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DOE OSTI2021

Observation of a dipole-bound excited state in 4-ethynylphenoxide and comparison with the quadrupole-bound excited state in the isoelectronic 4-cyanophenoxide

Negative ions do not possess Rydberg states, but can have Rydberg-like nonvalence excited states near the electron detachment threshold, including dipole-bound states (DBSs) and quadrupole-bound states (QBSs). While DBSs have been studied extensively, quadrupole-bound excited states have been more rarely observed. 4-cyanophenoxide (4CP – ) was the first anion observed to possess a quadrupole-bound exited state 20 cm-1 below its detachment threshold. Here we report the observation of a DBS in the isoelectronic 4-ethynylphenoxide anion (4EP – ), providing a rare opportunity to compare the behaviors of a dipole-bound and a quadrupole-bound excited state in a pair of very similar anions. Photodetachment spectroscopy (PDS) of cryogenically-cooled 4EP – reveals a DBS 76 cm -1 below its detachment threshold. Photoelectron spectroscopy (PES) at 266 nm shows that the electronic structure of 4EP – and 4CP – are nearly identical. The observed vibrational features in both the PDS and PES, as well as autodetachment from the nonvalence excited states, are also found to be similar for both anions. However, resonant two-photon detachment (R2PD) from the bound vibrational ground state is observed to be very different for the DBS in 4EP – and the QBS in 4CP – . The R2PD spectra reveal that decays take place from both the DBS and QBS to the respective anion ground electronic states within the 5 ns detachment laser pulse due to internal conversion followed by intramolecular vibrational redistribution (IVR), but the decay mechanisms appear to be very different. In the R2PD spectrum of 4EP – , we observe strong threshold electron signals, which are due to detachment, by the second photon, of highly rotationally excited anions resulted from the decay of the DBS. On the other hand, in the R2PD spectrum of 4CP – we observe well-resolved vibrational peaks due to the three lowest-frequency vibrational modes of 4CP – , which are populated from the decay of the QBS. Here, the different behaviors of the R2PD spectra suggest unexpected differences between the relaxation mechanisms of the dipole-bound and quadrupole-bound excited states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Tracking structural solvent reorganization and recombination dynamics following e – photoabstraction from aqueous I – with femtosecond x-ray spectroscopy and scattering

Here we present a sub-picosecond resolved investigation of the structural solvent reorganization and geminate recombination dynamics following 400 nm two-photon excitation and photodetachment of a valence p electron from the aqueous atomic solute, I–(aq). The measurements utilized time-resolved X-ray Absorption Near Edge Structure (TR-XANES) spectroscopy and X-ray Solution Scattering (TR-XSS) at the Linac Coherent Light Source x-ray free electron laser in a laser pump/x-ray probe experiment. The XANES measurements around the L 1 -edge of the generated nascent iodine atoms (I 0 ) yield an average electron ejection distance from the iodine parent of 7.4 ± 1.5 Å with an excitation yield of about 1/3 of the 0.1M NaI aqueous solution. The kinetic traces of the XANES measurement are in agreement with a purely diffusion-driven geminate iodine–electron recombination model without the need for a long-lived (I 0 :e–) contact pair. Nonequilibrium classical molecular dynamics simulations indicate a delayed response of the caging H 2 O solvent shell and this is supported by the structural analysis of the XSS data: We identify a two-step process exhibiting a 0.1 ps delayed solvent shell reorganization time within the tight H-bond network and a 0.3 ps time constant for the mean iodine–oxygen distance changes. The results indicate that most of the reorganization can be explained classically by a transition from a hydrophilic cavity with a well-ordered first solvation shell (hydrogens pointing toward I–) to an expanded cavity around I 0 with a more random orientation of the H 2 O molecules in a broadened first solvation shell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Wigner time delay in photoionization: a 1D model study

Abstract In scattering theory, the Wigner–Smith time delay, calculated through a phaseshift derivative or its multichannel generalization, has been demonstrated to measure the amount of delay or advance experienced by colliding particles during their interaction with the scattering potential. Fetic, Becker, and Milosevic argue that this concept cannot be extended to include photoionization, viewed as a half-scattering experiment. Their argument is based on the lack of information about scattering phaseshifts in the part of the wavefunction (satisfying the ingoing-wave boundary condition) going to the detector. This article aims to test this claim by examining a photodetachment process in a simple 1D model with a short-range symmetrical potential. Using time-dependent perturbation theory with a dipole interaction, the relevant wavepacket of the outgoing particle is analyzed and compared to the free wavepacket as a reference. Our findings confirm that, indeed, a time delay arises in the liberated fragmentation wavepacket, which is expressed as an energy derivative of the scattering phaseshift. Our study highlights that the source of the phaseshift content in the wavepacket arriving at the detector is the dipole matrix element, which is a direct consequence of imposing the ingoing-wave boundary condition. We illustrate our results through numerical simulations of both the non-free and free wavepackets. The amount of the observed time delay is found to be half of that appearing in a typical scattering experiment.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2021

Correlated single- and few-electron backgrounds milliseconds after interactions in dual-phase liquid xenon time projection chambers

In this work, we characterize single- and few-electron backgrounds that are observed in dual-phase liquid xenon time projection chambers at timescales greatly exceeding a maximum drift time after an interaction. These instrumental backgrounds limit a detector's sensitivity to dark matter and cosmogenic neutrinos. Using the ~150g liquid xenon detector at Purdue University, we investigate how these backgrounds, produced after 122keV 57 Co Compton interactions, behave under different detector conditions. We find that the rates of single- and few-electron signals follow power-laws with time after the interaction. We observe linearly increasing rates with increased extraction field, and increased rates in the single-electron background with increased drift field. Normalizing the rates to the primary interaction's measured ionization signal, the rates increase linearly with the depth of the interaction. We test the hypothesis that infrared photons (1550nm) would stimulate and accelerate electron emission via photodetachment from impurities, but find that even 1 Watt of infrared light fails to reduce these backgrounds. We thus provide a characterization that can inform background models for low-energy rare event searches.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1968

Interpretation of pre-sunrise electron densities and negative ions in the D-region.

