PbS quantum dots are promising active emitters for use with high-quality Si nanophotonic devices in the telecommunications-band. Measurements of low quantum dot densities are limited both because of low fluorescence levels and the challenges of single photon detection at these wavelengths. Here, we report on methods using a fiber taper waveguide to efficiently extract PbS quantum dot photoluminescence. Temperature dependent ensemble measurements reveal an increase in emitted photons concomitant with an increase in excited-state lifetime from 58.9 ns at 293 K to 657 ns at 40 K. Measurements are also performed on quantum dots on high-$Q$ ($>10^5$) microdisks using cavity-resonant, pulsed excitation.
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.
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-…
We report on enhanced fluorescence of lead sulfide quantum dots interacting with leaky modes of slab-type silicon photonic crystals. The photonic crystal slabs were fabricated supporting leaky modes in the near infrared wavelength range. Lead sulfite quantum dots which are resonant the same spectral range were prepared in a thin layer above the slab. We selectively excited the leaky modes by tuning wavelength and angle of incidence of the laser source and measured distinct resonances of enhanced fluorescence. By an appropriate experiment design, we ruled out directional light extraction effect…
We present a tunnel spectroscopy study of single PbS Quantum Dots (QDs) as function of temperature and gate voltage. Three distinct signatures of strong electron-phonon coupling are observed in the Electron Tunneling Spectrum (ETS) of these QDs. In the shell-filling regime, the $8\times$ degeneracy of the electronic levels is lifted by the Coulomb interactions and allows the observation of phonon sub-bands that result from the emission of optical phonons. At low bias, a gap is observed in the ETS that cannot be closed with the gate voltage, which is a distinguishing feature of the Franck-Condo…
We measure the photoluminescence (PL) lifetime, $τ$, of excitons in colloidal PbSe nanocrystals (NCs) at low temperatures to 270~mK and in high magnetic fields to 15~T. For all NCs (1.3-2.3~nm radii), $τ$ increases sharply below 10~K but saturates by 500~mK. In contrast to the usual picture of well-separated ``bright" and ``dark" exciton states (found, e.g., in CdSe NCs), these dynamics fit remarkably well to a system having two exciton states with comparable - but small - oscillator strengths that are separated by only 300-900 $μ$eV. Importantly, magnetic fields reduce $τ$ below 10~K, consist…
We examine the multiple exciton population dynamics in PbS quantum dots by ultrafast spectrally-resolved supercontinuum transient absorption (SC-TA). We simultaneously probe the first three excitonic transitions over a broad spectral range. Transient spectra show the presence of first order bleach of absorption for the 1S_h-1S_e transition and second order bleach along with photoinduced absorption band for 1P_h-1P_e transition. We also report evidence of the one-photon forbidden 1S_{h,e}-1P_{h,e} transition. We examine signatures of carrier multiplication (multiexcitons for the single absorbed…
This paper reviews recent progress in the synthesis of near-infrared (NIR) lead chalcogenide (PbX; PbX=PbS, PbSe, PbTe) quantum dots (QDs) and their applications in NIR QDs based light emitting diodes (NIR-QLEDs). It summarizes the strategies of how to synthesize high efficiency PbX QDs and how to realize high performance PbX based NIR-QLEDs.
The relaxation of strongly-confined electrons and holes between 1P and 1S levels in colloidal PbSe nanocrystals has been time-resolved using femtosecond transient absorption spectroscopy. In contrast to II-VI and III-V semiconductor nanocrystals, both electrons and holes are strongly confined in PbSe nanocrystals. Despite the large electron and hole energy level spacings (at least 12 times the optical phonon energy), we consistently observe picosecond time-scale relaxation. Existing theories of carrier relaxation cannot account for these experimental results. Mechanisms that could possibly cir…
We discuss photo-luminescence characteristics of CdSe core/shell quantum dots at cryogenic temperatures using a hybrid system of a single quantum dot and an optical nanofiber. The key point is to control the emission species of quantum dot to charged excitons, known as trions, which have superior characteristics to neutral excitons. We investigate the photocharging behavior for the quantum dots by varying the wavelength and intensity of irradiating laser light, and establish a method to create a permanently charged situation which lasts as long as the cryogenic temperature is maintained. The p…
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…
new defect-assisted mechanism of multiphonon intraband carrier relaxation in semiconductor quantum dots, where the carrier is found in a coherent superposition of the initial, final, and defect states, is proposed. It is shown that this mechanism is capable of explaining the observed trends in temperature dependences of the intraband relaxation rates for PbSe and CdSe colloidal nanocrystal quantum dots.
