Slice imaging study of NO2 photodissociation via the 1(2)B(2) and 2(2)B(2) states: the NO(X-2 Pi) + O(P-3(J)) product channel

Zhang, Zhaoxue1,2,3; Yang, Shuaikang2,3; Li, Zhenxing2,3; Chang, Yao2,3; Luo, Zijie2,3; Zhao, Yarui2,3; Yu, Shengrui1; Yuan, Kaijun2,3,4; Yang, Xueming2,3,4,5,6

2023-05-01

10.1039/d3cp00420a

PHYSICAL CHEMISTRY CHEMICAL PHYSICS   影响因子和分区

1463-9076

1463-9084

The state-resolved photodissociation of NO2 via the 1(2)B(2) and 2(2)B(2) excited states has been investigated by using time-sliced velocity-mapped ion imaging technique. The images of the O(P-3(J=2,1,0)) products at a series of excitation wavelengths are measured by employing a 1 + 1' photoionization scheme. The total kinetic energy release (TKER) spectra, NO vibrational state distributions and anisotropy parameters (beta) are derived from the O(P-3(J)=(2,1,)0) images. For the 1(2)B(2) state photodissociation of NO2, the TKER spectra mainly present a non-statistical vibrational state distribution of the NO co-products, and the profiles of most vibrational peaks display a bimodal structure. The beta values show a gradual decrease with the photolysis wavelength increasing except for a sudden increase at 357.38 nm. The results suggest that the NO2 photodissociation via the 1(2)B(2) state proceeds via the non-adiabatic transition between the 1(2)B(2) and (X) over tilde (2)A(1) states, leading to the NO(X-2 Pi) + O(P-3(J)) products with wavelength-dependent rovibrational distributions. As for photodissociation of NO2 via the 2(2)B(2) state, the NO vibrational state distribution is relatively narrow with the main peak shifting from v = 1, 2 at 235.43-249.22 nm to v = 6 at 212.56 nm. The beta values exhibit two distinctly different angular distributions, i.e., near isotropic at 249.22 and 246.09 nm and anisotropic at the rest of the excitation wavelengths. These results are consistent with the fact that the 2(2)B(2) state potential energy surface has a barrier, and the dissociation process is fast when the initial populated level is above this barrier. A bimodal vibrational state distribution is clearly observed at 212.56 nm, in which the main distribution (peaking at v = 6) is ascribed to dissociation via an avoided crossing with the higher electronically excited state while the subsidiary distribution (peaking at v = 11) likely arises due to dissociation via the internal conversion to the 1(2)B(2) state or to the (X) over tilde ground state.

SCI ; EI

英语

其他

National Natural Science Foundation of China["22241304","22225303","22173082"] ; National Natural Science Foundation of China (NSFC Center for Chemical Dynamics)[22288201] ; Scientific Instrument Developing Project of the Chinese Academy of Sciences[GJJSTD20220001] ; Innovation Program for Quantum Science and Technology[2021ZD0303304] ; Zhejiang Provincial Natural Science Foundation of China[LY22B030005] ; Guangdong Science and Technology Program["2019ZT08L455","2019JC01X091"] ; Shenzhen Science and Technology Program[ZDSYS20200421111001787] ; China Postdoctoral Science Foundation[2021M693118]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:001008207000001

ROYAL SOC CHEMISTRY

20232614325883

Angular distribution ; Anisotropy ; Excited states ; Ground state ; Kinetic energy ; Kinetics ; Nitrogen oxides ; Photolysis ; Potential energy ; Quantum chemistry

Fluid Flow, General:631.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Inorganic Compounds:804.2 ; Classical Physics; Quantum Theory; Relativity:931 ; Physical Properties of Gases, Liquids and Solids:931.2 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

CHEMISTRY

Web of Science

1.Zhejiang Normal Univ, Hangzhou Inst Adv Studies, 1108 Gengwen Rd, Hangzhou 311231, Zhejiang, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, 457 Zhongshan Rd, Dalian 116023, Liaoning, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Coherent Light Source, 457 Zhongshan Rd, Dalian 116023, Liaoning, Peoples R China
4.Hefei Natl Lab, Hefei 230088, Peoples R China
5.Southern Univ Sci & Technol, Coll Sci, Dept Chem, Shenzhen 518055, Peoples R China
6.Southern Univ Sci & Technol, Coll Sci, Ctr Adv Light Source Res, Shenzhen 518055, Peoples R China

Zhang, Zhaoxue,Yang, Shuaikang,Li, Zhenxing,et al. Slice imaging study of NO2 photodissociation via the 1(2)B(2) and 2(2)B(2) states: the NO(X-2 Pi) + O(P-3(J)) product channel[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2023,25(25):16872-16880.

Zhang, Zhaoxue.,Yang, Shuaikang.,Li, Zhenxing.,Chang, Yao.,Luo, Zijie.,...&Yang, Xueming.(2023).Slice imaging study of NO2 photodissociation via the 1(2)B(2) and 2(2)B(2) states: the NO(X-2 Pi) + O(P-3(J)) product channel.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,25(25),16872-16880.

Zhang, Zhaoxue,et al."Slice imaging study of NO2 photodissociation via the 1(2)B(2) and 2(2)B(2) states: the NO(X-2 Pi) + O(P-3(J)) product channel".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 25.25(2023):16872-16880.