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A representation of the search space in optical pulse shaping problems employing an acousto-optic programmable dispersive filter (AOPDF) is presented for use in closed-loop learning experiments where the optimal spectral phase function to some control problem is determined by an iterative learning algorithm. The representation allows the algorithm to select(More)
We propose an Internet based standard based on primary chemical MIME types to be used in conjuction with the WorldWide Web information delivery system. W e show how this allows the user to have access to and control of molecular structural and spectroscopic information transparently integrated into scientific publications. W e illustrate this with examples(More)
We experimentally investigate the transition to synchronization in a population of photochemical oscillators with weak global coupling. Above a critical coupling strength the oscillators join a one-phase group or two-phase clusters. The number of oscillators in each cluster depends on the initial phase distribution, and irregular switching of oscillators(More)
Ultrafast photodissociation of the 2 (1)A' state of ClNO, which has an absorption spectrum peaking at 335 nm, is studied by computational and experimental methods. New potential-energy surfaces are calculated for the 1 and 2 (1)A' states at the multireference configuration interaction (MRCI) level. Wavepacket dynamics simulations performed both exactly and(More)
Since the discovery of the halogen dance (HD) reaction more than 60 years ago, numerous insights into the mechanism have been unveiled. To date however, the reaction has not been investigated from a theoretical perspective. Density functional theory (DFT) was used to model the potential energy surface linking the starting reagents to the lithiated products(More)
We report on the application of an evolutionary algorithm to a noisy, dynamic optimization problem in chemistry: the maximization of three-photon absorption in molecular iodine. An evolution strategy is used in real-time in a closed loop experiment to search the space of physically realizable phase-modulated femtosecond laser pulses. The probability of(More)
Pump-probe photoionization has been used to map the relaxation processes taking place from highly vibrationally excited levels of the S(2) state of azulene, populated directly or via internal conversion from the S(4) state. Photoelectron spectra obtained by 1+2(') two-color time-resolved photoelectron imaging are invariant (apart from in intensity) to the(More)
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