Experimental demonstration of the coherent control of the molecular iodine vibrational dynamics by chirped femtosecond light pulses

Lozovoy, Vadim V.; Antipin, S. A.; Гостев, Ф. Е.; Titov, A. A.; Tovbin, D. G.; Sarkisov, O. M.; Vetchinkin, A. S.; Umanskii, S. Ya.

doi:10.1016/s0009-2614(97)01415-2

Cited by 33 publications

(25 citation statements)

References 12 publications

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“…33,34 Recently, an experimental demonstration of coherent control on I 2 on the B excited electronic state surface verified the importance of frequency chirping as a tool in effecting localization of the vibrational wave packet on the excited state surface. 35 Similarly, this study also confirms that use of a negatively chirped pulse leads to greater localization of the wave packet in coordinate space while a positively chirped pulse tends to hasten loss of vibrational coherence and wave packet spreading. Lozoyov et al 35 attributed this effect to the different initial distribution of molecular phases induced by use of different frequency chirped pulses.…”

Section: ͑27͒supporting

confidence: 75%

“…35 Similarly, this study also confirms that use of a negatively chirped pulse leads to greater localization of the wave packet in coordinate space while a positively chirped pulse tends to hasten loss of vibrational coherence and wave packet spreading. Lozoyov et al 35 attributed this effect to the different initial distribution of molecular phases induced by use of different frequency chirped pulses.…”

Section: ͑27͒supporting

confidence: 75%

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Quantum control of I2 wave packet localization in solid argon matrix

Guiang

Wyatt

2000

The Journal of Chemical Physics

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Dynamics and energy release in benzene/Ar cluster dissociationThe effect of coupled nonreactive modes on laser control of quantum wave packet dynamics J. Chem. Phys. 111, 6864 (1999); 10.1063/1.479978Time-dependent wave packet study of the one atom cage effect in I 2 -Ar Van der Waals complexes A hybrid quantum/classical approach for treating the vibrational and translational motion of the I 2 molecule inside a cold Ar matrix is implemented in the control of vibrational wave packet localization on the excited ͑A͒ electronic surface of I 2 . Quantum control was performed in the weak-field regime at six different temperatures to examine thermal effects on the dynamics of I 2 inside the lattice and on the degree of control that can be achieved for this system. It was found in this study that an increase in temperature from 0 to 75 K leads to a moderate decrease in the degree of control achieved. The role played by I 2 rotation on control was also shown to be minimal under the conditions examined in this work.

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Section: ͑27͒supporting

confidence: 75%

Section: ͑27͒supporting

confidence: 75%

Quantum control of I2 wave packet localization in solid argon matrix

Guiang

Wyatt

2000

The Journal of Chemical Physics

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“…This manipulation shapes the wave packet in each electronic state, allowing the focusing or spreading of the wave packet. [6][7][8]10 When the initial population distribution is not limited to a single vibrational state, the density matrix elements represent the evolution of all levels in the system after successive laser pulses. A coherent coupling arises within each electronic state as a consequence of interaction with the first two pulses.…”

Section: Theorymentioning

confidence: 99%

Control and Characterization of Intramolecular Dynamics with Chirped Femtosecond Three-Pulse Four-Wave Mixing

et al. 1999

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Experimental control and characterization of intramolecular dynamics are demonstrated with chirped femtosecond three-pulse four-wave mixing (FWM). The two-dimensional (spectrally dispersed and timeresolved) three-pulse FWM signal is shown to contain important information about the population and coherence of the electronic and vibrational states of the system. The experiments are carried out on gas-phase I 2 and the degenerate laser pulses are resonant with the X (ground) to B (excited) electronic transition. In the absence of laser chirp, control over population and coherence transfer is demonstrated by selecting specific pulse sequences. When chirped lasers are used to manipulate the optical phases of the pulses, the two-dimensional data demonstrate the transfer of coherence between the ground and excited states. Positive chirps are also shown to enhance the signal intensity, particularly for bluer wavelengths. A theoretical model based on the multilevel density matrix formalism in the perturbation limit is developed to simulate the data. The model takes into account two vibrational levels in the ground and the excited states, as well as different pulse sequences and laser chirp values. The analytical solution allows us to predict particular pulse sequences that control the final electronic state of the population. In a similar manner, the theory allows us to find critical chirp values that control the transfer of vibrational coherence between the two electronic states. Wave packet calculations are used to illustrate the process that leads to the observation of ground-state dynamics. All the calculations are found to be in excellent agreement with the experimental data. The ability to control population and coherence transfer in molecular systems is of great importance in the quest for controlling the outcome of laser-initiated chemical reactions.

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“…Previous studies employing femtosecond (fs) pulsed radiation were mainly devoted to the photodissociation of I 2 via the lowest excited covalent A and B states. [8][9][10][11] In ref.…”

Section: Introductionmentioning

confidence: 99%

Role of ion-pair states in the predissociation dynamics of Rydberg states of molecular iodine

Vangerow

Bogomolov

Dozmorov

et al. 2016

Phys. Chem. Chem. Phys.

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Using femtosecond pump-probe ion imaging spectroscopy, we establish the key role of I(+) + I(-) ion-pair (IP) states in the predissociation dynamics of molecular iodine I2 excited to Rydberg states. Two-photon excitation of Rydberg states lying above the lowest IP state dissociation threshold (1st tier) is found to be followed by direct parallel transitions into IP states of the 1st tier asymptotically correlating to a pair of I ions in their lowest states I(+)((3)P2) + I(-)((1)S0), of the 2nd tier correlating to I(+)((3)P0) + I(-)((1)S0), and of the 3rd tier correlating to I(+)((1)D2) + I(-)((1)S0). Predissociation via the 1st tier proceeds presumably with a delay of 1.6-1.7 ps which is close to the vibrational period in the 3rd tier state (3rd tier-mediated process). The 2nd tier IP state is concluded to be the main precursor for predissociation via lower lying Rydberg states proceeding with a characteristic time of 7-8 ps and giving rise to Rydberg atoms I(5s(2)5p(4)6s(1)). The channel generating I((2)P3/2) + I((2)P1/2) atoms with total kinetic energy corresponding to one-photon excitation is found to proceed via a pump - dump mechanism with dramatic change of angular anisotropy of this channel as compared with earlier nanosecond experiments.

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Experimental demonstration of the coherent control of the molecular iodine vibrational dynamics by chirped femtosecond light pulses

Cited by 33 publications

References 12 publications

Quantum control of I2 wave packet localization in solid argon matrix

Quantum control of I2 wave packet localization in solid argon matrix

Control and Characterization of Intramolecular Dynamics with Chirped Femtosecond Three-Pulse Four-Wave Mixing

Role of ion-pair states in the predissociation dynamics of Rydberg states of molecular iodine

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