Asymmetry in Photoelectron Emission from Chiral Molecules Induced by Circularly Polarized Light

Böwering, N.; Lischke, T.; Schmidtke, B.; Müller, Norbert; Khalil, Tarek E.; Heinzmann, Ulrich

doi:10.1103/physrevlett.86.1187

Cited by 344 publications

(283 citation statements)

References 26 publications

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“…Asymmetries in the interaction of polarized light with chiral molecular samples have been known since Pasteur's experiments on optical activity [7], and the theory of the effect has been reviewed [8]. Recently, direct measurements have been performed of CD in the photoelectron angular distributions (ADs) resulting from photoionization of free, randomly oriented chiral molecules [9].…”

Section: Brief Survey Of Dichroic Effects In Unpolarized Atom Photoprmentioning

confidence: 99%

“…Despite the many theoretical studies for multiphoton detachment, only the simplest cases of linear and/or circular polarizations of the laser field have been examined in the many papers cited above (with the exception of the perturbative treatment of [77] for H − ) 9 . The generalization of numerically intensive methods to the case of an arbitrary (elliptical) polarization is not straightforward and leads to much more tedious calculations owing to the larger number of dimensions that must be treated and to the consequent need for extended sets of basis functions, inclusion of higher angular momentum states, etc.…”

Section: Status Of Multiphoton Detachment Of Negative Ionsmentioning

confidence: 99%

“…In order to present our results in the most general form, it is convenient to use scaled units based on the single parameter κ of the model potential (8): the length unit is 1/κ; the energy and the frequency are measured in units of |E 0 | and |E 0 |/h; the field amplitude F is measured in units of the 'internal field', F 0 = 2m|E 0 | 3 /|e|h and the corresponding scaled unit of the intensity, I = cF 2 (9), which is self-consistent for the (one-parameter) δ-potential model. However, it is well known that for real negative ions more exact results may be obtained using, instead of N, a corrected normalization constant, N c , which may be obtained, e.g., by analysing the asymptotic behaviour of the wavefunction for large r (cf [29,128,140] for details).…”

Section: Definitions and Scaled Unitsmentioning

confidence: 99%

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Multiphoton detachment of a negative ion by an elliptically polarized, monochromatic laser field

Manakov

Frolov

Borca

et al. 2003

J. Phys. B: At. Mol. Opt. Phys.

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The quasistationary quasienergy state approach (QQES) is applied to the analysis of partial (n-photon) decay rates and angular distributions (ADs) of photoelectrons produced by an elliptically polarized laser field. The problem is formulated for a weakly bound electron with an energy E 0 in the threedimensional δ-model potential (which approximates the short-range potential of a negative ion) interacting with a strong monochromatic laser field having an electric vector F (ωt). The results presented cover weak (perturbative), strong (nonperturbative), and superstrong field regimes as well as a wide interval of frequencies ω extending from the tunnelling (hω |E 0 |) and multiphoton (hω < |E 0 |) cases up to the high frequency domain (hω > |E 0 |).For a weak laser field, exact equations for the normalization factor and for the Fourier coefficients of the QQES wavefunction at the origin (|r| → 0) (that are key elements of the QQES approach for a δ-model potential) as well as for the detachment amplitudes are analysed analytically using both standard RayleighSchrödinger perturbation theory (PT) in the intensity, I , of the laser field and Brillouin-Wigner PT expansions involving the exact (complex) quasienergy . The lowest-order perturbative results for the n-photon ADs are presented in analytic form, and the parametrization of ADs in terms of polarization-and angular-independent atomic parameters is discussed for the general case of elliptical polarization. The major emphasis is on the analysis of an ellipticity induced distortion of three-dimensional ADs and, especially, on the elliptic dichroism (ED) effect, i.e. the dependence of the photoelectron yield in a fixed direction n on the sign of the ellipticity (or on the helicity) of a laser field. The dominant role of binding potential effects for a correct description of ED and threshold effects is demonstrated, and the intimate relationship between atomic ED factors and scattering phases of the detached electron is established for multiphoton detachment, including the above-threshold case. For a strong laser field, we present an accurate derivation for the QQES wavefunction and decay rates in the Keldysh approximation (KA) from exact QQES equations, including analytical, first-order ('rescattering') corrections to the KA results. The symmetries of ADs and the existence of ED are established using the exact analytical result for the n-photon detachment amplitude. Accurate numerical results are presented for the variation of the structure of the ADs as well as of the ED effect with increasing laser intensity.For the high frequency case,hω > |E 0 |, a rigorous analytical treatment of higher-order PT effects is presented for one-photon detachment, taking into account corrections of higher orders in I to the well-known photodetachment cross section for a short-range potential. Together with the exact numerical analysis of the total and partial decay rates forhω > |E 0 |, these results demonstrate the existence of a quasistationary stabilization regime in the de...

