Intermolecular forces and correlations mediated by a phonon bath

article Intermolecular forces and correlations mediated by a phonon bath published yes Xiang Li author 4B7E523C-F248-11E8-B48F-1D18A9856A87 Enderalp Yakaboylu author 38CB71F6-F248-11E8-B48F-1D18A9856A870000-0001-5973-0874 Giacomo Bighin author 4CA96FD4-F248-11E8-B48F-1D18A9856A870000-0001-8823-9777 Richard Schmidt author Mikhail Lemeshko author 37CB05FA-F248-11E8-B48F-1D18A9856A870000-0002-6990-7802 Andreas Deuchert author 4DA65CD0-F248-11E8-B48F-1D18A9856A870000-0003-3146-6746 MiLe department RoSe department Quantum rotations in the presence of a many-body environment project Angulon: physics and applications of a new quasiparticle project A path-integral approach to composite impurities project Analysis of quantum many-body systems project Inspired by the possibility to experimentally manipulate and enhance chemical reactivity in helium nanodroplets, we investigate the effective interaction and the resulting correlations between two diatomic molecules immersed in a bath of bosons. By analogy with the bipolaron, we introduce the biangulon quasiparticle describing two rotating molecules that align with respect to each other due to the effective attractive interaction mediated by the excitations of the bath. We study this system in different parameter regimes and apply several theoretical approaches to describe its properties. Using a Born–Oppenheimer approximation, we investigate the dependence of the effective intermolecular interaction on the rotational state of the two molecules. In the strong-coupling regime, a product-state ansatz shows that the molecules tend to have a strong alignment in the ground state. To investigate the system in the weak-coupling regime, we apply a one-phonon excitation variational ansatz, which allows us to access the energy spectrum. In comparison to the angulon quasiparticle, the biangulon shows shifted angulon instabilities and an additional spectral instability, where resonant angular momentum transfer between the molecules and the bath takes place. These features are proposed as an experimentally observable signature for the formation of the biangulon quasiparticle. Finally, by using products of single angulon and bare impurity wave functions as basis states, we introduce a diagonalization scheme that allows us to describe the transition from two separated angulons to a biangulon as a function of the distance between the two molecules. AIP Publishing2020 eng Physical and Theoretical ChemistryGeneral Physics and Astronomy The Journal of Chemical Physics 0021-9606 1089-7690 1912.02658 32357791 00053044830000110.1063/1.5144759 15216 https://research-explorer.ista.ac.at/record/8958 Li, Xiang, et al. “Intermolecular Forces and Correlations Mediated by a Phonon Bath.” The Journal of Chemical Physics, vol. 152, no. 16, 164302, AIP Publishing, 2020, doi:<a href="https://doi.org/10.1063/1.5144759">10.1063/1.5144759</a>. Li X, Yakaboylu E, Bighin G, Schmidt R, Lemeshko M, Deuchert A. 2020. Intermolecular forces and correlations mediated by a phonon bath. The Journal of Chemical Physics. 152(16), 164302. Li X, Yakaboylu E, Bighin G, Schmidt R, Lemeshko M, Deuchert A. Intermolecular forces and correlations mediated by a phonon bath. The Journal of Chemical Physics. 2020;152(16). doi:<a href="https://doi.org/10.1063/1.5144759">10.1063/1.5144759</a> X. Li, E. Yakaboylu, G. Bighin, R. Schmidt, M. Lemeshko, A. Deuchert, The Journal of Chemical Physics 152 (2020). Li, X., Yakaboylu, E., Bighin, G., Schmidt, R., Lemeshko, M., & Deuchert, A. (2020). Intermolecular forces and correlations mediated by a phonon bath. The Journal of Chemical Physics. AIP Publishing. <a href="https://doi.org/10.1063/1.5144759">https://doi.org/10.1063/1.5144759</a> X. Li, E. Yakaboylu, G. Bighin, R. Schmidt, M. Lemeshko, and A. Deuchert, “Intermolecular forces and correlations mediated by a phonon bath,” The Journal of Chemical Physics, vol. 152, no. 16. AIP Publishing, 2020. Li, Xiang, Enderalp Yakaboylu, Giacomo Bighin, Richard Schmidt, Mikhail Lemeshko, and Andreas Deuchert. “Intermolecular Forces and Correlations Mediated by a Phonon Bath.” The Journal of Chemical Physics. AIP Publishing, 2020. <a href="https://doi.org/10.1063/1.5144759">https://doi.org/10.1063/1.5144759</a>. 85872020-09-30T10:33:17Z2026-04-08T07:26:09Z