Observation of multiple ionization pathways for OCS in an intense laser field resolved by three-dimensional covariance mapping and visualized by hierarchical ionization topology

The two- and three-body Coulomb explosion of carbonyl sulfide (OCS) by 790 nm, 50 fs laser pulses focused to {approx_equal}10{sup 16} W cm{sup -2} has been investigated by the three-dimensional covariance mapping technique. In a triatomic molecule, a single charge state, in this case the trication, has been observed to dissociate into two distinct energy channels. With the aid of a three-dimensional visualization technique to reveal the ionization hierarchy, evidence is presented for the existence of two sets of ionization pathways resulting from these two initial states. While one group of ions can be modeled using a classical enhanced ionization model, the second group, consisting of mainly asymmetric channels, cannot. The results provide clear evidence that an enhanced ionization approach must also be accompanied by an appreciation of the effects of excited ionic states and multielectronic processes.

[1]  Kevin F. Lee,et al.  Imaging the time-dependent structure of a molecule as it undergoes dynamics , 2005 .

[2]  K. Yamanouchi,et al.  Concerted and sequential Coulomb explosion processes of N2O in intense laser fields by coincidence momentum imaging. , 2005, The Journal of chemical physics.

[3]  R. Coffee,et al.  Identifying fragment vuv excitations with dissociation channels from the strong-field ionization of N 2 , 2005 .

[4]  K. Yamanouchi,et al.  Probing the ultrafast nuclear motion in CS2 2+ in intense laser fields. , 2005, The Journal of chemical physics.

[5]  C. Predescu,et al.  Thermodynamics and equilibrium structure of Ne38 cluster: quantum mechanics versus classical. , 2005, Journal of Chemical Physics.

[6]  R. Coffee,et al.  vuv fluorescence from selective high-order multiphoton excitation of N 2 , 2004 .

[7]  Kun Zhao,et al.  Strong-field dissociative ionization of a linear triatomic molecule: Relationship between Coulomb-explosion energies and bond angle , 2003 .

[8]  P. Corkum,et al.  Time-resolved double ionization with few cycle laser pulses. , 2003, Physical review letters.

[9]  Pengqian Wang,et al.  Dissociation of multiply ionized carbonyl sulfide due to electron impact , 2003 .

[10]  K. Yamanouchi,et al.  Sequential three-body Coulomb explosion of CS2 in intense laser fields appearing in momentum correlation map , 2002 .

[11]  M. Ivanov,et al.  Polyatomic molecules in strong laser fields: Nonadiabatic multielectron dynamics , 2002 .

[12]  P. McKenna,et al.  Suppression of multiple ionization of atomic ions in intense ultrafast laser pulses. , 2002, Physical review letters.

[13]  P. Taday,et al.  Coulombic and pre-Coulombic geometry evolution of carbonyl sulfide in an intense femtosecond laser pulse, determined by momentum imaging , 2002 .

[14]  K. Yamanouchi,et al.  Coincidence imaging of Coulomb explosion of CS2 in intense laser fields , 2001 .

[15]  H. Kono,et al.  Mechanism of enhanced ionization of linear H + 3 in intense laser fields , 2001 .

[16]  G. Gibson,et al.  Comprehensive analysis of strong-field ionization and dissociation of diatomic nitrogen , 2001 .

[17]  M. Shiota,et al.  A Theoretical Study of Electronic Dynamics and Deformation of CO2in Intense Laser Fields , 2001 .

[18]  P. Taday,et al.  A Detailed Study of Multiply Charged Ion Production Within a High Intensity Laser Focus , 2001 .

[19]  Cornaggia,et al.  Hydrodynamic description of laser-induced coulomb explosion for small molecules , 2000, Physical Review Letters.

[20]  P. Hering,et al.  Nonsequential double ionization of small molecules induced by a femtosecond laser field , 2000 .

[21]  Cornaggia,et al.  Experimental evidence of excited multicharged atomic fragments coming from laser-induced coulomb explosion of molecules , 2000, Physical review letters.

