Culling a Self-Assembled Quantum Dot as a Single-Photon Source Using X-ray Microscopy.

Introduction The advanced growth of semiconductor quantum dots (QDs) with high optical quality is one key to realizing novel devices in various research disciplines related to modern semiconductor technologies. Despite recent progress in the top-down lithographic fabrication of single semiconductor QD-like emitters [43], bottom-up fabrication methods are commonly applied for the realization of high quality light emitting QDs [7]. The exploitation of high-density QD arrays as an active material in laser diodes [17] and vertical cavity surface emitting lasers (VCSEL) resulted in a new class of devices featuring lower lasing thresholds and improved device performance (such as temperature stability) in comparison to devices with higher dimensional gain [2, 3]. Spintronics and quantum information processing are intensively studied fields in order to provide complementary or entirely novel routes to a future information technology [12, 5]. Single self-assembled quantum dots (QDs) grown in low-density arrays are promising candidates for realizing functional building blocks in these research fields as they allow to confine single charge carriers or spin carriers while providing a solid-state platform capable of electrical injection or manipulation. Extensive research has resulted in the realization of various devices relying on few or single QDs, for instance quantum light emitters such as single photon sources [23, 36], sources of pairs of entangled photons [1, 45], and fewto single-QD lasers [38]. Moreover, many milestone experiments have been performed with In(Ga)As QDs grown on GaAs, for instance the observation of the Purcell effect [10] or reaching the strong QD exciton–photon coupling regime [26], demonstration of the indistinguishability of photons emitted by a QD [29], or complete control of a single spin by ultrafast optical pulses [25].

The work presented in this thesis deals with optical studies of semiconductor quantum dots (QDs) in the InGaAs material system. It is shown that for self-assembled InAs QDs, the interaction with the surrounding GaAs barrier and the InAs wetting layer (WL) in particular, has a very large impact on their optical properties. The ability to control the charge state of individual QDs is demonstrated and attributed to a modulation in the carrier transport dynamics in the WL. After photo-excitation of carriers (electrons and holes) in the barrier, they will migrate in the sample and with a certain probability become captured into a QD. During this migration, the carriers can be affected by exerting them to an external magnetic field or by altering the temperature. An external magnetic field applied perpendicular to the carrier transport direction will lead to a decrease in the carrier drift velocity since their trajectories are bent, and at sufficiently high field strength become circular. In turn, this decreases the probability for the carriers to reach the QD since the probability for the carriers to get trapped in WL localizing potentials increases. An elevated temperature leads to an increased escape rate out of these potentials and again increases the flow of carriers towards the QD. These effects have significantly different strengths for electrons and holes due to the large difference in their respective masses and therefore it constitutes a way to control the supply of charges to the QD. Another effect of the different capture probabilities for electrons and holes into a QD that is explored is the ability to achieve spin polarization of the neutral exciton (X0). It has been concluded frequently in the literature that X0 cannot maintain its spin without application of an external magnetic field, due to the anisotropic electron – hole exchange interaction (AEI). In our studies, we show that at certain excitation conditions, the AEI can be by-passed since an electron is captured faster than a hole into a QD. The result is that the electron will populate the QD solely for a certain time window, before the hole is captured. During this time window and at polarized excitation, which creates spin polarized carriers, the electron can polarize the QD nuclei. In this way, a nuclear magnetic field is built up with a magnitude as high as ~ 1.5 T. This field will stabilize the X0 spin in a similar manner as an external magnetic field would. The build-up time for this nuclear field was determined to be ~ 10 ms and the polarization degree achieved for X0 is ~ 60 %. In contrast to the case of X0, the AEI is naturally cancelled for the negatively charged exciton (X-) and the positively charged exciton (X+) complexes. This is due to the fact that the electron (hole) spin is paired off in case of X- (X+). Accordingly, an even higher polarization degree (~ 73 %) is measured for the positively charged exciton. In a different study, pyramidal QD structures were employed. In contrast to fabrication of self-assembled QDs, the position of QDs can be controlled in these samples as they are grown in inverted pyramids that are etched into a substrate. After sample processing, the result is free-standing AlGaAs pyramids with InGaAs QDs inside. Due to the pyramidal shape of these structures, the light extraction is considerably enhanced which opens up possibilities to study processes un-resolvable in self-assembled QDs. This has allowed studies of Auger-like shake-up processes of holes in single QDs. Normally, after radiative recombination of X+, the QD is populated with a ground state hole. However, at recombination, a fraction of the energy can be transferred to the hole so that it afterwards occupies an excited state instead. This process is detected experimentally as a red-shifted luminescence satellite peak with an intensity on the order of ~ 1/1000 of the main X+ peak intensity. The identification of the satellite peak is based on its intensity correlation with the X+ peak, photoluminescence excitation measurements and on magnetic field measurements.

