Keeping the photon in the dark: Enabling quantum dot dark state control by chirped pulses and magnetic fields
Florian Kappe, René Schwarz, Yusuf Karli, Thomas K. Bracht, V. M. Axt, Saimon Filipe Covre da Silva, Armando Rastelli, Vikas Remesh, Doris E. Reiter, Gregor Weihs
Dark excitons in quantum dots are not directly optically accessible, which has limited their use in practical applications. Nevertheless, they offer promising features such as substantially longer lifetimes compared to bright excitons, making them attractive candidates for quantum information processing. While previous theoretical and experimental studies have explored their potential, their full capabilities remain largely untapped. In this work, we demonstrate an all-optical storage and retrieval of the spin-forbidden dark exciton in a quantum dot from the ground state using chirped pulses and an in-plane magnetic field. Our experimental findings are in excellent agreement with theoretical predictions of the dynamics calculated using state-of-the-art product tensor methods. Our scheme enables an all-optical control of dark states without relying on any preceding decays. This opens up an unexplored dimension for optimal quantum control and time-bin entangled photon pair generation from quantum dots.
Dark excitons in quantum dots are not directly optically accessible, which has limited their use in practical applications. Nevertheless, they offer promising features such as substantially longer lifetimes compared to bright excitons, making them attractive candidates for quantum information processing. While previous theoretical and experimental studies have explored their potential, their full capabilities remain largely untapped. In this work, we demonstrate an all-optical storage and retrieval of the spin-forbidden dark exciton in a quantum dot from the ground state using chirped pulses and an in-plane magnetic field. Our experimental findings are in excellent agreement with theoretical predictions of the dynamics calculated using state-of-the-art product tensor methods. Our scheme enables an all-optical control of dark states without relying on any preceding decays. This opens up an unexplored dimension for optimal quantum control and time-bin entangled photon pair generation from quantum dots.
Because dark excitons in quantum dots are not directly optically accessible, so far they have not played a significant role in using quantum dots for photon generation. They possess significantly longer lifetimes than their brighter counterparts and hence offer enormous potential for photon storage or manipulation. In this work, we demonstrate an all-optical storage and retrieval of the spin-forbidden dark exciton in a quantum dot from the ground state employing chirped pulses and an in-plane magnetic field. Our experimental findings are in excellent agreement with theoretical predictions of the dynamics calculated using state-of-the-art product tensor methods. Our scheme enables an all-optical control of dark states without relying on any preceding decays. This opens up a new dimension for optimal quantum control and time-bin entangled photon pair generation from quantum dots.
Temporal encodings of quantum information are prevalent in applications because of their suitability for long-distance quantum communication and their compatibility with optical fiber communication networks. Perhaps the simplest temporal encoding is time-bin encoding, i. e. in superpositions of two (or more) temporally separated optical pulses. Early attempts at generating time-bin entanglement from single quantum emitters was not able to avoid the problem of re-excitation or was converted probabilistically from polarization entangled photon pairs from a quantum dot. Direct generation requires a metastable level to carry the coherence and avoid double pair emission into the desired time bins. In order to use dark exciton states as metastable states we have worked on their efficient creation and coherent control in the presence of in-plane magnetic fields. Much of this is based on our recent work on advanced excitation schemes using chirped pulses. With chirped pulses we are now able to deterministically populate a dark exciton state and to transfer this population to the biexciton, which can then emit a photon pair.
Quantum dots are considered an attractive system for applications in quantum communication and quantum logic, confirmed by experimental demonstrations of quantum dot based single photon emission devices. Another key quantum optics resource is the on-demand generation of entangled photon pairs, for which the radiative decay of the biexciton state in a quantum dot has been proposed. The realization of such a device has been prevented due to polarization splitting of the exciton fine structure, caused by anisotropies of various structural parameters of the dot. We present the results of recent experiments that manage the splitting in quantum dots, in order to allow entangled photon emission. We demonstrate that dots with splitting within the homogeneous linewidth can be realized by carefully controlling the thickness of the dot layer. Furthermore, we show that the splitting can be reduced to zero by the application of an in-plane magnetic field. Polarization dependent correlation measurements on these dots will be presented that show characteristic features of entanglement, such as polarization correlation for all linear detection bases, and circular polarization anti-correlation. Our results indicate that for the first time, we have observed triggered entangled photon pair emission from a quantum dot.
