Pair Of Quantum Dots Research Articles

Unusual Fluorescent Properties of Stilbene Units and CdZnS/ZnS Quantum Dots Nanocomposites: White‐Light Emission in Solution versus Light‐Harvesting in Films

Nanocomposites with organic–inorganic properties represent a new field of basic research and offer prospects for many novel applications in extremely diverse fields, due to their remarkable emerging new properties and multifunctional nature. However, controllable manipulation of their fluorescent properties in different phases is still challenging, which seriously limits the related applications of nanocomposites. In this work, a convenient protocol to fabricate organic–inorganic nanocomposites composed of stilbene chromophores and CdZnS/ZnS quantum dots (QDs) pairs, with controllable fluorescent properties is presented. It is found that stable white‐light emission can be achieved only in solution phase, with negligible energy transfer or reabsorption between chromophores and QDs pairs. By contrast, when the nanocomposites are deposited as blended films, they cannot give rise to white‐light emission, no matter what donor/acceptor volume ratios are used. However, the blended films can exhibit near‐unity efficiency (94%) of Förster resonance energy transfer from QDs to chromophores. The underlying physical mechanisms are revealed through comprehensive steady‐state and time‐resolved spectroscopic analysis. This work suggests that the CdZnS/ZnS QDs/stilbene nanocomposites can be directly used for fluorescence sensors and probes in biological system as well as fundamental investigation of light‐harvesting, and also sheds light on developing other new materials for artificial photosynthesis and optoelectronics. image

Entanglement of two, three, or four plasmonically coupled quantum dots

We model the quantum dynamics of two, three, or four quantum dots (QDs) in proximity to a plasmonic system such as a metal nanoparticle or an array of metal nanoparticles. For all systems, an initial state with only one QD in its excited state evolves spontaneously into a state with entanglement between all pairs of QDs. The entanglement arises from the couplings of the QDs to the dissipative, plasmonic environment. Moreover, we predict that similarly entangled states can be generated in systems with appropriate geometries, starting in their ground states, by exciting the entire system with a single, ultrafast laser pulse. By using a series of repeated pulses, the system can also be prepared in an entangled state at an arbitrary time.

Manipulating the Phonon Bottleneck in Graphene Quantum Dots: Phonon-Induced Carrier Relaxation within the Linear Response Theory

Slow phonon-induced relaxation of excited carriers in quantum dots is crucial for next-generation photovoltaics; however, the phenomenon has been difficult to realize experimentally due to defects and ligands that introduce strongly coupled states. Graphene quantum dots are an intriguing system to avoid these problems due to chemical synthesis methods that minimize defects. Modeling electron–phonon interactions using a state-of-the-art method combining the reduced density matrix formalism with linear response theory, we find that 100 ps lifetimes are possible for electron–hole pairs in graphene quantum dots due to large transition energies and weak coupling to excited states near the band edge. By calculating carrier relaxation rates in dots with and without ligands, with armchair or zigzag edges, and of increasing size, we show how excited state lifetimes are sensitive to structural changes. In contrast to other types of quantum dots in which ligands can increase phonon-induced relaxation, carbon ligands...

Efficient Separation of Electron–Hole Pairs in Graphene Quantum Dots by TiO2 Heterojunctions for Dye Degradation

Water-soluble, single-crystalline, and amine-functionalized graphene quantum dots (GQDs) with absorption edge at ∼490 nm were synthesized by a molecular fusion method, and stably deposited onto anatase TiO2 nanoparticles under hydrothermal conditions. The effective incorporation of the GQDs extends the light absorption of the TiO2 nanoparticles from UV to a wide visible region. Moreover, amine-functionalized GQD–TiO2 heterojunctions can absorb more O2 than pure TiO2, which can generate more ·O2 species for MO degradation. Accordingly, the heterojunctions exhibit much higher photocatalytic performance for degrading methyl orange (MO) under visible-light irradiation than TiO2 alone. At optimum GQD content (1.0 wt %), an apparent MO decomposition rate constant is 15 times higher than that of TiO2 alone, and photocurrent intensity in response to visible-light excitation increases by 9 times. Compared with conventional sensitization by toxic, photounstable quantum dots such as CdSe QDs, the sensitization by en...

