The coupling between single photon emitters and integrated photonic circuits is an emerging topic relevant for quantum information science and other nanophotonic applications. We investigate the coupling between a hybrid system of colloidal quantum dots and propagating gap modes of a silicon nitride waveguide system. We furthermore explore the density of optical states of the system by using a scanning probe technique and find that the quantum dots couple significantly to the photonic circuit. Our results indicate that a scalable slot-waveguide might serve as a promising platform in future developments of integrated quantum circuitry.
Colloidal quantum dots have garnered active research interest as quantum emitters due to their robust synthesis process and straightforward integration with nanophotonic platforms. However, obtaining indistinguishable photons from the colloidal quantum dots at room temperature is fundamentally challenging because they suffer from an extremely large dephasing rate. Here we propose an experimentally feasible method of obtaining indistinguishable single photons from an incoherently pumped solution-processed colloidal quantum dot coupled to a system of nanocavities. We show that by coupling a coll…
We investigate coherent single surface-plasmon transport in a metal nanowire strongly coupled to two colloidal quantum dots. Analytical expressions are obtained for the transmission and reflection coefficients by solving the corresponding eigenvalue equation. Remote entanglement of the wave functions of the two quantum dots can be created if the inter-dot distance is equal to a multiple half-wavelength of the surface plasmon. Furthermore, by applying classical laser pulses to the quantum dots, the entangled states can be stored in metastable states which are decoupled from the surface plasmons…
The lattice mismatch strain field of core/multishell structures with spherical symmetry is modeled by a linear continuum elasticity approach. The effect of the strain on the energy structure and linear optical absorption in large core/shell/shell spherical semiconductor quantum dots is analyzed. Localization of the photoexcited carriers induced by coating is found to play an important role in explaining the optical stability of large CdSe/CdS/ZnS and ZnTe/ZnSe/ZnS quantum dots.
We present measurements of the beta-factor, describing the coupling efficiency of light emitted by single InAs/GaAs semiconductor quantum dots into a photonic crystal waveguide mode. The beta-factor is evaluated by means of time-resolved frequency-dependent photoluminescence spectroscopy. The emission wavelength of single quantum dots is temperature tuned across the band edge of a photonic crystal waveguide and the spontaneous emission rate is recorded. Decay rates up to 5.7 ns^(-1), corresponding to a Purcell factor of 5.2, are measured and beta-factors up to 85% are extracted. These results …
Future scalable photonic quantum information processing relies on the ability of integrating multiple interacting quantum emitters into a single chip. Quantum dots provide ideal on-chip quantum light sources. However, achieving quantum interaction between multiple quantum dots on-a-chip is a challenging task due to the randomness in their frequency and position, requiring local tuning technique and long-range quantum interaction. Here, we demonstrate quantum interactions between distant two quantum dots on a nanophotonic waveguide. We achieve a photon-mediated long-range interaction by integra…
Interfacing single emitters and photonic nanostructures enables modifying their emission properties, such as enhancing individual decay rates or controlling the emission direction. To achieve full control, the single emitter must be positioned in the nanostructures deterministically. Here, we use spectroscopy to gain spectral and spatial information about individual quantum dots in order to position each emitter in a pre-determined location in a unit cell of a photonic-crystal waveguide. Depending on the spatial and spectral positioning within the structured nanophotonic mode, we observe that …
The authors investigate the spontaneous emission dynamics of self-assembled InGaAs quantum dots embedded in GaAs photonic crystal waveguides. For an ensemble of dots coupled to guided modes in the waveguide we report spatially, spectrally, and time-resolved photoluminescence measurements, detecting normal to the plane of the photonic crystal. For quantum dots emitting in resonance with the waveguide mode, a ~21x enhancement of photoluminescence intensity is observed as compared to dots in the unprocessed region of the wafer. This enhancement can be traced back to the Purcell enhanced emission …
Coupling to phonon modes is a primary mechanism of excitonic dephasing and energy loss in semiconductors. However, low-energy phonons in colloidal quantum dots and their coupling to excitons are poorly understood, since their experimental signatures are weak and usually obscured by unavoidable inhomogeneous broadening of colloidal dot ensembles. We use multi-dimensional coherent spectroscopy at cryogenic temperatures to extract the homogeneous nonlinear optical response of excitons in a CdSe/CdZnS core/shell colloidal quantum dot ensemble. Comparison to simulation provides evidence that the ob…
Switching of a single plasmon interacting with equally spaced quantum dots coupled to one-dimensional surface plasmonic waveguide is investigated theoretically via the real-space approach. We showed that the transmission and reflection of a single plasmon can be switched on or off by dynamically tuning and changing the number of the equal transition frequencies of the quantum dots.
