Probing molecular chirality on a sub-femtosecond timescale

Cireasa, R.; Boguslavskiy, Andrey E.; Pons, B.; Wong, M. C. H.; Descamps, D.; Petit, S.; Ruf, H.; Thiré, Nicolas; Ferré, A.; Suárez, Jaime; Higuet, J.; Schmidt, Bruno E.; Alharbi, Abdullah; Légaré, François; Blanchet, Valérie; Fabre, B.; Patchkovskii, Serguei; Smirnova, Olga; Mairesse, Y.; Bhardwaj, V. R.

doi:10.1038/nphys3369

Cited by 288 publications

(319 citation statements)

References 40 publications

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“…Note that fenchone has also been used to demonstrate a pioneering chiroptical method based upon High Harmonic Generation (HHG) from a chiral molecule 38 , and both isomers have been studied by REMPI--UV Ion Yield CD 39 . To be validated in sensitivity and reliability laser--based PECD experiments need benchmarking with data obtained with more well--established and controlled experiments such as the one that can be carried out with pure--CPL SR sources.…”

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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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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“…Chiral dichroism at a few percent level for such almost linear fields observed in Ref. [14] demonstrates high potential for chiral discrimination of this new technique. However, as with any new technique, its first implementation may not be optimal.…”

Section: Introductionmentioning

confidence: 94%

“…In this section, we apply the approach we have already used in [14] to estimate the high harmonic signal vs ellipticity of the field given by Eq. (1).…”

Section: Chiral Discrimination Based On Hhg Spectral and Phase Measurmentioning

confidence: 99%

“…We set the ellipticities of both fields to be equal, 1 = 2 = . We will consider an epoxypropane molecule CH 3 CHCH 2 O (also known as 1,2-propylene oxide), which has been used in the first cHHG experiments [14].…”

Section: Chiral Discrimination Based On Hhg Spectral and Phase Measurmentioning

confidence: 99%

“…The chiral response can be monitored with ∆t ∼ 0.1 fsec resolution [14], orders of magnitude better than achieved so far (see e.g. [23]).…”

Section: Introductionmentioning

confidence: 99%

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Opportunities for chiral discrimination using high harmonic generation in tailored laser fields

Smirnova

Mairesse

Patchkovskii

2016

Conference on Lasers and Electro-Optics

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Abstract. Chiral discrimination with high harmonic generation (cHHG method) has been introduced in the recent work by R. Cireasa et al (Nat. Phys. 11, 654 -658, 2015). In its original implementation, the cHHG method works by detecting high harmonic emission from randomly oriented ensemble of chiral molecules driven by elliptically polarized field, as a function of ellipticity. Here we discuss future perspectives in the development of this novel method, the ways of increasing chiral dichroism using tailored laser pulses, new detection schemes involving high harmonic phase measurements, and concentration-independent approaches. Using the example of the epoxypropane molecule C 3 H 6 O (also known as 1,2-propylene oxide), we show theoretically that application of two-color counter-rotating elliptically polarized laser fields yields an order of magnitude enhancement of chiral dichroism compared to single color elliptical fields. We also describe how one can introduce a new functionality to cHHG: concentration-independent measurement of the enatiomeric excess in a mixture of randomly oriented left-handed and right-handed molecules. Finally, for arbitrary configurations of laser fields, we connect the observables of the cHHG method to the amplitude and phase of chiral response, providing a basis for reconstructing wide range of chiral dynamics from cHHG measurements, with femtosecond to sub-femtosecond temporal resolution.

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Chirality in Light–Matter Interaction

et al. 2022

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The scientific effort to control the interaction between light and matter has grown exponentially in the last 2 decades. This growth has been aided by the development of scientific and technological tools enabling the manipulation of light at deeply sub‐wavelength scales, unlocking a large variety of novel phenomena spanning traditionally distant research areas. Here, the role of chirality in light–matter interactions is reviewed by providing a broad overview of its properties, materials, and applications. A perspective on future developments is highlighted, including the growing role of machine learning in designing advanced chiroptical materials to enhance and control light–matter interactions across several scales.

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Probing molecular chirality on a sub-femtosecond timescale

Abstract: International audienc

Cited by 288 publications

References 40 publications

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

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

Opportunities for chiral discrimination using high harmonic generation in tailored laser fields

Chirality in Light–Matter Interaction

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