On the angular distributions of electrons photoejected from fixed-in-space and randomly oriented molecules
New theoretical expressions are devised from a dynamical perspective for molecular photoionization cross sections differential in electron ejection angles which facilitate comparisons between theory and experiment and provide a convenient basis for ab initio calculations. The cross sections obtained...
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| Published in: | Journal of electron spectroscopy and related phenomena Vol. 114; pp. 23 - 32 |
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| Main Authors: | , , , , , , , |
| Format: | Journal Article |
| Language: | English |
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Elsevier B.V
01-03-2001
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| Abstract | New theoretical expressions are devised from a dynamical perspective for molecular photoionization cross sections differential in electron ejection angles which facilitate comparisons between theory and experiment and provide a convenient basis for ab initio calculations. The cross sections obtained for fixed-in-space molecules, including the lowest-order (nondipole) effects of retardation, are given in terms of invariant molecular body-frame transition moments and related normalized angular-distribution amplitudes which can be calculated employing interaction-prepared states without reference to specific scattering boundary conditions. Corresponding expressions for molecular dipole and nondipole anisotropy factors appropriate for randomly oriented molecules are obtained in closed forms involving expectation values of harmonic polynomials over the fixed-in-space body-frame angular-distribution amplitudes. The expressions are seen to be in the spirit of corresponding results for atomic photoionization anisotropy factors, to which they reduce in appropriate limits. Interpretations of recently measured angular distributions of photoelectrons from the K-shell of molecular nitrogen illustrate how the development relates measurements on randomly oriented molecules to those performed on fixed-in-space molecules. The theoretical formalism provides results in excellent accord with measurements of the molecular nitrogen K-shell dipole anisotropy factor, and accounts for the origins of large nondipole effects observed at relatively low photon energies (ℏ
ω≤500 eV) in the measured angular distributions. |
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| AbstractList | New theoretical expressions are devised from a dynamical perspective for molecular photoionization cross sections differential in electron ejection angles which facilitate comparisons between theory and experiment and provide a convenient basis for ab initio calculations. The cross sections obtained for fixed-in-space molecules, including the lowest-order (nondipole) effects of retardation, are given in terms of invariant molecular body-frame transition moments and related normalized angular-distribution amplitudes which can be calculated employing interaction-prepared states without reference to specific scattering boundary conditions. Corresponding expressions for molecular dipole and nondipole anisotropy factors appropriate for randomly oriented molecules are obtained in closed forms involving expectation values of harmonic polynomials over the fixed-in-space body-frame angular-distribution amplitudes. The expressions are seen to be in the spirit of corresponding results for atomic photoionization anisotropy factors, to which they reduce in appropriate limits. Interpretations of recently measured angular distributions of photoelectrons from the K-shell of molecular nitrogen illustrate how the development relates measurements on randomly oriented molecules to those performed on fixed-in-space molecules. The theoretical formalism provides results in excellent accord with measurements of the molecular nitrogen K-shell dipole anisotropy factor, and accounts for the origins of large nondipole effects observed at relatively low photon energies (ℏ
ω≤500 eV) in the measured angular distributions. |
| Author | Lindle, D.W. Arce, J.C. Langhoff, P.W. Sheehy, J.A. Hemmers, O. Wang, H. Focke, P. Sellin, I.A. |
| Author_xml | – sequence: 1 givenname: P.W. surname: Langhoff fullname: Langhoff, P.W. email: langhoff@drifter.sdsc.edu organization: Department of Chemistry, Indiana University, Bloomington, IN 47405-4001, USA – sequence: 2 givenname: J.C. surname: Arce fullname: Arce, J.C. organization: Departamento de Quimica, Universidad del Valle, A.A. 25360 Cali, Colombia – sequence: 3 givenname: J.A. surname: Sheehy fullname: Sheehy, J.A. organization: Air Force Research Laboratory, AFRL/PRS, Edwards AFB, CA 93524-7680, USA – sequence: 4 givenname: O. surname: Hemmers fullname: Hemmers, O. organization: Department of Chemistry, University of Nevada, Las Vegas, NV 89154-4003, USA – sequence: 5 givenname: H. surname: Wang fullname: Wang, H. organization: Department of Chemistry, University of Nevada, Las Vegas, NV 89154-4003, USA – sequence: 6 givenname: P. surname: Focke fullname: Focke, P. organization: Department of Physics, University of Tennessee, Knoxville, TN 37996-1600, USA – sequence: 7 givenname: I.A. surname: Sellin fullname: Sellin, I.A. organization: Department of Physics, University of Tennessee, Knoxville, TN 37996-1600, USA – sequence: 8 givenname: D.W. surname: Lindle fullname: Lindle, D.W. organization: Department of Chemistry, University of Nevada, Las Vegas, NV 89154-4003, USA |
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| CitedBy_id | crossref_primary_10_1016_j_radphyschem_2005_11_009 crossref_primary_10_1103_PhysRevLett_89_033002 crossref_primary_10_1007_s00214_006_0212_3 crossref_primary_10_1016_j_elspec_2009_04_011 crossref_primary_10_1016_j_radphyschem_2003_12_010 crossref_primary_10_1016_j_elspec_2007_02_023 crossref_primary_10_1016_j_radphyschem_2005_03_004 crossref_primary_10_1039_C8CP00936H crossref_primary_10_1016_S0039_6028_01_01481_9 crossref_primary_10_1103_PhysRevLett_92_223002 crossref_primary_10_1103_PhysRevA_73_022716 crossref_primary_10_1380_ejssnt_2005_373 crossref_primary_10_1088_0953_4075_37_19_005 crossref_primary_10_1103_PhysRevLett_97_103006 crossref_primary_10_1103_PhysRevLett_87_273003 crossref_primary_10_1016_S0368_2048_02_00025_7 crossref_primary_10_1088_0953_4075_34_15_105 crossref_primary_10_1103_PhysRevA_91_053410 crossref_primary_10_1016_j_elspec_2010_02_001 crossref_primary_10_1016_S0368_2048_02_00014_2 crossref_primary_10_1088_0953_4075_39_2_L02 crossref_primary_10_1016_j_radphyschem_2003_12_009 crossref_primary_10_1016_j_radphyschem_2006_08_003 crossref_primary_10_1088_1674_1056_ab5c10 crossref_primary_10_1088_0953_4075_36_12_301 crossref_primary_10_1088_0953_4075_39_12_005 |
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| Copyright | 2001 Elsevier Science B.V. |
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| CorporateAuthor | Ernest Orlando Lawrence Berkeley National Lab., Advanced Light Source, Berkeley, CA (US) |
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| SubjectTerms | ADVANCED LIGHT SOURCE ADVANCED LIGHT SOURCE ALS ANGULAR DISTRIBUTION ELECTRONS PARTICLE ACCELERATORS |
| Title | On the angular distributions of electrons photoejected from fixed-in-space and randomly oriented molecules |
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