Dissociation of methane in intense laser fields

被引:50
作者
Wang, SF
Tang, XP
Gao, LR
Elshakre, ME
Kong, FN [1 ]
机构
[1] Chinese Acad Sci, Inst Chem, Beijing 100080, Peoples R China
[2] Cairo Univ, Coll Sci, Dept Chem, Cairo, Egypt
关键词
D O I
10.1021/jp022243e
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The dissociation of methane in the intense laser field has been investigated experimentally and theoretically. Using an amplified ultrafast Ti:sapphire laser around 800 nm coupled to a TOF mass spectrometer, all the primary and secondary ions were produced and detected at the laser intensities 10(13) to 10(14) W/cm(2). The experimental results show that the dissociation of methane proceeds via a stepwise mechanism by gradually increasing, the laser intensity. The maximum HI yield is formed when the linearly polarized laser field is parallel to the axis of the TOF tube. A quasi-diatomic theoretical model has been proposed and used to interpret the dissociation of polyatomic molecules. The model assumes that only the dissociative bond is considered and the rest of the molecular geometry is fixed during the dissociation. For each step, the profiles of the dressed potential energy surfaces (PESs) along the dissociative bond of the molecule at different laser intensities are calculated. Quasi-classical trajectories on the dressed PESs are calculated, showing that the wave packet is modulated by the sinusoidal laser field. Theoretical dissociation probabilities are thus calculated. The results can fully interpret the overall dissociation processes and the angular dependence of H+ yield.
引用
收藏
页码:6123 / 6129
页数:7
相关论文
共 34 条
[1]   Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses [J].
Assion, A ;
Baumert, T ;
Bergt, M ;
Brixner, T ;
Kiefer, B ;
Seyfried, V ;
Strehle, M ;
Gerber, G .
SCIENCE, 1998, 282 (5390) :919-922
[2]   Dynamic and geometric alignment of CS2 in intense laser fields of picosecond and femtosecond duration [J].
Banerjee, S ;
Kumar, GR ;
Mathur, D .
PHYSICAL REVIEW A, 1999, 60 (05) :R3369-R3372
[3]   Intensity-selective, field-induced dissociative ionization of CS2 by femtosecond-duration light pulses [J].
Banerjee, S ;
Kumar, GR ;
Mathur, D .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 1999, 32 (17) :4277-4292
[4]   Angle-resolved covariance mapping of spatially-aligned CO22+ in an intense picosecond laser field [J].
Bhardwaj, VR ;
Vijayalakshmi, K ;
Mathur, D .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 1999, 32 (05) :1087-1095
[5]   Spatial alignment of gas-phase polyatomic molecules by an intense laser field [J].
Bhardwaj, VR ;
Vijayalakshmi, K ;
Mathur, D .
PHYSICAL REVIEW A, 1997, 56 (03) :2455-2458
[6]   Dissociative ionization of benzene in intense laser fields of picosecond duration [J].
Bhardwaj, VR ;
Vijayalakshmi, K ;
Mathur, D .
PHYSICAL REVIEW A, 1999, 59 (02) :1392-1398
[7]   Subpicosecond ionization and dissociation of benzene and cyclic alkanes at 800 and 400 nm [J].
Castillejo, M ;
Couris, S ;
Koudoumas, E ;
Martin, M .
CHEMICAL PHYSICS LETTERS, 1998, 289 (3-4) :303-310
[8]   Ionization and fragmentation of aromatic and single-bonded hydrocarbons with 50 fs laser pulses at 800 nm [J].
Castillejo, M ;
Couris, S ;
Koudoumas, E ;
Martín, M .
CHEMICAL PHYSICS LETTERS, 1999, 308 (5-6) :373-380
[9]   Dissociative ionization of H-2(+) in an intense laser field: Charge-resonance-enhanced ionization, Coulomb explosion, and harmonic generation at 600 nm [J].
Chelkowski, S ;
Conjusteau, A ;
Zuo, T ;
Bandrauk, AD .
PHYSICAL REVIEW A, 1996, 54 (04) :3235-3244
[10]   COULOMB EXPLOSION OF CO2 IN AN INTENSE FEMTOSECOND LASER FIELD [J].
CORNAGGIA, C ;
SCHMIDT, M ;
NORMAND, D .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 1994, 27 (07) :L123-L130