Zeeman splitting of quantum-confined states of excitons in InGaAs quantum wells (QWs) is experimentally found to depend strongly on quantization energy. Moreover, it changes sign when the quantization energy increases with a decrease in the QW width. In the 87-nm QW, the sign change is observed for the excited quantum-confined states, which are above the ground state only by a few meV. A two-step approach for the numerical solution of the two-particle Schroedinger equation, taking into account the Coulomb interaction and valence-band coupling, is used for a theoretical justification of the observed phenomenon. The calculated variation of the g-factor convincingly follows the dependencies obtained in the experiments.
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.
We study an asymmetric double InGaAs quantum well using optical two-dimensional coherent spectroscopy. The collection of zero-quantum, one-quantum, and two-quantum two-dimensional spectra provides a unique and comprehensive picture of the double well coherent optical response. Coherent and incoherent contributions to the coupling between the two quantum well excitons are clearly separated. An excellent agreement with density matrix calculations reveals that coherent interwell coupling originates from many-body interactions.
We study the effects of the nonlinear piezoelectricity and the In distribution on the exciton energy, the electron-hole electric dipole moment, and the fine-structure splitting in stress-tunable InGaAs/GaAs quantum dots integrated onto a piezoelectric actuator. In particular, we investigate in detail the contributions of various elements of the expansion of the electrical polarization in terms of externally induced elastic strain on the latter two important quantum dot properties. Based on the comparison of the effects of first- and second-order piezoelectricity we provide a simple relation to…
We have measured weak antilocalization effects, universal conductance fluctuations, and Aharonov-Bohm oscillations in the two-dimensional electron gas formed in InGaAs/AlInAs heterostructures. This system possesses strong spin-orbit coupling and a high Landé factor. Phase-coherence lengths of 2$-$4 $μ$m at 1.5$-$4.2 K are extracted from the magnetoconductance measurements. The analysis of the coherence-sensitive data reveals that the temperature dependence of the decoherence rate complies with the dephasing mechanism originating from electron-electron interactions in all three experiments. Dis…
Quantum dots are arguably one of the best platforms for optically accessible spin based qubits. The paramount demand of extended qubit storage time can be met by using quantum-dot-confined dark exciton: a longlived electron-hole pair with parallel spins. Despite its name the dark exciton reveals weak luminescence that can be directly measured. The origins of this optical activity remain largely unexplored. In this work, using the atomistic tight-binding method combined with configuration-interaction approach, we demonstrate that atomic-scale randomness strongly affects oscillator strength of d…
We demonstrate that the exciton and biexciton emission energies as well as exciton fine structure splitting (FSS) in single (In,Ga)As/GaAs quantum dots (QDs) can be efficiently tuned using hydrostatic pressure in situ in an optical cryostat at up to 4.4 GPa. The maximum exciton emission energy shift was up to 380 meV, and the FSS was up to 180 $μ$eV. We successfully produced a biexciton antibinding-binding transition in QDs, which is the key experimental condition that generates color- and polarization-indistinguishable photon pairs from the cascade of biexciton emissions and that generates en…
The effect of irradiation by 30-keV Ga+ and 35-keV He+ ions (in relatively small doses) on the excitonic reflectivity spectra of single InGaAs/GaAs quantum-well structures is studied. It is found that the irradiation results in decreasing intensity and broadening of the excitonic resonances in the reflectivity spectra for all the doses. It is shown that these changes are not related to a decrease of the exciton transition oscillator strength and, therefore, to the irradiation-induced destruction of the excitonic states, but can be rather ascribed to a common cause, namely, to inhomogeneous bro…
Multiple quantum beats of a system of the coherently excited quantum confined exciton states in a high-quality heterostructure with a wide InGaAs/GaAs quantum well are experimentally detected by the spectrally resolved pump-probe method for the first time. The beat signal is observed as at positive as at negative delays between the pump and probe pulses. A theoretical model is developed, which allows one to attribute the QBs at negative delay to the four-wave mixing (FWM) signal detected at the non-standard direction. The beat signal is strongly enhanced by the interference of the FWM wave wit…
