Photoionization of randomly oriented chiral molecules with circularly polarized light leads to a strong forward/backward asymmetry in the photoelectron angular distribution. This chiroptical effect, referred to as Photoelectron Circular Dichroism (PECD), was shown to take place in all ionization regimes, from single photon to tunnel ionization. In the Resonance Enhanced Multiphoton Ionisation (REMPI) regime, where most of the table-top PECD experiments have been performed, understanding the role of the intermediate resonances is currently the subject of experimental and theoretical investigations. In an attempt to decouple the role of bound-bound and bound-continuum transitions in REMPI-PECD, we photoionized the (+)-limonene enantiomer using two-color laser fields in [1 + 1′] and [2 + 2′] ionization schemes, where the polarization state of each color can be controlled independently. We demonstrate that the main effect of the bound-bound transition is to break the sample isotropy by orientation-dependent photoexcitation, in agreement with recent theoretical predictions. We show that the angular distribution of PECD strongly depends on the anisotropy of photoexcitation to the intermediate state, which is different for circularly and linearly polarized laser pulses. On the contrary, the helicity of the pulse that drives the bound-bound transition is shown to have a negligible effect on the PECD.
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Multiphoton photoelectron circular dichroism of limonene with independent polarization state control of the bound-bound and bound-continuum transitions
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7 October 2018
Research Article|
October 01 2018
Multiphoton photoelectron circular dichroism of limonene with independent polarization state control of the bound-bound and bound-continuum transitions

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JCP Editors' Choice 2018
S. Beaulieu;
S. Beaulieu
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
2
Institut National de la Recherche Scientifique, Centre EMT
, Varennes, Quebec J3X 1S2, Canada
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A. Comby;
A. Comby
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
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D. Descamps
;
D. Descamps
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
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S. Petit;
S. Petit
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
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F. Légaré;
F. Légaré
2
Institut National de la Recherche Scientifique, Centre EMT
, Varennes, Quebec J3X 1S2, Canada
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B. Fabre;
B. Fabre
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
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V. Blanchet
;
V. Blanchet
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
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Y. Mairesse
Y. Mairesse
1
Université de Bordeaux—CNRS—CEA, CELIA, UMR5107
, F33405 Talence, France
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J. Chem. Phys. 149, 134301 (2018)
Article history
Received:
June 01 2018
Accepted:
August 09 2018
Connected Content
A companion article has been published:
Study decouples excitation and ionization steps in photoelectron circular dichroism
Citation
S. Beaulieu, A. Comby, D. Descamps, S. Petit, F. Légaré, B. Fabre, V. Blanchet, Y. Mairesse; Multiphoton photoelectron circular dichroism of limonene with independent polarization state control of the bound-bound and bound-continuum transitions. J. Chem. Phys. 7 October 2018; 149 (13): 134301. https://doi.org/10.1063/1.5042533
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