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## Full-Text Articles in Physics

Low-Energy Nondipole Effects In Molecular Nitrogen Valence-Shell Photoionization, Oliver Hemmers, Renaud Guillemin, D. Rolles, A. Wolska, Dennis W. Lindle, E. P. Kanter, B. Krassig, S. H. Southworth, R. Wehlitz, B. Zimmermann, V. Mckoy, P. W. Langhoff

#### Low-Energy Nondipole Effects In Molecular Nitrogen Valence-Shell Photoionization, Oliver Hemmers, Renaud Guillemin, D. Rolles, A. Wolska, Dennis W. Lindle, E. P. Kanter, B. Krassig, S. H. Southworth, R. Wehlitz, B. Zimmermann, V. Mckoy, P. W. Langhoff

*Environmental Studies Faculty Publications*

Observations are reported for the first time of significant nondipole effects in the photoionization of the outer-valence orbitals of diatomic molecules. Measured nondipole angular-distribution parameters for the 3σ_{g}, 1π_{u}, and 2σ_{u} shells of N_{2} exhibit spectral variations with incident photon energies from thresholds to ∼200 eV which are attributed via concomitant calculations to particular final-state symmetry waves arising from (E1)⊗(M1,E2) radiation-matter interactions first-order in photon momentum. Comparisons with previously reported K-edge studies in N_{2} verify linear scaling with photon momentum, accounting in part for the significantly enhanced nondipole behavior observed in inner-shell ionization ...

Nondipole Effects In The Photoionization Of Xe 4d5/2 And 4d3/2: Evidence For Quadrupole Satellites, Oliver Hemmers, Renaud Guillemin, D. Rolles, A. Wolska, Dennis W. Lindle, K. T. Cheng, W. R. Johnson, H. L. Zhou, S. T. Manson

#### Nondipole Effects In The Photoionization Of Xe 4d5/2 And 4d3/2: Evidence For Quadrupole Satellites, Oliver Hemmers, Renaud Guillemin, D. Rolles, A. Wolska, Dennis W. Lindle, K. T. Cheng, W. R. Johnson, H. L. Zhou, S. T. Manson

*Environmental Studies Faculty Publications*

Measurements of nondipole parameters in spin-orbit-resolved Xe 4d photoionization demonstrate dynamical differences arising from relativistic effects. The experimental data do not agree with relativistic random-phase approximation calculations of single ionization dipole and quadrupole channels. It is suggested that the discrepancy is due to the omission of multiple-excitation quadrupole channels, i.e., quadrupole satellite transitions.

Nearest-Neighbor-Atom Core-Hole Transfer In Isolated Molecules, Renaud Guillemin, Oliver Hemmers, D. Rolles, S. W. Yu, A. Wolska, I. Tran, A. C. Hudson, J. Baker, Dennis W. Lindle

#### Nearest-Neighbor-Atom Core-Hole Transfer In Isolated Molecules, Renaud Guillemin, Oliver Hemmers, D. Rolles, S. W. Yu, A. Wolska, I. Tran, A. C. Hudson, J. Baker, Dennis W. Lindle

*Environmental Studies Faculty Publications*

A new phenomenon sensitive only to next-door-neighbor atoms in isolated molecules is demonstrated using angle-resolved photoemission of site-selective core electrons. Evidence for this interatomic core-to-core electron interaction is observable only by measuring nondipolar angular distributions of photoelectrons. In essence, the phenomenon acts as a very fine atomic-scale sensor of nearest-neighbor elemental identity.

E1-E2 Interference In The Vuv Photoionization Of He, E. P. Kanter, B. Krassig, S. H. Southworth, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, R. Wehlitz, M. Ya Amusia, L. V. Chernysheva, N. L. S. Martin

#### E1-E2 Interference In The Vuv Photoionization Of He, E. P. Kanter, B. Krassig, S. H. Southworth, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, R. Wehlitz, M. Ya Amusia, L. V. Chernysheva, N. L. S. Martin

*Environmental Studies Faculty Publications*

We have measured the forward-backward asymmetry of photoelectron angular distributions produced in the vacuum ultraviolet photoionization of helium. This asymmetry, a consequence of the breakdown of the dipole approximation, measures the real part of the ratio of the quadrupole and dipole matrix elements. In the autoionization region, the strong energy dependence of the asymmetry permits an experimental separation of the ratio of those magnitudes from their phase difference. We experimentally determined the Fano parameters of the 2p^{2}^{1}D_{2} quadrupole resonance, and report improved values of the width Γ and line profile parameter q from those previously available ...

