Dissipative preparation of the exciton and biexciton in a self-assembled quantum dot on picosecond timescales
Per-Lennart Ardelt, Lukas Hanschke, Kevin A. Fischer, Kai Müller, Alexander Kleinkauf, Manuel Koller, Alexander Bechtold, Tobias Simmet, Jakob Wierzbowski, Hube… 展开作者
Per-Lennart Ardelt, Lukas Hanschke, Kevin A. Fischer, Kai Müller, Alexander Kleinkauf, Manuel Koller, Alexander Bechtold, Tobias Simmet, Jakob Wierzbowski, Hubert Riedl, Gerhard Abstreiter, Jonathan. J. Finley
Pulsed resonant fluorescence is used to probe ultrafast phonon-assisted exciton and biexciton preparation in individual self-assembled InGaAs quantum dots. By driving the system using large area ($\geq10π$) near resonant optical pulses, we experimentally demonstrate how phonon mediated dissipation within the manifold of dressed excitonic states can be used to prepare the neutral exciton with a fidelity $\geq 70\%$. By comparing the phonon-assisted preparation with resonant Rabi oscillations we show that the phonon-mediated process provides the higher fidelity preparation for large pulse areas and is less sensitive to pulse area variations. Moreover, by detuning the laser with respect to the exciton transition we map out the spectral density for exciton coupling to the bulk LA-phonon continuum. Similar phonon mediated processes are shown to facilitate direct biexciton preparation via two photon biexciton absorption, with fidelities $>80\%$. Our results are found to be in very good quantitative agreement with simulations that model the quantum dot-phonon bath interactions with Bloch-Redfield theory.
The contribution to the biexciton binding energy in quantum dots resulting from the interaction with longitudinal optical phonons is estimated by performing the configuration--interaction calculation of the few-particle states in a simple model of the confining potential and including the phonon corrections by means of a perturbation theory. It is found that the polaron contribution tends to compensate the Coulomb-related biexciton shift (binding energy) and reduces its value by several to even 30%, depending on the material parameters of the system.
We report on single InGaAs quantum dots embedded in a lateral electric field device. By applying a voltage we tune the neutral exciton transition into resonance with the biexciton using the quantum confined Stark effect. The results are compared to theoretical calculations of the relative energies of exciton and biexciton. Cascaded decay from the manifold of single exciton-biexciton states has been predicted to be a new concept to generate entangled photon pairs on demand without the need to suppress the fine structures splitting of the neutral exciton.
The use of ultrafast gating techniques allows us to resolve both spectrally and temporally the emission from short-lived neutral and negatively charged biexcitons in ultrasmall (sub-10 nm) CdSe nanocrystals (nanocrystal quantum dots). Because of forced overlap of electronic wave functions and reduced dielectric screening, these states are characterized by giant interaction energies of tens (neutral biexcitons) to hundreds (charged biexcitons) of meV. Both types of biexcitons show extremely short lifetimes (from sub-100 picoseconds to sub-picosecond time scales) that rapidly shorten with decrea…
The radiative recombination rates of interacting electron-hole pairs in a quantum dot are strongly affected by quantum correlations among electrons and holes in the dot. Recent measurements of the biexciton recombination rate in single self-assembled quantum dots have found values spanning from two times the single exciton recombination rate to values well below the exciton decay rate. In this paper, a Feynman path-integral formulation is developed to calculate recombination rates including thermal and many-body effects. Using real-space Monte Carlo integration, the path-integral expressions f…
The four-level exciton/biexciton system of a single semiconductor quantum dot acts as a two qubit register. We experimentally demonstrate an exciton-biexciton Rabi rotation conditional on the initial exciton spin in a single InGaAs/GaAs dot. This forms the basis of an optically gated two-qubit controlled-rotation (CROT) quantum logic operation where an arbitrary exciton spin is selected as the target qubit using the polarization of the control laser.