We demonstrate a straightforward way to obtain single well-isolated quantum dots emitting in the visible part of the spectrum and characterize the optical emission from single quantum dots using this method. Self-assembled InP quantum dots are grown using gas-source molecular-beam epitaxy over a wide range of InP deposition rates, using an ultralow growth rate of about 0.01 atomic monolayers/s, a quantum-dot density of 1 dot/μm2 is realized. The resulting isolated InP quantum dots embedded in an InGaP matrix are individually characterized without the need for lithographical patterning and masks on the substrate. Such low-density quantum dots show excitonic emission at around 670 nm with a linewidth limited by instrument resolution. This system is applicable as a single-photon source for applications such as quantum cryptography.

Quantum light from optically dressed quantum dot states in microcavities

We report on the magneto-optical study of spin polarized energetic fine structures for exciton complex in single CdSe quantum dot (QD) by using micro- photoluminescence (micro-PL) spectroscopy. The zero-field splitting of exciton luminescence peak arisen from the anisotropic exchange interaction of carriers in the QDs was observed. The g-factors for exciton and negatively-charged exciton, i.e. trion in a single QD were determined by fitting the magnetic field dependence of the corresponding PL peaks. By exciting the single QD with circularly polarized light of σ- and σ+ polarization, the spin-up and spin-down trions were selectively generated. The ratio, τ/τsf, of the exciton lifetime and the time constants for the spin-flipping process of trion in a single QD was estimated to be 0.13, which implies a long spin-lifetime in single CdSe QD.

Self-assembled quantum dots have excellent photonic properties. For instance, a single quantum dot is a high-brightness, narrow-linewidth source of single photons. Furthermore, the environment of a single quantum dot can be tailored relatively easily using semiconductor heterostructure and post-growth processing techniques, enabling electrical control of the quantum dot charge and control over the photonic modes with which the quantum dot interacts. A single electron or hole trapped inside a quantum dot has spintronics applications. Although the spin dephasing is rather rapid, a single spin can be manipulated using optical techniques on subnanosecond timescales. Optical experiments are also providing new insights into old issues, such as the central spin problem. This Review provides a snapshot of this active field, with some indications for the future. It covers the basic materials and optical properties of single quantum dots, techniques for initializing, manipulating and reading out single spin qubits, and the mechanisms that limit the electron-spin and hole-spin coherence.

The observation of photoluminescence spectra of self-assembled single InGaAs quantum dots at room temperature was performed under weak excitation conditions using a near-field scanning optical microscope. Operation in illumination-collection mode with a highly sensitive double-tapered optical fibre probe enabled detection of weak photoluminescence signals at room temperature with high efficiency and high spatial resolution. Each single quantum dot was imaged with a spatial resolution of about 250 nm, which corresponded to a quarter of the wavelength of the photoluminescence from quantum dots. The photoluminescence yields of individual quantum dots were widely distributed and were found to decrease with photoluminescence energy. This result serves as a clue to be pursued for better understanding of the thermal excitation of the carrier from confined states in quantum dots.

We demonstrate optical single-electron spin initialization, storage, and readout in a single self-assembled InGaAs quantum dot using a spin memory device. Single-electron spin relaxation is monitored over time scales exceeding $\ensuremath{\ge}30\text{ }\ensuremath{\mu}\text{s}$, defined only by extrinsic experimental parameters such as the optical detection efficiency. The selective generation of a single electron in the dot is performed by resonant optical excitation and subsequent partial exciton ionization; the hole is removed from the dot while the electron remains stored. When subject to a magnetic field applied in Faraday geometry, we show how the spin of the electron can be prepared with a well-defined spin projection relative to the light propagation direction simply by controlling the voltage applied to the gate electrode. The spin is stored then in the dot before being read out using an optical implementation of spin to charge conversion, whereby the spin projection of the electron is mapped onto a more robust variable, the charge state of the dot. After spin to charge conversion, we show how the charge occupancy can be repeatedly and nonperturbatively measured by pumping a luminescence recycling transition. The approach is shown to provide a readout signal ${10}^{4}$ times stronger per spin when compared to previous methods. In combination with spin manipulation using the optical Stark effect or microwaves, our approach provides an ideal basis for probing spin coherence in single self-assembled quantum dots over long-time scales and the development of methods for coherent spin control.