Solid-state quantum computers require classical electronics to control and readout individual qubits and to enable fast classical data processing [1-3]. Integrating both subsystems at deep cryogenic temperatures [4], where solid-state quantum processors operate best, may solve some major scaling challenges, such as system size and input/output (I/O) data management [5]. Spin qubits in silicon quantum dots (QDs) could be monolithically integrated with complementary metal-oxide-semiconductor (CMOS) electronics using very-large-scale integration (VLSI) and thus leveraging over wide manufacturing …
Steady-state access to intraband transitions in colloidal quantum dots (CQDs), via heavy doping, allows exploiting the electromagnetic spectrum at energies below the band gap. CQD intraband optoelectronics opens up a new path to cheap mid- and long-wavelength infrared photodetectors and light-emitting devices, which today employ mostly epitaxial materials. As a recent field of experimental research, thorough studies of the basic properties of intraband transitions in CQDs are still lacking. In this work, we investigate the size and temperature dependence of the intraband transition in heavily …
We report a photoluminescence imaging system for locating single quantum emitters with respect to alignment features. Samples are interrogated in a 4~K closed-cycle cryostat by a high numerical aperture (NA=0.9, 100$\times$ magnification) objective that sits within the cryostat, enabling high efficiency collection of emitted photons without image distortions due to the cryostat windows. The locations of single InAs/GaAs quantum dots within a $>50$~$μ$m~$\times$~50~$μ$m field of view are determined with $\approx4.5$~nm uncertainty (one standard deviation) in a 1~s long acquisition. The uncertai…
We investigate a quadruple quantum dot setup that can be employed to sense the temperature of an electrically isolated remote target reservoir. Such a setup was conceived earlier by Sánchez et. al. (New Journal of Physics, 19, 113040) as non-local thermodynamic engine and relies on the electrostatic interaction between Coulomb-coupled quantum dots. The conjugation of Coulomb-coupling and energy-filtering results in an overall change in conductance with remote reservoir temperature. The performance of the thermometer is then theoretically investigated using density matrix formulation, and it is…
Using a single-band model, the lowest transition energy was analysed between the lowest unoccupied molecular orbital (LUMO) of the conduction band and the highest occupied molecular orbital (HOMO) of the valence band. We focus on categorising the confinement strength in type-II core-shell quantum dots (CSQDs) based on the step-potential and show how it will affect their transition energy. Our model is applied to CSQDs of the heterostructures PbS/CdS and ZnTe/ZnSe through narrow and wide band gaps, respectively. It found that PbS/CdS CSQDs demonstrates a strong confinement in which their transi…
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…
A two quantum-dot device is coupled in parallel for studying the competition between the pseudo-spin Kondo effect and strongly hybridized molecular states. Cryogenic measurements are performed in the regime of weak coupling of the two dots to lead states under linear transport conditions. Detailed simulations verify the finding of the transition between the two different regimes.
On-chip calibrated radio-frequency measurement at cryogenic temperatures for determination of SrTiO3-based capacitor properties
Research Institute of Electrical Communication, Tohoku University（东北大学电气通信研究所）；Department of Electronic Engineering, Graduate School of Engineering, Tohoku University（东北大学工学研究科电子工程系）；WPI Advanced Institute for Materials Research, Tohoku University（东北大学材料研究高等研究院）；National Institute of Advanced Industrial Science and Technology (AIST)（产业技术综合研究所）；Faculty of Science and Engineering, Waseda University（早稻田大学理工学术院）；Research Center for Materials Nanoarchitechtonics (MANA), National Institute for Material Science (NIMS)（国立研究开发法人物质·材料研究机构纳米结构材料研究中心）
We report on the growth and optical characterisation of droplet GaAs quantum dots with extremely-thin (11 nm) capping layers. To achieve such result, an internal thermal heating step is introduced during the growth and its role in the morphological properties of the quantum dots obtained is investigated via scanning electron and atomic force microscopy. Photoluminescence measurements at cryogenic temperatures show optically stable, sharp and bright emission from single quantum dots, at near-infrared wavelengths. Given the quality of their optical properties and the proximity to the surface, su…
We study the exciton dynamics in an optically excited nanocrystal quantum dot. Multiple exciton formation is more efficient in nanocrystal quantum dots compared to bulk semiconductors due to enhanced Coulomb interactions and the absence of conservation of momentum. The formation of multiple excitons is dependent on different excitation parameters and the dissipation. We study this process within a Lindblad quantum rate equation using the full many-particle states. We optically excite the system by creating a single high energy exciton $E_{SX}$ in resonance to a double exciton $E_{DX}$. With Co…