Non-Dipolar Electron Angular Distributions From Fixed-In-Space Molecules, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, E. Shigemasa, K. Le Guen, D. Ceolin, C. Miron, N. Leclercq, P. Morin, Marc Simon, P. W. Langhoff

#### Non-Dipolar Electron Angular Distributions From Fixed-In-Space Molecules, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, E. Shigemasa, K. Le Guen, D. Ceolin, C. Miron, N. Leclercq, P. Morin, Marc Simon, P. W. Langhoff

*Environmental Studies Faculty Publications*

The first indication of nondipole effects in the azimuthal dependence of photoelectron angular distributions emitted from fixed-in-space molecules is demonstrated in N_{2}. Comparison of the results with angular distributions observed for randomly oriented molecules and theoretical derivations for the nondipole correction first order in photon momentum suggests that higher orders will be needed to describe distributions measured in the molecular frame.

Photoexcitation Of A Dipole-Forbidden Resonance In Helium, B. Krassig, E. P. Kanter, S. H. Southworth, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, R. Wehlitz, N. L. S. Martin

#### Photoexcitation Of A Dipole-Forbidden Resonance In Helium, B. Krassig, E. P. Kanter, S. H. Southworth, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, R. Wehlitz, N. L. S. Martin

*Environmental Studies Faculty Publications*

We have observed photoexcitation of the dipole-forbidden 1s^{2}^{1}S_{0}→2p^{2}^{1}D_{2} resonance in helium by measuring the nondipolar forward-backward asymmetry of photoelectron angular distributions in the 2ℓ2ℓ^{′} autoionizing region. By exploiting the electric dipole-quadrupole interference in the excitation of both the 2s2p^{1}P_{1} and 2p^{2}^{1}D_{2} levels, we have observed the quadrupole resonance in photoabsorption and extracted its Fano line shape parameters and the relative phase of the 1sEp and 1sEd continua. We find the quadrupole line profile index q_{2} to be markedly different from theoretical expectations.

Large Nondipole Effects In The Angular Distributions Of K-Shell Photoelectrons From Molecular Nitrogen, Oliver Hemmers, H. Wang, P. Focke, I. A. Sellin, Dennis W. Lindle, J. C. Arce, J. A. Sheehy, P. W. Langhoff

#### Large Nondipole Effects In The Angular Distributions Of K-Shell Photoelectrons From Molecular Nitrogen, Oliver Hemmers, H. Wang, P. Focke, I. A. Sellin, Dennis W. Lindle, J. C. Arce, J. A. Sheehy, P. W. Langhoff

*Environmental Studies Faculty Publications*

Measurements of angular distributions of K-shell electrons photoejected from molecular nitrogen are reported which reveal large deviations at relatively low photon energies ( ħω≤500eV) from emission patterns anticipated from the dipole approximation to interactions between radiation and matter. A concomitant theoretical analysis incorporating the effects of electromagnetic retardation attributes the observed large nondipole behaviors in N_{2} to bond-length-dependent terms in the E1⊗(E2,M1) photoelectron emission amplitudes which are indicative of a potentially universal nondipole behavior in molecular photoionization.

