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Electronic spectroscopy of cationic adamantane clusters and dehydrogenated adamantane in helium droplets.

ABSTRACT: We report the first helium-tagged electronic spectra of cationic adamantane clusters, along with its singly, doubly, and triply dehydrogenated analogues embedded in helium droplets. Absorption spectra were measured by recording the evaporation of helium atoms as a function of laser wavelength in the range of 300-2150 nm. Experimental spectra are coupled with simulated spectra obtained from quantum chemical calculations. The spectrum of cationic adamantane agrees with the electronic photodissociation spectrum measured previously, with an additional low-energy absorption at around 1000 nm. The spectra of the dehydrogenated molecules present broad absorptions exclusively in the high-energy region (300-600 nm). For the higher order adamantane dimer and trimer ions, strong absorptions are observed in the low-energy region (900-2150 nm), rationalised by transitions delocalised over two adamantane units.

SUBMITTER: Kappe M

PROVIDER: S-EPMC9533311 | biostudies-literature | 2022 Oct

REPOSITORIES: biostudies-literature

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Electronic spectroscopy of cationic adamantane clusters and dehydrogenated adamantane in helium droplets.

Kappe Miriam M Schiller Arne A Krasnokutski Serge A SA Ončák Milan M Scheier Paul P Cunningham Ethan M EM

Physical chemistry chemical physics : PCCP 20221005 38

We report the first helium-tagged electronic spectra of cationic adamantane clusters, along with its singly, doubly, and triply dehydrogenated analogues embedded in helium droplets. Absorption spectra were measured by recording the evaporation of helium atoms as a function of laser wavelength in the range of 300-2150 nm. Experimental spectra are coupled with simulated spectra obtained from quantum chemical calculations. The spectrum of cationic adamantane agrees with the electronic photodissocia ...[more]

PMID: 36148794

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Project description:We report doping of green fluorescent protein from an electrospray ionization (ESI) source into superfluid helium droplets. From analyses of the time profiles of the doped droplets, we identify two distinct groups of droplets. The faster group has a smaller average size, on the order of 106 helium atoms/droplet, and the slower group is much larger, by at least an order of magnitude. The relative populations of these two groups depend on the temperature of the droplet source: from 11 to 5 K, the signal intensity of the slower droplet group gradually increases, from near the detection limit to comparable to that of the faster group. We postulate that the smaller droplets are formed via condensation of gaseous helium upon expansion from the pulsed valve, while the larger droplets develop from fragmentation of ejected liquid helium. Our results on the size and velocity of the condensation peak at higher source temperatures (>7 K) agree with previous reports, but those at lower temperatures (<7 K) seem to be off. We attribute this discrepancy to the masking effect of the exceedingly large droplets from the fragmentation peak in previous measurements of droplet sizes. Within the temperature range of our investigation, although the expansion condition changes from subcritical to supercritical, there is no abrupt change in either the velocity distribution or the size distribution of the condensation peak, and the most salient effect is in the increasing intensity of the fragmentation peak. The absolute doping efficiency, as expressed by the ratio of ion-doped droplets over the total number of ions from the ESI source, is on the order of 10-4, while only hundreds of doped ions have been detected. Further improvements in the ESI source are key to extending the technology for future experiments. On the other hand, the separation of the two groups of droplets in velocity is beneficial for size selection of only the smaller droplets for future experiments of electron diffraction.

Dataset Information

Electronic spectroscopy of cationic adamantane clusters and dehydrogenated adamantane in helium droplets.

Publications

Electronic spectroscopy of cationic adamantane clusters and dehydrogenated adamantane in helium droplets.

Similar Datasets

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