We report on a magneto-photoluminescence (PL) study of Mn modulation-doped InAs/InGaAs/InAlAs quantum wells. Two PL lines corresponding to the radiative recombination of photoelectrons with free and bound-on-Mn holes have been observed. In the presence of a magnetic field applied in the Faraday geometry both lines split into two circularly polarized components. While temperature and magnetic field dependences of the splitting are well described by the Brillouin function, providing an evidence for exchange interaction with spin polarized manganese ions, the value of the splitting exceeds the ex…
Hereby, we present a comprehensive experimental and theoretical study of the electronic structure and optical properties of excitonic complexes in strain-engineered InGaAs/GaAs quantum dots (QDs) grown by metal-organic chemical vapour deposition and emitting at the 1300 nm telecommunication window. Single QD properties have been determined experimentally for a number of nanostructures by means of excitation-power-dependent and polarization-resolved microphotoluminescence and further compared with the results of confined states calculations employing the 8-band kp theory combined with the confi…
We report experimental evidence identifying acoustic phonons as the principal source of the excitation-induced-dephasing (EID) responsible for the intensity damping of quantum dot excitonic Rabi rotations. The rate of EID is extracted from temperature dependent Rabi rotation measurements of the ground-state excitonic transition, and is found to be in close quantitative agreement with an acoustic-phonon model.
We present results of atomistic empirical pseudopotential calculations and configuration interaction for excitons, positive and negative trions (X\pm), positive and negative quartons (X2\pm) and biexcitons. The structure investigated are laterally aligned InGaAs quantum dot molecules embedded in GaAs under a lateral electric field. The rather simple energetic of excitons becomes more complex in the case of charged quasiparticles but remains tractable. The negative trion spectrum shows four anticrossings in the presently available range of fields while the positive trion shows two. The magnitud…
In this paper, we study the exciton absorption spectra in InGaAs prolate ellipsoidal quantum dots when a strong pump laser resonant with electron quantized levels is active. Our obtained results by renormalized wavefunction theory show that, under suitable conditions, the initial exciton absorption peak is split into two new peaks as the evidence of the existence of the three-level optical Stark effect of excitons. We have suggested an explanation of the origin of the effect as well as investigating the effect of pump field energy, size, and geometric shape of the quantum dots on effect charac…
Recently, longitudinal acoustic phonons have been identified as the main source of the intensity damping observed in Rabi rotation measurements of the ground-state exciton of a single InAs/GaAs quantum dot. Here we report experiments of intensity damped Rabi rotations in the case of detuned laser pulses, the results have implications for the coherent optical control of both excitons and spins using detuned laser pulses.
Photoluminescence (PL) and reflectivity spectra of a high-quality InGaAs/GaAs quantum well structure reveal a series of ultra-narrow peaks attributed to the quantum confined exciton states. The intensity of these peaks decreases as a function of temperature, while the linewidths demonstrate a complex and peculiar behavior. At low pumping the widths of all peaks remain quite narrow ($< 0.1$ meV) in the whole temperature range studied, $4 - 30K$. At the stronger pumping, the linewidth first increases and than drops down with the temperature rise. Pump-probe experiments show two characteristic ti…
We study light emission properties of a population-inverted 2D electron-hole plasma in a quantizing magnetic field. We observe a series of superfluorescent bursts, discrete both in time and energy, corresponding to the cooperative recombination of electron-hole pairs from different Landau levels. The emission energies are strongly renormalized due to many-body interactions among the photogenerated carriers, exhibiting red-shifts as large as 20 meV at 15 T. However, the magnetic field dependence of the lowest Landau level emission line remains excitonic at all magnetic fields. Interestingly, ou…
