Spectroscopy on Rydberg states of sodium atoms on the surface of helium nanodroplets.

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.

[1]  C. Callegari,et al.  Perturbation method to calculate the interaction potentials and electronic excitation spectra of atoms in He nanodroplets. , 2011, The journal of physical chemistry. A.

[2]  M. Drabbels,et al.  Unusual Rydberg system consisting of a positively charged helium nanodroplet with an orbiting electron. , 2011, Physical review letters.

[3]  C. Callegari,et al.  One- and two-photon spectroscopy of highly excited states of alkali-metal atoms on helium nanodroplets. , 2010, The Journal of chemical physics.

[4]  C. Callegari,et al.  Alkali-metal electron spin density shift induced by a helium nanodroplet , 2010 .

[5]  C. Callegari,et al.  Molecular beam magnetic resonance in doped helium nanodroplets. A setup for optically detected ESR/NMR in the presence of unresolved Zeeman splittings. , 2009, The journal of physical chemistry. A.

[6]  C. Callegari,et al.  Coherent spin manipulation and ESR on superfluid helium nanodroplets. , 2009, Physical review letters.

[7]  A. Allouche,et al.  Ab initio potential energy curves and transition dipole moments for the interaction of a ground state He with Na(3s-3p) , 2009 .

[8]  A. Hernando,et al.  Absorption Spectrum of Na Atoms Attached to Helium Nanodroplets , 2009 .

[9]  C. Callegari,et al.  Electron spin pumping of Rb atoms on He nanodroplets via nondestructive optical excitation. , 2008, Physical review letters.

[10]  M. Mudrich,et al.  Quantum interference spectroscopy of rubidium-helium exciplexes formed on helium nanodroplets. , 2007, Physical Review Letters.

[11]  A. Hernando,et al.  Unraveling the absorption spectra of alkali metal atoms attached to helium nanodroplets. , 2007, The journal of physical chemistry. A.

[12]  M. Pi,et al.  Squeezing a helium nanodroplet with a Rydberg electron. , 2007, The journal of physical chemistry. A.

[13]  M. Drabbels,et al.  Photodissociation of alkyl iodides in helium nanodroplets. I. Kinetic energy transfer. , 2007, The Journal of chemical physics.

[14]  M. Drabbels,et al.  Excited state dynamics of Ag atoms in helium nanodroplets. , 2007, The journal of physical chemistry. A.

[15]  C. Callegari,et al.  Magnetic dichroism of potassium atoms on the surface of helium nanodroplets. , 2007, Physical review letters.

[16]  F. Spiegelman,et al.  Rydberg states of small NaAr(n)* clusters. , 2006, The Journal of chemical physics.

[17]  M. Pi,et al.  Helium Nanodroplets: An Overview , 2006 .

[18]  M. Drabbels,et al.  Simple procedure to extract speed distributions from ion images with a large background contribution , 2005 .

[19]  M. Pi,et al.  Alkali Atoms attached to 3He Nanodroplets , 2004, cond-mat/0410696.

[20]  M. Mudrich,et al.  Spectroscopy of Cs attached to helium nanodroplets. , 2004, The Journal of chemical physics.

[21]  F. Spiegelman,et al.  One-electron pseudopotential calculations of electronic properties of NaArn: Low-energy isomers and absorption spectra , 2004 .

[22]  F. Stienkemeier,et al.  Formation times of RbHe exciplexes on the surface of superfluid versus normal fluid helium nanodroplets. , 2004, Physical review letters.

[23]  J. Toennies,et al.  Superfluid helium droplets: a uniquely cold nanomatrix for molecules and molecular complexes. , 2004, Angewandte Chemie.

[24]  M. Pi,et al.  Surface location of sodium atoms attached to He 3 nanodroplets , 2003, cond-mat/0312281.

[25]  E. Draeger,et al.  Bose-Einstein condensation at a helium surface. , 2002, Physical Review Letters.

[26]  W. Ernst,et al.  Rb–He exciplex formation on helium nanodroplets , 2001 .

[27]  M. Vrakking.  An iterative procedure for the inversion of two-dimensional ion/photoelectron imaging experiments , 2001 .

