One- and Two-Color Resonant Photoionization Spectroscopy of Chromium-Doped Helium Nanodroplets

Koch, Markus; Kautsch, Andreas; Lackner, Florian; Ernst, Wolfgang

doi:10.1021/jp501285r

Cited by 12 publications

(32 citation statements)

References 43 publications

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“…Transitions involving the metastable 4 P states also exhibit comparatively narrow linewidths, which is again very unusual for helium nanodroplets. Narrow linewidths have been reported previously [14,22] and in some cases interpreted as being due to a very weak interaction between the metal atom and the surrounding helium atoms [22].…”

mentioning

confidence: 68%

“…There appears to be general agreement that alkali metal atoms reside on the surfaces of droplets [5,6], as do several of the alkaline earth metals [7][8][9][10][11][12][13]. Almost all such studies have concentrated on metal atoms with either no or one unpaired electron, and these have been added to the droplets in their electronic ground state; the only higher spin systems that have been investigated are chromium atoms, weakly bound alkali dimers and trimers, and the silver dimer [14][15][16][17][18].…”

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confidence: 99%

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Metastable Aluminum Atoms Floating on the Surface of Helium Nanodroplets

et al. 2015

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Metal atoms have proved to be sensitive probes of the properties of superfluid helium nanodroplets. To date, all experiments on the doping of helium droplets have concentrated on the attachment of metal atoms in their ground electronic states. Here we report the first examples of metal atoms in excited states becoming attached to helium nanodroplets. The atoms in question are aluminum, and they have been generated by laser ablation in a metastable quartet state, which attaches to and remains on the surface of helium droplets. Evidence for a surface location comes from electronic spectra, which consist of very narrow absorption profiles that show very small spectral shifts. Supporting ab initio calculations show there to be an energy incentive for a metastable Al atom to remain on the surface of a helium droplet rather than move to the interior. The results suggest that helium droplets may provide a method for the capture and transport of metastable excited atomic and molecular species.

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confidence: 68%

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confidence: 99%

Metastable Aluminum Atoms Floating on the Surface of Helium Nanodroplets

et al. 2015

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“…In this context, chromium (Cr) and copper (Cu) atoms embedded in He droplets were studied by means of REMPI spectroscopy [96][97][98]. The main outcome of that work has been that absorption lines are broadened and shifted by hundreds of cm −1 indicating that the dopants are located inside the droplets.…”

Section: Rempi Spectroscopymentioning

confidence: 99%

“…Even the transition metal atoms Ag [118,128], Cr and Cu [96][97][98], which are initially submerged in the He droplet interior, are found to partly desolvate upon excitation and to leave the droplets as free atoms (see section III).…”

Section: Ion Imagingmentioning

confidence: 99%

Photoionisaton of pure and doped helium nanodroplets

Mudrich

Stienkemeier

2014

International Reviews in Physical Chemistry

118

114

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Helium nanodroplets, commonly regarded as the "nearly ideal spectroscopic matrix", are being actively studied for more than two decades now. While they mostly serve as cold, weakly perturbing and transparent medium for high-resolution spectroscopy of embedded molecules, their intrinsic quantum properties such as microscopic superfluidity still are subject-matter of current research. This article reviews recent work on pure and doped He nanodroplets using PI spectroscopy, an approach which has greatly advanced in the past years. While the notion of the ideal spectroscopic matrix mostly no longer holds in this context, photoionization techniques provide detailed insights into the photo-physical properties of pure and doped He nanodroplets and their relaxation dynamics following electronic excitation. Exploiting nowadays available high laser fields, even highly ionized states of matter on the nanoscale can be formed. Our particular focus lies on recent experimental progress including fs time-resolved spectroscopy, photoion and electron imaging, and novel sources of highly energetic radiation.

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“…13,14 The location of a dopant is dictated by the interaction with helium (the pair potential) and can be estimated by the dimensionless Ancilotto parameter. This has been observed, for example, for Ag, [16][17][18] Cu, 19,20 Cr, [21][22][23] CF 3 ,24,25 and NO. This has been observed, for example, for Ag, [16][17][18] Cu, 19,20 Cr, [21][22][23] CF 3 ,24,25 and NO.…”

Section: Introductionmentioning

confidence: 63%

Photoinduced molecular dissociation and photoinduced recombination mediated by superfluid helium nanodroplets

Kautsch

Koch

Ernst

2015

Phys. Chem. Chem. Phys.

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We have investigated photoinduced chemical reaction dynamics of cold, isolated Cr2 molecules in helium nanodroplets (HeN), exploiting the quantum state specific spatial separation of solvated and surface locations on the droplet. The molecules are excited to achieve dissociation to a ground state (a(7)S3) and a metastable state (a(5)S2) atom. State specific spatial separation, in combination with efficient translational cooling to avoid ejection, causes the ground state atom to be solvated inside the droplet while the metastable atom migrates to the surface. A barrier between the two reactants formed by the HeN prevents recombination. We apply a resonance-enhanced multiphoton ionization scheme including the y(5)P°(1,2,3) <-- a(5)S(2) transition of the surface atom as well as a two-laser scheme including the y(7)P°(2,3,4) <-- a(7)S(3) transition of the solvated atom in order to verify the locations and separation of the dissociation products. Furthermore, ionization of the a(5)S2 surface atom triggers solvation followed by geminate recombination with the a(7)S3 atom, which is verified by the detection of Cr2(+) molecular ions. For small Cr clusters, our results indicate that they may be composed of chromium dimers that exhibit the same dissociation behavior.

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One- and Two-Color Resonant Photoionization Spectroscopy of Chromium-Doped Helium Nanodroplets

Cited by 12 publications

References 43 publications

Metastable Aluminum Atoms Floating on the Surface of Helium Nanodroplets

Metastable Aluminum Atoms Floating on the Surface of Helium Nanodroplets

Photoionisaton of pure and doped helium nanodroplets

Photoinduced molecular dissociation and photoinduced recombination mediated by superfluid helium nanodroplets

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