Dissociative recombination and low-energy inelastic electron collisions of the helium dimer ion

The dissociative recombination (DR) of He-3 He-4(+) has been investigated at the heavy-ion Test Storage Ring (TSR) in Heidelberg by observing neutral products from electron-ion collisions in a merged beams configuration at relative energies from near-zero (thermal electron energy about 10 meV) up to 40 eV. After storage and electron cooling for 35 s, an effective DR rate coefficient at near-zero energy of 3 x 10(-9) cm(3)s(-1) is found. The temporal evolution of the neutral product rates and fragment imaging spectra reveals that the populations of vibrational levels in the stored ion beam are nonthermal with fractions of similar to 0.1-1% in excited levels up to at least v=4, having a significant effect on the observed DR signals. With a pump-probe-type technique using DR fragment imaging while switching the properties of the electron beam, the vibrational excitation of the ions is found to originate mostly from ion collisions with the residual gas. Also, the temporal evolution of the DR signals suggests that a strong electron induced rotational cooling occurs in the vibrational ground state, reaching a rotational temperature near or below 300 K. From the absolute rate coefficient and the shape of the fragment imaging spectrum observed under stationary conditions, the DR rate coefficient from the vibrational ground state is determined; converted to a thermal electron gas at 300 K it amounts to (3.3 +/- 0.9) x 10(-10) cm(3)s(-1). The corresponding branching ratios from v=0 to the atomic final states are found to be (3.7 +/- 1.2) % for 1s2s S-3, (37.4 +/- 4.0) % for 1s2s S-1, (58.6 +/- 5.2) % for 1s2p P-3, and (2.9 +/- 3.0) % for 1s2p P-1. A DR rate coefficient in the range of 2 x 10(-7) cm(3)s(-1) or above is inferred for vibrational levels v=3 and higher. As a function of the collision energy, the measured DR rate coefficient displays a structure around 0.2 eV. At higher energies, it has one smooth peak around 7.3 eV and a highly structured appearance at 15-40 eV. The small size of the observed effective DR rate coefficient at near-zero energy indicates that the electron induced rotational cooling is due to inelastic electron-ion collisions and not due to selective depletion of rotational levels by DR.

[1]  Wing,et al.  Observation of the infrared spectrum of the helium molecular ion (3He 4He)+ , 1987, Physical review letters.

[2]  J. Tennyson,et al.  On the calculation of electron-impact rotational excitation cross sections for molecular ions , 1998 .

[3]  Hiroki Nakamura,et al.  Theoretical study of the dissociative recombination of NO+ with slow electrons , 1990 .

[4]  P. Stancil,et al.  The Deuterium Chemistry of the Early Universe , 1998 .

[5]  M Larsson Dissociative recombination with ion storage rings. , 1997, Annual review of physical chemistry.

[6]  R. Wester,et al.  NEAR-THRESHOLD PHOTODISSOCIATION OF COLD CH+ IN A STORAGE RING , 1998 .

[7]  Wolf,et al.  High-resolution measurement of the dielectronic recombination of fluorinelike selenium ions. , 1996, Physical review. A, Atomic, molecular, and optical physics.

[8]  J. Tennyson,et al.  Electron-impact rotational excitation of linear molecular ions , 2001 .

[9]  J. Rychlewski,et al.  Many‐electron explicitly correlated Gaussian functions. II. Ground state of the helium molecular ion He+2 , 1995 .

[10]  S. Brown,et al.  POSITIVE IONS IN THE AFTERGLOW OF A LOW PRESSURE HELIUM DISCHARGE. Technical Report No. 220 , 1952 .

[11]  A. Orel,et al.  Dissociative recombination of He 2 + molecular ions , 1999 .

[12]  T. S. Green Intense ion beams , 1974 .

[13]  L. Lammich,et al.  Physics with molecular ions in storage rings , 2003 .

[14]  Wolf,et al.  Dissociative recombination of CH+: Cross section and final states. , 1996, Physical review. A, Atomic, molecular, and optical physics.

[15]  M. Grieser,et al.  Upgrading of the Heidelberg accelerator facility with a new high current injector , 1993 .

[16]  D. R. Bates Dissociative Recombination: Crossing and Tunneling Modes , 1994 .

[17]  J. Tennyson,et al.  Calculated rotational and vibrational excitation rates for electron-HeH+ collisions , 1998 .

[18]  H. Poth Electron cooling: Theory, experiment, application , 1990 .

[19]  N. Arista,et al.  Energy-loss and exit-angle distributions of fragmented H 2 + ions after traversing carbon foils , 2000 .

[20]  Z. Vager,et al.  Dissociative recombination of vibrationally excited HD + : State-selective experimental investigation , 1999 .

[21]  Z. Vager,et al.  Coulomb explosion imaging at the heavy ion storage ring TSR , 1998 .

[22]  P. Monchicourt,et al.  High-pressure helium afterglow at room temperature , 1976 .