The influence of the tip-substrate bias induced electrical field in a scanning tunneling spectroscopy experiment on colloidal InAs nanocrystals has been studied. Calculating the Stark induced splitting of the degenerate 1P_e state perturbatively within a particle-in-a-sphere model, revealed a possible explanation of recently published experimental wave function mapping data by Millo et al. (Ref. 1).
Quantum dots play a promising role in the development of novel optical and biosensing devices. In this study, we investigated steady-state and time-dependent luminescence properties of InGaP/ZnS core/shell colloidal quantum dots in a solution phase at room temperature. The steady state experiments exhibited an emission maximum at 650 nm with full width at half maximum of ~ 85 nm, and strong first-excitonic absorption peak at 600 nm. The time-resolved luminescence measurements depicted a bi-exponential decay profile with lifetimes of τ1\sim 47 ns and τ 2\sim 142 ns at the emission maximum. Addi…
We report on the site-selected growth of bright single InAsP quantum dots embedded within InP photonic nanowire waveguides emitting at telecom wavelengths. We demonstrate a dramatic dependence of the emission rate on both the emission wavelength and the nanowire diameter. With an appropriately designed waveguide, tailored to the emission wavelength of the dot, an increase in count rate by nearly two orders of magnitude (0.4kcps to 35kcps) is obtained for quantum dots emitting in the telecom O-band. Using emission-wavelength-optimised waveguides, we demonstrate bright, narrow linewidth emission…
We study optical forces acting upon semiconductor quantum dots and the force driven motion of the dots in a colloid. In the spectral range of exciton transitions in uantum dots, when the photon energy is close to the exciton energy, the polarizability of the dots is drastically increased. It leads to a resonant increase of both the gradient and the scattering contributions to the optical force, which enables the efficient manipulation with the dots. We reveal that the optical grating of the colloid leads to the formation of a fluid photonic crystal with spatially periodic circulating fluxes an…
Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single quantum dot LEDs. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than twelve electrons and one hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot…
Chemically prepared colloidal semiconductor quantum dots have long been proposed as scalable and color-tunable single emitters in quantum optics, but they have typically suffered from prohibitively incoherent emission. We now demonstrate that individual colloidal lead halide perovskite quantum dots (PQDs) display highly efficient single photon emission with optical coherence times as long as 80 ps, an appreciable fraction of their 210 ps radiative lifetimes. These measurements suggest that PQDs should be explored as building blocks in sources of indistinguishable single photons and entangled p…
We report a valley photonic crystal (VPhC) waveguide in a GaAs slab with InAs quantum dots (QDs) as an internal light source exploited for experimental characterization of the waveguide. A topological interface state formed at the interface between two topologically-distinct VPhCs is used as the waveguide mode. We demonstrate robust propagation for near-infrared light emitted from the QDs even under the presence of sharp bends as a consequence of the topological protection of the guided mode. Our work will be of importance for developing robust photonic integrated circuits with small footprint…
Carrier-dopant exchange interactions in Mn-doped PbS colloidal quantum dots were studied by circularly polarized magneto-photoluminescence. Mn substitutional doping leads to paramagnetic behavior down to 5 K. While undoped quantum dots show negative circular polarization, Mn doping changes its sign to positive. A circular polarization value of 40% was achieved at T=7 K and B=7 tesla. The results are interpreted in terms of Zeeman splitting of the band edge states in the presence of carrier-dopant exchange interactions that are qualitatively different from the s,p-d exchange interactions in II-…
Luminescence spectroscopy experiments were realized for single colloidal quantum dots CdSe/ZnS in a broad temperature range above room temperature in a nitrogen atmosphere. Broadening and shifts of spectra due to the temperature change as well as due to spectral diffusion processes were detected and analyzed. A linear correlation between the positions of maxima and the squared linewidths of the spectra was found. This dependence was explained by a model which takes into account the slow variation of the electron-phonon coupling strength.
