Capturing electron-driven chiral dynamics in UV-excited molecules
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2023
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| author | Wanie, Vincent Bloch, Etienne Månsson, Erik P. Colaizzi, Lorenzo Ryabchuk, Sergey Saraswathula, Krishna Ordonez, Andres F. Ayuso, David Smirnova, Olga Trabattoni, Andrea Blanchet, Valérie Amor, Nadia Ben Heitz, Marie-Catherine Mairesse, Yann Pons, Bernard Calegari, Francesca |
| author_facet | Wanie, Vincent Bloch, Etienne Månsson, Erik P. Colaizzi, Lorenzo Ryabchuk, Sergey Saraswathula, Krishna Ordonez, Andres F. Ayuso, David Smirnova, Olga Trabattoni, Andrea Blanchet, Valérie Amor, Nadia Ben Heitz, Marie-Catherine Mairesse, Yann Pons, Bernard Calegari, Francesca |
| contents | Molecular chirality is a key design property for many technologies including bioresponsive imaging, circularly polarized light detection and emission, molecular motors and switches. Imaging and manipulating the primary steps of transient chirality is therefore central for controlling numerous physical, chemical and biological properties that arise from chiral molecules in response to external stimuli. So far, the manifestation of electron-driven chiral dynamics in neutral molecules has not been demonstrated at their intrinsic timescale. Here, we use time-resolved photoelectron circular dichroism (TR-PECD) with an unprecedented instrument response function of 2.9 fs to image the dynamics of coherent electronic motion activated by prompt UV-excitation in neutral chiral molecules, disclosing its impact on the molecular chiral response. We find that electronic beatings between Rydberg states lead to periodic modulations of the chiroptical response on the few-femtosecond timescale, showing a sign inversion in less than 10 fs. Calculations including both the molecular UV-excitation and subsequent photoionization confirm this interpretation and provide further evidence that the combination of the resulting photoinduced chiral current with a circularly polarized probe pulse realizes an enantio-selective filter of molecular orientations upon photoionization, opening up a route towards enantio-selective charge-directed reactivity. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2301_02002 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Capturing electron-driven chiral dynamics in UV-excited molecules Wanie, Vincent Bloch, Etienne Månsson, Erik P. Colaizzi, Lorenzo Ryabchuk, Sergey Saraswathula, Krishna Ordonez, Andres F. Ayuso, David Smirnova, Olga Trabattoni, Andrea Blanchet, Valérie Amor, Nadia Ben Heitz, Marie-Catherine Mairesse, Yann Pons, Bernard Calegari, Francesca Chemical Physics Atomic Physics Optics Molecular chirality is a key design property for many technologies including bioresponsive imaging, circularly polarized light detection and emission, molecular motors and switches. Imaging and manipulating the primary steps of transient chirality is therefore central for controlling numerous physical, chemical and biological properties that arise from chiral molecules in response to external stimuli. So far, the manifestation of electron-driven chiral dynamics in neutral molecules has not been demonstrated at their intrinsic timescale. Here, we use time-resolved photoelectron circular dichroism (TR-PECD) with an unprecedented instrument response function of 2.9 fs to image the dynamics of coherent electronic motion activated by prompt UV-excitation in neutral chiral molecules, disclosing its impact on the molecular chiral response. We find that electronic beatings between Rydberg states lead to periodic modulations of the chiroptical response on the few-femtosecond timescale, showing a sign inversion in less than 10 fs. Calculations including both the molecular UV-excitation and subsequent photoionization confirm this interpretation and provide further evidence that the combination of the resulting photoinduced chiral current with a circularly polarized probe pulse realizes an enantio-selective filter of molecular orientations upon photoionization, opening up a route towards enantio-selective charge-directed reactivity. |
| title | Capturing electron-driven chiral dynamics in UV-excited molecules |
| topic | Chemical Physics Atomic Physics Optics |
| url | https://arxiv.org/abs/2301.02002 |