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Probing exciton/exciton interactions with entangled photons: theory

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 Added by Eric R. Bittner
 Publication date 2019
  fields Physics
and research's language is English




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Quantum entangled photons provide a sensitive probe of many-body interactions and offer an unique experimental portal for quantifying many-body correlations in a material system. In this paper, we present a theoretical demonstration of how photon-photon entanglement can be generated via interactions between coupled qubits. Here we develop a model for the scattering of an entangled pair of photons from a molecular dimer. We develop a diagrammatic theory for the scattering matrix and show that one can correlate the von Neumann entropy of the outgoing bi-photon wave function to exciton exchange and repulsion interactions. We conclude by discussing possible experimental scenarios for realizing these ideas.



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Coherent coupling between excitons is at the heart of many-body interactions with transition metal dichalcogenide (TMD) heterostructures as an emergent platform for the investigation of these interactions. We employ multi-dimensional coherent spectroscopy on monolayer MoSetextsubscript{2}/WSetextsubscript{2} heterostructures and observe coherent coupling between excitons spatially localized in monolayer MoSe$_2$ and WSe$_2$. Through many-body spectroscopy, we further observe the absorption state arising from free interlayer electron-hole pairs. This observation yields a spectroscopic measurement of the interlayer exciton binding energy of about 250 meV.
We study the effect of the exciton fine-structure splitting on the polarisation-entanglement of photon pairs produced by the biexciton cascade in a single quantum dot. The entanglement is found to persist despite separations between the intermediate energy levels of up to 4 micro-eV. Measurements demonstrate that entanglement of the photon pair is robust to the dephasing of the intermediate exciton state responsible for the first order coherence time of either single photon. We present a theoretical framework taking into account the effects of spin-scattering, background light and dephasing. We distinguish between the first-order coherence time, and a parameter which we measure for the first time and define as the cross-coherence time.
We investigate the excitonic dynamics in MoSe2 monolayer and bulk samples by femtosecond transient absorption microscopy. Excitons are resonantly injected by a 750-nm and 100-fs laser pulse, and are detected by a probe pulse tuned in the range of 790 - 820 nm. We observe a strong density-dependent initial decay of the exciton population in monolayers, which can be well described by the exciton-exciton annihilation. Such a feature is not observed in the bulk under comparable conditions. We also observe the saturated absorption induced by exciton phase-space filling in both monolayers and the bulk, which indicates their potential applications as saturable absorbers.
We present an input/output analysis of photon-correlation experiments whereby a quantum mechanically entangled bi-photon state interacts with a material sample placed in one arm of a Hong-Ou-Mandel (HOM) apparatus. We show that the output signal contains detailed information about subsequent entanglement with the microscopic quantum states in the sample. In particular, we apply the method to an ensemble of emitters interacting with a common photon mode within the open-system Dicke Model. Our results indicate considerable dynamical information concerning spontaneous symmetry breaking can be revealed with such an experimental system.
A new approach to the theory of anisotropic exciton based on Fock transformation, i.e., on a stereographic projection of the momentum to the unit 4-dimensional (4D) sphere, is developed. Hyperspherical functions are used as a basis of the perturbation theory. The binding energies, wave functions and oscillator strengths of elongated as well as flattened excitons are obtained numerically. It is shown that with an increase of the anisotropy degree the oscillator strengths are markedly redistributed between optically active and formerly inactive states, making the latter optically active. An approximate analytical solution of the anisotropic exciton problem taking into account the angular momentum conserving terms is obtained. This solution gives the binding energies of moderately anisotropic exciton with a good accuracy and provides a useful qualitative description of the energy level evolution.
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