Multiply-excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room temperature single-particle spectroscopy of their emission has so far proved elusive due to the temporal and spectral overlap with emission from the singly-excited and charged states. Here we introduce biexciton heralded spectroscopy, enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton-exciton emission cascades an…
Spontaneous emission from excitonic transitions in InAs/GaAs quantum dots embedded in photonic crystal waveguides at 5K into non-guided and guided modes is determined by direct hyperspectral imaging. This enables measurement of the absolute coupling efficiency into the guided modes, the beta-factor, directly, without assumptions on decay rates used previously. Notably, we found beta-factors above 90% over a wide spectral range of 40meV in the fast light regime, reaching a maximum of (99 $\pm$ 1)%. We measure the directional emission of the circularly polarized transitions in a magnetic field i…
Chiral light-matter interaction between photonic nanostructures with quantum emitters shows great potential to implement spin-photon interfaces for quantum information processing. Position-dependent spin momentum locking of the quantum emitter is important for these chiral coupled nanostructures. Here, we report the position-dependent chiral coupling between quantum dots (QDs) and cross waveguides both numerically and experimentally. Four quantum dots distributed at different positions in the cross section are selected to characterize the chiral properties of the device. Directional emission i…
Multiple exciton generation is a process in which more than one electron hole pair is generated per absorbed photon. It allows us to increase the efficiency of solar energy harvesting. Experimental studies have shown the multiple exciton generation yield of 1.2 in isolated colloidal quantum dots. However real photoelectric devices require the extraction of electron hole pairs to electric contacts. We provide a systematic study of the corresponding quantum coherent processes including extraction and injection and show that a proper design of extraction and injection rates enhances the yield sig…
Single-photon emitters integrated into quantum optical circuits will enable new, miniaturized quantum optical devices. Here, we numerically investigate semiconductor quantum dots embedded to low refractive index contrast waveguides. We discuss a model to compute the coupling efficiency of the emitted light field to the fundamental propagation mode of the waveguide, and we optimize the waveguide dimensional parameters for maximum coupling efficiency. Further, we show that for a laterally cropped waveguide the interplay of Purcell-enhancement and optimized field profile can enhance the coupling …
Colloidal core/shell InP/ZnSe quantum dots (QDs), recently produced using an improved synthesis method, have a great potential in life-science applications as well as in integrated quantum photonics and quantum information processing as single-photon emitters. Single-particle spectroscopy of 10-nm QDs with 3.2-nm cores reveals strong photon antibunching attributed to fast (70-ps) Auger recombination of multiple excitons. The QDs exhibit very good photostability under strong optical excitation. We demonstrate that the antibunching is preserved when the QDs are excited above the saturation inten…
We report a study of the quantum dot emission in short photonic crystal waveguides. We observe that the quantum dot photoluminescence intensity and decay rate are strongly enhanced when the emission energy is in resonance with Fabry-Perot cavity modes in the slow-light regime of the dispersion curve. The experimental results are in agreement with previous theoretical predictions and further supported by three-dimensional finite element simulation. Our results show that the combination of slow group velocity and Fabry-Perot cavity resonance provides an avenue to efficiently channel photons from…
We explore the dynamics and directionality of spontaneous emission from self-assembled In(Ga)As quantum dots into TE-polarised guided modes in GaAs two-dimensional photonic crystal waveguides. The local group velocity of the guided waveguide mode is probed, with values as low as $\sim 1.5\%\times c$ measured close to the slow-light band edge. By performing complementary continuous wave and time-resolved measurements with detection along, and perpendicular to the waveguide axis we probe the fraction of emission into the waveguide mode ($β$-factor). For dots randomly positioned within the unit c…