Two-photon absorption by a quantum dot pair

The biexciton absorption spectrum of a pair of InAs/GaAs quantum dots is being studied by photoluminescence excitation spectroscopy. An absorption resonance with the characteristics of an instantaneous two-photon process reveals a coherent interdot two-photon transition. Pauli-selective tunneling is being used to demonstrate the transduction of the two-photon coherence into a nonlocal spin singlet state. The two-photon transition can be tuned spectrally by electric field, enabling amplification of its transition strength.

Electronic Coupling in Nanoscale InAs/GaAs Quantum Dot Pairs Separated by a Thin Ga(Al)As Spacer.

The electronic coupling in vertically aligned InAs/GaAs quantum dot (QD) pairs is investigated by photoluminescence (PL) measurements. A thin Al0.5Ga0.5As barrier greatly changes the energy transfer process and the optical performance of the QD pairs. As a result, the QD PL intensity ratio shows different dependence on the intensity and wavelength of the excitation laser. Time-resolved PL measurements give a carrier tunneling time of 380 ps from the seed layer QDs to the top layer QDs while it elongates to 780 ps after inserting the thin Al0.5Ga0.5As barrier. These results provide useful information for fabrication and investigation of artificial QD molecules for implementing quantum computation applications.

Entanglement dynamics and Mollow nonuplets between two coupled quantum dots in a nanowire photonic-crystal system

We introduce a nanowire-based photonic crystal waveguide system capable of controllably mediating the photon coupling between two quantum dots which are macroscopically separated. Using a rigorous Green-function-based master equation approach, our two-dot system is shown to provide a wide range of interesting quantum regimes. In particular, we demonstrate the formation of long-lived entangled states and study the resonance fluorescence spectrum which contains clear signatures of the coupled quantum dot pair. Depending upon the operating frequency, one can obtain a modified Mollow triplet spectrum or a Mollow nonuplet, namely a spectrum with nine spectral peaks. These multiple peaks are explained in the context of photon-exchange-mediated dressed states. Results are robust with respect to scattering loss, and spatial filtering via propagation allows for each quantum dot's emission to be observed individually.

Chaotic oscillation and random-number generation based on nanoscale optical-energy transfer.

By using nanoscale energy-transfer dynamics and density matrix formalism, we demonstrate theoretically and numerically that chaotic oscillation and random-number generation occur in a nanoscale system. The physical system consists of a pair of quantum dots (QDs), with one QD smaller than the other, between which energy transfers via optical near-field interactions. When the system is pumped by continuous-wave radiation and incorporates a timing delay between two energy transfers within the system, it emits optical pulses. We refer to such QD pairs as nano-optical pulsers (NOPs). Irradiating an NOP with external periodic optical pulses causes the oscillating frequency of the NOP to synchronize with the external stimulus. We find that chaotic oscillation occurs in the NOP population when they are connected by an external time delay. Moreover, by evaluating the time-domain signals by statistical-test suites, we confirm that the signals are sufficiently random to qualify the system as a random-number generator (RNG). This study reveals that even relatively simple nanodevices that interact locally with each other through optical energy transfer at scales far below the wavelength of irradiating light can exhibit complex oscillatory dynamics. These findings are significant for applications such as ultrasmall RNGs.

Single photoelectron detection after selective excitation of electron heavy-hole and electron light-hole pairs in double quantum dots

We demonstrate the real-time detection of single photogenerated electrons in two different lateral double quantum dots made in AlGaAs/GaAs/AlGaAs quantum wells having a thin or a thick AlGaAs barrier layer. The observed incident laser power and photon energy dependences of the photoelectron detection efficiency both indicate that the trapped photoelectrons are, for the thin barrier sample, predominantly photogenerated in the buffer layer followed by tunneling into one of the two dots, whereas for the thick barrier sample they are directly photogenerated in the well. For the latter, single photoelectron detection after selective excitation of the heavy and light hole state in the dot is well resolved. This ensures the applicability of our quantum well-based quantum dot systems for the coherent transfer from single photon polarization to single electron spin states.

Resolving single plasmons generated by multiquantum-emitters on a silver nanowire.

