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Physical Review Letters

Magnetic Dichroism of Potassium Atoms on the Surface of Helium Nanodroplets

Johann Nagl, Gerald Auböck, Carlo Callegari, Wolfgang Ernst

Published Feb 14, 2007• 24 citations
Publisher

Abstract

The population ratio of Zeeman sublevels of atoms on the surface of superfluid helium droplets (T=0.37 K) has been measured. Laser induced fluorescence spectra of K atoms are measured in the presence of a moderately strong magnetic field (2.9 kG). The relative difference between the two states of circular polarization of the exciting laser is used to determine the electron spin polarization of the ensemble. Equal fluorescence levels indicate that the two spin sublevels of the ground-state K atom are equipopulated, within 1%. Thermalization to 0.37 K would give a population ratio of 0.35. We deduce that the rate of spin relaxation induced by the droplet must be <520/s. For the K2 triplet dimer we find instead full thermalization of the spin.

DOI
10.1103/physrevlett.98.075301

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Physical Review A•Mar 1, 1991•6 citations
The population ratio of Zeeman sublevels of atoms on the surface of superfluid helium droplets (T=0.37 K) has been measured. Laser induced fluorescence spectra of K atoms are measured in the presence of a moderately strong magnetic field (2.9 kG). The relative difference between the two states of circular polarization of the exciting laser is used to determine the electron spin polarization of the ensemble. Equal fluorescence levels indicate that the two spin sublevels of the ground-state K atom are equipopulated, within 1%. Thermalization to 0.37 K would give a population ratio of 0.35. We deduce that the rate of spin relaxation induced by the droplet must be <520/s. For the K2 triplet dimer we find instead full thermalization of the spin.
We measured laser-induced-fluorescence (LIF) and beam-depletion (BD) spectra of rubidium atoms (5S-5P transition) on the surface of superfluid helium nanodroplets (M-He_{N} with M=Rb). It is known that when M is a lighter alkali atom electronic excitation always leads to detachment of the excited atom (M;{*}). The dissociation energy, few tens cm;{-1}, comes either as photon excess energy or from the barrierless formation of a M;{*}-He exciplex. We observe that this picture does not hold when M=Rb and the photon excess energy is small: we are able to excite atoms without detaching them from the droplet, thanks to a barrier preventing formation of the exciplex. This system is ideally suited for optical spin pumping in a He nanodroplet, whose achievement we explicitly demonstrate in a pump-probe magnetic circular dichroism experiment.
Superfluid helium nanodroplets provide a versatile substrate to cool atoms and molecules, and to assemble weakly bound complexes. Absence of spin-relaxation mechanisms makes He nanodroplets ideal to isolate open-shell atoms and create a spin-polarized system. Here, we show the first coherent manipulation of such a system by resonant excitation of a magnetic-dipole transition. Observation of approximately 50 Rabi oscillations demonstrates coherent population transfer with minimal dephasing. Ours is also the first application of ESR spectroscopy to doped He nanodroplets. This unique environment results in extremely sharp lines and hyperfine-resolved spectra: those of single 39K and 85Rb dopant atoms presented here denote an increase of the Fermi contact interaction, which we can follow as a function of droplet size, reflecting the distortion of the valence-electron wave function due to the surrounding He.
Silver atoms, initially embedded in nanodroplets of superfluid helium (roughly 104{10}^{4}104 atoms in size), are found to move to the surface and desorb when excited to the broadened 5p5p5p level. The absorption of a second photon within less than 10 ns leads to the population of previously unobserved Rydberg states (20<n<60)(20<n<60)(20<n<60) of free silver atoms. This is the first result showing laser induced movement of a foreign atom from the inside to the surface of a nanodroplet of superfluid helium.
