The role of pulse sequences in controlling ultrafast intramolecular dynamics with four-wave mixing
Апстракт
This article seeks to provide a fundamental understanding of time-resolved four-wave mixing (FWM) processes based on a large body of experimental measurements on a model system consisting of isolated iodine molecules. The theoretical understanding is based primarily on a diagrammatic approach. Double-sided Feynman diagrams are used to classify and describe the coherent FWM processes involved in the signal obtained with each pulse sequence. Different pulse sequences of degenerate femtosecond pulses are shown to control the optical phenomena observed, that is transient grating, reverse-transient grating, photon echo and virtual photon echo. The experimental data reveal clear differences between the nonlinear optical phenomena. We find that the virtual photon echo sequence k(1) - k(2) + k(3) is the most efficient for controlling the observation of ground-or excited-state dynamics. The strategy followed to make this assessment was to compare transients when the time delay between two of th...e three pulses set in or out of phase with the excited-state vibrational dynamics. We have obtained a signal from pulse sequences k(1) + k(2) - k(3) for which FWM signal generation for this two-electronic-level system is forbidden. This signal can be explained by the cascading of a first-order polarization and a second-order process to generate the FWM signal. The implications of our findings are discussed in the context of multiple-pulse methods for the control of intramolecular dynamics.
Извор:
International Reviews in Physical Chemistry, 2000, 19, 4, 531-552
DOI: 10.1080/014423500750040609
ISSN: 0144-235X
WoS: 000165785400002
Scopus: 2-s2.0-0034527686
Колекције
Институција/група
VinčaTY - JOUR AU - Lozovoy, VV AU - Pastirk, Igor AU - Brown, EJ AU - Grimberg, BI AU - Dantus, M PY - 2000 UR - https://vinar.vin.bg.ac.rs/handle/123456789/2395 AB - This article seeks to provide a fundamental understanding of time-resolved four-wave mixing (FWM) processes based on a large body of experimental measurements on a model system consisting of isolated iodine molecules. The theoretical understanding is based primarily on a diagrammatic approach. Double-sided Feynman diagrams are used to classify and describe the coherent FWM processes involved in the signal obtained with each pulse sequence. Different pulse sequences of degenerate femtosecond pulses are shown to control the optical phenomena observed, that is transient grating, reverse-transient grating, photon echo and virtual photon echo. The experimental data reveal clear differences between the nonlinear optical phenomena. We find that the virtual photon echo sequence k(1) - k(2) + k(3) is the most efficient for controlling the observation of ground-or excited-state dynamics. The strategy followed to make this assessment was to compare transients when the time delay between two of the three pulses set in or out of phase with the excited-state vibrational dynamics. We have obtained a signal from pulse sequences k(1) + k(2) - k(3) for which FWM signal generation for this two-electronic-level system is forbidden. This signal can be explained by the cascading of a first-order polarization and a second-order process to generate the FWM signal. The implications of our findings are discussed in the context of multiple-pulse methods for the control of intramolecular dynamics. T2 - International Reviews in Physical Chemistry T1 - The role of pulse sequences in controlling ultrafast intramolecular dynamics with four-wave mixing VL - 19 IS - 4 SP - 531 EP - 552 DO - 10.1080/014423500750040609 ER -
@article{ author = "Lozovoy, VV and Pastirk, Igor and Brown, EJ and Grimberg, BI and Dantus, M", year = "2000", abstract = "This article seeks to provide a fundamental understanding of time-resolved four-wave mixing (FWM) processes based on a large body of experimental measurements on a model system consisting of isolated iodine molecules. The theoretical understanding is based primarily on a diagrammatic approach. Double-sided Feynman diagrams are used to classify and describe the coherent FWM processes involved in the signal obtained with each pulse sequence. Different pulse sequences of degenerate femtosecond pulses are shown to control the optical phenomena observed, that is transient grating, reverse-transient grating, photon echo and virtual photon echo. The experimental data reveal clear differences between the nonlinear optical phenomena. We find that the virtual photon echo sequence k(1) - k(2) + k(3) is the most efficient for controlling the observation of ground-or excited-state dynamics. The strategy followed to make this assessment was to compare transients when the time delay between two of the three pulses set in or out of phase with the excited-state vibrational dynamics. We have obtained a signal from pulse sequences k(1) + k(2) - k(3) for which FWM signal generation for this two-electronic-level system is forbidden. This signal can be explained by the cascading of a first-order polarization and a second-order process to generate the FWM signal. The implications of our findings are discussed in the context of multiple-pulse methods for the control of intramolecular dynamics.", journal = "International Reviews in Physical Chemistry", title = "The role of pulse sequences in controlling ultrafast intramolecular dynamics with four-wave mixing", volume = "19", number = "4", pages = "531-552", doi = "10.1080/014423500750040609" }
Lozovoy, V., Pastirk, I., Brown, E., Grimberg, B.,& Dantus, M.. (2000). The role of pulse sequences in controlling ultrafast intramolecular dynamics with four-wave mixing. in International Reviews in Physical Chemistry, 19(4), 531-552. https://doi.org/10.1080/014423500750040609
Lozovoy V, Pastirk I, Brown E, Grimberg B, Dantus M. The role of pulse sequences in controlling ultrafast intramolecular dynamics with four-wave mixing. in International Reviews in Physical Chemistry. 2000;19(4):531-552. doi:10.1080/014423500750040609 .
Lozovoy, VV, Pastirk, Igor, Brown, EJ, Grimberg, BI, Dantus, M, "The role of pulse sequences in controlling ultrafast intramolecular dynamics with four-wave mixing" in International Reviews in Physical Chemistry, 19, no. 4 (2000):531-552, https://doi.org/10.1080/014423500750040609 . .