Research Interest
Quantum wavepacket calculations in chemical reaction dynamics
Quantum wavepacket calculations provide results that can be compared in detail about the
dynamics of a chemical reaction with those obtained in the experiments, and serve as one of the
most rigorous tests of the accuracy of potential energy surfaces (PESs) for chemical reactions.
We have developed initial state selected wavepacket (ISSWP) simulations to study dynamics in
multiple channels for elementary chemical reactions, e.g., H2 (v1, j1) +H2/D2 (v2, j2) in collision
induced dissociation (CID), four-center (4C), and single exchange (SE) channels. Also, we have
extended wavepacket calculations to high dimensional space in poly-atomic systems, e.g., the
abstraction reaction of H+CH4/CD4, as well as simultaneously constructing accurate potential
energy surfaces for the reaction.
FIG. (a)–(c) The six-dimensional reaction flux distribution for the H2 (v1 = 10, j1 = 0) + D2 (v2 =
0, j2 = 0) reaction at a translational energy of 0.5 eV on the planes S[rF1 ], S[rF2 ], and S[RF ]; (d)
|ψ+i (E)|2 as a function of rmin and rCPmin.
“CO2 family” van der Waals clusters
The “CO2 family” molecules include CO2, N2O, OCS, and CS2. Their dimers and trimers, have
been the focus of experiment over the past few years. Recently some new structures have been
experimentally observed for these complexes, including the polar isomers of N2O dimer and OCS
dimer, planar cyclic isomer of CO2 trimer and two distinct structures of OCS-CO2 complex. Some
interesting questions arose, such as the relative stability of the isomers and the interconversion
mechanism between these isomers.
We have studied the NO2 dimer theoretically through the construction of very high accuracy
inter-molecular potential energy surface and the calculation of bound states on the PES. Three coplanar local minima are found on this PES. They correspond to a nonpolar isomer with slippedantiparallel planar structure and two equivalent polar isomers with slipped-parallel planar
structures. The nonpolar isomer is energetically more stable by 162 cm-1 than the polar ones. The
calculated vibrational frequencies are in good agreement with the available experimental data.
Quantum tunneling effect between the two equivalent polar structures has been found in the
higher vibrational excited states. Microwave spectra of the polar structure are also calculated. The
accuracy of the PES has been validated by the good agreement between theoretical and
experimental results of transition frequencies and spectroscopic parameters. More work will be
performed to study other dimers and trimers.
FIG. The θ 1- θ 2 contour plots of the wave functions and the schematic diagrams of
corresponding vibrational modes. (a) Disrotation mode of the nonpolar isomer; (b) Conrotation
mode of the nonpolar isomer; (c) Disrotation mode of the polar isomer; (d) Conrotation mode of
the polar isomer.
Ab initio calculations in chemistry
We have been working on ab initio calculations to understand organocatalysis reaction
mechanism, e.g., aminoxylation catalyzed by chiral Bronsted acid, in collaboration with
experimental group in CBC. We have also performed electronic structure calculations to
understand tungsten-phosphinidene complex.
Selected Publications
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H W Song, Y P Lu and S Y Lee, Full-dimensional time-dependent wave packet dynamics
of H2 + D2 reaction. The Journal of Chemical Physics, 135, 041305 (2011) (Among the top
20 most downloaded articles in the journal in August 2011)
H W Song, Y P Lu and S Y Lee, Three-dimensional wave packet dynamics of H2 + D2
reaction. Chemical Physics, 381, 72 (2011)
L M Zheng, Y P Lu, S Y Lee, H Fu, M H Yang, Theoretical studies of the N2O van der
Waals dimer: Ab initio potential energy surface, intermolecular vibrations and rotational
transition frequencies. The Journal of Chemical Physics, 134, 054311 (2011)
H T H Ngoc, Y P Lu, F Mathey, Oligomerization of Terminal Phosphinidene Complexes,
Organometallics, 30, 1734-1737 (2011)
M Lu, Y P Lu, D Zhu, X F Zeng, X S Li, G F Zhong, Chiral Bronsted Acid Catalyzed
Enantioselective alpha-Aminoxylation of Enecarbamates. Angewandte ChemieInternational, 49, 8588 (2010)
W Q Zhang, Y Zhou, G R Wu, Y P Lu, H L Pan, B N Fu, Q A Shuai, L Liu , S Liu, L L
Zhang, B Jiang, D X Dai, S Y Lee, Z Xie, B J Braams, J M Bowman, M A Collins, D H
Zhang, and X M Yang, Depression of reactivity by collision energy in the single barrier
H+CD4 → HD+CD3 reaction. Proceedings of the National Academy of Sciences of the
United States of America, 107 (2010): 12782-12785.