We study experimentally the dependence of dynamic nuclear spin polarization on the power of non-resonant optical excitation in two types of individual neutral semiconductor quantum dots: InGaAs/GaAs and GaAs/AlGaAs. We show that the mechanism of nuclear spin pumping via second order recombination of optically forbidden (''dark'') exciton states recently reported in InP/GaInP quantum dots [Phys. Rev. B 83, 125318 (2011)] is relevant for material systems considered in this work. In the InGaAs/GaAs dots this nuclear spin polarization mechanism is particularly pronounced, resulting in Overhauser s…
The Stranski-Krastanov (SK) growth-mode facilitates the self-assembly of quantum dots (QDs) using lattice-mismatched semiconductors, for instance InAs and GaAs. SK QDs are defect-free and can be embedded in heterostructures and nano-engineered devices. InAs QDs are excellent photon emitters: QD-excitons, electron-hole bound pairs, are exploited as emitters of high quality single photons for quantum communication. One significant drawback of the SK-mode is the wetting layer (WL). The WL results in a continuum rather close in energy to the QD-confined-states. The WL-states lead to unwanted scatt…
Non-linear Zeeman splitting of neutral excitons is observed in composition engineered In(x)Ga(1-x)As self-assembled quantum dots and its microscopic origin is explained. Eight-band k.p simulations, performed using realistic dot parameters extracted from cross-sectional scanning tunneling microscopy, reveal that a quadratic contribution to the Zeeman energy originates from a spin dependent mixing of heavy and light hole orbital states in the dot. The dilute In-composition (x<0.35) and large lateral size (40-50 nm) of the quantum dots investigated is shown to strongly enhance the non-linear exci…
We have observed the Zeeman-split excited state of a spin-1/2 multi-electron Si/SiGe depletion quantum dot and measured its spin relaxation time T1 in magnetic fields up to 2 T. Using a new step-and-reach technique, we have experimentally verified the g-value of 2.0 +/- 0.1 for the observed Zeeman doublet. We have also measured T1 of single- and multi-electron spins in InGaAs quantum dots. The lifetimes of the Si/SiGe system are appreciably longer than those for InGaAs dots for comparable magnetic field strengths, but both approach one second at sufficiently low fields (< 1 T for Si, and < 0.2…
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and tripl…
We investigated the electron transport property of the InGaAs/GaAs double quantum dots, the electron g-factors of which are different from each other. We found that in a magnetic field, the resonant tunneling is suppressed even if one of the Zeeman sublevels is aligned. This is because the other misaligned Zeeman sublevels limit the total current. A finite broadening of the misaligned sublevel partially relieves this bottleneck effect, and the maximum current is reached when interdot detuning is half the Zeeman energy difference.
Photoluminescence (PL) and highly circularly-polarized magneto-PL (up to 50% at 6 T) from two-step bandgap InAs/InGaAs/InAlAs quantum wells (QWs) are studied. Bright PL is observed up to room temperature, indicating a high quantum efficiency of the radiative recombination in these QW. The sign of the circular polarization indicates that it stems from the spin polarization of heavy holes caused by the Zeeman effect. Although in magnetic field the PL line are strongly circularly polarized, no energy shift between the counter-polarized PL lines was observed. The results suggest that the electron …
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…
We present a comprehensive optical study of the excitonic Zeeman effects in transition metal dichalcogenide monolayers, which are discussed comparatively for selected materials: MoSe$_2$, WSe$_2$ and WS$_2$. We introduce a simple semi-phenomenological description of the magnetic field evolution of individual electronic states in fundamental sub-bands by considering three additive components: valley, spin and orbital terms. We corroborate the validity of the proposed description by inspecting the Zeeman-like splitting of neutral and charged excitonic resonances in absorption-type spectra. The v…
Exciton spin and related optical polarization in self-assembled InAs/In$_{0.53}$Ga$_{0.23}$Al$_{0.24}$As/InP(001) quantum dashes emitting at 1.55 μm are investigated by means of polarization- and time-resolved photoluminescence, as well as photoluminescence excitation spectroscopy, at cryogenic temperature. We investigate the influence of highly non-resonant and quasi-resonant optical spin pumping conditions on spin polarization and spin memory of the quantum dash ground state. We show that a spin pumping scheme, utilizing the longitudinal-optical-phonon-mediated coherent scattering process, c…