The unique success story of semiconductor physics and technology relies on the ability to highly integrate micro- and nanometer sized functional units on a single chip. Within the last few years single nanostructures, e.g., individual and coupled pairs of quantum dots and single molecules moved more and more into the focus of many research groups to study the exciting physics and to exploit their tremendous potential for device applications. The full advantage of their superior properties can be utilized if a controlled positioning or growth of the nanostructure inside a more complex device structure can be realized, thereby defining precise coupling between the microscopic nanostructure and the macroscopic periphery. single-photon sources coupled quantum-dot gates single quantum-dot tunneling diodes. electroluminescence of single electrically-driven molecules at room temperature controlling quantum-dot emission by integration of semiconductor nanomembranes onto piezoelectric actuators controlled coupling of individual self-assembled quantum dots to plasmonic nanoantennas quantum light emission of two lateral tunnel-coupled (In,Ga)As/GaAs quantum dots controlled by a tunable static electric field realization of vertically stacked and laterally ordered InP and InAs quantum dots for quantum gate applications development of site-controlled SiGe islands on patterned Si(001) and realization of tunneling diodes ultrafast transient reflection spectroscopy of a single self-assembled GaAs quantum dot. We hope that this collection of ideas and results of controlled positioning of single nanostructures stimulates many fascinating experiments and clever applications of quantum objects. We wish to thank all people involved in the research group for their excellent work, the DFG for the financial support and Wiley for the opportunity to publish this volume. On behalf of all applicants being funded by DFG over the years, M. Lippitz and P. Michler Stuttgart, March 2012

Single photon sources are important components for future quantum communication networks. Lights emitting diodes with emission from an embedded self-organized quantum dot offer compact semiconductor sources that can be easily fabricated using standard photolithographic techniques. In this paper, progress towards an electrically driven 1300 nm quantum dot single photon emitter for fiber optic based applications are addressed. Low density longer wavelength emissions were achieved by exploiting the second critical growth threshold for large self-assembled InAs quantum dots on GaAs. The single photon collection efficiency was improved by incorporating the quantum dots between GaAs/AlxGa1-xAs distributed Bragg reflector mirror stacks and laterally confined inside etched micropillars. Resonance of the microcavity mode with the InAs quantum dot emission leads to an enhancement in the collection intensity. Emission from an active quantum dot was collected using a confocal microscope and coupled directly into a single mode fiber. Strong suppression in the multiphoton emission rate was verified by a custom Hanbury-Brown and Twiss interferometer set-up with optical fibers and InGaAs single photon avalanche photodetectors. Integration of electrical contacts with a planar resonant microcavity structure for a single photon light emitting diode is also discussed. Electroluminescence spectra recorded on such a device revealed sharp lines due to the charge recombination in a quantum dot. Correlation measurements on a single quantum dot line showed the suppression of multiphoton emission for an electrically driven source near 1300 nm for the first time.

Single-photon emitters are crucial for the applications in quantum communication, random number generation and quantum information processing. Self-assembled InAs/GaAs quantum dots (QDs) have demonstrated to have singlephoton emission with high extraction efficiency, single-photon purity, and photon indistinguishability. Thus they are considered as the promising deterministic single-photon emitters. To extend the emission wavelength of InAs/GaAs QDs to telecom band, several methods have been developed, such as the strain engineered metamorphic quantum dots, the use of strain reducing layers and the strain-coupled bilayer of QDs. In fact, it is reported on single-photon emissions based on InAs/InP QDs with an emission wavelength of 1.55μm, but it is difficult to combine such QDs with a high-quality distributed Bragg reflector (DBR) cavity because the refractive index difference between InP and InGaAsP is too small to obtain a DBR cavity with high quality factor. Here we investigate 1.3μm single-photon emissions based on selfassembled strain-coupled bilayer of InAs QDs embedded in micropillar cavities. The studied InAs/GaAs self-assembled QDs are grown by molecular beam epitaxy on a semi-insulating (100) GaAs substrate through strain-coupled bilayer of InAs QDs, where the active QDs are formed on the seed QDs capped with an InGaAs layer, and two-layer QDs are vertically coupled with each other. In such a structure the emission wavelength of QDs can be extended to 1.3μm. The QDs with a low density of about 6×10<sup>8</sup> cm<sup>-2</sup> are embedded inside a planar 1-<sup>λ</sup> GaAs microcavity sandwiched between 20 and 8 pairs of Al<sup>0.9</sup>Ga<sup>0.1</sup>As/GaAs as the bottom and top mirror of a DBR planar cavity, respectively. Then the QD samples are etched into 3μm diameter micropillar by photolithography and dry etching. The measured quality factor of studied pillar cavity has a typical value of approximately 300. Photoluminescence (PL) spectra of QDs at a temperature of 5 K are examined by using a micro-photoluminescence setup equipped with a 300 mm monochromator and an InGaAs linear photodiode array detector. A diode laser with a continuous wave or a pulsed excitation repetition rate of 80 MHz and an excitation wavelength of 640 nm is used to excite QDs through an near-infrared objective (<sup>NA</sup> 0.5), and the PL emission is collected by the same objective. The time-resolved PL of the QDs is obtained by a time-correlated single photon counting. The second-order correlation function is checked by a Hanbury-Brown and Twiss setup through using ID 230 infrared single-photon detectors.<br/>In summary, we find that the 1.3μm QD exciton lifetime at 5 K is measured to be approximately 1 ns, which has the same value as the 920 nm QD exciton lifetime. The second-order correlation function is measured to be 0.015, showing a good characteristic of 1.3μm single photon emission. To measure the coherence time, i.e., to perform highresolution linewidth measurements, of the QDs emitted at the wavelength of 920 and 1300 nm, we insert a Michelson interferometer in front of the spectrometer. The obtained coherence time for 1.3μm QDs is 22 ps, corresponding to a linewidth of approximately 30μeV. Whereas, the coherence time is 216 ps for 920 nm QDs, corresponding to a linewidth of approximately 3μeV. Furthermore, both emission spectral lineshapes are different. The former is of Gaussian-like type, while the latter is of Lorentzian type.

