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At least 73 records · Page 4

Observation of bound valence excited electronic states of deprotonated 2-hydroxytriphenylene using photoelectron, photodetachment, and resonant two-photon detachment spectroscopy of cryogenically cooled anions

Polycyclic aromatic hydrocarbons (PAHs) are common atmospheric pollutants, and they are also ubiquitous in the interstellar medium. Here, we report the study of a complex O-containing PAH anion, the deprotonated 2-hydroxytriphenylene (2-OtPh–), using high-resolution photoelectron imaging and photodetachment spectroscopy of cryogenically cooled anions. Vibrationally resolved photoelectron spectra yield the electron affinity of the 2-OtPh radical as 2.629(1) eV and several vibrational frequencies for its ground electronic state. Photodetachment spectroscopy reveals bound valence excited electronic states for the 2-OtPh– anion, with unprecedentedly rich vibronic features. Evidence is presented for a low-lying triplet state (T1) and two singlet states (S1 and S2) below the detachment threshold. Single-color resonant two-photon photoelectron spectroscopy uncovers rich photophysics for the 2-OtPh– anion, including vibrational relaxation in S1, internal conversion to the ground state of 2-OtPh–, intersystem crossing from S2 to T1, and a long-lived autodetaching shape resonance about 1.3 eV above the detachment threshold. The rich electronic structure and photophysics afforded by the current study suggest that 2-OtPh– would be an interesting system for pump–probe experiments to unravel the dynamics of the excited states of this complex PAH anion.

Chemistry↗

Two-dimensional correlation analysis for x-ray photoelectron spectroscopy

Abstract X-ray photoelectron spectroscopy (XPS) measures the binding energy of core-level electrons, which are well-localised to specific atomic sites in a molecular system, providing valuable information on the local chemical environment. The technique relies on measuring the photoelectron spectrum upon x-ray photoionisation, and the resolution is often limited by the bandwidth of the ionising x-ray pulse. This is particularly problematic for time-resolved XPS, where the desired time resolution enforces a fundamental lower limit on the bandwidth of the x-ray source. In this work, we report a novel correlation analysis which exploits the correlation between the x-ray and photoelectron spectra to improve the resolution of XPS measurements. We show that with this correlation-based spectral-domain ghost imaging method we can achieve sub-bandwidth resolution in XPS measurements. This analysis method enables XPS for sources with large bandwidth or spectral jitter, previously considered unfeasible for XPS measurements.

47 OTHER INSTRUMENTATION↗

Hard x-ray photoelectron spectroscopy: a snapshot of the state-of-the-art in 2020

Hard X-ray photoelectron spectroscopy (HAXPES) is establishing itself as an essential technique for the characterisation of materials. The number of specialised photoelectron spectroscopy techniques making use of hard X-rays is steadily increasing and ever more complex experimental designs enable truly transformative insights into the chemical, electronic, magnetic, and structural nature of materials. This paper begins with a short historic perspective of HAXPES and spans from developments in the early days of photoelectron spectroscopy to provide an understanding of the origin and initial development of the technique to state-of-the-art instrumentation and experimental capabilities. The main motivation for and focus of this paper is to provide a picture of the technique in 2020, including a detailed overview of available experimental systems worldwide and insights into a range of specific measurement modi and approaches. Herein, we also aim to provide a glimpse into the future of the technique including possible developments and opportunities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Polarized photoelectrons from converging vector waves

Abstract This paper investigates the spin characteristics of photoelectrons when hydrogen-like ions are centro-symmetrically irradiated with converging vector waves—a non-paraxial form of structured light. For a photon with given total angular momentum and third component thereof, photoelectrons with both helicities are obtained—in contrast to the fixed helicities produced by left- or right-circularly polarized light. The angular distribution of photoelectrons is broadly tunable through the radiation mode numbers, and opposite helicities can be extracted in synchronism.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Resonant control of photoelectron directionality by interfering one- and two-photon pathways

Coherent control of interfering one- and two-photon processes has for decades been the subject of research to achieve the redirection of photocurrent. The present study develops two-pathway coherent control of ground-state helium atom above-threshold photoionization for energies up to the N = 2 threshold, based on a multichannel quantum defect and R-matrix calculation. Three parameters are controlled in our treatment: the optical interference phase ΔΦ, the reduced electric field strength χ = $\mathscr{E}^2_ω$$\mathscr{E}_{2ω}$, and the final state energy ε. A small energy change near a resonance is shown to flip the emission direction of photoelectrons with high efficiency, through an example where 90% of photoelectrons whose energy is near the 2p 2 1 S e resonance flip their emission direction. However, the large fraction of photoelectrons ionized at the intermediate state energy, which are not influenced by the optical control, make this control scheme challenging to realize experimentally.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Rocket measurements of conjugate photoelectrons during the total solar eclipse of 7 March 1970 over Wallops Island.