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Section: Brief Survey Of Dichroic Effects In Unpolarized Atom Photoprmentioning

confidence: 99%

Section: Status Of Multiphoton Detachment Of Negative Ionsmentioning

confidence: 99%

Section: Definitions and Scaled Unitsmentioning

confidence: 99%

See 1 more Smart Citation

Multiphoton detachment of a negative ion by an elliptically polarized, monochromatic laser field

Manakov

Frolov

Borca

et al. 2003

J. Phys. B: At. Mol. Opt. Phys.

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“…Since its formal prediction in 1976 1 , its first precise calculated values in 2000 2,3 , and its first experimental evidence in 2001 4 , Photoelectron Circular Dichroism (PECD) has been the subject of a large number of both theoretical and experimental studies 5--7 , mainly carried out with Synchrotron Radiation (SR), for valence and core--shell ionization. PECD is an orbital--specific chiroptical effect which manifests itself as a forward/backward asymmetry, with respect to the photon axis, of the electron angular distribution produced by the photoionization with Circularly Polarized Light (CPL) of randomly--oriented pure enantiomers of a chiral system.…”

Section: Introductionmentioning

confidence: 99%

Determination of accurate electron chiral asymmetries in fenchone and camphor in the VUV range: sensitivity to isomerism and enantiomeric purity

Nahon

Nag

Garcia

et al. 2016

Phys. Chem. Chem. Phys.

122

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Ivan (2016) Determination of accurate electron chiral asymmetries in fenchone and camphor in the VUV range: sensitivity to isomerism and enantiomeric purity. Physical Chemistry Chemical Physics . ISSN 1463-9084 Access from the University of Nottingham repository: http://eprints.nottingham.ac.uk/32734/1/PECD_PCCP2016_Accepted_manuscript.pdf Copyright and reuse:The Nottingham ePrints service makes this work by researchers of the University of Nottingham available open access under the following conditions. This article is made available under the University of Nottingham End User licence and may be reused according to the conditions of the licence. For more details see: http://eprints.nottingham.ac.uk/end_user_agreement.pdf A note on versions:The version presented here may differ from the published version or from the version of record. If you wish to cite this item you are advised to consult the publisher's version. Please see the repository url above for details on accessing the published version and note that access may require a subscription.For more information, please contact eprints@nottingham.ac.uk This is an Accepted Manuscript, which has been through the Royal Society of Chemistry peer review process and has been accepted for publication.Accepted Manuscripts are published online shortly after acceptance, before technical editing, formatting and proof reading. Using this free service, authors can make their results available to the community, in citable form, before we publish the edited article. We will replace this Accepted Manuscript with the edited and formatted Advance Article as soon as it is available.You can find more information about Accepted Manuscripts in the Information for Authors.Please note that technical editing may introduce minor changes to the text and/or graphics, which may alter content. Photoelectron circular dichroism (PECD) manifests itself as an intense forward/backward asymmetry in the angular distribution of photoelectrons produced from randomly--oriented enantiomers by photoionization with circularly--polarized light (CPL). As a sensitive probe of both photoionization dynamics and of the chiral molecular potential, PECD attracts much interest especially with the recent performance of related experiments with visible and VUV laser sources. Here we report, by use of quasi--perfect CPL VUV synchrotron radiation and using a double imaging photoelectron/photoion coincidence (i 2 PEPICO) spectrometer, new and very accurate values of the corresponding asymmetries on showcase chiral isomers: camphor and fenchone. These data have additionally been normalized to the absolute enantiopurity of the sample as measured by a chromatographic technique. They can therefore be used as benchmarking data for new PECD experiments, as well as for theoretical models. In particular we found, especially for the outermost orbital of both molecules, a good agreement with CMS--Xα PECD modeling over the whole VUV range. We also report a spectacular sensitivity of PECD to isomerism for slow electrons, ...

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“…Accordingly, CD in photoemission from solids has been widely used for the investigation of local magnetization and other properties of solids and surfaces (for example, refs 10,11). In atomic and molecular physics, circularly polarized photon beams have been applied for example in studies of electron spin-related phenomena and its polarization control 12,13 as well as of symmetry breaking in chiral molecules 14,15 . With FERMI many experimental techniques, already well established for applications of CD using synchrotron radiation, high order harmonics or optical lasers [16][17][18][19][20][21] , can now be extended to studies at FEL sources.…”

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confidence: 99%

Determining the polarization state of an extreme ultraviolet free-electron laser beam using atomic circular dichroism

et al. 2014

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Ultrafast extreme ultraviolet and X-ray free-electron lasers are set to revolutionize many domains such as bio-photonics and materials science, in a manner similar to optical lasers over the past two decades. Although their number will grow steadily over the coming decade, their complete characterization remains an elusive goal. This represents a significant barrier to their wider adoption and hence to the full realization of their potential in modern photon sciences. Although a great deal of progress has been made on temporal characterization and wavefront measurements at ultrahigh extreme ultraviolet and X-ray intensities, only few, if any progress on accurately measuring other key parameters such as the state of polarization has emerged. Here we show that by combining ultra-short extreme ultraviolet free electron laser pulses from FERMI with near-infrared laser pulses, we can accurately measure the polarization state of a free electron laser beam in an elegant, non-invasive and straightforward manner using circular dichroism.

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Asymmetry in Photoelectron Emission from Chiral Molecules Induced by Circularly Polarized Light

Cited by 344 publications

References 26 publications

Multiphoton detachment of a negative ion by an elliptically polarized, monochromatic laser field

Multiphoton detachment of a negative ion by an elliptically polarized, monochromatic laser field

Determination of accurate electron chiral asymmetries in fenchone and camphor in the VUV range: sensitivity to isomerism and enantiomeric purity

Determining the polarization state of an extreme ultraviolet free-electron laser beam using atomic circular dichroism

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