Dynamical Relativistic Effects In Photoionization: Spin-Orbit-Resolved Angular Distributions Of Xenon 4d Photoelectrons Near The Cooper Minimum, H. Wang, G. Snell, Oliver Hemmers, M. M. Sant'anna, I. A. Sellin, N. Berrah, Dennis W. Lindle, P. C. Deshmukh, N. Haque, S. T. Manson

#### Dynamical Relativistic Effects In Photoionization: Spin-Orbit-Resolved Angular Distributions Of Xenon 4d Photoelectrons Near The Cooper Minimum, H. Wang, G. Snell, Oliver Hemmers, M. M. Sant'anna, I. A. Sellin, N. Berrah, Dennis W. Lindle, P. C. Deshmukh, N. Haque, S. T. Manson

*Environmental Studies Faculty Publications*

Two decades ago, it was predicted [Y. S. Kim et al., Phys. Rev. Lett. 46, 1326 (1981)] that relativistic effects should alter the dynamics of the photoionization process in the vicinity of Cooper minima. The present experimental and theoretical study of the angular distributions of Xe 4d_{3/2} and 4d_{5/2} photoelectrons demonstrates this effect for the first time. The results clearly imply that relativistic effects are likely to be important for intermediate- Z atoms at most energies.

Relativistic Effects On Interchannel Coupling In Atomic Photoionization: The Photoelectron Angular Distribution Of Xe, Oliver Hemmers, S. T. Manson, M. M. Sant'anna, P. Focke, H. Wang, I. A. Sellin, Dennis W. Lindle

#### Relativistic Effects On Interchannel Coupling In Atomic Photoionization: The Photoelectron Angular Distribution Of Xe, Oliver Hemmers, S. T. Manson, M. M. Sant'anna, P. Focke, H. Wang, I. A. Sellin, Dennis W. Lindle

*Environmental Studies Faculty Publications*

Measurements of the photoelectron angular-distribution asymmetry parameter β for Xe 5s photoionization have been performed in the 80–200 eV photon-energy region. The results show a substantial deviation from the nonrelativistic value of β=2 and provide a clear signature of significant relativistic effects in interchannel coupling.

Electric-Octupole And Pure-Electric-Quadrupole Effects In Soft X-Ray Photoemission, Andrei Derevianko, Oliver Hemmers, S. Oblad, P. Glans, H. Wang, S. B. Whitfield, R. Wehlitz, I. A. Sellin, W. R. Johnson, Dennis W. Lindle

#### Electric-Octupole And Pure-Electric-Quadrupole Effects In Soft X-Ray Photoemission, Andrei Derevianko, Oliver Hemmers, S. Oblad, P. Glans, H. Wang, S. B. Whitfield, R. Wehlitz, I. A. Sellin, W. R. Johnson, Dennis W. Lindle

*Environmental Studies Faculty Publications*

Second-order [ O(k^{2}), k = ω/c] nondipole effects in soft-x-ray photoemission are demonstrated via an experimental and a theoretical study of angular distributions of neon valence photoelectrons in the 100–1200 eV photon-energy range. A newly derived theoretical expression for nondipolar angular distributions characterizes the second-order effects using four new parameters with primary contributions from pure-quadrupole and octupole-dipole interference terms. Independent-particle calculations of these parameters account for a significant portion of the existing discrepancy between experiment and theory for Ne 2p first-order nondipole parameters.

Beyond The Dipole Approximation: Angular-Distribution Effects In The 1s Photoemission From Small Molecules, Dennis W. Lindle, Oliver Hemmers, H. Wang, P. Focke, I. A. Sellin, J. D. Mills, J. A. Sheehy, P. W. Langhoff

#### Beyond The Dipole Approximation: Angular-Distribution Effects In The 1s Photoemission From Small Molecules, Dennis W. Lindle, Oliver Hemmers, H. Wang, P. Focke, I. A. Sellin, J. D. Mills, J. A. Sheehy, P. W. Langhoff

*Environmental Studies Faculty Publications*

Over the past two decades, the dipole approximation has facilitated a basic understanding of the photoionization process in atoms and molecules. Recent experiments on the 1*s* inner shells of small molecules at relatively low photon energies (⩽ 1000 eV) show strong nondipole effects. They are significant and measurable at energies close to threshold, in conflict with a common assumption that the dipole approximation is valid for photon energies below 1 keV.

