Weak-field laser phase modulation coherent control of asymptotic photofragment distributions
Literature Information
Coherent control of the asymptotic photofragment state-resolved distributions by means of laser phase modulation in the weak-field limit is demonstrated computationally for a polyatomic molecule. The control scheme proposed applies a pump laser field consisting of two pulses delayed in time. Phase modulation of the spectral bandwidth profile of the laser field is achieved by varying the time delay between the pulses. The underlying equations show that such a phase modulation is effective in order to produce control effects on the asymptotic, long-time limit photofragment distributions only when the bandwidths of the two pulses overlap in a frequency range. The frequency overlap of the pulses gives rise to an interference term which is responsible for the modulation of the spectral profile shape. The magnitude of the range of spectral overlap between the pulses becomes an additional control parameter. The control scheme is illustrated computationally for the asymptotic photofragment state distributions produced from different scenarios of the Ne–Br2 predissociation. An experimental application of the control scheme is found to be straightforward.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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