Optimal quantum control (OQC) enabled by femtosecond laser pulse shaping techniques provides a highly flexible approach to quantum states manipulation in solid-state qubit systems. Here we apply OQC to optimize the form of the triggering laser pulse for a single photon source. The use of a frequency-swept laser pulse possessing a notch resonant with the transition energy of the quantum emitter enables the spectral isolation of the emitted photon stream in conjunction with resonant driving for good indistinguishability. We show that the robustness of this scheme would enable spectral multiplexing of quantum light sources using a single triggering laser pulse.
In this presentation I will describe a new laser driving scheme for triggered high-brightness single photon emitters using a chirped laser pulse possessing a spectral hole resonant with the transition energy of the emitter, referred to as Notch-filtered adiabatic rapid passage (NARP). When combined with optimized photonic structures for enhanced collection efficiency and commercial filters we estimate that NARP would provide less than 10-8 scattered photons per emitted photon with a 4% detection loss together with resonant driving for high photon indistinguishability. We demonstrate inversion using NARP experimentally in a single semiconductor QD.
Semiconductor quantum dots (QDs) may be applied to solid-state quantum emitters of interest for quantum light sources or nodes in distributed quantum networks. For such emitters, resonant optical driving results in the highest degree of photon indistinguishability, but leads to the need to reject scattered light from the laser used to drive the emitter. In this work, we apply femtosecond pulse shaping techniques to the development of quantum state inversion strategies for QD emitters that optimize fidelity and source brightness. The control protocols we have developed would be applicable to a wide range of solid-state QE systems.
Interest in the hybrid organic-inorganic perovskite semiconductors has skyrocketed in recent years due to unprecedented high performance as solution-processable absorber layers in solar cells [1]. These materials also have potential for applications in semiconductor spintronics due to their large spin-orbit interaction. Theoretical studies predict a large Rashba spin splitting [2], and recent experiments have revealed a large photoinduced magnetization [3-5] and spin-dependent optical Stark effect [6], yet still relatively little is known about the spin-related properties of these materials. Here we report polarization-dependent pump probe studies of the 2D perovskite butylammonium methylammonium lead iodide. Our experiments indicate a strong influence of the Rashba spin splitting on the carrier kinetics in this system, consistent with our recent four-wave mixing studies of bulk CH3NH3PbI3.
[1] https://www.nrel.gov/pv/assets/images/efficiency_chart.jpg.
[2] M. Kepenekian and J. Even, J. Phys. Chem. Lett. 8, 3362 (2017).
[3] D. Giovanni et al. Nano Lett. 15, 1553 (2015).
[4] C. Zhang et al. Nat. Phys. 11, 427 (2015).
[5] P. Odenthal et al. Nat. Phys. 13, 894 (2017).
[6] D. Giovanni et al. Science Advances 2, e1600477 (2016).
The lead halide hybrid perovskites have gained considerable attention in recent years due to their stellar performance as absorber layers in solution-processed solar cells, with efficiencies recently reaching over 22 percent [1]. Owing to their large spin-orbit coupling, these materials are also of interest for spintronic applications, in which the presence of lead may be less of an impediment to their adoption [2]. Measurements of spin dynamics in bulk CH3NH3PbI3-xClx have been reported in recent years [3,4,5], the spin-dependent optical Stark effect was demonstrated in 4F-PEPI [6], and a large Rashba effect has been predicted in both bulk and 2D perovskites [2], highlighting the need for further studies of the spin-related properties of these materials. Here we report spin-dependent measurements of carrier kinetics in butylammonium methylammonium lead iodide 2D perovskite and measurements of the coherent carrier response in 3D CH3NH3PbI3. Both experiments provide direct evidence of the impact of Rashba on the carrier kinetics in these systems, further supporting the potential for developing spin-optoelectronic devices using these materials.
[1] https://www.nrel.gov/pv/assets/images/efficiency_chart.jpg.
[2] M. Kepenekian and J. Even, J. Phys. Chem. Lett. 8, 3362 (2017).
[3] D. Giovanni et al. Nano Lett. 15, 1553 (2015).
[4] C. Zhang et al. Nat. Phys. 11, 427 (2015).
[5] P. Odenthal et al. Nat. Phys. 13, 894 (2017).
[6] D. Giovanni et al. Science Advances 2, e1600477 (2016).
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