Spin beats in the photoluminescence polarization dynamics of charged excitons in InP/(In,Ga)P quantum dots in presence of nuclear quadrupole interaction
S. V. Nekrasov, I. A. Akimov, Yu. G. Kusrayev, D. R. Yakovlev, M. Bayer
The spin dynamics of positively (X$^{+}$) and negatively (X$^{-}$) charged excitons in InP/In$_{0.48}$Ga$_{0.52}$P quantum dots subject to a magnetic field is studied. We find that a characteristic feature of the system under study is the presence of nuclear quadrupole interaction, which leads to stabilization of the nuclear and electron spins in a quantum dot in zero external magnetic field. In detail, the nuclear quadrupole interaction leads to pinning of the Overhauser field along the quadrupole axis, which is close to the growth axis of the heterostructure. The nuclear effects are observed only when resident electrons are confined in the quantum dots, i.e. for X$^{-}$ trion photoexcitation. The presence of X$^{-}$ and X$^{+}$ trion contributions to the photoluminescence together with the quadrupole interaction significantly affects the dynamics of optical orientation in Voigt magnetic field. In absence of dynamic nuclear spin polarization the time evolution of the photoluminescence polarization was fitted by a form which describes the electron spin relaxation in "frozen" nuclear field fluctuations. In relatively large external magnetic fields exceeding 60 mT good agreement between theory and experiment is achieved.
Color centers in hexagonal boron nitride (hBN) show stable single photon emission even at room temperature, making these systems a promising candidate for quantum information applications. Besides this remarkable property, also their interaction with longitudinal optical (LO) phonons is quite unique because they lead to dominant phonon sidebands (PSBs), well separated from the zero phonon line (ZPL). In this work we utilize this clear spectral separation to theoretically investigate the influence of phonon decay dynamics on time-dependent photoluminescence (PL) signals. Our simulations show, t…
We propose an unconventional scheme of photoluminescence in a semiconductor thin film, where the nonlocal correlation between an excitonic wave and a light wave prominently enhances the exciton-light coupling beyond the long-wavelength approximation (the so-called excitonic superradiance regime). On the basis of the developed method extending input-output theory, we elucidate atypical photoluminescence effects due to the strong wave-wave correlation. In particular, the up-converted photoluminescence based on the coherent superposition of excitons is found to be highly efficient, i.e., it can b…
We investigate the thermal quenching of the multimodal photoluminescence from InAs/InP (001) self-assembled quantum dots. The temperature evolution of the photoluminescence spectra of two samples is followed from 10 K to 300 K. We develop a coupled rate-equation model that includes the effect of carrier thermal escape from a quantum dot to the wetting layer and to the InP matrix, followed by transport, recapture or non-radiative recombination. Our model reproduces the temperature dependence of the emission of each family of quantum dots with a single set of parameters. We find that the main es…
The demonstration of strong photoluminescence polarization anisotropy in semiconducting nanowires embodies both technological promise and scientific challenge. Here we present progress on both fronts through the study of the photoluminescence polarization anisotropy of randomly oriented nanowire ensembles in materials without/with crystalline anisotropy, small/wide bandgap, and both III-V/II-VI chemistry (InP/ZnO nanowires, respectively). Comprehensive control of the polarization anisotropy is realized by dielectric matching with conformally deposited Ta2O5 (dielectric ratios of 9.6:4.41 and 4…
Kinetics of polarized photoluminescence of the negatively charged InP quantum dots in weak magnetic field is studied experimentally. Effect of both the nuclear spin fluctuations and the dynamical nuclear polarization on the electron spin orientation is observed.