[23]  R. Stokstad,et al.  First experiments with the heidelberg test storage ring TSR , 1989 .

[24]  R. S. Mulliken RARE-GAS AND HYDROGEN MOLECULE ELECTRONIC STATES, NONCROSSING RULE, AND RECOMBINATION OF ELECTRONS WITH RARE-GAS AND HYDROGEN IONS , 1964 .

[25]  J. Tennyson,et al.  Dissociative recombination without curve crossing: study of HeH+ , 1994 .

[26]  F. O. Ellison Intensities of Vibrational and Rotational Spectra of Charged Diatomic Molecules , 1962 .

[27]  L. H. Andersen,et al.  Dissociative recombination of NO , 1998 .

[28]  Hiroki Nakamura,et al.  Dissociative recombination of H+2, HD+, and D+2 by collisions with slow electrons , 1987 .

[29]  Ubachs,et al.  Comment on "First measurement of the rotational constants for the homonuclear molecular ion He( +)(2)" , 2000, Physical review letters.

[30]  M. Grieser,et al.  Electron cooling and recombination experiments with an adiabatically expanded electron beam , 1996 .

[31]  R. Naaman,et al.  Coulomb Explosion Imaging of Small Molecules , 1989, Science.

[32]  M. Grieser,et al.  Development of seven-gap resonators for the Heidelberg high current injector , 1993 .

[33]  T. Mārk,et al.  Laser-induced photodissociation of He+2 , 1980 .

[34]  S. Peyerimhoff,et al.  Ab initio calculation of the X2Σ+u state of He+2 and adjustment governed by translational spectroscopic measurements , 1976 .

[35]  Guberman Dissociative recombination without a curve crossing. , 1994, Physical review. A, Atomic, molecular, and optical physics.

[36]  Kanter,et al.  Influence of multiple scattering on the Coulomb-explosion imaging of fast molecules. , 1992, Physical review. A, Atomic, molecular, and optical physics.

[37]  Orel,et al.  Resonance-enhanced dissociation of a molecular ion below its electronic excitation threshold. , 1996, Physical Review A. Atomic, Molecular, and Optical Physics.

[38]  M. Larsson,et al.  Absolute high-resolution rate coefficients for dissociative recombination of electrons with HD+: Comparison of results from three heavy-ion storage rings , 2003 .

[39]  Wolf,et al.  New resonances in the dissociative recombination of vibrationally cold CD+ , 1994, Physical review letters.

[40]  J. Cohen Diabatic-states representation for He * (n>=3)+ He collisions , 1976 .

[41]  L. V. Søgaard,et al.  Storage ring study of the dissociative recombination of He+2 , 2005 .

[42]  M. Grieser,et al.  Rate coefficients and final states for the dissociative recombination of LiH+. , 2001, Physical review letters.

[43]  J. Ackermann,et al.  Adiabatic calculations and properties of the He2+ molecular ion , 1991 .

[44]  S. Guberman Mechanism for the green glow of the upper ionosphere , 1997 .

[45]  S. Brown,et al.  Measurement of electron-ion recombination , 1949 .

[46]  L. Lammich,et al.  Evidence for subthermal rotational populations in stored molecular ions through state-dependent dissociative recombination. , 2003, Physical review letters.

[47]  C. Greene,et al.  Unified theoretical treatment of dissociative recombination of D3h triatomic ions: Application to H3+ and D3+ , 2003 .

[48]  Wolf,et al.  High-resolution measurement of dielectronic recombination of lithiumlike Cu26+ , 1992, Physical review. A, Atomic, molecular, and optical physics.

[49]  D. R. Bates Electron Recombination in Helium , 1950 .

[50]  K. Noda,et al.  Evidence of Superelastic Electron Collisions from H 2 + Studied by Dissociative Recombination Using an Ultracold Electron Beam from a Cooler Ring , 1999 .

[51]  M. Grieser,et al.  Electron cooling of heavy ions , 1990 .

[52]  Dirk Schwalm,et al.  Coulomb-explosion imaging of CH2 + : Target-polarization effects and bond-angle distribution , 2004 .

[53]  J. P. Molnar,et al.  MASS SPECTROMETRIC STUDIES OF MOLECULAR IONS IN THE NOBLE GASES , 1951 .

[54]  L. H. Andersen,et al.  The Source of Green Light Emission Determined from a Heavy-Ion Storage Ring Experiment , 1997 .

[55]  Zajfman,et al.  Rotational and vibrational lifetime of isotopically asymmetrized homonuclear diatomic molecular ions. , 1994, Physical review. A, Atomic, molecular, and optical physics.

[56]  R. Wester,et al.  Electron-induced vibrational deexcitation of H 2 + , 2000 .

[57]  K. Hardy,et al.  First Measurement of the Rotational Constants for the Homonuclear Molecular Ion He + 2 , 1999 .

[58]  Hardy,et al.  Hardy and wang reply: , 2000, Physical review letters.

[59]  G. Herzberg,et al.  Spectra of diatomic molecules , 1950 .