The capability to embed self-assembled quantum dots (QDs) at predefined positions in nanophotonic structures is key to the development of complex quantum photonic architectures. Here, we demonstrate that QDs can be deterministically positioned in nanophotonic waveguides by pre-locating QDs relative to a global reference frame using micro-photoluminescence ($μ$PL) spectroscopy. After nanofabrication, $μ$PL images reveal misalignments between the central axis of the waveguide and the embedded QD of only $(9\pm46$) nm and $(1\pm33$) nm, for QDs embedded in undoped and doped membranes, respectivel…
We use an optical fiber taper waveguide to probe PbS quantum dots (QDs) dried on Si photonic crystal cavities near 1.55 $μ$m. We demonstrate that a low density ($\lesssim 100 μ$m$^{-2}$) of QDs does not significantly degrade cavity quality factors as high as $\approx3\times10^4$. We also show that the tapered fiber can be used to excite the QDs and collect the subsequent cavity-filtered photoluminescence, and present measurements of reversible photodarkening and QD saturation. This method represents an important step towards spectroscopy of single colloidal QDs in the telecommunications band.
The study of charge and spin transport through semiconductor quantum dots is experiencing a renaissance due to recent advances in nano-fabrication and the realization of quantum dots as candidates for quantum computing. In this work, we combine atomistic electronic structure calculations with quantum master equation methods to study the transport of electrons and holes through strongly confined quantum dots coupled to two leads with a voltage bias. We find that a competition between the energy spacing between the two lowest quasiparticle energy levels and the strength of the exchange interacti…
Many photonic quantum information processing applications would benefit from a high brightness, fiber-coupled source of triggered single photons. Here, we present a fiber-coupled photonic-crystal waveguide single-photon source relying on evanescent coupling of the light field from a tapered out-coupler to an optical fiber. A two-step approach is taken where the performance of the tapered out-coupler is recorded first on an independent device containing an on-chip reflector. Reflection measurements establish that the chip-to-fiber coupling efficiency exceeds 80 %. The detailed characterization …
We study the effect of Coulomb correlation on the emission properties of the ground state exciton in zincblende CdSe/ZnS core-shell and in wurtzite ZnO quantum dots. We validate our theory model by comparing results of computed exciton energies of CdSe/ZnS quantum dots to photoluminescence and scanning near-field optical microscopy measurements. We use that to estimate the diameter of the quantum dots using a simple model based on infinitely deep quantum well and compare the results with the statistics of the atomic force microscopy scans of CdSe/ZnS dots, obtaining excellent agreement. Therea…
Luminescence properties of colloidal quantum dots have found applications in imaging, light-sources, and displays. Despite wide interest, several experimental observations from these quantum dots, such as the short lifetime on the scale of microseconds and a zero-longitudinal optical phonon line in low-temperature photoluminescence spectrum, remain unexplained by existing models. Here we propose a model including the effect of solid-state environment on luminescence by capturing coherent and incoherent interactions of band-edge exciton with phonon modes. Our model predicts the formation of dre…
The excitonic finestructure of colloidal quantum dots (CQDs) is comprised of a manifold of transitions, of which only the lowest are populated and contribute to photoluminescence. This leads to a Stokes shift in emission relative to absorption. Here we show experimentally that the Stokes shift in Pb and Cd-based chalcogenide CQDs is correlated with the degree of surface passivation, and develop a model that explains how coupling to the surface affects the core electronic states. Dark and bright transitions can reorder and split, increasing the Stokes shift even without the formation of deep tr…