GaN and the heterostructures are attractive in condensed matter science and applications for electronic devices. We measure the electron transport in GaN/AlGaN field-effect transistors (FETs) at cryogenic temperature. We observe formation of quantum dots in the conduction channel near the depletion of the 2-dimensional electron gas (2DEG). Multiple quantum dots are formed in the disordered potential induced by impurities in the FET conduction channel. We also measure the gate insulator dependence of the transport properties. These results can be utilized for the development of quantum dot devi…
High resolution coherent nonlinear optical spectroscopy of an ensemble of red-emitting InGaN quantum dots in GaN nanowires is reported. The data show a pronounced atom-like interaction between resonant laser fields and quantum dot excitons at low temperature that is difficult to observe in the linear absorption spectrum due to inhomogeneous broadening from indium fluctuation effects. We find that the nonlinear signal persists strongly at room temperature. The robust atom-like room temperature response indicates the possibility that this material could serve as the platform for proposed exciton…
A simple, single-color method for permanent marking of the position of individual self-assembled semiconductor Quantum Dots (QDs) at cryogenic temperatures is reported. The method combines in situ photolithography with standard micro-photoluminescence spectroscopy. Its utility is proven by a systematic magnetooptical study of a single CdTe/ZnTe QD containing a Mn2+ ion, where a magnetic field of up to 10 T in two orthogonal, Faraday and Voigt, configurations is applied to the same QD. The presented approach can be applied to a wide range of solid state nanoemitters.
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…
Graphene is an attractive material for broadband photodetection but suffers from weak light absorption. Coating graphene with quantum dots can significantly enhance light absorption and create extraordinarily high photo gain. This high gain is often explained by the classical gain theory which is unfortunately an implicit function and may even be questionable. In this work, we managed to derive explicit gain equations for hybrid graphene-quantum-dot photodetectors. Due to the work function mismatch, lead sulfide (PbS) quantum dots coated on graphene will form a surface depletion region near th…
III-Nitride quantum dots have emerged as a new chip-scale system for quantum information science, which combines electrical and optical interfaces on a semiconductor chip that is compatible with non-cryogenic operating temperatures. Yet most work has been limited to optical excitations. To enable single-spin based quantum optical and quantum information research, we demonstrate here quantized charging in optically active, site-controlled III-Nitride quantum dots. Single-electron charging was confirmed by the voltage dependence of the energy, dipole moment, fine structures and polarization prop…
Phonon-enhanced strain sensitivity of quantum dots in two-dimensional semiconductors
School of Physical Sciences, Indian Institute of Technology Goa（印度理工学院果阿分校物理科学学院）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国家材料科学研究所电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国家材料科学研究所材料纳米架构研究中心）
Molybdenum disulfide nanoribbons and nanotubes are quasi-1D semiconductors with strong spin-orbit interaction, a nanomaterial highly promising for quantum electronic applications. Here, it is demonstrated that a bismuth semimetal layer between the contact metal and this nanomaterial strongly improves the properties of the contacts. Two-point resistances on the order of 100k$Ω$ are observed at room temperature. At cryogenic temperature, Coulomb blockade is visible. The resulting stability diagrams indicate a marked absence of trap states at the contacts and the corresponding disorder, compared …
We demonstrate a 36$\times$36 gate electrode crossbar that supports 648 narrow-channel field effect transistors (FET) for gate-defined quantum dots, with a quadratic increase in quantum dot count upon a linear increase in control lines. The crossbar is fabricated on an industrial $^{28}$Si-MOS stack and shows 100% FET yield at cryogenic temperature. We observe a decreasing threshold voltage for wider channel devices and obtain a normal distribution of pinch-off voltages for nominally identical tunnel barriers probed over 1296 gate crossings. Macroscopically across the crossbar, we measure an a…
