Four-Tool Control of Competing Photochemical Channels

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A single Hamiltonian and physical input–output optical network are constructed for coherent control of two competing channels in a CH3I-inspired, 266-nm photodissociation model. The electronic doublet, a three-level C–I stretch, a two-level umbrella vibration, and two rotational branches produce a 25-dimensional reactive Hilbert space. Intramolecular vibrational redistribution (IVR), nonadiabatic mixing, product-selective absorbing jumps, electronic dephasing, and a thermally balanced IVR relaxation pair are included explicitly. Gaussian amplitude and chirp, a three-port T 3 phase control, a ring-resonator (solid-torus) cavity, and a half-twist polarization-exchange interferometer act on the same physical electric field. Using the stipulated illustrative parameters, a bounded numerical search followed by local open-system refinement obtains a thermal target product probability of 12.83%, selectivity 43.15%, and total reaction probability 29.73%, from 1.120176 pJ of incident UV energy. A Jones-optimized direct Gaussian reference under the same input budget obtains 20.28%, 46.61%, and 43.51%, respectively; hence this numerical benchmark does not demonstrate a four-tool selectivity or yield advantage. The four-tool intrinsic optical loss is lower (14.34% versus 20.78% of incident energy). We prove (i) exact 100% channel selectivity is equivalent to absence of occupation of every competing jump’s support while the target yield is nonzero; (ii) strictly positive electronic dephasing prohibits exact 100% selectivity in the specified model for any coherent pump that reacts; and (iii) passive optical preprocessing cannot outperform unrestricted direct pulse synthesis under identical local modes and energy. R02 further derives an exact integrated electronic-channel Gram matrix and … [source excerpt; see complete PDF]

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