Quantum Control from the Gas to Condensed Phase

Recent experiments by Herek, Materny and Zewail [Chem. Phys. Lett. 1994, 228, 15] have demonstrated that the timing between two transform-limited, ultrafast laser pulses can be used to control the branching ratio of Na* (electronically excited atomic sodium) to Na in the photodissociation of NaI. In this work, we theoretically show that, by varying the linear chirp of the first pulse without changing its power spectrum or field strength versus time, the Na* to Na branching ratio can be controlled over a large range with a fixed interpulse delay time and a fixed form of the second pulse. Theory predicts that at 0 K the branching ratio can be varied by a factor of 3, while at high temperatures (1000 K), the factor drops to approximately 1.2 due to the effect of the wide distribution of initial states. Experimental results at 1000 K are presented and are found to be consistent with theory. Several possible experimental methods are discussed to overcome the effects of the thermal distribution of initial states.

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Chirality-induced signals in coherent multidimensional spectroscopy of excitons

Abramavičius

Mukamel

2006

The Journal of Chemical Physics

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The nonlocal second- and third-order susceptibilities of an isotropic ensemble of aggregates are calculated by solving the nonlinear exciton equations which map the system into coupled anharmonic oscillators. Both electric and magnetic contributions are included using the minimal-coupling Hamiltonian. The various tensor components are evaluated to first order in the optical wave vector k. Additional structural information about the interchromophore distances, which is not accessible through zeroth-order contributions (the dipole approximation), is contained to the first order in k. New resonant second- and third-order signals predicted for chiral molecules provide multidimensional extensions of circular dichroism spectroscopy. Numerical simulations demonstrate the sensitivity of third-order signals to the secondary structural motiffs of peptides.

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Quantum Control from the Gas to Condensed Phase

Cited by 3 publications

References 4 publications

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

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

Quantum Control of NaI Photodissociation Reaction Product States by Ultrafast Tailored Light Pulses

Chirality-induced signals in coherent multidimensional spectroscopy of excitons

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