Surface plasmons, the collective oscillations of electrons at metal surface, provide the ability to enhance the weak interaction between individual quantum emitters and photons for quantum information applications. The generation of single plasmons by coupling silver nanowire with single quantum emitters opens the prospects of using quantum optical techniques to control single surface plasmons and designing novel quantum plasmonic devices. However, the real applications will deal with multiple plasmons generated from multiple quantum emitters. Here we report the first experimental demonstration of resolving single plasmons generated by a pair of quantum dots (QDs) on a silver nanowire waveguide. The accurate positions of the two QDs with separation ranging from micrometers to 200 nm within the diffraction limit are determined by using super-resolution imaging method. The efficiency of plasmon generation due to the exciton-plasmon coupling is obtained for each QD. Our research takes a crucial step toward the experimental study of coupled systems of multiple quantum emitters and plasmonic waveguides and would shed new light on the study of light-matter interactions for potential quantum optics and quantum information applications.

Vertically stacked quantum dot pairs fabricated by nanohole filling

Strain-free, vertically coupled GaAs quantum dots (QDs) with an ultra-low density below are fabricated by filling of self-assembled nanoholes with a GaAs/AlGaAs/GaAs layer sequence. The sizes of the two QDs, forming a QD pair (QDP), as well as the AlGaAs tunnel-barrier between the dots are tuned independently. We present atomic force microscopy studies of the QDP formation steps. We have performed photoluminescence studies of single QDPs with varied dot size and tunnel-barrier thickness. The data indicate non-resonant tunnelling between the dots. Furthermore, we apply the quantum confined Stark effect to tune the photoluminescence energy by up to 25 meV.

Introducing singleMn2+ions into spontaneously coupled quantum dot pairs

We present the photoluminescence excitation study of the self-assembled CdTe/ZnTe quantum dots doped with manganese ions. We demonstrate the identification method of spontaneously coupled quantum dots pairs containing single Mn2+ ions. As the result of the coupling, the resonant absorption of the photon in one quantum dot is followed by the exciton transfer into a neighboring dot. It is shown that the Mn2+ ion might be present in the absorbing, emitting or both quantum dots. The magnetic properties of the Mn2+ spin are revealed by a characteristic sixfold splitting of the excitonic line. The statistics of the value of this splitting is analyzed for the large number of the dots and gives the information on the maximum density of the neutral exciton wave function.

Optophononics with coupled quantum dots

Modern technology is founded on the intimate understanding of how to utilize and control electrons. Next to electrons, nature uses phonons, quantized vibrations of an elastic structure, to carry energy, momentum and even information through solids. Phonons permeate the crystalline components of modern technology, yet in terms of technological utilization phonons are far from being on par with electrons. Here we demonstrate how phonons can be employed to render a single quantum dot pair optically transparent. This phonon-induced transparency is realized via the formation of a molecular polaron, the result of a Fano-type quantum interference, which proves that we have accomplished making typically incoherent and dissipative phonons behave in a coherent and non-dissipative manner. We find the transparency to be widely tunable by electronic and optical means. Thereby we show amplification of weakest coupling channels. We further outline the molecular polaron's potential as a control element in phononic circuitry architecture.

Demonstrating nonlocality-induced teleportation through Majorana bound states in a semiconductor nanowire

Abstract It was predicted by Tewari et al. (2008) [15] that a teleportation-like electron transfer phenomenon is one of the novel consequences of the existence of Majorana fermion, because of the inherently nonlocal nature. In this work we consider a concrete realization and measurement scheme for this interesting behavior, based on a setup consisting of a pair of quantum dots which are tunnel-coupled to a semiconductor nanowire and are jointly measured by two point-contact detectors. We analyze the teleportation dynamics in the presence of measurement back-action and discuss how the teleportation events can be identified from the current trajectories of strong response detectors.

Generation of Multiple Excitons in Ag2S Quantum Dots: Single High-Energy versus Multiple-Photon Excitation

We explored biexciton generation via carrier multiplication (or multiple-exciton generation) by high-energy photons and by multiple-photon absorption in Ag2S quantum dots (QDs) using femtosecond broad-band transient absorption spectroscopy. Irrespective of the size of the QDs and how the multiple excitons are generated in the Ag2S QDs, two distinct characteristic time constants of 9.6-10.2 and 135-175 ps are obtained for the nonradiative Auger recombination of the multiple excitons, indicating the existence of two binding excitons, namely, tightly bound and weakly bound excitons. More importantly, the lifetimes of multiple excitons in Ag2S QDs were about 1 and 2 orders of magnitude longer than those of comparable size PbS QDs and single-walled carbon nanotubes, respectively. This result is significant because it suggests that by utilizing an appropriate electron acceptor, there is a higher possibility to extract multiple electron-hole pairs in Ag2S QDs, which should improve the performance of QD-based solar cell devices.

