Calculated angular distributions of photoelectrons using the orthogonalized plane-wave approximation

Rabalais, J. W.; Debies, T.; Berkosky, Jeffrey L.; Huang, Jan-Tsyu J.; Ellison, Frank O.

doi:10.1063/1.1681927

Cited by 33 publications

(6 citation statements)

References 17 publications

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“…Assuming that the wavefunction for the outgoing photoelectron is a plane wave orthogonalized to filled molecular orbitals 14 yields {3 values for the B 2~: state which are significantly lower than those calculated for the x~; state (see Table II). We conclude that no theoretical calculation to date which neglects the role of autoionization via continuum nuclear states can satisfactorily account for the experimental results.…”

Section: Other Sources For the Xmentioning

confidence: 90%

Energy dependence of the differential photoelectron cross sections of molecular nitrogen

Mintz

Kuppermann

1978

The Journal of Chemical Physics

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The angular distribution of photoelectron intensity for molecular nitrogen was studied using He I and Ne 1 resonance line discharge light sources. Studies of photoelectron angular distributions covering a range of photon energies, and thus a range of photoelectron energies, are possible using the weaker high order lines in each discharge as well as the principal lines. Peaks in three photoelectron bands of N 2 were studied at the photon energies 16.85, 19.78, 21.22, 23.09, and 23.74 eV, where possible. We find that the v' = 0 peak of the X 2 I.i band has abnormally high intensity and, at the higher photon energies, an abnormally low angular distribution asymmetry parameter, /3. Several mechanisms for this anomaly are discussed, including autoionization, the variation of electric dipole transition moments with internuclear distance, and possible shape resonance phenomena. None of these explanations is completely in agreement with all theoretical and experimental evidence.

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Section: Other Sources For the Xmentioning

confidence: 90%

Energy dependence of the differential photoelectron cross sections of molecular nitrogen

Mintz

Kuppermann

1978

The Journal of Chemical Physics

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“…-Theoretical progress on angular distributions of molecules has likewise been spotty, and, as of yet, no flexible, realistic means is readily available for the purpose of mapping the wavelengthdependent p's for molecules of arbitrary complexity, although this problem may be overcome soon. A large volume of earlier work (see, e.g., [68]) in this area utilized plane wave or orthogonalized plane waves for final states. Owing to the importance of phase shift information to angular distributions, these models, which neglect both the Coulomb field of the ion and the phase shift of photoelectrons, canhot be considered realistic in the VUV Snergy range.…”

Section: Photoelectron Angular Distributionsmentioning

confidence: 99%

Angular Distributions of Photoelectrons and Non-Thermal Photoions From Atoms and Molecules

Dehmer

1978

J. Phys. Colloques

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RCsumC. -Durant ces dix dernikres annees, les distributions angulaires des photo-electrons ont kte exclusivement utilisees pour ktudier la dynamique des processus de photoionisation dans les atomes et les molkcules. Nous faisons le point, ici, sur les resultats les plus marquants survenus depuis la dernikre Conference Internationale d'il y a trois ans. De loin, les plus grands progres ont eu lieu pour les atomes, l'interst s'etant plus particulierement port6 sur les points suivants : amelioration de l'ordre zero (Hartree-Slater, Cooper-Zare), comprehension du paramttre d'asymetrie P(&), en considerant les correlations Clectroniques, les effets relativistes, les interactions de 1'Ctat final anisotropique. L'etude des gaz rares a bkneficik de l'ttroite coordination entre l'expkrience et la theorie, tandis que l'etude des atomes non spheriques est restee principalement theorique, mis a part les mesures rkcentes sur I'oxygkne atomique. Les etudes de distribution angulaire sur les molecules sont encore a un stade t r b preliminaire de dtveloppement. Ceci resulte du manque de mesures en fonction de la longueur d'onde, mises a part les experiences trks recentes, et l'absence de methodes theoriques pratiques et realistes. Le point sera donc fait sur ce travail recent, ainsi que sur une selection de travaux plus anciens concernant les molCcules et obtenus avec des raies de resonance. De plus, une nouvelle serie d'ktudes angulaires sur les molCcules -la distribution angulaire des ions non thermiques formes par photoionisation dissociative -fournissant des informations complCmentaires sur les mesures correspondantes avec des photoClectrons, sera presentee.Abstract. -During the last ten years, photoelectron angular distributions have been used extensively to study the dynamics of the photoionization process in atoms and molecules. Here we review some major advances in this body of work, with special emphasis on results emerging since the last Conference on VUV Radiation Physics three years ago. By far the greatest progress has occurred for atoms, where interest is focussed on improving our zero-order (Hartree-Slater, Cooper-Zare) understanding of the asymmetry parameter P(&), by considering electron correlations, relativistic effects, and anisotropic final-state interactions. The study of the rare gases has benefitted from extensive coordination between experiment and theory, whereas work on non-spherical atoms has been mainly theoretical, with the only measurements being performed very recently on atomic oxygen. Angular distribution studies on molecules are in a much earlier stage of development. Progress has been impeded by the lack of practical, realistic theoretical methods and wavelength-dependent measurements, both of which are becoming available only now. This recent work, together with selected topics from earlier resonance-line work on molecules will be reviewed. In addition, a new class of angle-dependent stud~es of molecules will be discussed -the angular distribution of non-thermal ions formed by dissociative ph...

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“…Thus, the conditions of the applicability of the plane-wave approximation mentioned in the previous section are satisfied. The angle-resolved photoelectron spectra calculated with the photoelectron wave function |φ e = |q e − α |φ α φ α |q e [39], which is a plane wave orthogonalized to the occupied molecular orbitals of the cation, φ α (r), are shown in Fig. 8 in Appendix B and are almost identical to those shown in Fig.…”

Section: B Angle-resolved Photoelectron Spectramentioning

confidence: 70%

“…which is a plane wave |q e = e iq·r / (2π ) 3 orthogonalized to the molecular orbitals of the cation φ α (r) [39]. The probe-pulse parameters are the same as assumed for the calculation of the time-and angle-resolved photoelectron probability in Fig.…”

Section: Appendix A: Derivation Of the Time-and Angle-resolved Photoementioning

confidence: 99%

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

2016

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We theoretically study how time-and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time-and angle-resolved photoelectron spectra. We show how a Fourier analysis of time-and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.

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Calculated angular distributions of photoelectrons using the orthogonalized plane-wave approximation

Cited by 33 publications

References 17 publications

Energy dependence of the differential photoelectron cross sections of molecular nitrogen

Energy dependence of the differential photoelectron cross sections of molecular nitrogen

Angular Distributions of Photoelectrons and Non-Thermal Photoions From Atoms and Molecules

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

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