Single self-assembled CdSe quantum dots (QDs) are shown to exhibit random fluctuations of the ground state emission energy as well as a spontaneous on/off blinking of the luminescence. A comparison of samples with different densities of extendend crystal defects indicates that Frenkel stacking faults are involved in the mechanism of these phenomena. We demonstrate that single emission lines originating from the same QD show a strong correlation of their transient energy shifts as well as simultaneous blinking.

A system of quantum dots based on Al x In1−xAs/Al y Ga1−yAs solid solutions is investigated. The use of Al x In1−xAs wide-gap solid solutions as the basis of quantum dots substantially extends the spectral emission range to the short-wavelength region, including the wavelength region near 770 nm, which is of interest for the development of aerospace systems of quantum cryptography. The optical characteristics of Al x In1−xAs single quantum dots grown by the Stranski–Krastanov mechanism were studied by cryogenic microphotoluminescence. The statistics of the emission of single quantum dot excitons was studied using a Hanbury Brown–Twiss interferometer. The pair photon correlation function indicates the sub-Poissonian nature of the emission statistics, which directly confirms the possibility of developing single-photon emitters based on Al x In1−xAs quantum dots. The fine structure of quantum dot exciton states was investigated at wavelengths near 770 nm. The splitting of the exciton states is found to be similar to the natural width of exciton lines, which is of great interest for the development of entangled photon pair emitters based on Al x In1−xAs quantum dots.

We demonstrate full charge control, narrow optical linewidths, and optical spin pumping on single self-assembled InGaAs quantum dots embedded in a $162.5\,\text{nm}$ thin diode structure. The quantum dots are just $88\,\text{nm}$ from the top GaAs surface. We design and realize a p-i-n-i-n diode that allows single-electron charging of the quantum dots at close-to-zero applied bias. In operation, the current flow through the device is extremely small resulting in low noise. In resonance fluorescence, we measure optical linewidths below $2\,\mu\text{eV}$, just a factor of two above the transform limit. Clear optical spin pumping is observed in a magnetic field of $0.5\,\text{T}$ in the Faraday geometry. We present this design as ideal for securing the advantages of self-assembled quantum dots -- highly coherent single photon generation, ultra-fast optical spin manipulation -- in the thin diodes required in quantum nano-photonics and nano-phononics applications.

Colloidal semiconductor quantum dots (QDs) have strong light absorption, continuously adjustable narrowband emission, and high photoluminescence quantum yields, thereby making them promising materials for light-emitting diodes, solar cells, detectors, and lasers. Single-QD photoluminescence spectroscopy can remove the ensemble average to reveal the structure information and exciton dynamics of QD materials at a single-particle level. The study of single-QD spectroscopy can provide guidelines for rationally designing the QDs and giving the mechanism basis for QD-based applications. We can also carry out the research of the interaction between light and single QDs on a nanoscale, and prepare QD-based single-photon sources and entangled photon sources. Here, we review the recent research progress of single-QD photoluminescence spectroscopy and exciton dynamics, mainly including photoluminescence blinking dynamics, and exciton and multi-exciton dynamics of single colloidal CdSe-based QDs and perovskite QDs. Finally, we briefly discuss the possible future development trends of single-QD spectroscopy and exciton dynamics.