Breakdown Of The Independent Particle Approximation In High-Energy Photoionization, E. W. B. Dias, H. S. Chakraborty, P. C. Deshmukh, S. T. Manson, Oliver Hemmers, P. Glans, D. Hansen, H. Wang, S. B. Whitfield, Dennis W. Lindle, R. Wehlitz, Jon C. Levin, I. A. Sellin

#### Breakdown Of The Independent Particle Approximation In High-Energy Photoionization, E. W. B. Dias, H. S. Chakraborty, P. C. Deshmukh, S. T. Manson, Oliver Hemmers, P. Glans, D. Hansen, H. Wang, S. B. Whitfield, Dennis W. Lindle, R. Wehlitz, Jon C. Levin, I. A. Sellin

*Environmental Studies Faculty Publications*

The independent particle approximation is shown to break down for the photoionization of both inner and outer nℓ (ℓ>0) electrons of all atoms, at high enough energy, owing to interchannel interactions with the nearby ns photoionization channels. The effect is illustrated for Ne 2p in the 1 keV photon energy range through a comparison of theory and experiment. The implications for x-ray photoelectron spectroscopy of molecules and condensed matter are discussed.

Kinetic-Energy- And Angular-Resolved Fragmentation Of Co In Vibrational-Resolved C 1s Excitation, N. Saito, Franz Heiser, Oliver Hemmers, K. Wieliczek, J. Viefhaus, U. Becker

#### Kinetic-Energy- And Angular-Resolved Fragmentation Of Co In Vibrational-Resolved C 1s Excitation, N. Saito, Franz Heiser, Oliver Hemmers, K. Wieliczek, J. Viefhaus, U. Becker

*Environmental Studies Faculty Publications*

Angular distributions of C^{+}+O^{+} from CO were measured, following vibrationally resolved C 1s excitations into the 2pπ, 3sσ, and 3pπ orbitals as well as into higher unresolved orbitals. A time-of-flight mass spectrometer, with a multihit-type position-sensitive anode, was used for the measurements. The anisotropy parameters (β) of C^{+}+O^{+} approach their theoretically expected values as the released kinetic energy in the fragmentation increases. The value of the β parameters remains constant for all vibrational states within each orbital.

Auger Resonant Raman Spectroscopy Used To Study The Angular Distributions Of The Xe 4d5/2 → 6p Decay Spectrum, B. Langer, N. Berrah, A. Farhat, Oliver Hemmers, J. Bozek

#### Auger Resonant Raman Spectroscopy Used To Study The Angular Distributions Of The Xe 4d5/2 → 6p Decay Spectrum, B. Langer, N. Berrah, A. Farhat, Oliver Hemmers, J. Bozek

*Environmental Studies Faculty Publications*

The Auger resonant Raman effect can be used as a method to eliminate natural lifetime broadening in resonant Auger spectra. We have coupled this method with high-resolution photons from the Advanced Light Source to study angular distributions and decay rates of the Xe4d_{5/2}→6p resonant Auger lines. The angular distribution parameters β of almost all possible final ionic 5p^{4}(^{3}P, ^{1}D, ^{1}S)6p states have been determined. Our data, which remove the discrepancy between previous lower-resolution experimental results, are compared to different theoretical results.

Angle-Resolved Photoelectron Spectroscopy Of C60, T. Liebsch, O. Plotzke, Franz Heiser, U. Hergenhahn, Oliver Hemmers, R. Wehlitz, J. Viefhaus, B. Langer, S. B. Whitfield, U. Becker

#### Angle-Resolved Photoelectron Spectroscopy Of C60, T. Liebsch, O. Plotzke, Franz Heiser, U. Hergenhahn, Oliver Hemmers, R. Wehlitz, J. Viefhaus, B. Langer, S. B. Whitfield, U. Becker

*Environmental Studies Faculty Publications*

Angle-resolved photoelectron spectra of gaseous C_{60} were recorded in the photon energy regions from 21 to 108 eV and from 295 to 320 eV. Partial cross sections σ and the angular distribution anisotropy parameter β vary significantly with photon energy, particularly in the near-threshold region of the valence and the core ionization regimes. Some of these effects may be attributed to scattering of the outgoing photoelectron by the atoms of the ionized C_{60} molecule. Our results indicate that the observed satellites of the C(1s) main line are most likely of shake-up character. Low-energy electrons emitted below the ...

