Alkali-metal electron spin density shift induced by a helium nanodroplet

Koch, Markus; Callegari, Carlo; Ernst, Wolfgang

doi:10.1080/00268971003623401

Cited by 9 publications

(21 citation statements)

References 45 publications

(58 reference statements)

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“…The omission of this additional effect can possibly explain the early convergence of our model description, which seems to be challenged by the experimental results for clusters beyond our size limit, which are still showing a marginal increase for He droplets with N = 15 000. [4] Nevertheless we believe that our model, which is based on a single empirical parameter applied to all alkalimetal dopants, can be of value for future ESR experiments on doped He droplets.…”

Section: Resultsmentioning

confidence: 98%

“…A significant increase of a HFS is observed for all species at short distances. This behavior is explained by the compression of the s-orbitals due to Pauli repulsion from the doubly occupied helium shells 4, 46, 47. Tentative scans of even shorter distances (not shown in the graph) prove that a HFS approaches a maximum value at a certain distance before it drops down rather steeply, which can be explained by a strong intermixing of the s orbitals with orbitals of higher angular momentum.…”

Section: Theorymentioning

confidence: 97%

“…[3] In ref. [4] our group presented hyperfine-resolved spectra of ESR transitions of rubidium atoms attached to superfluid helium nanodroplets. The high sensitivity of this experimental technique led to the observation of hyperfine shifts in the ESR spectra caused by the chemically inert but physically disturbing helium environment: shifts of the well-known hyperfine structure constants of 85 Rb and 87 Rb were detected as a function of the droplet size.…”

Section: Introductionmentioning

confidence: 99%

“…the resulting helium density distribution of such a weakly bound system, are density functional theory (DFT) or quantum Monte Carlo (QMC) approaches. A detailed study of dimple structures for alkalimetal-doped 3 He and 4 He droplets based on the latter is given in ref. [7].…”

Section: Introductionmentioning

confidence: 99%

“…id quantum liquid such as a 4 He droplet. The second condition, a reasonable scaling with the size of the system, prevents us from using highly sophisticated standard methods of MObased quantum chemistry.…”

Section: Introductionmentioning

confidence: 99%

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Shifts in the ESR Spectra of Alkali‐Metal Atoms (Li, Na, K, Rb) on Helium Nanodroplets

et al. 2012

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He-droplet-induced changes of the hyperfine structure constants of alkali-metal atoms are investigated by a combination of relativistically corrected ab initio methods with a simulation of the helium density distribution based on He density functional theory. Starting from an accurate description of the variation of the hyperfine structure constant in the M–He diatomic systems (M=Li, Na, K, Rb) as a function of the interatomic distance we simulate the shifts induced by droplets of up to 10 000 4He atoms. All theoretical predictions for the relative shifts in the isotropic hyperfine coupling constants of the alkali-metal atoms attached to helium droplets of different size are then tied to a single, experimentally derived parameter of Rb.

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Section: Resultsmentioning

confidence: 98%

Section: Theorymentioning

confidence: 97%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Shifts in the ESR Spectra of Alkali‐Metal Atoms (Li, Na, K, Rb) on Helium Nanodroplets

et al. 2012

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Helium Droplets as Nanocryostats for Molecular Spectroscopy—from the Vacuum Ultraviolet to the Microwave Regime

Callegari

Ernst

2011

Handbook of High‐resolution Spectroscopy

109

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We report on the investigation of mixed alkali metal (Ak) -alkaline earth metal (Ake) molecules on the surface of helium nanodroplets (HeN ). These molecules have recently attracted considerable attention as candidates for the formation of ultracold molecules with a magnetic and an electronic dipole moment a . In our experiments, LiCa and RbSr molecules are formed in a sequential pick-up process in their X 2 Σ + ground state and cool down rapidly to the droplet temperature of 0.38 K b . Excitation spectra of LiCa and RbSr were recorded by using resonance enhanced multi-photon ionization time-of-flight (REMPI-TOF) spectroscopy and laser induced fluorescence (LIF) spectroscopy. On the helium droplet, vibronic transitions in Ak-Ake molecules are broadened and show a characteristic asymmetric peak form, which is caused by the interaction between the molecule and the superfluid HeN environment. For the lower electronic transitions in LiCa and RbSr progressions of vibrational bands excited from the X 2 Σ + (ν ′′ = 0) state are observed. The LiCa spectra can be compared to molecular beam experiments c , which enables the assignment of three band systems near 15260 cm −1 , 19300 cm −1 and 22120 cm −1 as 2 Σ + , 2 ΠΩ and 2 Π band, respectively. In the RbSr excitation spectrum we observe a vibrationally resolved band system near 14020 cm −1 . Upon electronic excitation, a fraction of the molecules desorb from the droplet surface and dispersed fluorescence spectra allow to study the X 2 Σ + ground state and excited states of free Ak-Ake molecules.

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Spectroscopy on Rydberg States of Sodium Atoms on the Surface of Helium Nanodroplets

et al. 2011

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One- and two-photon excitation spectra of sodium atoms on the surface of helium droplets are reported. The spectra are recorded by monitoring the photoionization yield of desorbed atoms as function of excitation frequency. The excitation spectra involving states with principal quantum number up to n = 6 can be reproduced by a pseudodiatomic model where the helium droplet is treated as a single atom. For the lowest excited states of sodium, the effective interaction potentials for this system can be approximated by the sum of NaHe pair potentials. For the higher excited states, the interaction of the sodium valence electron with the helium induces significant configuration mixing, leading to a failure of this approach. For these states, effective interaction potentials based on a perturbative treatment of the interactions between the valence electron, the alkali positive core, and the helium, as described in detail in the accompanying publication, yield excellent agreement with experiment.

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Alkali-metal electron spin density shift induced by a helium nanodroplet

Cited by 9 publications

References 45 publications

Shifts in the ESR Spectra of Alkali‐Metal Atoms (Li, Na, K, Rb) on Helium Nanodroplets

Shifts in the ESR Spectra of Alkali‐Metal Atoms (Li, Na, K, Rb) on Helium Nanodroplets

Helium Droplets as Nanocryostats for Molecular Spectroscopy—from the Vacuum Ultraviolet to the Microwave Regime

Spectroscopy on Rydberg States of Sodium Atoms on the Surface of Helium Nanodroplets

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