Photoelectron chiral dichroism induced by lasers without helicity via chiral hole wave-packets
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| Format: | Preprint |
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2025
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| author | Bouskila, Gal Fleischer, Avner Neufeld, Ofer |
| author_facet | Bouskila, Gal Fleischer, Avner Neufeld, Ofer |
| contents | Photoelectron circular dichroism (PECD) is a method where randomly oriented chiral molecules are photoionized due to irradiation by circularly-polarized lasers, yielding large chiral signals in the photoelectron momentum distribution. Recently, PECD was explored with polarization-tailored light such as bi-chromatic and non-collinear drivers, which still produces significant chiral signals. Yet, all known PECD configurations to date exhibit non-zero time-local chirality. That is, they are driven by an intrinsically helical light source. Nonetheless, 'chiral' light can also be non-helical if its chirality manifests on longer timescales (e.g. an optical centrifuge). It remains unknown whether PECD can arise from non-helical coherent light. Here we predict that PECD indeed emerges from non-helical light by employing a train of linearly-polarized intense laser pulses with a rotating polarization axis, which are phase-coherent and time-delayed. We find strong PECD in the model chiral molecule CBrClFH under a wide parameter regime that can be optimized up to ~8% by tuning delays between pulses, suggesting quantum interference. We directly show that the physical mechanism for this type of PECD differs from the standard case, relying on a chiral hole attosecond wave-packet evolving in the molecule, induced by the first linear pulse. Our work shows that multiple mechanisms can give rise to PECD on longer timescales and provides a novel approach for ultrafast chirality spectroscopy and coherent chiral wave-packet manipulation. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2512_12412 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Photoelectron chiral dichroism induced by lasers without helicity via chiral hole wave-packets Bouskila, Gal Fleischer, Avner Neufeld, Ofer Optics Chemical Physics Photoelectron circular dichroism (PECD) is a method where randomly oriented chiral molecules are photoionized due to irradiation by circularly-polarized lasers, yielding large chiral signals in the photoelectron momentum distribution. Recently, PECD was explored with polarization-tailored light such as bi-chromatic and non-collinear drivers, which still produces significant chiral signals. Yet, all known PECD configurations to date exhibit non-zero time-local chirality. That is, they are driven by an intrinsically helical light source. Nonetheless, 'chiral' light can also be non-helical if its chirality manifests on longer timescales (e.g. an optical centrifuge). It remains unknown whether PECD can arise from non-helical coherent light. Here we predict that PECD indeed emerges from non-helical light by employing a train of linearly-polarized intense laser pulses with a rotating polarization axis, which are phase-coherent and time-delayed. We find strong PECD in the model chiral molecule CBrClFH under a wide parameter regime that can be optimized up to ~8% by tuning delays between pulses, suggesting quantum interference. We directly show that the physical mechanism for this type of PECD differs from the standard case, relying on a chiral hole attosecond wave-packet evolving in the molecule, induced by the first linear pulse. Our work shows that multiple mechanisms can give rise to PECD on longer timescales and provides a novel approach for ultrafast chirality spectroscopy and coherent chiral wave-packet manipulation. |
| title | Photoelectron chiral dichroism induced by lasers without helicity via chiral hole wave-packets |
| topic | Optics Chemical Physics |
| url | https://arxiv.org/abs/2512.12412 |