2023
DOI: 10.1093/nsr/nwad158
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Exploring the vacuum ultraviolet photochemistry of astrochemically important triatomic molecules

Abstract: The recently constructed vacuum ultraviolet (VUV) free electron laser (FEL) at the Dalian Coherent Light Source (DCLS) is yielding a wealth of new and exquisitely detailed information about the photofragmentation dynamics of many small gas phase molecules. This Review focuses particular attention on five triatomic molecules – H2O, H2S, CO2, OCS and CS2. Each shows excitation wavelength dependent dissociation dynamics, yielding photofragments that populate a range of electronic and (in the case of diatomic frag… Show more

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Cited by 12 publications
(11 citation statements)
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“…HNCO photodissociation at 215 and 217 nm was investigated using a sliced velocity map ion imaging setup, which has been described previously. , In brief, a pulsed molecular beam was produced by expanding 2% HNCO in argon at total pressures of ∼1 bar. The mixtures were expanded into the source chamber through a 0.5 mm diameter pulsed nozzle.…”
Section: Methodsmentioning
confidence: 99%
“…HNCO photodissociation at 215 and 217 nm was investigated using a sliced velocity map ion imaging setup, which has been described previously. , In brief, a pulsed molecular beam was produced by expanding 2% HNCO in argon at total pressures of ∼1 bar. The mixtures were expanded into the source chamber through a 0.5 mm diameter pulsed nozzle.…”
Section: Methodsmentioning
confidence: 99%
“…The fraction of high vibrational excited O 2 (a 1 Δ g ) products was determined to be ~0.4 to 0.6. To the best of our knowledge, no distinguishable bimodal vibrational distribution has been observed previously in SO 2 photodissociation at shorter photolysis wavelengths ( 41 ), or in other triatomic molecular photodissociation processes ( 23 27 ). The similarity between the energy distribution within the products of S( 1 D) + O 2 (a 1 Δ g ) channel in the range of 132 to 134 nm and the molecular products resulting from formaldehyde photolysis ( 1 ) leads to speculation that the high vibrational excited O 2 (a 1 Δ g ) was likely produced through the roaming dynamics.…”
Section: Experimental Evidence Of Roaming Pathway In Highly Excited S...mentioning
confidence: 59%
“…Triatomic molecules have served as textbook examples for the study of unimolecular reaction dynamics and recent advances show that we still have much to learn from these typical molecules ( 23 ). Chemical intuition suggests that the absorption of a high-energy photon by a triatomic molecule such as CO 2 would give rise to a single bond fission and produce CO+O fragments.…”
mentioning
confidence: 99%
“…Similar to state-selective excitation in molecules, , quantum materials, , and bulk materials through frequency tuning, site-selective excitation (SSE) can also be realized by making use of the characteristic absorption at distinct local environment sites and functional groups of materials. SSE can be used in unimolecular reactions to regulate the dynamics and in doped crystals to analyze the structure and manipulate the emission spectra. For proteins and biological membranes, SSE provides an additional dimension in fluorescence spectroscopy to study structures, dynamics, and interactions. In photosynthesis materials, excitation takes place at photosensitizer sites and charges transfer to catalytic active sites to initiate reactions. Sometimes, the roles of these two kinds of sites can be reversed, providing a chance to manipulate reactions …”
Section: Introductionmentioning
confidence: 99%