Femtosecond transient stimulated emission pumping studies of ozone visible photodissociation

Chen, Y.; Hunziker, Lukas E.; Ludowise, P.; Morgen, Mike

doi:10.1063/1.463102

Cited by 39 publications

(17 citation statements)

References 17 publications

(4 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…20 The outline of the paper is as follows: In section 11, a discussion of the approach is given. The experimental description is given in section 111, followed by the results in section IV.…”

Section: Introductionmentioning

confidence: 99%

Femtosecond real-time probing of reactions. 12. Vectorial dynamics of transition states

Baumert¹,

Pedersen²,

Zewail³

1993

J. Phys. Chem.

View full text Add to dashboard Cite

Femtosecond time-resolved techniques with KETOF (kinetic energy time-of-flight) detection in a molecular beam are developed for studies of the vectorial dynamics of transition states. Application to the dissociation reaction of IHgI is presented. For this system, the complex [I-.Hg.I]t* is unstable and, through the symmetric and asymmetric stretch motions, yields different product fragments: [I*-Hg.-I] t* -HgI(X2Z+) + I(2P~/2) [or I*(2Pl/2)] (la); [I-.Hg-I]t* -Hg('S0) + I(2P3/2) + I(2P3/2) [or I*(2P1/2)] (lb). These twochannels, ( l a )and (1 b), lead to different kinetic energy distributions in the products. It is shown that the motion of the wave packet in the transition-state region can be observed by MPI mass detection; the transient time ranges from 120 to 300 fs depending on the available energy. With polarized pulses, the vectorial properties (transition moments alignment relative to recoil direction) are studied for fragment separations on the femtosecond time scale. The results indicate the nature of the structure (symmetry properties) and the correlation to final products. For 311-nm excitation, no evidence of crossing between the I and I* potentials is found at the internuclear separations studied. (Results for 287-nm excitation are also presented.) Molecular dynamics simulations and studies by laser-induced fluorescence support these findings.

show abstract

Section: Introductionmentioning

confidence: 99%

Femtosecond real-time probing of reactions. 12. Vectorial dynamics of transition states

Baumert¹,

Pedersen²,

Zewail³

1993

J. Phys. Chem.

View full text Add to dashboard Cite

show abstract

“…The photodissociation of ozone has been extensively investigated both theoretically and experimentally, [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] not only because of its importance in atmospheric chemistry, but also because of its interesting electronic spectroscopy which provides a platform for studying the more fundamental aspects of photodissociation reaction dynamics. Perhaps the most sophisticated experimental study of dynamics associated with the Chappuis band of ozone has been the work of Chen et al 9 who developed a zero-background, multiplex-selected femtosecond transition-state spectroscopic technique that allowed direct visualization of the wave packet motion. However, despite the rich information content in the experimental data of this powerful transient stimulated emission pumping ͑TSEP͒ technique, the signals are the result of complicated dynamics of a polyatomic system, the details of which cannot be extracted by a cursory examination of the results.…”

Section: Introductionmentioning

confidence: 99%

Semiclassical molecular dynamics simulations of ultrafast photodissociation dynamics associated with the Chappuis band of ozone

Batista

Miller

1998

The Journal of Chemical Physics

View full text Add to dashboard Cite

In this paper we investigate the nonadiabatic ultrafast dynamics of interconversion between the two lower lying excited states of 1 AЉ symmetry ͑1 1 AЉ and 2 1 AЉ) of ozone following photoexcitation of the molecule in the gas phase with visible light. Our algorithm involves a semiclassical initial value representation method which is able to describe electronically nonadiabatic processes within the time dependent picture through the quantization of the classical electron-nuclear model Hamiltonian of Meyer and Miller ͓J. Chem. Phys. 70, 7 ͑1979͔͒. We explore the capabilities of these techniques as applied to studying the dynamics of a realistic reaction of photodissociation on full ab initio electronic potential energy surfaces. Our semiclassical results provide an intuitive understanding of the most fundamental dynamical features involved in the process of predissociation, such as decay and recurrence events, as well as an interpretation of experimental studies of the Chappuis band of ozone in the frequency domain.

show abstract

“…Rapid dissociation takes place on the lower surface, corresponding to Eq. (1), with a timescale of approximately 60 fs, leading to a highly diffuse and complex absorption spectrum [13,16,19,20].…”

Section: Introductionmentioning

confidence: 99%

The photodissociation of ozone: A quasi-classical approach to a quantum dynamics problem

Penfold

Worth

2007

Journal of Molecular Graphics and Modelling

View full text Add to dashboard Cite

Femtosecond transient stimulated emission pumping studies of ozone visible photodissociation

Cited by 39 publications

References 17 publications

Femtosecond real-time probing of reactions. 12. Vectorial dynamics of transition states

Femtosecond real-time probing of reactions. 12. Vectorial dynamics of transition states

Semiclassical molecular dynamics simulations of ultrafast photodissociation dynamics associated with the Chappuis band of ozone

The photodissociation of ozone: A quasi-classical approach to a quantum dynamics problem

Contact Info

Product

Resources

About