The observation of spin-related phenomena of microcavity polaritons has been limited due to weak Zeeman effect of non-magnetic semiconductors. We demonstrate that the incorporation of magnetic ions into quantum wells placed in a non-magnetic microcavity results in enhanced effects of magnetic field on exciton-polaritons. We show that in such a structure the Zeeman splitting of exciton-polaritons strongly depends on the photon - exciton detuning and polariton wavevector. Our experimental data are explained by a model where the impact of magnetic field on the lower polariton state is directly in…
Using integrated superconducting single photon detectors we probe ultra-slow exciton capture and relaxation dynamics in single self-assembled InGaAs quantum dots embedded in a GaAs ridge waveguide. Time-resolved luminescence measurements performed with on- and off-chip detection reveal a continuous decrease in the carrier relaxation time from 1.22 $\pm$ 0.07 ns to 0.10 $\pm$ 0.07 ns upon increasing the number of non-resonantly injected carriers. By comparing off-chip time-resolved spectroscopy with spectrally integrated on-chip measurements we identify the observed dynamics in the rise time ($…
Charge carriers in two-dimensional transition metal dichalcogenides (TMDs), such as WSe$_2$, have their spin and valley-pseudospin locked into an optically-addressable index that is proposed as a basis for future information processing. The manipulation of this spin-valley index requires tuning its energy, typically through external magnetic field (B), which is cumbersome. Thus, other efficient routes like all-optical control of spin-valley index are desirable. Here, we show that many-body interactions amongst interlayer excitons in WSe$_2$/MoSe$_2$ heterobilayer induce a steady-state valley Z…
The dependence of the excitonic photoluminescence (PL) spectrum of monolayer transition metal dichalcogenides (TMDs) on the tilt angle of an applied magnetic field is studied. Starting from a four-band Hamiltonian we construct a theory which quantitatively reproduces the available experimental PL spectra for perpendicular and in-plane magnetic fields. In the presence of a tilted magnetic field, we demonstrate that the dark exciton PL peaks brighten due to the in-plane component of the magnetic field and split for light with different circular polarization as a consequence of the perpendicular …
We report on the experimental and theoretical investigation of magnetic-field-induced second harmonic generation (SHG) and two-photon absorption (TPA) of excited exciton states ($n \geq 3$) of the yellow series in Cu$_2$O. In this centrosymmetric material, SHG can occur due to constructive interplay of electric dipole and electric quadrupole/magnetic dipole transitions for light propagating along the low-symmetry directions [111] or [112]. By application of a magnetic field in Voigt configuration, SHG gets also allowed for excitation along the [110]-axis and even the high-symmetry cubic direct…
We demonstrate fast initialization of a single hole spin captured in an InGaAs quantum dot with a fidelity F>99% by applying a magnetic field parallel to the growth direction. We show that the fidelity of the hole spin, prepared by ionization of a photo-generated electron-hole pair, is limited by the precession of the exciton spin due to the anisotropic exchange interaction.
We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of $\mp$ 0.12 meV/T for emission arising, respectively, from the K and K' valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley degeneracy. The magnitude of the Zeeman shift agrees with predicted magnetic moments for carriers in the conduction and valence bands. The relative intensity of neutral and charged exciton emission is m…
We study optically driven Rabi rotations of a quantum dot exciton transition between 5 and 50 K, and for pulse-areas of up to $14π$. In a high driving field regime, the decay of the Rabi rotations is nonmonotonic, and the period decreases with pulse-area and increases with temperature. By comparing the experiments to a weak-coupling model of the exciton-phonon interaction, we demonstrate that the observed renormalization of the Rabi frequency is induced by fluctuations in the bath of longitudinal acoustic phonons, an effect that is a phonon analogy of the Lamb-shift.
