Quantum entanglement is one of the most intriguing features of quantum mechanics. To investigate the entanglement between two excitons in a biexciton, an experimental technique called density matrix spectroscopy (DMS) has recently been developed. DMS combines stimulated emission tomography and pump-probe techniques to obtain a time-resolved density matrix of the polarization state of a photon pair emitted from the biexciton. The reconstructed density matrix is expected to encode information about the biexciton state and its entanglement dynamics, but the precise nature of this connection has remained unclear. In this paper, we derive an analytical relationship between the density matrix obtained by DMS and the biexciton state. In addition, we perform numerical simulations to compare the entanglement dynamics obtained by DMS with the biexciton's entanglement dynamics in a two-dimensional electron-hole system using an extended ionic Hubbard model. We find that DMS can partially capture the entanglement in the biexciton, in particular, the dynamics of the difference
Sbi−Sk, where
Sbi is the entanglement entropy of the biexciton and
Sk is the entanglement in terms of the wavevectors of the excitons that constitute the biexciton. These results demonstrate the validity of DMS for obtaining information about the entanglement dynamics of the biexciton.
Spectroscopy is an indispensable tool for understanding the structures and dynamics of molecular systems. However, computational modeling of spectroscopy is challenging due to the exponential scaling of computational complexity with system sizes unless drastic approximations are made. Quantum computers could potentially overcome these classically intractable computational tasks, but the existing approaches using quantum computers to simulate spectroscopy can only handle isolated and static molecules. In this work, we develop a workflow that combines multi-scale modeling and a time-dependent variational quantum algorithm to compute the linear spectroscopy of systems interacting with their condensed-phase environment via the relevant time correlation function. We demonstrate the feasibility of our approach by numerically simulating the UV-vis absorption spectra of organic semiconductors. We show that our dynamical approach captures several spectral features that are otherwise overlooked by static methods. Our method can be directly used for other linear condensed-phase spectroscopy and could potentially be extended to nonlinear multi-dimensional spectroscopy.