We have studied the size dependence of the exciton g-factor in self-assembled InAs/InP quantum dots. Photoluminescence measurements on a large ensemble of these dots indicate a multimodal height distribution. Cross-sectional Scanning Tunneling Microscopy measurements have been performed and support the interpretation of the macro photoluminescence spectra. More than 160 individual quantum dots have systematically been investigated by analyzing single dot magneto-luminescence between 1200nm and 1600 nm. We demonstrate a strong dependence of the exciton g-factor on the height and diameter of the…
Thermal quenching is one of the essential factors in reducing the efficiency of radiative processes in luminophores of various nature. The emission activity of low dimensional structures is influenced also by multiplicity of parameters that are related to synthesis processes, treatment regimes, etc. In the present work, we have investigated the temperature dependence of photoluminescence caused by exciton and defect-related transitions in ensembles of biocompatible InP/ZnS core/shell nanocrystals with an average size of 2.1 and 2.3 nm. The spread in the positions of energy levels is shown to b…
We have fabricated an array of closely spaced quantum dashes starting from a planar array of self-assembled semiconductor quantum wires. The array is embedded in a metallic nanogap which we investigate by micro-photoluminescence as a function of a lateral electric field. We demonstrate that the net electric charge and emission energy of individual quantum dashes can be modified externally with performance limited by the size inhomogeneity of the self-assembling process.
We report on the coherent dynamics of the spin of an individual magnetic atom coupled to carriers in a semiconductor quantum dot which has been investigated by resonant photoluminescence of the positively charged exciton (X+). We demonstrate that a positively charged CdTe/ZnTe quantum dot doped with a single Mn atom forms an ensemble of optical Lambda systems which can be addressed independently. We show that the spin dynamics of the X+Mn complex is dominated by the electron-Mn exchange interaction and report on the coherent dynamics of the electron-Mn spin system that is directly observed in …
Effects of both the dynamic nuclear polarization (DNP) created by circularly polarized light and the fluctuations of average nuclear spin in a quantum dot (QD) on the electron spin orientation are studied for singly negatively charged InP QDs. From the dependence of the negative circular polarization of photoluminescence on the applied longitudinal magnetic field, the hyperfine field B_N of a few mT appearing due to DNP and the effective magnetic field B_f of a few tens of mT arising from nuclear spin fluctuations (NSF) are estimated. A lifetime of about 1 microsecond is estimated for NSF.
Isolated InAs/InP self-assembled quantum wires have been grown using in situ accumulated stress measurements to adjust the optimal InAs thickness. Atomic force microscopy imaging shows highly asymmetric nanostructures with average length exceeding more than ten times their width. High resolution optical investigation of as-grown samples reveals strong photoluminescence from individual quantum wires at 1.5 microns. Additional sharp features are related to monolayer fluctuations of the two dimensional InAs layer present during the early stages of the quantum wire self-assembling process.
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…
We report millisecond-range spin memory of resident electrons in an ensemble of InP quantum dots (QDs) under a small magnetic field of 0.1 T applied along the optical excitation axis at temperatures up to about 5 K. A pump-probe photoluminescence (PL) technique is used for optical orientation of electron spins by the pump pulses and for study of spin relaxation over the long time scale by measuring the degree of circular polarization of the probe PL as a function of pump-probe delay. Dependence of spin decay rate on magnetic field and temperature suggests two-phonon processes as the dominant s…
Optical transitions in coupled InAs/InP self-assembled quantum wires are studied within the single-band effective mass approximation including effects due to strain. Both vertically and horizontally coupled quantum wires are investigated and the ground state, excited states and the photoluminescence peak energies are calculated. Where possible we compare with available photo-luminescence data from which it was possible to determine the height of the quantum wires. An anti-crossing of the energy of excited states is found for vertically coupled wires signaling a change of symmetry of the excito…
We demonstrate control by applied electric field of the charge states in single self-assembled InP quantum dots placed in GaInP Schottky structures grown by metalorganic vapor phase epitaxy. This has been enabled by growth optimization leading to suppression of formation of large dots uncontrollably accumulating charge. Using bias- and polarization-dependent micro-photoluminescence, we identify the exciton multi-particle states and carry out a systematic study of the neutral exciton state dipole moment and polarizability. This analysis allows for the characterization of the exciton wavefunctio…
