Pulse trains in molecular dynamics and coherent spectroscopy: a theoretical study

Voll, Judith; Vivie‐Riedle, Regina de

doi:10.1088/1367-2630/11/10/105036

Cited by 21 publications

(14 citation statements)

References 59 publications

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“…It is also worth noting that the two antiphased subpulses of I min (t) are of nearly equal intensity in order to achieve increased cancellation of the wavefunction in this particular normal mode of S 1 ; constructive reinforcement of the wavefunction takes place for any ratio of subpulse intensities. Accordingly, the control mechanism is inferred to be a variant of wavepacket interferometry 52,56,57 induced by a phase-locked intrapulse pair (phase-locking here refers to a constant phase relationship between various subpulses of the temporal envelope). Within a few picoseconds, energy flows across the entire molecular framework [intramolecular vibrational energy redistribution (IVR) 58 ] and redistributes the initially localized vibrational excitation; hence, the controlled interference is destroyed and differences in the coupling to higher electronic states are eliminated (e.g., Figs.…”

Section: A Learning Stagementioning

confidence: 99%

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Roslund

Roth

Guyon

et al. 2011

The Journal of Chemical Physics

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Fundamental molecular selectivity limits are probed by exploiting laser-controlled quantum interferences for the creation of distinct spectral signatures in two flavin molecules, erstwhile nearly indistinguishable via steady-state methods. Optimal dynamic discrimination (ODD) uses optimally shaped laser fields to transiently amplify minute molecular variations that would otherwise go unnoticed with linear absorption and fluorescence techniques. ODD is experimentally demonstrated by combining an optimally shaped UV pump pulse with a time-delayed, fluorescence-depleting IR pulse for discrimination amongst riboflavin and flavin mononucleotide in aqueous solution, which are structurally and spectroscopically very similar. Closed-loop, adaptive pulse shaping discovers a set of UV pulses that induce disparate responses from the two flavins and allows for concomitant flavin discrimination of ∼16σ . Additionally, attainment of ODD permits quantitative, analytical detection of the individual constituents in a flavin mixture. The successful implementation of ODD on quantum systems of such high complexity bodes well for the future development of the field and the use of ODD techniques in a variety of demanding practical applications.

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Section: A Learning Stagementioning

confidence: 99%

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Roslund

Roth

Guyon

et al. 2011

The Journal of Chemical Physics

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“…The resulting pulse shape is plotted in Figure 2b, and the measured ion growth curve is shown in Figure 2c. The spacing of the peaks of the pulse train is much larger than (and not commensurate with 24,25 ) the periods of the vibrational modes of the molecule. 22 The calculated ion growth curve in Figure 2c is in excellent agreement with the data.…”

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confidence: 99%

Coherent Control of the Photoionization of Pyrazine

Singha

Zhao

et al. 2012

J. Phys. Chem. Lett.

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Most attempts to control the absorption of resonant light by quantum mechanical interference have been limited to atoms and small molecules with specialized state configurations and selection rules. Here we illustrate experimentally the possibility of creating laser-induced transparencies in complex molecular systems. Our approach takes advantage of the nonadiabatic excited-state dynamics characteristic of polyatomic molecules. Specifically, we show that it is possible to construct femtosecond pulses using a genetic algorithm to suppress the ionization of isolated pyrazine molecules at a prespecified time. The data suggest that transparency is achieved by localization of a wave packet in a region of the coupled S 1 /S 2 potential energy surfaces, where a vertical transition to the ionic state is energetically forbidden. This approach is general and does not require prior knowledge of the molecular Hamiltonian.

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“…A variety of phase functions were applied to the AOM to produce different shaped UV laser pulses. These included a sine phase to generate sequences of evenly spaced TL pulses, [29][30][31][32] a V-shaped phase to produce a pulse pair, and a quadratic phase to produce chirped pulses.…”

Section: Methodsmentioning

confidence: 99%

Coherent phase control of internal conversion in pyrazine

Seideman

Singha

et al. 2015

The Journal of Chemical Physics

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Shaped ultrafast laser pulses were used to study and control the ionization dynamics of electronically excited pyrazine in a pump and probe experiment. For pump pulses created without feedback from the product signal, the ion growth curve (the parent ion signal as a function of pump/probe delay) was described quantitatively by the classical rate equations for internal conversion of the S 2 and S 1 states. Very different, non-classical behavior was observed when a genetic algorithm (GA) was used to minimize the ion signal at some pre-determined target time, T. Two qualitatively different control mechanisms were identified for early (T< 1.5 ps) and late (T> 1.5 ps) target times. In the former case, the ion signal was largely suppressed for t < T , while for t T the ion signal produced by the GA-optimized pulse and a transform limited (TL) pulse coalesced. In contrast, for T > 1.5 ps the ion growth curve followed the classical rate equations for t < T , while for t T the quantum yield for the GA-optimized pulse was much smaller than for a TL pulse. We interpret the first type of behavior as an indication that the wave packet produced by the pump laser is localized in a region of the S 2 potential energy surface where the vertical ionization energy exceeds the probe photon energy, whereas the second type of behavior may be described by a reduced absorption cross section for S 0 → S 2 followed by incoherent decay of the excited molecules. * rjgordon@uic.edu 2

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Pulse trains in molecular dynamics and coherent spectroscopy: a theoretical study

Cited by 21 publications

References 59 publications

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Coherent Control of the Photoionization of Pyrazine

Coherent phase control of internal conversion in pyrazine

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