Using laser-induced Coulomb explosion of aligned chiral molecules to determine their absolute configuration

Christensen, Lars Rune; Nielsen, Jens Hedegaard; Slater, Craig S.; Lauer, Alexandra; Brouard, M.; Stapelfeldt, Henrik

doi:10.1103/physreva.92.033411

Cited by 33 publications

(27 citation statements)

References 26 publications

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“…The appearance of long-time orientation in a gas sample can be detected by means of Coulomb explosion [7,8,14,17,18,43] and nonlinear optics through high harmonic generation of various orders [54][55][56][57], especially by means of the second harmonic generation. Another approach to detecting the induced orientation is by measuring THz emission due to free induction decay of coherently oscillating molecular dipoles [58][59][60].…”

Section: Numerical Simulationsmentioning

confidence: 99%

Laser-induced persistent orientation of chiral molecules

et al. 2019

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We show, both classically and quantum mechanically, enantioselective orientation of gas phase chiral molecules excited by laser fields with twisted polarization. Counterintuitively, the induced orientation, whose direction is laser controllable, does not disappear after the excitation, but stays approximately constant long after the end of the laser pulses, behavior unique to chiral systems. We computationally demonstrate this long-lasting orientation using propylene oxide molecules (CH3CHCH2O, or PPO) as an example, and consider two kinds of fields with twisted polarization: a pair of delayed cross-polarized pulses, and an optical centrifuge. This novel chiral effect opens new avenues for detecting molecular chirality, measuring enantiomeric excess and separating enantiomers with the help of inhomogeneous external fields.

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Section: Numerical Simulationsmentioning

confidence: 99%

Laser-induced persistent orientation of chiral molecules

et al. 2019

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“…Other enantio-sensitive methods on dilute targets have been recently proposed making this field very lively nowadays [18], including high harmonic generation (HHG) from a chiral gaseous medium [19]. It is worth mentioning recent experiments on the Coulomb explosion induced by either laser [20,21], synchrotron radiation [22], or beam foil [23], which allowed direct imaging and deciphering of the absolute configuration of a racemic (50% left/50% right) mixture of a chiral species in the gas phase for the first time. New innovative and very sensitive chiroptical spectroscopic methods based on non-coplanar bound-bound transition dipoles in the MW by three wave-mixing [24,25] and in the UV by use of CPL fs-pulses creating a coherent helical motion of bound electrons [26] appear very promising especially for their potential ability to separate enantiomers [27], which is still a challenge in stereochemistry and asymmetric catalysis.…”

Section: Introductionmentioning

confidence: 99%

Electron asymmetries in the photoionization of chiral molecules: possible astrophysical implications

Hadidi

Božanić

Garcia

et al. 2018

Advances in Physics: X

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Photoelectron circular dichroism (PECD) is an intense orbital-specific chiroptical effect observed as asymmetries in the angular distribution of photoelectrons produced by photoionization of randomly oriented pure enantiomers with circularly polarized light. After a broad introduction placing this effect in the context of new physical chiralsensitive methods, we review the main characteristics of PECD in terms of molecular photoionization dynamics. We stress also the analytical capabilities of PECD to retrieve enantiomeric excesses (e.es.) and to probe subtle details of the whole molecular potential, some of them exemplified by the showcase camphor and fenchone molecules. We then present the case of the amino acid alanine for which an interplay between PECD and conformer population is rationalized. Based on this study, we propose a photophysical astrophysical scenario for the origin of life's homochirality, relying upon the asymmetry of the associated recoiling alanine parent ion that could lead at the relevant Lyman-α energy to an e.e. of up to 4% in a given line of sight, which appears independent of the temperature. In an attempt to generalize this scenario to other amino acids, new data on proline showing an e.e. of 12%, of the same sign as alanine, are also presented.

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“…Recently, a number of new techniques have been developed for investigating chiral molecules in the gas phase. These include photoelectron circular dichroism using intense laser pulses or synchrotron radiation, 136,138,139 CEI, 133,135,[140][141][142] microwave three-wave mixing, 134,137,143,144 and orienting chiral molecules using a pair of cross-polarized laser pulses. The last approach was theoretically suggested in Ref.…”

Section: Partial Transient and Persistent Orientation Of Chiral Molecmentioning

confidence: 99%

Spatiotemporal rotational dynamics of laser-driven molecules

Lin

Tutunnikov

et al. 2020

Adv. Photon.

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Molecular alignment and orientation by laser fields has attracted significant attention in recent years, mostly due to new capabilities to manipulate the molecular spatial arrangement. Molecules can now be efficiently prepared for ionization, structural imaging, orbital tomography, and more, enabling, for example, shooting of dynamic molecular movies. Furthermore, molecular alignment and orientation processes give rise to fundamental quantum and classical phenomena like quantum revivals, Anderson localization, and rotational echoes, just to mention a few. We review recent progress on the visualization, coherent control, and applications of the rich dynamics of molecular rotational wave packets driven by laser pulses of various intensities, durations, and polarizations. In particular, we focus on the molecular unidirectional rotation and its visualization, the orientation of chiral molecules, and the three-dimensional orientation of asymmetric-top molecules. Rotational echoes are discussed as an example of nontrivial dynamics and detection of prepared molecular states.

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Using laser-induced Coulomb explosion of aligned chiral molecules to determine their absolute configuration

Cited by 33 publications

References 26 publications

Laser-induced persistent orientation of chiral molecules

Laser-induced persistent orientation of chiral molecules

Electron asymmetries in the photoionization of chiral molecules: possible astrophysical implications

Spatiotemporal rotational dynamics of laser-driven molecules

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