Semiconductor Quantum dots are potentially an attractive source of non-classical light. They can confine bound electron-hole pairs, excitons, in all three spatial dimensions giving them discrete optical emission energies, much like the electronic states in atomic systems. The semiconductor nature of the system allows quantum dots to be integrated into complicated device structures including optical cavities [1] and electrical injection [2]. The radiative exciton emission from a semiconductor quantum dot can provide the simplest form of quantum light, a single photon source [2]. The finite re-excitation time following the radiative decay of an exciton in a quantum dot prevents the dot from emitting more than one photon if excited with a short optical or electronic pulse. In a similar fashion excitation of the biexciton state, consisting of two electrons and holes, in the quantum dot results in the emission of a pair of photons at the energy of the biexciton and exciton transitions. The biexciton state was, in fact, proposed as a possible source of polarisation-entangled photons in 2000 by Benson et al. [3] as it consists of two polarisation-correlated decay paths which could potentially be indistinguishable. The condition of indistinguishability is fundamental to the generation of entangled photons and is, in general, not true of the two decay paths from the biexciton state in a quantum dot; physical anisotropy causes the intermediate exciton states to hybridise and separate in energy providing ‘which-path’ information about the route taken through the biexciton decay. We demonstrate how the splitting between the intermediate exciton states in a single InAs quantum dot can be controlled by growth [4], rapid thermal annealing [5] and the application of an external magnetic field [6]. Each of these three techniques can be used to make the intermediate exciton states degenerate allowing the biexciton decay to produce singe pairs of entangled photons triggered by short laser pulses [7,8]. Entangled photon pair sources are essential for applications such as entanglement based quantum key distribution, and optical quantum computing. For these applications it is important that no more than one entangled photon pair is generated in a cycle, a requirement met by our quantum dot source which is not possible with traditional methods for generating entangled pairs of photons. Entanglement also enables quantum interferometry and metrology, the basis of image resolution beyond that possible with equivalent classical light. Biphoton interferometry using entangled emission from the biexciton decay reveals fringes with half the period of classical light [9], and less that that of the laser. In addition, interferometry suggests that this type of entangled light source is not limited by decoherence, we fine the biphoton is surprising robust against dephasing, in stark contrast to the devastating effect of decoherence upon single photons emitted by similar structures.
Semiconductor quantum dots have been featured in a number of proposals for quantum computing because of the advantages afforded by confinement on the nanoscale, such as well separated, discrete energy levels and ease of optical manipulation. In addition, they can leverage established semiconductor fabrication techniques and, like the quantum dots used in this work, can be designed to match the telecommunication band, improving the scalability and potential integration of the platform into existing technologies. This thesis work applied optical pulse engineering to manipulate exciton qubits in self-assembled InAs quantum dots. Optimal quantum control theory was used to design pulse shapes that implement high fidelity single-qubit and two-qubit operations, with constraints on the numerical optimization that ensure that the pulses can be accurately implemented using a commercial 4f pulse shaper. In the case of single-qubit operations, the results showed that two uncoupled qubits can be manipulated in parallel using a single phase-shaped laser pulse, provided their optoelectronic properties are sufficiently different. It was demonstrated that targeted differences in inversion and phase between the qubits can be achieved on an ultrafast timescale with high fidelity. In the case of two-qubit operations, the controlled-rotation gate was optimized using amplitude-only and phase-only pulse shaping schemes. The shaped pulses for both schemes were shown to produce higher fidelity operations. The ability to implement robust state inversion on short timescales is particularly useful for technologies such as ultrafast optical switches, single-photon sources, and entangled-photon sources. This work has demonstrated state inversion in a single InAs quantum dot via adiabatic rapid passage using linearly chirped laser pulses. The achieved gate times were an order of magnitude shorter than previous demonstrations. Theoretical predictions of the dependence of the inversion efficiency of the exciton on the sign of the pulse chirp were also verified experimentally, allowing for the identification of phonon-mediated dephasing as the dominant source of decoherence.
The dark exciton state in semiconductor quantum dots (QDs) constitutes a long-lived solid-state qubit which has the potential to play an important role in implementations of solid-state-based quantum information architectures. In this work, we exploit deterministically fabricated QD microlenses which promise enhanced photon extraction, to optically prepare and read out the dark exciton spin and observe its coherent precession. The optical access to the dark exciton is provided via spin-blockaded metastable biexciton states acting as heralding states, which are identified by deploying polarization-sensitive spectroscopy as well as time-resolved photon cross-correlation experiments. Our experiments reveal a spin-precession period of the dark exciton of (0.82 ± 0.01) ns corresponding to a fine-structure splitting of (5.0 ± 0.7) μeV between its eigenstates ↑⇑±↓⇓. By exploiting microlenses deterministically fabricated above pre-selected QDs, our work demonstrates the possibility to scale up implementations of quantum information processing schemes using the QD-confined dark exciton spin qubit, such as the generation of photonic cluster states or the realization of a solid-state-based quantum memory.