Photodetachment of electrons from negative ions by solar UV and visible radiation determined from presunrise electron densities and VLF absorption in D region

Sechrist, C. F., Jr.↗

NASA NTRS1970

An investigation of the ionospheric D region at sunrise

The growth over sunrise of the C and D layers of the ionosphere is investigated. The model which is analyzed includes the negative ion species O(-), O2(-), O3(-), O4(-), NO3(-), CO3(-), and CO4(-). Ionization sources due to galactic cosmic rays, precipitated electrons, ionization of NO by scattered Lyman alpha radiation, and the direct solar radiation ionization are also included. The photodetachment of most of the negative ions is discussed, as well as the time variation of these parameters. The time variations of the electron, negative ion, and positive ion densities are calculated over sunrise. From these data, the mesospheric C and D layer development is plotted. Several model parameters are varied until the best agreement with experimentally determined electron densities is obtained. The results are discussed in light of several atmospheric parameters including the O and NO concentrations and the electron-ion recombination coefficient.

Turco, R. P.↗

NASA NTRS1974

The energy distribution cross section in threshold electron-atom impact ionization

The flatness of the energy differential cross section in impact ionization is derived analytically in the Wannier theory. However it is shown that the Wannier zone is confined to a region of the order E/5 is less than or equal to epsilon is less than or equal to 4E/5, where E is the available energy and epsilon is the energy of the electrons. By contrasting the known results of photoionization and photodetachment, one can cogently argue that in the complementary region where electrons share their energy very unequally the cross section rises to a value independent of E, and that this region determines the form of the threshold law.

Temkin, A.↗

NASA NTRS1974

Absorption of laser radiation in a H-He plasma. I - Theoretical calculation of the absorption coefficient

The theory for calculating the absorption of laser radiation by hydrogen is outlined for the temperatures and pressures of common laboratory plasmas. Nonhydrogenic corrections for determining the absorption by helium are also included. The coefficients for the absorption of He-Ne laser radiation at the wavelengths of 0.633, 1.15, and 3.39 microns in a H plasma is presented for temperatures in the range from 10,000 to 40,000 K and electron number densities in the range from 10 to the 15th power to 10 to the 18th power per cu cm. The total absorption of a H-He plasma calculated from this theory is compared with the measured absorption. The theoretical composition of the H-He absorption is analyzed with respect to the significant absorption processes, inverse bremsstrahlung, photoionization, resonance excitation, and photodetachment.

Stallcop, J. R.↗

NASA NTRS1975

Altitudinal, diurnal and latitudinal dependences for ionic concentrations formed by corpuscular fluxes in the stratosphere and mesosphere

On the basis of over 15 rocket measurements of ionic concentrations below 80 km, the height, daily and latitudinal dependences between positive ionic concentrations and cosmic ray intensity below 60 km as well as between ionic concentrations and corpuscular streams within the 60-80 km altitude range are compared. It is shown that ionic concentration and cosmic ray intensity below 60 km at night are likely to be interrelated, in conformity with Chapman's theory of the simple layer. In daytime, all phenomena are aggravated by photodetachment and ion exchange reactions with the participation of ozone. Between 60-80 km, besides ordinary cosmic rays, there must exist an additional corpuscular stream.

Bragin, Y. A.↗

NASA NTRS1981

Negative ions in the ionospheres of planetary bodies without atmospheres

It is noted that negative ions may be formed in the ionospheres of Mercury, the moon, and Jupiter's satellites with densities of a few percent of the ionospheric electron density. Negative ions result from three mechanisms at the planetary surface: charge inversion during energetic proton scattering, with simultaneous secondary negative ion emission, and micrometeorite impacts. The density and distribution of negative ions around planetary bodies depends primarily on the negative ion lifetimes determined through photodetachment by solar radiation.

Wekhof, A.↗

NASA NTRS1985

A Sensitive Infrared Photodetector

Technique utilizing photodetachment of negative ions incorporated into sensitive photodetector which allows detection of low-energy infrared photons, without resorting to cryogenic cooling.

Srivastava, S. K.↗

NASA NTRS1986

High-Flux Atomic-Oxygen Source

Beams of pure ground-state oxygen atoms produced. Accelerated electrons strike beam of O2 gas in dissociative-attachment region, producing O- ions. O- ions accelerated to desired final energy and pass through photodetachment region to form 0(3P) atoms. These pass between electric field plates to remove O- and e and strike target. Designed specifically to study degradation of materials and spacecraft glow phenomena in low Earth orbits, used to study gas-phase collision phenomena involving energetic oxygen atoms.

Chutjian, A.↗

NASA NTRS1988

Theoretical study of the electron affinities of Cu, Cu2, and Cu3

The modified pair functional method is used here to compute the electron affinities of the negative ions of Cu, Cu2, and Cu3 to equal relative accuracy. The results show that, while the extra electron in Cu2(-) occupies a sigma(u) antibonding orbital, the orbital is polarized to reduce the density in the internuclear rergion. The calculations also show that Cu3(-) is a closed-shell linear molecule in its ground state, and that there is an excited triplet state about 0.7 eV higher in energy. This strongly suggests that photodetachment from the excited triplet state is responsible for the low energy structure observed in the photoelectron spectrum of Cu3(-).