Using a polaron master equation approach we investigate the resonance fluorescence spectra from coherently driven quantum dots (QDs) coupled to an acoustic phonon bath and a photonic crystal waveguide with a rich local density of photon states (LDOS). Resonance fluorescence spectra from QDs in semiconductor crystals are known to show strong signatures of electron-phonon interactions, but when coupled to a structured photonic reservoir, the QD emission properties are also determined by the frequency dependence of the LDOS of the photon reservoir. Here, we investigate the simultaneous role of co…
Polariton emission from optical cavities integrated with various luminophores has been extensively studied recently due to the wide variety of possible applications in photonics, particularly promising in terms of fabrication of low-threshold sources of coherent emission. Tuneable microcavities allow extensive investigation of the photophysical properties of matter placed inside the cavity by deterministically changing the coupling strength and controllable switching from weak to strong and ultra-strong coupling regimes. Here we demonstrate room temperature strong coupling of exciton transitio…
We report measurements of low-frequency electronic noise in ordered superlattice, weakly-ordered and random-packed thin films of 6.5 nm PbSe quantum dots prepared using several different ligand chemistries. For all samples, the normalized noise spectral density of the dark current revealed a Lorentzian component, reminiscent of the generation-recombination noise, superimposed on the 1/f background (f is the frequency). An activation energy of 0.3 eV was extracted from the temperature dependence of the noise spectra. The noise level in the ordered films was lower than that in the weakly-ordered…
Coherent spin dynamics in colloidal CdSe quantum dots (QDs) typically show two spin components with different Larmor frequencies, whose origin is an open question. We exploit the photocharging approach to identify their origin and find that surface states play a key role in the appearance of the spin signals. By controlling the photocharging with electron or hole acceptors, we show that the specific spin component can be enhanced by the choice of acceptor type. In core/shell CdSe/ZnS QDs, the spin signals are significantly weaker. Our results exclude the neutral exciton as the spin origin and …
We exploit hyperfine interactions in a single Mn-ion confined in a quantum dot (QD) to create a qudit, i.e. a multi-level quantum-bit system, with well defined, addressable and robust set of spin states for the realization of universal quantum gates. We generate and probe an arbitrary superposition of states between selected hyperfine energy level pairs by using electron double resonance detected nuclear magnetic resonance (EDNMR). This enables the observation of Rabi oscillations and the experimental realization of NOT and SWAP universal quantum gates that are robust against decoherence. Our …
We report on a temporal evolution of photoluminescence (PL) spectroscopy of CuInS$_{2}$/ZnS colloidal quantum dots (QDs) by drop-casting on SiO$_{2}$/Si substrates and high quality factor microdisks (MDs) under different atmospheric conditions. Fast PL decay, peak blueshift and linewidth broadening due to photooxidation have been observed at low excitation power. With further increasing of the excitation power, the PL peak position shows a redshift and linewidth becomes narrow, which is ascribed to the enhanced F$\ddot{o}$rster resonant energy transfer between different QDs by photoinduced agg…
Colloidal quantum dots are robust, efficient, and tunable emitters now used in lighting, displays, and lasers. Consequently, when the spaser, a laser-like source of surface plasmons, was first proposed, quantum dots were specified as the ideal plasmonic gain medium. Subsequent spaser designs, however, have required a single material to simultaneously provide gain and define the plasmonic cavity, an approach ill-suited to quantum dots and other colloidal nanomaterials. Here we develop a more open architecture that decouples the gain medium from the cavity, leading to a versatile class of quantu…
We theoretically investigate the magnitude and range of the photon-mediated interaction between two quantum dots embedded in a photonic crystal waveguide, including fabrication disorder both in the crystal and in the dot positioning. We find that disorder-induced light localization has a drastic effect on the excitation transfer rate - as compared to an ideal structure - and that this rate varies widely among different disorder configurations. Nevertheless, we also find that significant rates of 50 micro-eV at a range of 10 micro-meters can be achieved in realistic systems.
