Polar and azimuthal dependence of the molecular frame photoelectron angular distributions of spatially oriented linear molecules

Lucchese, Robert R.; Lafosse, A.; Brenot, J. C.; Guyon, P. M.; Houver, J. C.; Lebech, M.; Raşeev, G.; Dowek, D.

doi:10.1103/physreva.65.020702

Cited by 83 publications

(93 citation statements)

References 22 publications

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“…In the present work, approximate cross sections may be retrieved by multiplying the asymptotic transition probabilities by a factor 3ω/8T I [40]. As shown in [31], Eq. (19) for MFPADs is formally and computationally equivalent to Eq.…”

Section: Theoretical Methodsmentioning

confidence: 99%

“…For instance, the multichannel Schwinger configuration-interaction method (MC-SCI) of Lucchese and co-workers [33][34][35] has been shown to provide accurate predictions of molecular-frame photoemission observables measured for a series of molecular targets [20][21][22]30,31]. Density functional theory (DFT) calculations have also been conducted and predict richly structured measured angular distributions from fixed-in-space small polyatomic molecules [36], with recent developments involving time-dependent DFT [37].…”

Section: Theoretical Methodsmentioning

confidence: 99%

“…(1), the dependence on the azimuthal angle φ e and the molecular orientation angle χ is factorized in terms of simple trigonometric functions and associated Legendre polynomials P LN , respectively, so that complete dynamical information about the dissociative photoionization reaction is fully described by the five F LN (θ e ) functions [31]. These functions can be determined experimentally by performing a Legendre-Fourier analysis in (χ , φ e ) of the MFPAD I (χ,θ e ,φ e ), using expression (1).…”

Section: Circular Dichroism For Photoemission In the Molecular Framementioning

confidence: 99%

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Circular dichroism in molecular-frame photoelectron angular distributions in the dissociative photoionization ofH2andD2molecules

et al. 2014

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The presence of net circular dichroism in the photoionization of nonchiral homonuclear molecules has been put in evidence recently through the measurement of molecular-frame photoelectron angular distributions in dissociative photoionization of H 2 [Dowek et al., Phys. Rev. Lett. 104, 233003 (2010)]. In this work we present a detailed study of circular dichroism in the photoelectron angular distributions of H 2 and D 2 molecules, oriented perpendicularly to the propagation vector of the circularly polarized light, at different photon energies (20, 27, and 32.5 eV). Circular dichroism in the angular distributions at 20 and to a large extent 27 eV exhibits the usual pattern in which inversion symmetry is preserved. In contrast, at 32.5 eV, the inversion symmetry breaks down, which eventually leads to total circular dichroism after integration over the polar emission angle. Time-dependent ab initio calculations support and explain the observed results for H 2 in terms of quantum interferences between direct photoionization and delayed autoionization from the Q 1 and Q 2 doubly excited states into ionic states (1sσ g and 2pσ u ) of different inversion symmetry. Nevertheless, for D 2 at 32.5 eV, there is a particular case where theory and experiment disagree in the magnitude of the symmetry breaking: when D + ions are produced with an energy of around 5 eV. This reflects the subleties associated to such simple molecules when exposed to this fine scrutiny.

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Section: Theoretical Methodsmentioning

confidence: 99%

Section: Theoretical Methodsmentioning

confidence: 99%

Section: Circular Dichroism For Photoemission In the Molecular Framementioning

confidence: 99%

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Circular dichroism in molecular-frame photoelectron angular distributions in the dissociative photoionization ofH2andD2molecules

et al. 2014

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“…The (V A+ , V e , ê) correlation leads to the MFPAD which is a function of three angles I ( , e , e ), where is the polar angle which characterizes the orientation of the molecule with respect to the polarization axis ê, and ( e , e ) characterize the emission direction of the photoelectron in the molecular frame [18]. Considering a non-linear molecule, the MFPAD is a function of increasing complexity: valence shell PI producing generally a single charged fragment cannot give access to the complete MFPAD.…”

Section: Uvx 2008mentioning

confidence: 99%

“…In order to derive the MFPADs for selected processes in the KECDs, we use the general formalism developed earlier in the dipole approximation for one-photon photoionization of a linear molecule induced by linearly [18] or circularly [3] polarized light. In the general expression of the I ( , e , e ) MFPAD, all the dynamical information is contained in five one-dimensional F LN ( e ) functions, the dependence in terms of the molecular axis orientation with respect to the light propagation axis k and the photoelectron azimuthal emission angle in the molecular frame e being expressed by simple geometrical functions (see ref.…”

