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تسجيل مستخدم جديدMolecular photodissociation
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Photodissociation is the dominant removal process of molecules in any region exposed to intense ultraviolet (UV) radiation. This includes diffuse and translucent interstellar clouds, dense photon-dominated regions, high velocity shocks, the surface layers of protoplanetary disks, and cometary and exoplanetary atmospheres. The rate of photodissociation depends on the cross sections for absorption into a range of excited electronic states, as well as on the intensity and shape of the radiation field at each position into the region of interest. Thus, an acccurate determination of the photodissociation rate of even a simple molecule like water or carbon monoxide involves many detailed considerations ranging from its electronic structure to its dissociation dynamics and the specifics of the radiation field that the molecule is exposed to. In this review chapter, each of these steps in determining photodissociation rates is discussed systematically and examples are provided.
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We propose a strategy for enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon. The large possible coupling on the single-molecule level combined with the highly lossy nature of plasmonic modes, wit
h lifetimes on the order of femtoseconds, opens an ultrafast decay channel for the molecule. For plasmon mode frequencies below the vertical photoexcitation energy of the molecule, the difference between excitation and emission energy is converted into vibrational energy on the molecular ground state in a Raman-like process. Under the correct conditions, this energy can be high enough to enable efficient photodissociation on the electronic ground state. We demonstrate the concept using numerical simulations of the Lindblad master equation for the hydrogen molecule in the vicinity of an aluminum nanoparticle, and explore the photodissociation efficiency as a function of various system parameters.
Photodissociation of a molecule produces a spatial distribution of photofragments determined by the molecular structure and the characteristics of the dissociating light. Performing this basic chemical reaction at ultracold temperatures allows its qu
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Astronomical observations have shown that small carbonaceous molecules can persist in interstellar clouds exposed to intense ultraviolet radiation. Current astrochemical models lack quantitative information on photodissociation rates in order to inte
rpret these data. We here present ab initio multi-reference configuration-interaction calculations of the vertical excitation energies, transition dipole moments and oscillator strengths for a number of astrophysically relevant molecules: C3, C4, C2H, l- and c-C3H, l- and c-C3H2, HC3H, l-C4H and l-C5H. Highly excited states up to the 9th root of each symmetry are computed, and several new states with large oscillator strengths are found below the ionization potentials. These data are used to calculate upper limits on photodissociation rates in the unattenuated interstellar radiation field by assuming that all absorptions above the dissociation limit lead to dissociation.
We use (1+1$$) resonance-enhanced multiphoton photodissociation (REMPD) to detect the population in individual rovibronic states of trapped HfF$^+$ with a single-shot absolute efficiency of 18%, which is over 200 times better than that obtained with
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