It is demonstrated how the exciton and the biexciton state of a quantum dot can be prepared with high fidelity on a picosecond time-scale by driving the dot with a strong laser pulse that is tuned above the exciton resonance for exciton preparation and in resonance with the exciton transition for biexciton preparation. The proposed schemes make use of the phonon-induced relaxation towards photon dressed states in optically driven quantum dots and combine the simplicity of Rabi flopping with the robustness of adiabatic rapid passage schemes. Our protocols allow for an on-demand, fast and almost…
We investigate both experimentally and theoretically a simple yet more robust and flexible alternative to Rabi oscillation-type biexciton preparation protocols traditionally used for semiconductor quantum dots. The quantum dot is excited by a strong laser pulse positively detuned from the two-photon resonance yielding an on demand initialization of the biexciton state by making use of the phonon-induced thermalization of the photon dressed states. It is shown that for excitation pulses in the picosecond range, a stable and high fidelity of up to $f_{XX}=0.98\pm 0.01$ is reached. Notably, the g…
We present a spectroscopic study of excitation dynamics in self assembled CdTe/ZnTe quantum dots. Insight into details of kinetics is obtained from the time resolved micro-photoluminescence, single photon correlation and subpicosecond excitation correlation measurements done on single quantum dots. It is shown that the pulsed excitation in energy above the energy gap of the barrier material results in separate capture of electrons and holes. The capture of carriers of different charge take place at different delay from excitation.
We present a theory of the optical control of the spin of an electron in an InAs quantum dot. We show how two Raman-detuned laser pulses can be used to obtain arbitrary single-qubit rotations via the excitation of an intermediate trion state. Our theory takes into account a finite in-plane hole $g$-factor and hole-mixing. We show that such rotations can be performed to high fidelities with pulses lasting a few tens of picoseconds.
We demonstrate control over the spin state of a semiconductor quantum dot exciton using a polarized picosecond laser pulse slightly detuned from a biexciton resonance. The control pulse follows an earlier pulse, which generates an exciton and initializes its spin state as a coherent superposition of its two non-degenerate eigenstates. The control pulse preferentially couples one component of the exciton state to the biexciton state, thereby rotating the exciton's spin direction. We detect the rotation by measuring the polarization of the exciton spectral line as a function of the time-differen…
We present a comparative study of two self-assembled quantum dot (QD) systems based on II-VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X$^+$, X$^-$) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X-XX transition energy difference 12 meV (24 meV); fine-structure splitting $δ_{1}=$0.14 meV ($δ_{1}=$0.47 meV); $g$-factor $g=$2.12 ($g=$1.71…
I present a systematic study of self-assembled InAs/InP and InAs/GaAs quantum dots single particle and many body properties as a function of quantum dot-surrounding matrix valence band offset. I use an atomistic, empirical tight-binding approach and perform numerically demanding calculations for half-million atom nanosystems. I demonstrate that the overall confinement in quantum dots is a nontrivial interplay of two key factors: strain effects and the valence band offset. I show that strain effects determine both the peculiar structure of confined hole states of lens type InAs/GaAs quantum dot…
We study theoretically phonon-assisted relaxation processes in a system consisting of one or two electrons confined in two vertically stacked self-assembled quantum dots. The calculation is based on a k.p approximation for single particle wave functions in a strained self-assembled structure. From these, two-particle states are calculated by including the Coulomb interaction and the transition rates between the lowest energy eigenstates are derived. We take into account phonon couplings via deformation potential and piezoelectric interaction and show that they both can play a dominant role in …
Biexciton cascade process in self-assembled quantum dots (QDs) provides an ideal system for deterministic entangled photon pair source, which is essential in quantum information science. The entangled photon pairs have recently be realized in experiments after eliminating the FSS of exciton using a number of different methods. However, so far the QDs entangled photon sources are not scalable, because the wavelengths of the QDs are different from dot to dot. Here we propose a wavelength tunable entangled photon emitter on a three dimensional stressor, in which the FSS and exciton energy can be …
The emission spectrum of exciton complexes formed in individual self-assembled quantum dots (QDs) embedded into a p-n junction is theoretically studied using an effective mass model. We calculate the particle Coulomb interactions, eletron-hole overlaps and transition energies of exciton complexes for the different strength and direction of electric field. Both redshifts and blueshifts are observed in exciton, trions and biexciton. The Stark effect may be applied to manipulate the spontaneous emission rate of individual QDs embedded in microcavities.