Trion quantum coherence in site-controlled pyramidal InGaAs quantum dots
Department of Physics, University of Strathclyde（斯特拉斯克莱德大学物理系）；Sussex Centre for Quantum Technologies, University of Sussex（苏塞克斯大学苏塞克斯量子技术中心）；Tyndall National Institute, University College Cork（科克大学学院廷德尔国家研究所）
Monolayers and multilayers of semiconducting transition metal dichalcogenides (TMDCs) offer an ideal platform to explore valley-selective physics with promising applications in valleytronics and information processing. Here we manipulate the energetic degeneracy of the $\mathrm{K}^+$ and $\mathrm{K}^-$ valleys in few-layer TMDCs. We perform high-field magneto-reflectance spectroscopy on WSe$_2$, MoSe$_2$, and MoTe$_2$ crystals of thickness from monolayer to the bulk limit under magnetic fields up to 30 T applied perpendicular to the sample plane. Because of a strong spin-layer locking, the gro…
The electron-phonon coupling in self-assembled InGaAs quantum dots is relatively weak at low light intensities, which means that the zero-phonon line in emission is strong compared to the phonon sideband. However, the coupling to acoustic phonons can be dynamically enhanced in the presence of an intense optical pulse tuned within the phonon sideband. Recent experiments have shown that this dynamic vibronic coupling can enable population inversion to be achieved when pumping with a blue-shifted laser and for rapid de-excitation of an inverted state with red detuning. In this paper we confirm th…
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…
We report circularly-polarized optical reflection spectroscopy of monolayer WS$_2$ and MoS$_2$ at low temperatures (4~K) and in high magnetic fields to 65~T. Both the A and the B exciton transitions exhibit a clear and very similar Zeeman splitting of approximately $-$230~$μ$eV/T ($g\simeq -4$), providing the first measurements of the valley Zeeman effect and associated $g$-factors in monolayer transition-metal disulphides. These results complement and are compared with recent low-field photoluminescence measurements of valley degeneracy breaking in the monolayer diselenides MoSe$_2$ and WSe$_…
We study the zero-temperature phase diagram and fractional excitation when a thin film of 3D topological insulator has two competing masses: T- symmetric exciton condensation and T- breaking Zeeman effect. Two topologically distinct phases are identified: in one, the quasiparticles can be viewed as in a quantum spin Hall phase, and in the other a quantum anomalous Hall phase. The vortices of the exciton order parameter can carry fractional charge and statistics of electrons in both phases. When the system undergoes the quantum phase transition between these two phases, the charges, statistics …
We calculate the emission spectrum of neutral and charged excitons in a pair of laterally coupled InGaAs quantum dots with nearly degenerate energy levels. As the interdot distance decreases, a number of changes take place in the emission spectrum which can be used as indications of molecular coupling. These signatures ensue from the stronger tunnel-coupling of trions as compared to that of neutral excitons.
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…
We consider theoretically a system of exciton-polariton micropillars arranged in a honeycomb lattice. The naturally present TE-TM splitting and an alternating Zeeman splitting, where the different sublattices experience opposite Zeeman splitting, shifts the Dirac points in energy, giving rise to antichiral behavior. In a strip geometry having zigzag edges, two pairs of edge states exist and propagate in the same direction (including the states at the opposite edges). The edge modes localized at the opposite edges have opposite spins (circular polarizations), which leads to co-propagating "+-" …
The theory for light-hole Zeeman splitting developed in [Physica E 44, 797 (2012)] is compared with experimental data found in literature for GaAs/AlGaAs, InGaAs/InP and CdTe/CdMgTe quantum wells. It is shown that the description of experiments is possible with account for excitonic effects and peculiarities of the hole energy spectrum in a quantum well including complex structure of the valence band and the interface mixing of light and heavy holes. It is demonstrated that the absolute values and the sign of the light-hole $g$-factor are extremely sensitive to the parametrization of the Lutti…
We show how resonant laser spectroscopy of the trion optical transitions in a self-assembled quantum dot can be used to determine the temperature of a nearby electron reservoir. At finite magnetic field the spin-state occupation of the Zeeman-split quantum dot electron ground states is governed by thermalization with the electron reservoir via co-tunneling. With resonant spectroscopy of the corresponding excited trion states we map out the spin occupation as a function of magnetic field to establish optical thermometry for the electron reservoir. We demonstrate the implementation of the techni…
Magnetically doped semiconductors are well known for their giant Zeeman splittings which can reach several meV even in relatively small external magnetic fields. After preparing a nonequilibrium exciton distribution via optical excitation, the spin dynamics in diluted magnetic semiconductor quantum wells is typically governed by spin-flip scattering processes due to the exciton-impurity exchange interaction. Our theoretical calculations show that the giant Zeeman splitting in these materials in combination with the influence of longitudinal acoustic phonons lead to a quantum ratchet-type dynam…
