In recent years the physics of two-dimensional semiconductors was revived by the discovery of the class of transition metal dichalcogenides. In these systems excitons dominate the optical response in the visible range and open many perspectives for nonlinear spectroscopy. To describe the coherence and polarization dynamics of excitons after ultrafast excitation in these systems, we employ the Bloch equation model of a two-level system extended by a local field describing the exciton–exciton interaction. We calculate four-wave mixing (FWM) signals and analyze the dependence of the temporal and spectral signals as a function of the delay between the exciting pulses. Exact analytical results obtained for the case of ultrafast (δ-shaped) pulses are compared to numerical solutions obtained for finite pulse durations. If two pulses are used to generate the nonlinear signal, characteristic spectral line splittings are restricted to short delays. When considering a three-pulse excitation the line splittings, induced by the local field effect, persist for long delays. All of the found features are instructively explained within the Bloch vector picture and we show how the exciton occupation dynamics govern the different FWM signals.
Color centers in hexagonal boron nitride show stable single photon emission even at room temperature, making these systems a promising candidate for quantum information applications. Besides this remarkable property, also their interaction with longitudinal optical (LO) phonons is quite unique because they lead to dominant phonon sidebands, well separated from the zero phonon line. In this work we utilize this clear spectral separation to theoretically investigate the influence of phonon decay dynamics on time-dependent photoluminescence (PL) signals. Our simulations show, that by using tailored optical excitation schemes it is possible to create a superposition between the two LO modes, leading to a phonon quantum beat that manifests in the time-dependent PL signal.
The coupling between single-photon emitters and phonons opens many possibilities to store and transmit quantum properties. In this paper we apply the independent boson model to describe the coupling between an optically driven two-level system and a discrete phonon mode. Tailored optical driving allows not only to generate coherent phonon states, but also to generate coherent superpositions in the form of Schrödinger cat states in the phonon system. We analyze the influence of decay and dephasing of the two-level system on these phonon preparation protocols. We find that the decay transforms the coherent phonon state into a circular distribution in phase space. Although the dephasing between two exciting laser pulses leads to a reduction of the interference ability in the phonon system, the decay conserves it during the transition into the ground state. This allows to store the phonon quantum state properties in the ground state of the single-photon emitter.
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