We present here an atomistic theory of the electronic and optical properties of hexagonal InAsP quantum dots in InP nanowires in the wurtzite phase. These self-assembled quantum dots are unique in that their heights, shapes, and diameters are well known. Using a combined valence-force-field, tight-binding, and configuration-interaction approach we perform atomistic calculations of single-particle states and excitonic, biexcitonic and trion complexes as well as emission spectra as a function of the quantum dot height, diameter and As versus P concentration. The atomistic tight-binding parameter…
We report on recent progress in the acousto-electrical control of self-assembled quantum dot and quantum post using radio frequency surface acoustic waves (SAWs). We show that the occupancy state of these optically active nanostructures can be controlled via the SAW-induced dissociation of photogenerated excitons and the resulting sequential bipolar carrier injection which strongly favors the formation of neutral excitons for quantum posts in contrast to conventional quantum dots. We demonstrate high fidelity preparation of the neutral biexciton which makes this approach suitable for determini…
We demonstrate a one to one correspondence between the polarization state of a light pulse tuned to neutral exciton resonances of single semiconductor quantum dots and the spin state of the exciton that it photogenerates. This is accomplished using two variably polarized and independently tuned picosecond laser pulses. The first "writes" the spin state of the resonantly excited exciton. The second is tuned to biexcitonic resonances, and its absorption is used to "read" the exciton spin state. The absorption of the second pulse depends on its polarization relative to the exciton spin direction.…
We have shown theoretically that efficient multiple exciton generation (MEG) by a single photon can be observed in small nanocrystals (NCs). Our quantum simulations that include hundreds of thousands of exciton and multi-exciton states demonstrate that the complex time-dependent dynamics of these states in a closed electronic system yields a saturated MEG effect on a picosecond timescale. Including phonon relaxation confirms that efficient MEG requires the exciton--biexciton coupling time to be faster than exciton relaxation time.
We study spectrally resolved dynamics of Forster energy transfer in single monolayers and bilayers of semiconductor nanocrystal quantum dots assembled using Langmuir-Blodgett (LB) techniques. For a single monolayer, we observe a distribution of transfer times from ~50 ps to ~10 ns, which can be quantitatively modeled assuming that the energy transfer is dominated by interactions of a donor nanocrystal with acceptor nanocrystals from the first three shells surrounding the donor. We also detect an effective enhancement of the absorption cross section (up to a factor of 4) for larger nanocrystals…
The self-assembled quantum dots (QDs) provide an ideal platform for realization of quantum information technology because it provides on demand single photons, entangled photon pairs from biexciton cascade pro- cess, single spin qubits, and so on. The fine structure splitting (FSS) of exciton is a fundamental property of QDs for thees applications. From the symmetry point of view, since the two bright exciton states belong to two different representations for QDs with C2v symmetry, they should not only have different energies, but also have different lifetimes, which is termed exciton lifetime…
A hole spin is a potential solid-state q-bit, that may be more robust against nuclear spin induced dephasing than an electron spin. Here we propose and demonstrate the sequential preparation, control and detection of a single hole spin trapped on a self-assembled InGaAs/GaAs quantum dot. The dot is embedded in a photodiode structure under an applied electric-field. Fast, triggered, initialization of a hole spin is achieved by creating a spin-polarized electron-hole pair with a picosecond laser pulse, and in an applied electric-field, waiting for the electron to tunnel leaving a spin-polarized …
The effects resulting due to dressing of an exciton with phonons are analysed as the source of unavoidable decoherence of orbital degrees of freedom in quantum dots. The dressing with longitudinal optical phonons results in energetic shift of order of a few meV even of the ground state of exciton in a state-of-the-art InAs/GaAs dot and the mediating role of longitudinal acoustical phonons is essential in this process. The characteristic time needed for dressing of the exciton with optical phonons is of a picosecond order. That time can be regarded as the lowest limit for decoherence for optica…
We report the sub-picosecond initialization of a single heavy hole spin in a self-assembled quantum dot with >98.5 % fidelity and without external magnetic field. Using an optically adressable charge and spin storage device we tailor the relative electron and hole tunneling escape timescales from the dot and simultaneously achieve high-fidelity initialization, long hole storage times and high efficiency readout via a photocurrent signal. We measure electric field-dependent Rabi oscillations of the neutral and charged exciton transitions in the ultrafast tunneling regime and demonstrate that tu…
