A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Thermal disorder prevents the suppression of ultra-fast photochemistry in the strong light-matter coupling regime (2024)


Dutta, A., Tiainen, V., Sokolovskii, I., Duarte, L., Markešević, N., Morozov, D., Qureshi, H. A., Pikker, S., Groenhof, G., & Toppari, J. J. (2024). Thermal disorder prevents the suppression of ultra-fast photochemistry in the strong light-matter coupling regime. Nature Communications, 15, Article 6600. https://doi.org/10.1038/s41467-024-50532-5


JYU-tekijät tai -toimittajat


Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: Dutta, Arpan; Tiainen, Ville; Sokolovskii, Ilia; Duarte, Luís; Markešević, Nemanja; Morozov, Dmitry; Qureshi, Hassan A.; Pikker, Siim; Groenhof, Gerrit; Toppari, J. Jussi

Lehti tai sarja: Nature Communications

eISSN: 2041-1723

Julkaisuvuosi: 2024

Ilmestymispäivä: 04.08.2024

Volyymi: 15

Artikkelinumero: 6600

Kustantaja: Nature Publishing Group

Julkaisumaa: Britannia

Julkaisun kieli: englanti

DOI: https://doi.org/10.1038/s41467-024-50532-5

Julkaisun avoin saatavuus: Avoimesti saatavilla

Julkaisukanavan avoin saatavuus: Kokonaan avoin julkaisukanava

Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/96750


Tiivistelmä

Strong coupling between molecules and confined light modes of optical cavities to form polaritons can alter photochemistry, but the origin of this effect remains largely unknown. While theoretical models suggest a suppression of photochemistry due to the formation of new polaritonic potential energy surfaces, many of these models do not account for the energetic disorder among the molecules, which is unavoidable at ambient conditions. Here, we combine simulations and experiments to show that for an ultra-fast photochemical reaction such thermal disorder prevents the modification of the potential energy surface and that suppression is due to radiative decay of the lossy cavity modes. We also show that the excitation spectrum under strong coupling is a product of the excitation spectrum of the bare molecules and the absorption spectrum of the molecule-cavity system, suggesting that polaritons can act as gateways for channeling an excitation into a molecule, which then reacts normally. Our results therefore imply that strong coupling provides a means to tune the action spectrum of a molecule, rather than to change the reaction.


YSO-asiasanat: valokemia; molekyylit; kvasihiukkaset; polaritonit; fotonit


Liittyvät organisaatiot


Hankkeet, joissa julkaisu on tehty


OKM-raportointi: Kyllä

VIRTA-lähetysvuosi: 2024

Alustava JUFO-taso: 3


Viimeisin päivitys 2024-14-10 klo 15:08