Observation Of Parity-Unfavored Transitions In The Nonresonant Photoionization Of Argon, B. Langer, J. Viefhaus, Oliver Hemmers, A. Menzel, R. Wehlitz, U. Becker

#### Observation Of Parity-Unfavored Transitions In The Nonresonant Photoionization Of Argon, B. Langer, J. Viefhaus, Oliver Hemmers, A. Menzel, R. Wehlitz, U. Becker

*Environmental Studies Faculty Publications*

Single-photon ionization of an atom or molecule can be subdivided into parity-favored and -unfavored transitions, the latter characterized by electron emission, preferentially perpendicular to the electric vector. The nonresonant existence of these transitions is shown experimentally and studied over an extended energy range for a variety of satellite transitions in atomic argon. The spectra exhibit several clearly resolved satellite lines with strongly negative β values close to -1, independent of the photon energy. The results confirm the corresponding predictions of angular-momentum transfer theory.

Observation Of Non-Isotropic Auger Angular Distribution In The C(1s) Shape Resonance Of Co, Oliver Hemmers, Franz Heiser, J. Eiben, R. Wehlitz, U. Becker

#### Observation Of Non-Isotropic Auger Angular Distribution In The C(1s) Shape Resonance Of Co, Oliver Hemmers, Franz Heiser, J. Eiben, R. Wehlitz, U. Becker

*Environmental Studies Faculty Publications*

Angle-resolved high-resolution C(KVV) Auger spectra of CO were taken in the vicinity of the C(1s) σ^{*} shape resonance. These spectra show clear evidence for the theoretically predicted anisotropic K-shell Auger emission in molecules. Complementary results from angle-resolved photoion spectroscopy show that the small size of the observed effect is, besides the varying intrinsic anisotropy of the Auger decay, also due to a smaller anisotropy in the primary absorption process than originally predicted but in good agreement with more recent calculations. Contrary to this, satellite Auger transitions show unexpectedly large anisotropies.

Electron-Energy And –Angular Distributions In The Double Photoionization Of Helium, R. Wehlitz, Franz Heiser, Oliver Hemmers, B. Langer, A. Menzel, U. Becker

#### Electron-Energy And –Angular Distributions In The Double Photoionization Of Helium, R. Wehlitz, Franz Heiser, Oliver Hemmers, B. Langer, A. Menzel, U. Becker

*Environmental Studies Faculty Publications*

Photoelectron spectra of helium have been measured at different angles and at various energies above the double-ionization threshold up to 120 eV to investigate the behavior of the energy and angular distributions, of shake-off electrons. Both energy and angular distributions clearly show a U-shaped profile which turns to a flat curve near threshold pointing to a uniform intensity distribution over the kinetic energy for all angles in this excitation energy regime. Our results for the angular-distribution asymmetry parameter indicate qualitative agreement with theoretical predictions but fail to provide them quantitatively.

High-Resolution Photoelectron Spectrometry Study Of Conjugate Shakeup Processes In The Li 1s Threshold Region, B. Langer, J. Viefhaus, Oliver Hemmers, A. Menzel, U. Becker

#### High-Resolution Photoelectron Spectrometry Study Of Conjugate Shakeup Processes In The Li 1s Threshold Region, B. Langer, J. Viefhaus, Oliver Hemmers, A. Menzel, U. Becker

*Environmental Studies Faculty Publications*

Partial cross sections and angular-distribution asymmetry parameters of diagram and satellite lines associated with Li 1s photoionization were measured using synchrotron-radiation excitation. Special emphasis was given to a high-resolution study of the ^{1}P and ^{3}P conjugate shakeup satellite lines testing qualitative predictions of the conjugate shakeup model: increasing σ and decreasing β values towards threshold, both being verified. Comparison with recent relaxed Hartree-Fock calculations shows good agreement for the ^{1}P satellite, but demonstrates also that the present theory does not seem to be able to describe the cross-section behavior of the ^{3}P satellite correctly.