[22]  C. E. Brion,et al.  Dipole (e,e+ ion) coincidence studies of the ionic photofragmentation and photoionization of carbonyl sulfide in the valence shell and S 2p, 2s and C 1s inner shell regions (10–300 eV) , 2000 .

[23]  P. Taday,et al.  Laser-induced Coulomb explosion, geometry modification and reorientation of carbon dioxide , 2000 .

[24]  K. Yamanouchi,et al.  Ultrafast structural deformation of NO2 in intense laser fields studied by mass-resolved momentum imaging , 1999 .

[25]  K. Yamanouchi,et al.  Ultrafast Deformation of the Geometrical Structure of CO 2 Induced in Intense Laser Fields , 1999 .

[26]  P. Corkum,et al.  DISSOCIATION OF MOLECULAR CHLORINE IN A COULOMB EXPLOSION : POTENTIAL CURVES, BOUND STATES, AND DEVIATION FROM COULOMBIC BEHAVIOR FOR CL2N+ (N = 2,3,4 ,6,8,10) , 1999 .

[27]  P. Taday,et al.  GEOMETRY MODIFICATIONS AND ALIGNMENT OF H2O IN AN INTENSE FEMTOSECOND LASER PULSE , 1999 .

[28]  P. Hering,et al.  Coulomb explosion of N 2 and CO 2 using linearly and circularly polarized femtosecond laser pulses , 1999 .

[29]  J. Eland,et al.  Dissociative photoionisation of OCS from threshold to 40.8 eV , 1999 .

[30]  Charles G. Durfee,et al.  High power ultrafast lasers , 1998 .

[31]  S. Nanbu,et al.  NONADIABATIC BENDING DISSOCIATION IN 16 VALENCE ELECTRON SYSTEM OCS , 1998 .

[32]  P. Taday,et al.  Alignment and bending of by intense femtosecond laser pulses , 1998 .

[33]  M. Walker,et al.  INTENSITY-RESOLVED MULTIPHOTON IONIZATION : CIRCUMVENTING SPATIAL AVERAGING , 1998 .

[34]  K. Yamanouchi,et al.  Mass-resolved two-dimensional momentum imaging of the Coulomb explosion of N2 and SO2 in an intense laser field , 1998 .

[35]  C. Clark,et al.  Multielectron Dissociative Ionization of Molecules by Intense Laser Radiation , 1996, physics/9611024.

[36]  A. Giles,et al.  Field-ionization, Coulomb explosion of diatomic molecules in intense laser fields , 1996 .

[37]  Cornaggia.  Large-amplitude nuclear motions in the laser-induced Coulomb explosion of carbon dioxide molecules. , 1996, Physical review. A, Atomic, molecular, and optical physics.

[38]  Ivanov,et al.  Role of electron localization in intense-field molecular ionization. , 1995, Physical review letters.

[39]  A. Bandrauk,et al.  Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers. , 1995, Physical review. A, Atomic, molecular, and optical physics.

[40]  M. Schmidt,et al.  Coulomb explosion of CO2 in an intense femtosecond laser field , 1994 .

[41]  C. Wahlström,et al.  Multielectron Dissociative Ionization of Co2 In Intense Laser Fields , 1994 .

[42]  L. Frasinski,et al.  Multiphoton multiple ionisation of N2O probed by three-dimensional covariance mapping , 1991 .

[43]  L. Frasinski,et al.  Covariance Mapping: A Correlation Method Applied to Multiphoton Multiple Ionization , 1989, Science.

[44]  Gerard Mourou,et al.  Compression of amplified chirped optical pulses , 1985 .

[45]  S. Okada.  Measurements of energy loss spectra in ion-pair formation reactions for the K + HCl system , 1979 .

[46]  I. Mclaren,et al.  TIME-OF-FLIGHT MASS SPECTROMETER WITH IMPROVED RESOLUTION , 1955 .