Deterministic generation of bright single resonance fluorescence photons from a Purcell-enhanced quantum dot-micropillar system

The authors acknowledge financial support by the State of Bavaria and the German Ministry of Education and Research (BMBF) within the projects Q.com-H and the Chist-era project SSQN. Y.-M. H. acknowledges support from the Sino-German (CSC-DAAD) Postdoc Scholarship Program.We report on the observation of bright emission of single photons under pulsed resonance fluorescence conditions from a single quantum dot (QD) in a micropillar cavity. The brightness of the QD fluorescence is greatly enhanced via the coupling to the fundamental mode of a micropillar, allowing us to determine a single photon extraction efficiency of (20.7 ± 0.8) % per linear polarization basis. This yields an overall extraction efficiency of (41.4 ± 1.5) % in our device. We observe the first Rabi-oscillation in a weakly coupled quantum dot-micropillar system under coherent pulsed optical excitation, which enables us to deterministically populate the excited QD state. In this configuration, we probe the single photon statistics of the device yielding g(2)(0) = 0.072 ± 0.011 at a QD-cavity detuning of 75 μeV.PostprintPeer reviewe

Observation of resonance fluorescence and the Mollow triplet from a coherently driven site-controlled quantum dot

This work was funded by project SIQUTE (contract EXL02) of the European Metrology Research Programme (EMRP). The EMRP is jointly funded by the EMRP participating countries within EURAMET and the European Union. Support was provided from the Villum Foundation via the VKR Centre of Excellence NATEC.Resonant excitation of solid state quantum emitters has the potential to deterministically excite a localized exciton while ensuring maximally coherent emission. In this work, we demonstrate the coherent coupling of an exciton localized in a lithographically positioned, site-controlled semiconductor quantum dot to an external resonant laser field. For strong continuous-wave driving we observe the characteristic Mollow triplet and analyze the Rabi splitting and sideband widths as a function of driving strength and temperature. The sideband widths increase linearly with temperature and the square of the driving strength, which we explain via coupling of the exciton to longitudinal acoustic phonons. We also find an increase of the Rabi splitting with temperature, which indicates a temperature-induced delocalization of the excitonic wave function resulting in an increase of the oscillator strength. Finally, we demonstrate coherent control of the exciton excited state population via pulsed resonant excitation and observe a damping of the Rabi oscillations with increasing pulse area, which is consistent with our excitonx2013;photon coupling model. We believe that our work outlines the possibility to implement fully scalable platforms of solid state quantum emitters. Such scalability is one of the key prerequisites for more advanced, integrated nanophotonic quantum circuits.PostprintPeer reviewe

Bulk AlInAs on InP(111) as a novel material system for pure single photon emission

In this letter, we report on quantum light emission from bulk AlInAs grown on InP(111) substrates. We observe indium rich clusters in the bulk Al0:48In0:52As (AlInAs), resulting in quantum dot-like energetic traps for charge carriers, which are confirmed via cross-sectional scanning tunnelling microscopy (XSTM) measurements and 6-band k•p simulations. We observe quantum dot (QD)-like emission signals, which appear as sharp lines in our photoluminescence spectra at near infrared wavelengths around 860 nm, and with linewidths as narrow as 50 meV. We demonstrate the capability of this new material system to act as an emitter of pure single photons as we extract g(2)-values as low as g(2)/cw (0) = 0:05+0:17/-0:05 for continuous wave (cw) excitation and g (2) pulsed, corr. = 0:24 ± 0:02 for pulsed excitation.PostprintPeer reviewe

High-throughput ab initio reaction mechanism exploration in the cloud with automated multi-reference validation

Quantum chemical calculations on atomistic systems have evolved into a standard approach to study molecular matter. These calculations often involve a significant amount of manual input and expertise although most of this effort could be automated, which would alleviate the need for expertise in software and hardware accessibility. Here, we present the AutoRXN workflow, an automated workflow for exploratory high-throughput lectronic structure calculations of molecular systems, in which (i) density functional theory methods are exploited to deliver minimum and transition-state structures and corresponding energies and properties, (ii) coupled cluster calculations are then launched for optimized structures to provide more accurate energy and property estimates, and (iii) multi-reference diagnostics are evaluated to back check the coupled cluster results and subject hem to automated multi-configurational calculations for potential multi-configurational cases. All calculations are carried out in a cloud environment and support massive computational campaigns. Key features of all omponents of the AutoRXN workflow are autonomy, stability, and minimum operator interference. We highlight the AutoRXN workflow at the example of an autonomous reaction mechanism exploration of the mode of action of a homogeneous catalyst for the asymmetric reduction of ketones.Comment: 29 pages, 11 figure

Intrinsic and environmental effects on the interference properties of a high-performance quantum dot single-photon source

We acknowledge support by the State of Bavaria and the German Ministry of Education and Research (BMBF) within the project Q.com. J.I.-S. and J.M. acknowledge support from the Danish Research Council (DFF-4181-00416) and Villum Fonden (NATEC Centre). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No. 703193.We report a joint experimental and theoretical study of the interference properties of a single-photon source based on a In(Ga)As quantum dot embedded in a quasiplanar GaAs microcavity. Using resonant laser excitation with a pulse separation of 2 ns, we find near-perfect interference of the emitted photons, and a corresponding indistinguishability of I=(99.6^+0.4_−1.4)%. For larger pulse separations, quasiresonant excitation conditions, increasing pump power, or with increasing temperature, the interference contrast is progressively and notably reduced. We present a systematic study of the relevant dephasing mechanisms and explain our results in the framework of a microscopic model of our system. For strictly resonant excitation, we show that photon indistinguishability is independent of pump power, but strongly influenced by virtual phonon-assisted processes which are not evident in excitonic Rabi oscillations.Publisher PDFPeer reviewe

Cascaded emission of linearly polarized single photons from positioned InP/GaInP quantum dots

This content may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This material originally appeared in Appl. Phys. Lett. 103, 191113 (2013) and may be found at https://doi.org/10.1063/1.4828354.We report on the optical characterization of site-controlled InP/GaInP quantum dots (QDs). Spatially resolved low temperature cathodoluminescence proves the long-range ordering of the buried emitters, revealing a yield of ∼90% of optically active, positioned QDs and a strong suppression of emitters on interstitial positions. The emission of single QDs shows a pronounced degree of linear polarization along the [0,−1,1] crystal axis with an average degree of polarization of 94%. Photon correlation measurements of the emission from a single QD indicate the single-photon character of the exciton and biexciton emission lines as well as the cascaded nature of the photon pair