We present a new physical model resolving a long-standing mystery of the power-law distributions of the blinking times in single colloidal quantum dot fluorescence. The model considers the non-radiative relaxation of the exciton through multiple recombination centers. Each center is allowed to switch between two quasi-stationary states. We point out that the conventional threshold analysis method used to extract the exponents of the distributions for the on-times and off-times has a serious flaw: The qualitative properties of the distributions strongly depend on the threshold value chosen for …
The dephasing time of the lowest bright exciton in CdSe/ZnS wurtzite quantum dots is measured from 5 K to 170 K and compared with density dynamics within the exciton fine structure using a sensitive three-beam four-wave-mixing technique unaffected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing of 109 ps at 5 K, much faster than the ~10 ns exciton radiative lifetime. The zero-phonon line dephasing is explained by phonon-assisted spin-flip from the lowest bright state to dark exciton states. This is…
CdSe quantum dots (QDs) with different organic linker molecules are attached to ZnO nanowires (NWs) to study the luminescence dynamics and the electron tunneling from the QDs to the nanowires in time-resolved photoluminescence (PL) and photoconductivity measurements. The PL transients of the QD luminescence indicate two different recombination channels: the direct recombination inside the QD core and the recombination via QD surface defect states. After linking the QDs to the ZnO NW surface, photo-induced electron tunneling from an excited state of the QD into the conduction band of the nanowi…
Doping a semiconductor quantum dot with just a single impurity atom can completely transform its physical properties. Here, we report and analyze the magnetic circular dichroism (MCD) spectra of colloidal CdSe quantum dot samples containing on average fewer than one Mn2+ per quantum dot. Even at this sub-single-dopant level, the low-temperature low-field data are dominated by impurity-induced Zeeman splittings caused by dopant-carrier sp-d exchange. Unlike in more heavily doped quantum dots, however, the MCD intensity at the first CdSe exciton shows a field-induced sign flip as the field stren…
The quest for an integrated quantum optics platform has motivated the field of semiconductor quantum dot research for two decades. Demonstrations of quantum light sources, single photon switches, transistors, and spin-photon interfaces have become very advanced. Yet the fundamental problem that every quantum dot is different prevents integration and scaling beyond a few quantum dots. Here, we address this challenge by patterning strain via local phase transitions to selectively tune individual quantum dots that are embedded in a photonic architecture. The patterning is implemented with in oper…
We preform large-scale \emph{ab initio} density functional theory calculations to study the lattice strain and the vibrational properties of colloidal semiconductor core-shell nanoclusters with up to one thousand atoms (radii up to 15.6~Å). For all the group IV, III-V and II-VI semiconductors studied, we find that the atom positions of the shell atoms, seem unaffected by the core material. In particular, for group IV core-shell clusters the shell material remains unstrained, while the core adapts to the large lattice mismatch (compressive or tensile strain). For InAs-InP and CdSe-CdS, both the…
Doping of bulk semiconductors has revealed widespread success in optoelectronic applications. In the past few decades, substantial effort has been engaged for doping at the nanoscale. Recently, doped zero-dimensional quantum dots made of semiconductor nanocrystals have been demonstrated to be promising materials for luminescent solar concentrators (LSCs) as they can be engineered for providing Stokes-shifted tunable emission in the solar spectrum. However, existing doped colloidal quantum dots suffer from moderately low quantum efficiency and intrinsically small absorption cross-section, which…
We present optical investigations of hybrid plasmonic nanosystems consisting of lithographically defined plasmonic Au-waveguides or beamsplitters on GaAs substrates coupled to proximal self-assembled InGaAs quantum dots. We designed a sample structure that enabled us to precisely tune the distance between quantum dots and the sample surface during nano-fabrication and demonstrated that non-radiative processes do not play a major role for separations down to $\sim 10 nm$. A polarized laser beam focused on one end of the plasmonic nanostructure generates propagating surface plasmon polaritons th…
