Search

The H + D (Formula presented.) (v = 0,1 and 2) charge transfer reaction is studied using an accurate wave packet method, using recently proposed coupled diabatic potential energy surfaces. The state-to-state cross section is obtained for three different channels: non-reactive charge transfer, reactive charge transfer, and exchange reaction. The three processes proceed via the electronic transition from the first excited to the ground electronic state. The cross section for the three processes increases with the initial vibrational excitation. The non-reactive charge transfer process is the dominant channel, whose branching ratio increases with collision energy, and it compares well with experimental measurements at collision energies around 0.5 eV. For lower energies the experimental cross section is considerably higher, suggesting that it corresponds to higher vibrational excitation of D (Formula presented.) (v) reactants. Further experimental studies of this reaction and isotopic variants are needed, where conditions are controlled to obtain a better analysis of the vibrational effects of the D (Formula presented.) reagents.

info:eu-repo/semantics/nonPublished

We have measured the production of Lyman α and Balmer α fluorescence from atomic H and D for the photodissociation of H2, HD and D2 by linearly-polarized photons with energies between 22 and 64 eV. We discuss systematic uncertainties associated with our data, and compare our results with previous experimental results and ab initio calculations of the dissociation process. We comment on the discrepancies.

The collision-energy resolved rate coefficient for dissociative recombination of HD(+) ions in the vibrational ground state is measured using the photocathode electron target at the heavy-ion storage ring TSR. Rydberg resonances associated with rovibrational excitation of the HD(+) core are scanned as a function of the electron collision energy with an instrumental broadening below 1 meV in the low-energy limit. The measurement is compared to calculations using multichannel quantum defect theory, accounting for rotational structure and interactions and considering the six lowest rotational energy levels as initial ionic states. Using thermal-equilibrium-level populations at 300 K to approximate the experimental conditions, close correspondence between calculated and measured structures is found up to the first vibrational excitation threshold of the cations near 0.24 eV. Detailed assignments, including naturally broadened and overlapping Rydberg resonances, are performed for all structures up to 0.024 eV. Resonances from purely rotational excitation of the ion core are found to have similar strengths as those involving vibrational excitation. A dominant low-energy resonance is assigned to contributions from excited rotational states only. The results indicate strong modifications in the energy dependence of the dissociative recombination rate coefficient through the rotational excitation of the parent ions, and underline the need for studies with rotationally cold species to obtain results reflecting low-temperature ionized media.

Rate coefficients for dissociative recombination (DR), dissociative excitation (DE), and vibrational excitation between the helium dimer ion He-4(2)+ and electrons from a few meV up to 40 eV were measured using fast (3.8 and 8.3 MeV) ion beams stored for up to 85 s. Vibrational relaxation to greater than 95% in the v = 0 level was achieved by collisions with cold electrons over 50 s. Low-energy, strongly v-dependent DR rate coefficients are given for v = 0, 1, and >= 2. The rate coefficients at higher energies for v = 0, with DR and DE given on an absolute scale, are compared to results from recent wave-packet calculations on the fast dissociation dynamics of the doubly excited helium dimer, where the three processes occur as competing reaction channels. Also given are rate coefficients for vibrationally superelastic electron collisions at near 10 meV average energy and the approximate vibrational excitation cross section for fast collisions with the residual gas.

A method for the active feedback reduction of optical instrumental intensity asymmetries is presented. It is based on the fast chopping of two spatially separated beams of light with orthogonal linear polarizations that are recombined and passed through a quarter-wave plate to yield a single beam with rapidly flipping helicity. Active electro-optic feedback has been successfully employed to maintain this asymmetry below 10−5.

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. T