Charge-Transfer Chemical Reactions in Nanofluidic Fabry-Pérot Cavities
| dc.contributor.author | MAURO, L | |
| dc.contributor.author | CAICEDO, K | |
| dc.contributor.author | JONUSAUSKAS, G | |
| hal.structure.identifier | Laboratoire Ondes et Matière d'Aquitaine [LOMA] | |
| dc.contributor.author | AVRILLER, Rémi | |
| dc.date.issued | 2021-04-13 | |
| dc.identifier.issn | 1098-0121 | |
| dc.description.abstractEn | We investigate the chemical reactivity of molecular populations confined inside a nanofluidic Fabry-Pérot cavity. Due to strong light-matter interactions developing between a resonant electromagnetic cavity-mode and the electric dipole moment of the confined molecules, a polariton is formed. The former gets dressed by environmental vibrational and rotational degrees of freedom of the solvent. We call the resulting polariton dressed by its cloud of environmental excitation a "reacton", since it further undergoes chemical reactions. We characterize how the reacton formation modifies the kinetics of a photoisomerization chemical reaction involving an elementary charge-transfer process. We show that the reaction driving-force and reorganization energy are both modulated optically by the reactant concentration, the vacuum Rabi splitting and the de-tuning between the Fabry-Pérot cavity frequency and targeted electronic transition. Finally, we compute the ultrafast picosecond dynamics of the whole photochemical reaction. We predict that despite optical cavity losses and solvent-mediated non-radiative relaxation, measurable signatures of the reacton formation can be found in state-of-the-art pump-probe experiments. | |
| dc.description.sponsorship | Réactions Chimiques, Transfert de Charges et d'Energie en Cavité Electromagnétique - ANR-18-CE30-0006 | |
| dc.description.sponsorship | University of Bordeaux Graduate Scholl in Light Sciences & Technologies - ANR-17-EURE-0027 | |
| dc.language.iso | en | |
| dc.publisher | American Physical Society | |
| dc.subject.en | Atoms | |
| dc.subject.en | ions | |
| dc.subject.en | molecules in cavities | |
| dc.subject.en | Chemical physics and physical chemistry | |
| dc.subject.en | Polaritons | |
| dc.subject.en | Light-latter interaction | |
| dc.subject.en | Optical microcavities | |
| dc.title.en | Charge-Transfer Chemical Reactions in Nanofluidic Fabry-Pérot Cavities | |
| dc.type | Article de revue | |
| dc.identifier.doi | 10.1103/PhysRevB.103.165412 | |
| dc.subject.hal | Physique [physics]/Matière Condensée [cond-mat]/Systèmes mésoscopiques et effet Hall quantique [cond-mat.mes-hall] | |
| dc.identifier.arxiv | 2010.05524 | |
| bordeaux.journal | Physical Review B: Condensed Matter and Materials Physics (1998-2015) | |
| bordeaux.peerReviewed | oui | |
| hal.identifier | hal-02962814 | |
| hal.version | 1 | |
| hal.origin.link | https://hal.archives-ouvertes.fr//hal-02962814v1 | |
| bordeaux.COinS | ctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.jtitle=Physical%20Review%20B:%20Condensed%20Matter%20and%20Materials%20Physics%20(1998-2015)&rft.date=2021-04-13&rft.eissn=1098-0121&rft.issn=1098-0121&rft.au=MAURO,%20L&CAICEDO,%20K&JONUSAUSKAS,%20G&AVRILLER,%20R%C3%A9mi&rft.genre=article |
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