Highly sensitive turn-on fluorescent detection of cartap via a nonconjugated gold nanoparticle–quantum dot pair mediated by inner filter effect

The well-dispersed AuNPs exhibited a tendency to aggregate when exposed to cartap with positively charged amine groups, which induced an absorption band transition from 522 nm to the long-wavelength band, and restored the IFE-decreased emission of CdTe QDs for cartap detection.

Resonant Excitation of CdTe/ZnTe Quantum Dot Pairs as a Tool for Spectroscopic Study of the Excitonic p-States

Resonant Excitation of CdTe/ZnTe Quantum Dot Pairs as a Tool for Spectroscopic Study of the Excitonic p-States

Magnetically tunable singlet-triplet spin qubit in a four-electron InGaAs coupled quantum dot.

A pair of self-assembled InGaAs quantum dots filled with two electrons can act as a singlet-triplet spin qubit that is robust against nuclear spin fluctuations as well as charge noise. This results in a T2* coherence time two orders of magnitude longer than that of a single electron, provided the qubit is operated at a particular “sweet spot” in gate voltage. However, at this fixed operating point the ground-state splitting can no longer be tuned into resonance with e.g. another qubit, limiting the options for coupling multiple qubits. Here, we propose using a four-electron coupled quantum dot to implement a singlet-triplet qubit that features a magnetically tunable level splitting. As a first step towards full experimental realization of this qubit design, we use optical spectroscopy to demonstrate the tunability of the four-electron singlet-triplet splitting in a moderate magnetic field.

Longitudinal Plasmon Modes of Ag Nanorod Coupled with a Pair of Quantum Dots

The longitudinal plasmon modes of an elongated Ag nanorod induced by an obliquely incident plane wave were analyzed theoretically. Our results show that the proximities at the two apexes of the nanorod are the hotspots at the dipole (m = 1), quadrupole (m = 2), sextupole (m = 3), octupole (m = 4), decapole (m = 5) and duodecapole (m = 6) modes. This phenomenon implies that a pair of quantum dots (QDs) located at these hotspots might be excited simultaneously through these plasmon modes. Consequently, the coherent spontaneous emission of the paired QDs could be induced through these modes. Furthermore, the coherent emission of the pair of excited QDs was studied, where these QDs were modeled as two electric dipoles (bi-dipole) oscillating with anti-symmetric or symmetric configurations. The radiative and nonradiative powers show that the maximum Purcell factors occur at these modes; the odd modes enhance the emission of the anti-symmetric configuration, and the even modes the symmetric one. However, only those bi-dipoles emitting at the lower-order (e.g., dipole, quadrupole and sextupole) modes of Ag nanorod are with high apparent quantum yields. In addition, the correlation of these plasmon modes of Ag nanorod with the dispersion relation of Ag nanowire was discussed.

Highly Sensitive Detection of Caspase-3 Activities via a Nonconjugated Gold Nanoparticle–Quantum Dot Pair Mediated by an Inner-Filter Effect

We describe here a simple fluorometric assay for the highly sensitive detection of caspase-3 activities on the basis of the inner-filter effect of gold nanoparticles (AuNPs) on CdTe quantum dots (QDs). The method takes advantage of the high molar absorptivity of the plasmon band of gold nanoparticles as well as the large absorption band shift from 520 to 680 nm upon nanoparticle aggregation. When labeled with a peptide possessing the caspase-3 cleavage sequence (DEVD), the monodispersed Au-Ps (peptide-modified AuNPs) exhibited a tendency to aggregate when exposed to caspase-3, which induced the absorption band transition from 520 to 680 nm and turned on the fluorescence of the CdTe QDs for caspase-3 sensing. Under optimum conditions, a high sensitivity towards caspase-3 was achieved with a detection limit as low as 18 pM, which was much lower than the corresponding assays based on absorbance or other approaches. Overall, we demonstrated a facile and sensitive approach for caspase-3 detection, and we expected that this method could be potentially generalized to design more fluorescent assays for sensing other bioactive entities.