented Talent Training Model in the Demonstration Center for Experimental Chemistry Education. University Chemistry, 2024, 39(7): 188-192. doi: 10.12461/PKU.DXHX202405107
13. [13]
  Miaomiao He , Zhiqing Ge , Qiang Zhou , Jiaqing He , Hong Gong , Lingling Li , Pingping Zhu , Wei Shao . Exploring the Fascinating Realm of Quantum Dots. University Chemistry, 2024, 39(6): 231-237. doi: 10.3866/PKU.DXHX202310040
14. [14]
  Mingjie Lei , Wenting Hu , Kexin Lin , Xiujuan Sun , Haoshen Zhang , Ye Qian , Tongyue Kang , Xiulin Wu , Hailong Liao , Yuan Pan , Yuwei Zhang , Diye Wei , Ping Gao . Accelerating the reconstruction of NiSe₂ by Co/Mn/Mo doping for enhanced urea electrolysis. Acta Physico-Chimica Sinica, 2025, 41(8): 100083-0. doi: 10.1016/j.actphy.2025.100083
15. [15]
  Yingxian Wang , Tianye Su , Limiao Shen , Jinping Gao , Qinghe Wu . Introduction of Chinese Lacquer from the Perspective of Chemistry: Popularizing Chemistry in Lacquer and Inherit Lacquer Art. University Chemistry, 2024, 39(5): 371-379. doi: 10.3866/PKU.DXHX202312015
16. [16]
  Yuanyuan Cheng , Di Zhao , Zhicheng Zhang . Practical Exploration of AI-Enabled Rain Classroom in Blended Teaching of Physical Chemistry. University Chemistry, 2025, 40(9): 196-205. doi: 10.12461/PKU.DXHX202503029
17. [17]
  Ruoxi Sun , Yiqian Xu , Shaoru Rong , Chunmiao Han , Hui Xu . The Enchanting Collision of Light and Time Magic: Exploring the Footprints of Long Afterglow Lifetime. University Chemistry, 2024, 39(5): 90-97. doi: 10.3866/PKU.DXHX202310001
18. [18]
  Shengli Chen , Xinxin Zhao , Mingxue Xing , Xintai Li , Xiaojie Zhang , Xiuli Hu , Jimin Zhang . “一触即发”：聚羧酸减水剂和水泥的魔力碰撞. University Chemistry, 2025, 40(8): 315-322. doi: 10.12461/PKU.DXHX202410036
19. [19]
  Yanhui Zhong , Ran Wang , Zian Lin . Analysis of Halogenated Quinone Compounds in Environmental Water by Dispersive Solid-Phase Extraction with Liquid Chromatography-Triple Quadrupole Mass Spectrometry. University Chemistry, 2024, 39(11): 296-303. doi: 10.12461/PKU.DXHX202402017
20. [20]
  Yinuo Wu , Sheng Yin , Wenhao Hu , Tian-Miao Ou . Exploration and Practice in Cultivating Innovative Pharmaceutical Talent through Strengthening Fundamental Education and Interdisciplinary Integration: A Case Study of School of Pharmaceutical Science at Sun Yat-Sen University. University Chemistry, 2025, 40(10): 72-77. doi: 10.12461/PKU.DXHX202412016

Get Citation

PDF

XML

Metrics

PDF Downloads(2474)
Abstract views(3561)
HTML views(45)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142