Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. II. Three- and four-photon ionization of fenchone and camphor

Müller, Anne D.; Artemyev, A. N.; Demekhin, Ph. V.

doi:10.1063/1.5032295

Cited by 21 publications

(28 citation statements)

References 67 publications

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“…The time-dependent single center method, developed in Paper I [22] and tested on bicyclic ketones in Paper II [23], is applied here to study the multiphoton PECD of fenchone in different ionization regimes. The present multiphoton PECDs of the 3PI, 4ATI, and 5ATI electrons, computed for the 400 nm pulses, are in a very good agreement with the experimental results from Refs.…”

Section: Discussionmentioning

confidence: 99%

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. III. Photoionization of fenchone in different regimes

Müller

Kutscher

Artemyev

et al. 2020

The Journal of Chemical Physics

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Photoelectron circular dichroism (PECD) in different regimes of multiphoton ionization of fenchone is studied theoretically using the time-dependent single center method. In particular, we investigate the chiral response to the one-color multiphoton or strong-field ionization by circularly polarized 400 and 814 nm optical laser pulses or 1850 nm infrared pulse. In addition, the broadband ionization by short coherent circularly polarized 413-1240 nm spanning pulse is considered.Finally, the two-color ionization by the phase-locked 400 and 800 nm pulses, which are linearly polarized in mutually-orthogonal directions, is investigated. The present computational results on the one-color multiphoton ionization of fenchone are in agreement with the available experimental data. For the ionization of fenchone by broadband and bichromatic pulses, the present theoretical study predicts substantial multiphoton PECDs.

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Section: Discussionmentioning

confidence: 99%

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. III. Photoionization of fenchone in different regimes

Müller

Kutscher

Artemyev

et al. 2020

The Journal of Chemical Physics

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“…In addition, an impact of the nuclear and electron dynamics during multiphoton ionization of chiral molecules have been demonstrated by pump-probe experiments [17][18][19][20]. Theoretical approaches to describe the multiphoton PECD range from time-independent perturbative ab-initio calculation of the two-photon absorption followed by one-photon ionization in hydrogenic continuum spectrum [21] to nonperturbative time-dependent methods [22,23].Employing overlapping bichromatic laser pulses is a particularly important example of coherent control schemes [24,25]. Here, interference between the nphoton route of one of the fields and the m-photon route of the other field can be controlled through the relative phase.…”

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“…In order to verify this hypothesis, we simulated the proposed experiment theoretically. Calculations were carried out by the time-dependent Single Center (TDSC) method and code [22,23]. It consists in the propagation of the wave packet of a single-active-electron, which is driven in the potential of a chiral ion by an intense short laser pulse.…”

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Photoelectron Circular Dichroism with Two Overlapping Laser Pulses of Carrier Frequencies ω and 2ω Linearly Polarized in Two Mutually Orthogonal Directions

et al. 2018

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Using a model methane-like chiral system, we theoretically demonstrate a possibility to access photoelectron circular dichroism (PECD) by a single experiment with two overlapping laser pulses of carrier frequencies ω and 2ω, which are linearly polarized in two mutually-orthogonal directions. Depending on the relative phase, the resulting electric field can be tailored to have two different rotational directions in the upper and lower hemispheres along the polarization of the ω-pulse. We predict a strong forward/backward asymmetry in the emission of photoelectrons from randomly oriented samples, which has an opposite sign in the upper and lower hemispheres. The predicted PECD effect is phase-and enantiomer-sensitive, providing new insight in this fascinating fundamental phenomenon. The effect can be optimized by varying relative intensities of the pulses. 33.20.Xx, 33.55.+b, 81.05.Xj In 1976, it was predicted theoretically that photoionization of chiral molecules is sensitive to the helicity of ionizing light [1]. The effect emerges already in the electric-dipole approximation and manifests itself as a forward/backward asymmetry in the emission of photoelectrons from randomly oriented chiral molecules in the gas phase. It took about 25 years to verify these theoretical predictions experimentally [2,3]. Later on, this enantiomer-and helicity-selective effect was termed as photoelectron circular dichroism (PECD) [4]. During the last decade, one-photon ionization of chiral molecules by circularly polarized radiation, and the emerging PECD effects, were studied in the numerous experimental and theoretical works (see, e.g., review articles [5][6][7]).Recently [8,9], a similar PECD effect has been observed in the multiphoton ionization of chiral molecules by circularly polarized laser pulses. Since then, extensive experimental studies provided many important details on the multiphoton PECD, like, e.g., on its dependence on the pulse intensity and ellipticity [10-12], on the enantiomeric excess of the target [13,14], or on the intermediate electronic states involved in different multiphoton ionization schemes [15,16]. In addition, an impact of the nuclear and electron dynamics during multiphoton ionization of chiral molecules have been demonstrated by pump-probe experiments [17][18][19][20]. Theoretical approaches to describe the multiphoton PECD range from time-independent perturbative ab-initio calculation of the two-photon absorption followed by one-photon ionization in hydrogenic continuum spectrum [21] to nonperturbative time-dependent methods [22,23].Employing overlapping bichromatic laser pulses is a particularly important example of coherent control schemes [24,25]. Here, interference between the nphoton route of one of the fields and the m-photon route of the other field can be controlled through the relative phase. According to the selection rules for multiphoton transitions in atoms, there are two control scenarios [24].If n and m are both odd or even numbers, the integral and differential cross section ca...

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“…These variations reflect the competition between linearly and circularly polarized photons in the photoexcitation process, which determines the anisotropy of the photoexcited molecular ensemble. From a fundamental point of view, extrapolating the linear behavior of PEELD measurements near S 3 = 0 to S 3 = 1 provides an interesting physical quantity—the photoelectron circular dichroism that would be measured by photoexciting molecules with linear photons and ionizing them with circular photons—which can be particularly useful to benchmark calculations of REMPI-PECD 32 , 37 , 38 . In the same spirit, the 3D-PEELD distributions that we have measured exhibit very characteristic features, depending on the molecular species, and are certainly very sensitive probes of the quality of quantum chemistry calculations in chiral molecules.…”

Section: Discussionmentioning

confidence: 99%

Real-time determination of enantiomeric and isomeric content using photoelectron elliptical dichroism

et al. 2018

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The fast and accurate analysis of chiral chemical mixtures is crucial for many applications but remains challenging. Here we use elliptically-polarized femtosecond laser pulses at high repetition rates to photoionize chiral molecules. The 3D photoelectron angular distribution produced provides molecular fingerprints, showing a strong forward-backward asymmetry which depends sensitively on the molecular structure and degree of ellipticity. Continuously scanning the laser ellipticity and analyzing the evolution of the rich, multi-dimensional molecular signatures allows us to observe real-time changes in the chemical and chiral content present with unprecedented speed and accuracy. We measure the enantiomeric excess of a compound with an accuracy of 0.4% in 10 min acquisition time, and follow the evolution of a mixture with an accuracy of 5% with a temporal resolution of 3 s. This method is even able to distinguish isomers, which cannot be easily distinguished by mass-spectrometry.

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Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. II. Three- and four-photon ionization of fenchone and camphor

Cited by 21 publications

References 67 publications

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. III. Photoionization of fenchone in different regimes

Photoelectron circular dichroism in the multiphoton ionization by short laser pulses. III. Photoionization of fenchone in different regimes

Photoelectron Circular Dichroism with Two Overlapping Laser Pulses of Carrier Frequencies ω and 2ω Linearly Polarized in Two Mutually Orthogonal Directions

Real-time determination of enantiomeric and isomeric content using photoelectron elliptical dichroism

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