Multidimensional spectroscopy in optical cavities based on photon correlations

Sergey K. Andrukhovich, A.V. Berestov, B. A. Martsynkevich +2 more

Gerace, Tureci, Ferretti +4 more

Konstantin E. Dorfman, Shaul Mukamel

The strong coupling of atoms and molecules to radiation field modes in optical cavities creates dressed matter/field states known as polaritons with controllable dynamical and energy transfer properties. We propose a multidimensional optical spectroscopy technique for monitoring polariton dynamics. The response of a two-level atom to the time-dependent coupling to a single-cavity mode is monitored through time-and-frequency-resolved single-photon coincidence measurements of spontaneous emission. Polariton population and coherence dynamics and its variation with cavity photon number and controlled by gating parameters are predicted by solving the Jaynes-Cummings model.

R. v. Baltz

Arunangshu Debnath, Ángel Rubio

We present a theoretical formulation of the frequency domain multidimensional pump-probe analog spectroscopy, which utilizes the spectral–temporal entanglement features of the biphoton sources. It has been shown, via a compact multi-time, convolutional Green’s function expression and the accompanying numerical simulations, that utilizing the correlation properties of non-classical sources offers a viable scheme for the exploration of dissipative kinetics of the cavity confined quantum aggregates. The cooperative and competitive modifications brought in by the photonic cavity mode and the auxiliary vibrational modes into the scattering and dephasing properties of the exciton–polaritons have been explored via their signatures in the multidimensional correlation maps. The study offers a new parameter window for the investigation of the dynamical polariton characteristics and warrants the usage of multi-mode entanglement properties of the external photonic sources in future studies.

Daniela Gallego-Valencia, Lars Mewes, Johannes Feist +1 more

The fast dynamics of molecular polaritonics is scrutinized theoretically through the implementation of two-dimensional spectroscopy protocols. We derive conceptually simple and computationally efficient formulas to calculate two-dimensional spectra for molecules, each of them modeled as a system of two electronic states including vibrational relaxation, immersed in an optical cavity, thus coupled to quantized radiation. Cavity photon losses and molecular relaxation are incorporated into the Hamiltonian dynamics to form an open quantum system that is solved through a master equation. In the collective case, the relaxation dynamics into dark states is revealed to be the crucial factor to explain the asymmetries in both the diagonal and cross peaks of two-dimensional spectra for long waiting times between excitation and detection, a feature shown by recent experiments. Our theoretical method provides a deeper insight in those processes that yield relevant signals in multidimensional molecular spectroscopy.