[28]  F. Stienkemeier,et al.  Formation of K*He exciplexes on the surface of helium nanodroplets studied in real time. , 2001, Physical review letters.

[29]  G. Jeung,et al.  Undulating potential curves of the Rydberg states of NaHe , 2001 .

[30]  G. Scoles,et al.  Alkali-helium exciplex formation on the surface of helium nanodroplets. I. Dispersed emission spectroscopy , 2000 .

[31]  G. Scoles,et al.  Alkali-helium exciplex formation on the surface of helium nanodroplets. II. A time-resolved study , 2000 .

[32]  F. Stienkemeier,et al.  Langmuir–Taylor surface ionization of alkali (Li, Na, K) and alkaline earth (Ca, Sr, Ba) atoms attached to helium droplets , 2000 .

[33]  L. Reatto,et al.  Fluctuation effects at the free surface of superfluid 4He , 2000 .

[34]  I. Hertel,et al.  COHERENCE AND RELAXATION IN POTASSIUM-DOPED HELIUM DROPLETS STUDIED BY FEMTOSECOND PUMP-PROBE SPECTROSCOPY , 1999 .

[35]  H. Lee,et al.  Undulations of the potential-energy curves for highly excited electronic states in diatomic molecules related to the atomic orbital undulations , 1999 .

[36]  J. Harms,et al.  Density of superfluid helium droplets , 1997, cond-mat/9705070.

[37]  G. Scoles,et al.  Beam Depletion Spectroscopy of Alkali Atoms (Li, Na, K) Attached to Highly Quantum Clusters , 1998 .

[38]  G. Scoles,et al.  Spin–orbit effects in the formation of the Na–He excimer on the surface of He clusters , 1997 .

[39]  G. Scoles,et al.  Spectroscopy of alkali atoms (Li, Na, K) attached to large helium clusters , 1996 .

[40]  Griffin,et al.  Surface region of superfluid helium as an inhomogeneous Bose-condensed gas. , 1995, Physical review letters.

[41]  M. W. Cole,et al.  Physics of solvation , 1995 .

[42]  G. Scoles,et al.  Spectroscopy of alkali atoms and molecules attached to liquid He clusters , 1995 .

[43]  Hartmann,et al.  Rotationally Resolved Spectroscopy of SF6 in Liquid Helium Clusters: A Molecular Probe of Cluster Temperature. , 1995, Physical review letters.

[44]  Ernst,et al.  Laser spectroscopy of alkali-doped helium clusters. , 1995, Physical review letters.

[45]  J. Toennies,et al.  High-resolution infrared spectroscopy of SF6 embedded in He clusters , 1994 .

[46]  A. Golov,et al.  Rydberg branch of electronic excitations of helium clusters , 1994 .

[47]  I. Petsalakis,et al.  Potential energy curves and radiative lifetimes of Rydberg states of NaHe , 1993 .

[48]  A. Golov,et al.  A new type of excimer atom: electron + ionized helium cluster , 1993 .

[49]  J. Toennies,et al.  A new scattering deflection method for determining and selecting the sizes of large liquid clusters of 4He , 1993 .

[50]  Goyal,et al.  Vibrational spectroscopy of sulfur hexafluoride attached to helium clusters. , 1992, Physical review letters.

[51]  S. Patil.  ADIABATIC POTENTIALS FOR ALKALI INERT-GAS SYSTEMS IN THE GROUND-STATE , 1991 .

[52]  S. Stringari,et al.  Density of states and evaporation rate of helium clusters , 1990 .

[53]  Toennies,et al.  Capture of neon atoms by 4He clusters. , 1990, Physical review letters.

[54]  J. Pascale.  Use of l-dependent pseudopotentials in the study of alkali-metal-atom--He systems. The adiabatic molecular potentials , 1983 .

[55]  M. Aymar.  Influence of core-polarisation effects on the photoionisation cross sections of the ground level and excited ns levels of neutral sodium , 1978 .

[56]  M. Aymar,et al.  Theoretical investigation on photoionization from Rydberg states of lithium, sodium and potassium , 1976 .