Section: Dpi Of H 2 and D 2 : Molecular Frame Photoemissionmentioning

confidence: 99%

Electron-ion vector correlations for the study of photoionization of molecules in the UVX range: From synchrotron radiation to short light pulses

Elkharrat

Picard

Billaud

et al. 2009

UVX 2008 - 9e Colloque Sur Les Sources Cohérentes Et Incohérentes UV, VUV Et X : Applications Et Développements Récents

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Abstract. Molecular frame photoemission is a very sensitive probe of the photoionization (PI) dynamics of molecules. The electron-ion vector correlation (VC) method takes advantage of dissociative photoionization (DPI) reactions of small molecules to measure such observables. It relies on the coincident detection of the photoelectron and the ion fragment emitted from the same DPI event and the determination of their velocity vectors. Most of the VC studies so far have been performed using synchrotron radiation (SR) light sources which benefit from a high repetition rate (1-10 MHz) favorable for coincidence experiments. In this paper we discuss the extension of this method to the study of PI processes induced by ultra-short VUV light sources, which provide the capability for investigating processes characterized by femtosecond or subfemtosecond dynamics. We first illustrate the VC method by the report of recent results of a comparative study of resonant photoionization of the H 2 and D 2 molecules induced by VUV circularly polarized synchrotron radiation at SOLEIL in the region involving resonant excitation of Q 1 and Q 2 doubly excited state series. This problem is of particular interest since autoionization and dissociation of selected Q 1 or Q 2 states occur on a comparable time scale of few femtoseconds, which implies a coupling between the electronic and nuclear motion. The extension of the VC method using femtosecond laser sources is then demonstrated by results for multiphoton PI of the Xe atom induced by 70 fs pulses centered at 400 nm delivered by the SOFOCKLE and PLFA sources (SLIC, CEA-Saclay) after frequency doubling of a 1 kHz Ti:sapphire laser.

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Angular Distributions in Molecular Photoionization

Lucchese

Dowek

2014

Attosecond and XUV Physics

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Photoelectron angular distributions (PADs) in molecular photoionization can provide detailed information about the geometry of a molecule, the initial electronic state and the electronic state of the product molecular ion. In general, the molecular frame photoelectron angular distribution (MFPAD) can be a function of four angles for linearly and circularly polarized light and five angles for elliptically polarized light. In this chapter, we show how, for dipole transitions, these multidimensional distributions can be reduced to a limited number of one-dimensional functions. PADs must be determined relative to the molecular frame of reference and we consider experimental distributions that can be obtained with post-ionization analysis of the molecular frame orientation, using coincidence detection of the photoelectron and at least one ionic fragment. We also consider concurrent orientation, where a multiphoton process modifies the alignment of the molecule, helping the analysis of the PAD. And finally, we consider the form of the PAD when the molecule is preoriented, as can be achieved with impulsive alignment by intense infrared lasers. IntroductionThe ionization of molecules by absorption of light is significantly different from absorption where the final state is a bound state. In the case of ionization, the continuous nature of the final state leads to a lack of quantization for the total energy of the system. The infinite degeneracy of the continuum allows ejection of the photoelectron in any direction relative to the molecular frame (MF), that is, in any direction in the coordinate system of the molecule. The differential cross-section for this photoemission process is the molecular frame photoelectron angular distribution (MFPAD). This observable results from the coherent superposition of all partial waves contributing to the continuum electronic wavefunction: it therefore provides a very sensitive probe of the potentials and interactions governing the quantum dynamics of the emitted photoelectrons. In molecules, the MFPAD is a function of Attosecond and XUV Physics, First Edition. Edited by Thomas Schultz and Marc Vrakking.

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Polar and azimuthal dependence of the molecular frame photoelectron angular distributions of spatially oriented linear molecules

Cited by 83 publications

References 22 publications

Circular dichroism in molecular-frame photoelectron angular distributions in the dissociative photoionization ofH2andD2molecules

Circular dichroism in molecular-frame photoelectron angular distributions in the dissociative photoionization ofH2andD2molecules

Electron-ion vector correlations for the study of photoionization of molecules in the UVX range: From synchrotron radiation to short light pulses

Angular Distributions in Molecular Photoionization

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