Superfluid helium droplets represent a unique state of matter, which are large clusters of helium typically containing approximately 103-1011 helium atoms and exhibit remarkable properties such as superfluidity, a very low temperature (0.37 K) and high thermal conductivity. This PhD project investigates two novel aspects of superfluid helium droplets: the use of superfluid helium nanodroplets as the nanoreactors to grow magnetic nanoparticles and the generation and exploration of quantum vortices in a controlled manner. In the first part, we exploit the very low temperature and rapid cooling to develop a new approach for fabricating magnetic nanoparticles. For the very low temperature and the ultrahigh thermal conductivity, superfluid helium can suppress thermal effects during the atom-by-atom growth of magnetic nanoparticles, making the relatively weak exchange interactions (compared with metallic bonding) the driving force. As a result, the atomic spins align for ferromagnetic elements and thus the magnetic moments of nanoparticles are maximized. In particular, we focus on iron nanoparticles coated by a gold shell and investigate their properties by electron microscopy (for structural investigation) and x-ray circular dichroism (XMCD), for magnetic property measurement) at the Diamond Light Source. We first study mass spectrometry of small iron clusters and observed abnormal behaviours. Unlike other molecular clusters formed in helium droplets such as water, gold and silver, which typically follow a Poisson distribution, Fe+ channel was found to be far greater than that of FeN+ (N = 2-8) clusters. We postulate this as an indicator for the formation of high-spin iron clusters inside superfluid helium and attempt to provide an interpretation based on DFT calculations. However, XMCD showed an expected low magnetisation for Fe/Au core-shell nanoparticles which is even lower than iron oxide nanoparticles, indicating that the neutral Fe atoms are oxidized into Fe2+ within the nanoparticles which is magnetically inert. This is accounted by the very high electron negativity of Au atoms and the alloying effect during the growth of nanoparticles, which dismisses the magnetic properties. Our work shows that the choice of protective shell is important to maintain the magnetic properties of iron nanoparticles and points the direction for the next-step research. The second part presents a breakthrough in quantum vortex research. We demonstrate a novel method for generating controlled vortex arrays in superfluid helium droplets through collisions with cesium ions. Subsequential addition of metal atoms (Ag and Au) to helium droplets and the formation of nanodroplets allow the vortex lattices to be imaged after the nanoparticles are deposited onto a solid surface. By this approach we have revealed a record-high vortex density of 5.6×10¹⁴ m⁻², exceeding previous observations in bulk superfluid helium by more than six orders of magnitude. This unprecedented vortex density opens new possibilities for studying quantum hydrodynamics at extreme angular momenta and investigating quantum turbulence in previously inaccessible regimes. Through detailed theoretical analysis and experimental characterization, this work establishes superfluid helium droplets as a versatile platform for both materials synthesis and fundamental research. Our findings not only advance the understanding of superfluidity but also provide a new pathway for developing high-performance magnetic nanomaterials that can potentially revolutionize biomedical science and technologies.
The theory of how excited-state hyperfine structure can be determined using a magnetic field to decouple the nuclear and electronic angular momentum is presented. The initial excited state is assumed to have an anisotropic Zeeman sublevel population distribution, which can be conveniently created by a laser-induced multiphoton excitation of an unpolarized atom. The Zeeman sublevel populations are subsequently mixed by the hyperfine interaction. The degree of mixing is controlled by a magnetic field applied along the quantization axis. The relative Zeeman sublevel populations can be monitored by detecting the polarization of fluorescence emitted when the excited state radiatively decays. It is convenient to take the ratio of two time-integrated fluorescent signals measured for orthogonal linear polarizations, since this is independent of the excited-state number density. The plot of this ratio versus magnetic field is very well approximated by a Lorentzian curve whose half-width is proportional to the magnetic dipole hyperfine coupling constant. This method was used to determine the magnitude of the magnetic dipole constant of the cesium 8D3/2{\mathit{D}}_{3/2}D3/2​ state to be 3.92\ifmmode\pm\else\textpm\fi{}0.10 MHz, which is in excellent agreement with previous results.