Measurement of multiple quantum devices on a single chip increases characterization throughput and enables testing of device repeatability, process yield, and systematic variations in device design. We present a method that uses on-chip field-effect transistor switches to enable multiplexed cryogenic measurements of double quantum dot Si/SiGe devices. Multiplexing makes it feasible to characterize a number of devices that scales exponentially with the number of external wires, a key capability given the significant constraints on cryostat wiring currently in common use. We use this approach to…
We predict a spin pure dephasing channel in electron relaxation between states with unequal Zeeman splittings, exemplified by a spin-preserving electron tunneling between quantum dots in a magnetic field. The dephasing is caused by a mismatch in electron $g$-factors in the dots leading to distinguishability of phonons emitted during tunneling with opposite spins. Combining multiband $\boldsymbol{k}{\cdot}\boldsymbol{p}$ modeling and dynamical simulations via a Master equation we show that this fundamental effect of spin measurement effected by the phonon bath may be widely controlled by the si…
We propose and investigate thermometry of a setup employing dual quantum dots with staircase ground state configuration. The stair-case ground state configuration actuates thermally controlled inelastic tunnelling, which translates into a temperature sensitive conductance, thereby inducing thermometry. The performance of the set-up is then analyzed employing quantum master equation (QME) for such systems in the sequential tunnelling regime. In particular, it is demonstrated that the system performance, in terms of temperature sensitivity and efficiency, is maximum in the regime of low temperat…
Photo-induced Wavelength-tuning of Telecom-band Quantum Dot Nanowires Embedded in a Phase Change Material
CNRS, ECL, INSA Lyon, UCBL, CPE Lyon, INL, UMR 5270（法国国家科学研究中心，里昂高等师范学校，里昂国立应用科学学院，里昂第一大学，里昂高等化学物理学院，国家科研中心）；CNRS, INSA Lyon, Université Claude Bernard Lyon 1, MATEIS, UMR 5510（法国国家科学研究中心，里昂国立应用科学学院，克洛德·贝尔纳里昂第一大学）；Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière, UMR5306（克洛德·贝尔纳里昂第一大学，法国国家科学研究中心，光物质研究所）
We have investigated spin relaxation times in CdTe quantum dots doped with a single Mn atom, a prototype of a system where the interaction between a single charge carrier and a single spin takes place. A theoretical model that was used includes the electron-Mn spin exchange interaction responsible for mixing of the states of different spin in the basic Hamiltonian and electron-phonon interaction as a perturbation responsible for transitions between the states. It was found that the dominant electron-phonon interaction mechanism responsible for spin relaxation is the interaction with acoustic p…
Spins in silicon quantum devices are promising candidates for large-scale quantum computing. Gate-based sensing of spin qubits offers compact and scalable readout with high fidelity, however further improvements in sensitivity are required to meet the fidelity thresholds and measurement timescales needed for the implementation of fast-feedback in error correction protocols. Here, we combine radio-frequency gate-based sensing at 622 MHz with a Josephson parametric amplifier (JPA), that operates in the 500-800 MHz band, to reduce the integration time required to read the state of a silicon doubl…
Emergent Bell Phase in an Electro-Nanomechanical Quantum Simulator
Universitat Autònoma de Barcelona（巴塞罗那自治大学）；ICFO - Institut De Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究院）；ICREA（加泰罗尼亚高级研究院）
Photoluminescence spectroscopy of single InAs quantum dots at cryogenic temperatures (~14 K) is performed using a micron-scale optical fiber taper waveguide as a near-field optic. The measured collection efficiency of quantum dot spontaneous emission into the fundamental guided mode of the fiber taper is estimated at 0.1%, and spatially-resolved measurements with ~600 nm resolution are obtained by varying the taper position with respect to the sample and using the fiber taper for both the pump and collection channels.
Efficient, high rate photon sources with high single photon purity are essential ingredients for quantum technologies. Single photon sources based on solid state emitters such as quantum dots are very advantageous for integrated photonic circuits, but they can suffer from a high two-photon emission probability, which in cases of non-cryogenic environment cannot be spectrally filtered. Here we propose two temporal purification-by-heralding methods for using a two photon emission process to yield highly pure and efficient single photon emission, bypassing the inherent problem of spectrally overl…
Quantum dots (QDs) based on III-nitride semiconductors are promising for single photon emission at non-cryogenic temperatures due to their large exciton binding energies. Here, we demonstrate GaN QD single photon emitters operating at 300 K with $g^{(2)}(0) = 0.17 \pm 0.08$ under continuous wave excitation. At this temperature, single photon emission rates up to $6\times10^6 \, \text{s}^{-1}$ are reached while $g^{(2)}(0) \leq 0.5$ is maintained. Our results are achieved for GaN QDs embedded in a planar AlN layer grown on silicon, representing a promising pathway for future interlinkage with o…
