Degree of chirality of electromagnetic fields and maximally chiral light

Neufeld, Ofer; Tzur, Matan Even; Cohen, Oren

doi:10.1103/physreva.101.053831

Cited by 16 publications

(16 citation statements)

References 39 publications

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“…Here we re-formulate PECD with non-collinear and bi-chromatic laser pulses that are 'locallychiral' [29,35]. The electric field generated by locally-chiral light carries nonzero chirality-density within the electric-dipole approximation, and is highly effective for enantio-selectivity.…”

Section: Introductionmentioning

confidence: 99%

“…We demonstrate these effects and their generality through ab-initio calculations in the chiral molecules: Bromochlorofluoromethane, Limonene, Fenchone, and Camphor. We also explore the correspondence between light's degree of chirality (DOC) [35], and the chiral-signal conversion efficiency, finding a strong correlation between the two. This result supports the use of the newly derived DOC as an effective measure to quantify chiral-light-chiral-matter interactions.…”

Section: Introductionmentioning

confidence: 99%

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Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

Neufeld

Hübener

Rubio

et al. 2021

Phys. Rev. Research

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We derive here a new highly selective photoelectron-based chirality-sensing technique that utilizes 'locally-chiral' laser pulses. We show that this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting dichroism is much larger and more robust than conventional PECD, is found in all hemispheres, and is not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, a CD of up to 10% survives in the angularly-integrated above-threshold ionization (ATI) spectra, and of up to 5% in the total ionization rates. We demonstrate these results through ab-initio calculations in the chiral molecules Bromochlorofluoromethane, Limonene, Fenchone, and Camphor. We also explore the parameter-space of the locally-chiral field and show that the observed CD is strongly correlated to the degree of chirality of the light, validating it as a measure for chiralinteraction strengths. Our results pave the way for highly selective probing of ultrafast chirality in ATI, can potentially lead to all-optical enantio-separation, and motivate the use of locally-chiral light for enhancing ultrafast spectroscopies.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

Neufeld

Hübener

Rubio

et al. 2021

Phys. Rev. Research

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“…In all the experiments reported above, the tailored polarization profile was confined to the (x, y)-plane perpendicular to the propagation direction of the pulse. Building on recent theoretical proposals [209][210][211][212]226], we envision the next challenge in experimental coherent control to be the generation and tailoring of full 3D light fields by superimposing two polarization-shaped laser pulses propagating non-collinearly in different directions.…”

Section: Discussionmentioning

confidence: 99%

“…These results demonstrate that MPI of chiral molecules with circularly polarized few-cycle pulses can be used to control the axial asymmetry via the PECD and, moreover, the lateral asymmetry via the CEP. Very recently, fully 3D polarization-tailored laser fields, generated by superposition of two polarization-controlled multichromatic laser pulses propagating non-collinearly in different directions, have been proposed as novel tools for the investigation of chiral light-matter interactions [209][210][211][212]. These so-called superchiral light fields [213] promise an unprecedented enantio-sensitivity which makes them highly attractive for chiral discrimination applications.…”

Section: Asymmetries In the Photoemission From Chiral Moleculesmentioning

confidence: 99%

Multichromatic Polarization-Controlled Pulse Sequences for Coherent Control of Multiphoton Ionization

et al. 2021

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In this review, we report on recent progress in the generation and application of multichromatic polarization-tailored pulse sequences for the coherent control of multiphoton ionization (MPI) dynamics and present unpublished experimental results that complement our previous findings. Specifically, we utilize single-color, bichromatic, and trichromatic polarization-controlled pulse sequences generated by spectral amplitude, phase and polarization modulation of a carrier-envelope phase (CEP)-stable white light supercontinuum for MPI. The analysis of the number of ionization pathways and the number of distinct final free electron states shows that both increase significantly, but scale differently with the number of absorbed photons and the number of pulses in the sequence. In our experiments, ultrafast polarization shaping is combined with high-resolution photoelectron tomography to generate, control, and reconstruct three-dimensional photoelectron momentum distributions from atomic and molecular MPI. We discuss the use of polarization-controlled single-color and bichromatic pulse sequences in perturbative and non-perturbative coherent control of coupled electron-nuclear dynamics in molecules, atomic spin-orbit wave packet dynamics and the directional photoemission from atoms and chiral molecules. We compare the coherent control of CEP-insensitive intraband multipath interference in the MPI with a fixed number of photons with CEP-sensitive interband multipath interference in the ionization with a different number of photons. The generation and control of free electron vortices with even-numbered rotational symmetry by MPI with single-color pulse sequences is contrasted with the bichromatic control of CEP-sensitive electron vortices with odd-numbered rotational symmetry. To illustrate the potential of multichromatic pulse sequences for coherent control, we present a trichromatic scheme for shaper-based quantum state holography.

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“…For instance, many efforts are currently invested in photoelectron circular dichroism [7][8][9]. Yet, others focus on nonlinear optical signals that depend on the sign of the electric fields with which the molecules interact [10,11] including photoexcitation circular dichroism [12], the use of synthetic chiral fields [13][14][15][16], and microwave three-wave mixing [17][18][19][20][21]. More precisely, the latter technique can be understood through cyclic three-level models [22][23][24][25][26][27][28] where the product of three light-matter couplings [hereafter referred to as the Kral-Shapiro (KS) product] differs by a π phase between the two enantiomers.…”

mentioning

confidence: 99%

Enantioselective Topological Frequency Conversion

Schwennicke¹,

Yuen-Zhou²

2021

Preprint

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Two molecules are enantiomers if they are non-superimposable mirror images of each other. Electric dipole-allowed cyclic transitions, and R, S label the two enantiomers. Here we generalize the concept of topological frequency conversion to an isotropic ensemble of molecular enantiomers. We show that, within a rotating-frame, the pumping power between fields of frequency ω1 and ω2 is sensitive to enantiomeric excess, P2→1 =(NR − NS), where Ni is the number of enantiomers i and C R − ∝ sgnO R is an isotropically averaged Chern number. Connections with chiroptical microwave spectroscopy are made.

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Degree of chirality of electromagnetic fields and maximally chiral light

Cited by 16 publications

References 39 publications

Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

Multichromatic Polarization-Controlled Pulse Sequences for Coherent Control of Multiphoton Ionization

Enantioselective Topological Frequency Conversion

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