Results of measurements made with a retarding potential analyzer on a Nike-Tomahawk rocket during the totality of the solar eclipse, showing definite evidence for the existence of photoelectrons from the conjugate hemisphere. Photoelectrons are observed in the altitude range from 120 to 260 km. The observed flux in the energy range from 2 to 30 eV is relatively constant above about 200 km, but decreased below that altitude. The flux of 5-eV energy electrons above 200 km altitude is about 10 to the 7th power electrons/cm/sec/eV. Higher-energy electrons were also observed, and it is possible that the energy content of these observed fluxes of conjugate-point photoelectrons is sufficient to maintain the observed electron densities and temperatures during the total eclipse.

Maier, E. J.↗

The 6300 A predawn enhancement - Excitation by photoelectrons from the magnetic conjugate point.

Incoherent scatter and tilting filter photometer data from Arecibo Observatory were combined to search for a contribution to the 6300 A predawn enhancement due to impact excitation by photoelectrons from the magnetic conjugate point. Prior to about 105 deg conjugate solar zenith angle, calculations of the 6300 A intensities due to dissociative recombination gave good agreement with the observed intensities. Then, with the arrival of conjugate photoelectrons (confirmed by plasma line enhancements), the observed intensities rose above the calculated, the difference increasing until a plateau was achieved at a conjugate solar zenith angle of about 95 deg. The difference or residual intensity is attributed to direct photoelectron impact excitation. Significant day-to-day variations in the onset angle and intensity have a strong negative correlation with ionospheric electron density.

Wickwar, V. B.↗

Direct observation of the lunar photoelectron layer.

The Charged-Particle Lunar Environment Experiment (CPLEE), a part of the Apollo 14 ALSEP, is an ion-electron spectrometer capable of measuring ions and electrons with energies between 40 eV and 50 keV. Accordingly, the instrument, with apertures 26 cm above the surface, has detected a layer of photoelectrons, or photoelectron gas above the sunlit lunar surface with energies ranging up to 200 eV. The experimental data for periods when the moon was in the earth's magnetotail for electron energies between 40 and 200 eV follows a defined power-law spectrum. The implications of this measurement are two-fold in that the lunar surface potential can be immediately determined to be at least 200 V, and a value of the photoelectron yield of the lunar surface material for photon energies above 40 eV may be computed.

Reasoner, D. L.↗

Photoelectrons and solar wind/lunar limb interaction.

It is suggested that boundary conditions for solar wind/lunar limb interactions are active. The 'whole-moon' limb does not evoke a shock cone, because warm (approximately equal 13 eV/electron) solar wind electrons are replaced by cool (less than or equal to 2 eV/electron) photoelectrons that are ejected from the generally smooth areas of the lunar terminator illuminated at glazing angles by the sun. A localized volume of low thermal pressure is created in the solar wind by these cool photoelectrons. The solar wind expands into this turbulence-suppressive volume without shock production. Conversely, directly illuminated highland areas exchange hot photoelectrons (greater than 20 eV/electron) for warm solar wind electrons. The hot electrons generate a localized pressure increase in the adjacent solar wind flow which evokes a shock streamer in the solar wind. Shock streamers are identifiable by a coincident increase in the magnitude of the solar wind magnetic field immediately external to the lunar wake. Shock occurrence is controlled by lunar topography, solar activity in the hard ultraviolet (greater than 20 eV), solar wind electron density and thermal velocity, and the intensity of the solar wind magnetic field.

Criswell, D. R.↗

Photoelectron angular distributions as a probe of anisotropic electron-ion interactions

Expressions are given for atomic photoelectron angular distributions in LS coupling in which the role of anisotropic final state electron-ion interactions emerges explicitly. Calculations of photoelectron angular distributions for atomic sulfur are presented in which these anisotropic interactions produce pronounced deviations from the predictions of the Cooper-Zare model. Such effects are expected to be a general feature of photoelectron angular distributions for most open shell atoms.

Dill, D.↗

The effect of conjugate photoelectron impact ionization on the pre-dawn ionosphere

The measured photoelectron fluxes are used to show that ionization by photoelectrons is not sufficiently large to affect significantly the nighttime ionosphere. The measured downward photoelectron flux used in the calculations is shown in a table. This flux was measured on December 9, 1971 at an altitude of 1400 km, when the local zenith angle was 159 deg and the conjugate zenith angle was 85.2 deg.

