Quantum interference in H plus HD → H2 + D between direct abstraction and roaming insertion pathways

被引:64
作者
Xie, Yurun [1 ,2 ]
Zhao, Hailin [1 ]
Wang, Yufeng [1 ]
Huang, Yin [1 ]
Wang, Tao [3 ]
Xu, Xin [1 ]
Xiao, Chunlei [1 ]
Sun, Zhigang [1 ]
Zhang, Dong H. [1 ]
Yang, Xueming [1 ,3 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
[2] ShanghaiTech Univ, Sch Phys Sci & Technol, 100 Haike Rd, Shanghai 201210, Peoples R China
[3] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
基金
中国国家自然科学基金;
关键词
DIFFERENTIAL CROSS-SECTIONS; GEOMETRIC PHASE; VIBRATIONAL-EXCITATION; RESONANCES; SCATTERING; DYNAMICS; ENERGY; PATHWAYS;
D O I
10.1126/science.abb1564
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Understanding quantum interferences is essential to the study of chemical reaction dynamics. Here, we provide an interesting case of quantum interference between two topologically distinct pathways in the H + HD -> H-2 + D reaction in the collision energy range between 1.94 and 2.21 eV, manifested as oscillations in the energy dependence of the differential cross section for the H-2 (v' = 2, j' = 3) product (where v' is the vibrational quantum number and j' is the rotational quantum number) in the backward scattering direction. The notable oscillation patterns observed are attributed to the strong quantum interference between the direct abstraction pathway and an unusual roaming insertion pathway. More interestingly, the observed interference pattern also provides a sensitive probe of the geometric phase effect at an energy far below the conical intersection in this reaction, which resembles the Aharonov-Bohm effect in physics, clearly demonstrating the quantum nature of chemical reactivity.
引用
收藏
页码:767 / +
页数:22
相关论文
共 48 条
  • [1] SIGNIFICANCE OF ELECTROMAGNETIC POTENTIALS IN THE QUANTUM THEORY
    AHARONOV, Y
    BOHM, D
    [J]. PHYSICAL REVIEW, 1959, 115 (03): : 485 - 491
  • [2] General explanation of geometric phase effects in reactive systems: Unwinding the nuclear wave function using simple topology
    Althorpe, SC
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2006, 124 (08)
  • [3] A refined H-3 potential energy surface
    Boothroyd, AI
    Keogh, WJ
    Martin, PG
    Peterson, MR
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1996, 104 (18) : 7139 - 7152
  • [4] Strong geometric-phase effects in the hydrogen-exchange reaction at high collision energies
    Bouakline, Foudhil
    Althorpe, Stuart C.
    Ruiz, Daniel Pelaez
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2008, 128 (12)
  • [5] Quantum theory of chemical reaction dynamics
    Clary, DC
    [J]. SCIENCE, 1998, 279 (5358) : 1879 - 1882
  • [6] State-to-state three-atom time-dependent reactive scattering in hyperspherical coordinates
    Crawford, Jeff
    Parker, Gregory A.
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2013, 138 (05)
  • [7] Interference of quantized transition-state pathways in the H+D2→D+HD chemical reaction
    Dai, DX
    Wang, CC
    Harich, SA
    Wang, XY
    Yang, XM
    Chao, SD
    Skodje, RT
    [J]. SCIENCE, 2003, 300 (5626) : 1730 - 1734
  • [8] Using quantum rotational polarization moments to describe the stereodynamics of the H+D2(v=0,j=0)→HD(v′,j′)+D reaction
    de Miranda, MP
    Clary, DC
    Castillo, JF
    Manolopoulos, DE
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1998, 108 (08) : 3142 - 3153
  • [9] Chemical "double slits": Dynamical interference of photodissociation pathways in water
    Dixon, RN
    Hwang, DW
    Yang, XF
    Harich, S
    Lin, JJ
    Yang, X
    [J]. SCIENCE, 1999, 285 (5431) : 1249 - 1253
  • [10] Eyles CJ, 2011, NAT CHEM, V3, P597, DOI [10.1038/NCHEM.1071, 10.1038/nchem.1071]