The strong confinement of semiconductor excitons in a quantum dot gives rise to atom-like behavior. The full benefit of such a structure is best observed in resonant excitation where the excited state can be deterministically populated and coherently manipulated. Due to large refractive index and device geometry it remains challenging to observe resonantly excited emission that is free from laser scattering in III/V self-assembled quantum dots. Here we exploit the biexciton binding energy to create an extremely clean single photon source via two-photon resonant excitation of an InAs/GaAs quant…
We show that the non-parabolic confinement potential is responsible for the non-monotonic behavior and sign change of the exciton fine-structure splitting (FSS) in optically active self-assembled quantum dots. This insight is important for the theoretical understanding and practical control by electric fields of the quantum state of the emitted light from a biexciton cascade recombination process. We find that a hard-wall (box) confinement potential leads to a FSS that is in better agreement with experimentally measured FSS than a harmonic potential. We then show that a finite applied electric…
We report on coherent emission of the neutral exciton state in a single semiconductor self-assembled InAs/GaAs quantum dot embedded in a one-dimensional waveguide, under resonant picosecond pulsed excita- tion. Direct measurements of the radiative lifetime and coherence time are performed as a function of excitation power and temperature. The characteristic damping of Rabi oscillations which is observed, is attributed to an excitation-induced dephasing due to a resonant coupling between the emitter and the acoustic phonon bath of the matrix. Other sources responsible for the decrease of the co…
High-quality sources of single photons are of paramount importance for quantum communication, sensing and metrology. To these ends, resonantly excited two-level systems based on self-assembled quantum dots have recently generated widespread interest. Nevertheless, we have recently shown that for resonantly excited two-level systems, emission of a photon during the presence of the excitation laser pulse and subsequent re-excitation results in a degradation of the obtainable single-photon purity. Here, we demonstrate that generating single photons from self-assembled quantum dots with a scheme b…
Long distance quantum communication is one of the prime goals in the field of quantum information science. With information encoded in the quantum state of photons, existing telecommunication fiber networks can be effectively used as a transport medium. To achieve this goal, a source of robust entangled single photon pairs is required. While time-bin entanglement offers the required robustness, currently used parametric down-conversion sources have limited performance due to multi-pair contributions. We report the realization of a source of single time-bin entangled photon pairs utilizing the …
We employ ultrafast pump-probe spectroscopy with photocurrent readout to directly probe the dynamics of a single hole spin in a single, electrically tunable self-assembled quantum dot molecule formed by vertically stacking InGaAs quantum dots. Excitons with defined spin configurations are initialized in one of the two dots using circularly polarized picosecond pulses. The time-dependent spin configuration is probed by the spin selective optical absorption of the resulting few Fermion complex. Taking advantage of sub-5 ps electron tunneling to an orbitally excited state of the other dot, we ini…
Energy-time entanglement from a monolithically integrated quantum dot on silicon
Institute for Physics and Astronomy, Technical University of Berlin（柏林工业大学物理与天文学研究所）；mar.quest | Marburg Center for Quantum Materials and Sustainable Technologies, Philipps University Marburg（马尔堡大学量子材料与可持续技术中心 (mar.quest)）；Department of Physics, Philipps University Marburg（马尔堡大学物理系）
We study Rabi rotations arising in intensity-dependent photon echoes from an ensemble of self-assembled InGaAs quantum dots. To achieve a uniform distribution of intensities within the excited ensemble, we introduce flattop intensity profiles of picosecond laser pulses. This allows us to overcome the damping of Rabi rotations imposed by the spatial inhomogeneity of Rabi frequencies by a Gaussian laser profile. Using photon echo polarimetry, we distinguish between the coherent optical responses from exciton and trion ensembles. Here, we demonstrate that a photo-induced charging of the quantum d…
Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a novel concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2pi area. Dependi…
The spectral properties of one exciton trapped in a self-assembled multi-layered quantum dot is obtained using a high precision variational numerical method. The exciton Hamiltonian includes the effect of the polarization charges, induced by the presence of the exciton in the quantum dot, at the material interfaces. The method allows to implement rather easily the matching conditions at the interfaces of the hetero-structure. The numerical method also provides accurate approximate eigenfunctions that enable the study of the separability of the exciton eigenfunction in electron and hole states.…