Nagy, A. F.↗

Photoelectrons and lunar limb shocks

It is suggested that boundary conditions for solar wind/lunar limb interactions are active. The 'whole-moon' limb does not evoke a shock cone because warm solar wind electrons are replaced by cool photoelectrons that are ejected from the generally smooth areas of the lunar terminator illuminated at glancing angles by the sun. A localized volume of low thermal pressure is created in the solar wind by these cool photoelectrons. The solar wind expands into this volume without shock production. Directly illuminated highland areas exchange hot photoelectrons for warm solar wind electrons. The hot electrons generate a localized pressure increase in the adjacent solar wind flow which evokes a shock streamer in the solar wind. Shock streamers are identifiable by a coincident increase in the magnitude of the solar wind magnetic field. Shock occurrence is controlled by lunar topography, solar activity in the hard ultraviolet, solar wind electron density and thermal velocity, and the density of the solar wind magnetic field.

Criswell, D. R.↗

Photoelectron angular distributions as a probe of anisotropic electron-ion interactions

Expressions are given for atomic photoelectron angular distributions in LS coupling in which the role of anisotropic final state electron-ion interactions emerges explicitly. Calculations of photoelectron angular distributions for atomic sulfur are presented in which these anisotropic interactions produce clear deviations from the predictions of the Cooper-Zare model. Such effects are expected to be a general feature of photoelectron angular distributions for most open-shell atoms.

Dill, D.↗

Calculated photoelectron pitch angle and energy spectra

Calculations of the steady-state photoelectron energy and angular distribution in the altitude region between 120 and 1000 km are presented. The distribution is found to be isotropic at all altitudes below 250 km, while above this altitude anisotropies in both pitch angle and energy are found. The isotropy found in the angular distribution below 250 km implies that photoelectron transport below 250 km is insignificant, while the angular anisotropy found above this altitude implies a net photoelectron current in the upward direction.

Mantas, G. P.↗

Observations of OI 7774 emission excited by conjugate photoelectrons

Observations and computer calculations of O I 7774 A airglow emissions excited by conjugate photoelectrons have been carried out. The observations were made at McDonald Observatory, Texas using a 2 m grille spectrometer from December 1972 to June 1973. The zenithal emission intensity during conjugate photoelectron precipitation was fairly constant at 2-4 R until conjugate sunset, after which it diminished steadily and ceased near a conjugate solar zenith angle of 105 (plus or minus 3) deg. A predawn enhancement in both O I 7774 A and forbidden O I 6300 A was observed to commence near 102 deg. The computations utilize the two-stream technique of Nagy and Banks (1970) to obtain the escaping photoelectron flux and the local excitation rates of the oxygen emissions. Good agreement with the observations is obtained for the dependence of the emission rate on conjugate solar zenith angle.

Christensen, A. B.↗

On the energy deposition of photoelectrons in the atmosphere of Venus

Vertical components of photoelectron fluxes in the atmosphere of Venus are computed by solving an appropriate form of the Boltzmann equation in the cases where there is no flux of either photoelectrons or solar-wind particles across the ionopause and where photoelectrons are free to escape from the atmosphere. It is assumed that Venus has no magnetic field and that the atmosphere is composed of carbon dioxide, atomic oxygen, and helium. The results are plotted as a function of altitude for several energies in the range from 100 eV to a cutoff of the order of 1 eV. Heating rates for the two upper boundary conditions and the case of no spatial transport are determined which show that transport effects dominate at altitudes greater than about 200 km. Electron temperatures are calculated for the adopted model atmosphere and ionosphere by solving the pertinent conservation equation, and excitation rates are computed for the CO Cameron band as well as the CO2(+) A and B bands.

Mccormick, P. T.↗

Comparison between calculated and measured photoelectron fluxes from Atmosphere Explorer C and E

The two-stream method has been used to calculate photoelectron fluxes. These results have been compared to those obtained by the photoelectron spectrometer on Atmosphere Explorers C and E. At both low altitudes, and higher altitudes (where transport effects are significant) the calculated and measured photoelectron fluxes yield good agreement. It is suggested that (1) better photoionization and scattering cross-section data will yield improved flux calculations, and (2) measurements of the pitch angle distribution are necessary for better high-altitude comparisons.

Nagy, A. F.↗

Photoelectrons in the upper atmosphere - A formulation incorporating effects of transport

A technique for solving the problem of photoelectron spatial transport and spectral degradation is presented. The developed model, which allows for a relatively complete description of the relevant transport and collisional physics, can be applied to study processes at either low or high altitude, and may be used to investigate interhemispheric transport. The technique involves dividing the spatial dimension into a set of discrete ordinates and calculating the photoelectron intensity for a specific energy at each point in space and at a set of angle points. The selected range of the energy spectrum was covered completely by a set of energy bins, and the photoelectron intensity in the highest energy bin was calculated first by assuming that the only source term was derived from photoionization. The method is similar to a method used in radiative transfer theory. Spatial and angular redistribution of electrons play a dominant role at heights above 400 km.

Prather, M. J.↗