Experimental investigation of nuclear spin effects on the electron spin polarization in singly negatively charged InP quantum dots is reported. Pump-probe photoluminescence measurements of electron spin relaxation in the microsecond timescale are used to estimate the time-period $T_{N}$ of the Larmor precession of nuclear spins in the hyperfine field of electrons. We find $T_{N}$ to be $\sim 1$ $μ$s at $T \approx 5$ K, under the vanishing external magnetic field. From the time-integrated measurements of electron spin polarization as a function of a longitudinally applied magnetic field at $T \…
We investigate the long wavelength (1.2 to 1.55 micro-m) photoluminescence of high-density InAs quantum dots and dashes, which were grown on InP substrates. We analyze the temperature dependence of the recombination and carrier distribution on the alloy composition of the barrier materials, InGaAlAs, and on the existence of a wetting layer. Carrier escape and transfer are discussed based on temperature dependent photoluminescence measurements and theoretical considerations about the heterostructures' confinement energies and band structure. We propose two different contributions to the thermal…
The spin splitting of conduction band electrons in inversion-asymmetric InGaAs/InP quantum wells is studied by Shubnikov-de Haas measurements combining the analysis of beating patterns and coincidence measurements in doubly tilted magnetic fields. The method allows us to determine the absolute values of the Rashba and linear Dresselhaus spin-orbit interaction coefficients, their relative sign and the full Landé g-tensor. This is achieved by analyzing the anisotropy of the beat node positions with respect to both polar and azimuthal angles between the magnetic field direction and the quantum we…
We report on both experimental and theoretical study of conduction-electron spin polarization dynamics achieved by pulsed optical pumping at room temperature in GaAs(1-x)N(x) alloys with a small nitrogen content (x = 2.1, 2.7, 3.4%). It is found that the photoluminescence circular polarization determined by the mean spin of free electrons reaches 40-45% and this giant value persists within 2 ns. Simultaneously, the total free-electron spin decays rapidly with the characteristic time ~150 ps. The results are explained by spin-dependent capture of free conduction electrons on deep paramagnetic c…
Photoluminescence data from single, self-assembled InAs/InP quantum dots in magnetic fields up to 7 T are presented. Exciton g-factors are obtained for dots of varying height, corresponding to ground state emission energies ranging from 780 meV to 1100 meV. A monotonic increase of the g-factor from -2 to +1.2 is observed as the dot height decreases. The trend is well reproduced by sp3 tight binding calculations, which show that the hole g-factor is sensitive to confinement effects through orbital angular momentum mixing between the light-hole and heavy-hole valence bands. We demonstrate tunabi…
We use photoluminescence spectroscopy of ''bright'' and ''dark'' exciton states in single InP/GaInP quantum dots to measure hyperfine interaction of the valence band hole with nuclear spins polarized along the sample growth axis. The ratio of the hyperfine constants for the hole (C) and electron (A) is found to be C/A~-0.11. In InP dots the contribution of spin 1/2 phosphorus nuclei to the hole-nuclear interaction is weak, which enables us to determine experimentally the value of C for spin 9/2 indium nuclei as C_In~-5 micro-eV. This high value of C is in good agreement with recent theoretical…
The coupling between Zeeman spin splitting and Rashba spin-orbit terms has been studied experimentally in a gated InGaAs/InP quantum well structure by means of simultaneous measurements of the weak antilocalization (WAL) effect and beating in the SdH oscillations. The strength of the Zeeman splitting was regulated by tilting the magnetic field with the spin-zeros in the SdH oscillations, which are not always present, being enhanced by the tilt. In tilted fields the spin-orbit and Zeeman splittings are not additive, and a simple expression is given for the energy levels. The Rashba parameter an…
The groundstate properties of an exciton in a self-assembled quantum disk are calculated in the presence of a perpendicular magnetic field. For sufficient wide and thin dots, the strain field leads to a confinement of the heavy hole within the dot and the system is type I, while the light hole is confined outside the dot and the system is type II. However, with increasing disk thickness, the strain induces a transition of the heavy hole from inside the disk towards the radial boundary outside the disk. For the exciton, we predict a heavy-hole to light-hole transition as a function of the disk …
Crystal-phase low-dimensional structures offer great potential for the implementation of photonic devices of interest for quantum information processing. In this context, unveiling the fundamental parameters of the crystal phase structure is of much relevance for several applications. Here, we report on the anisotropy of the g-factor tensor and diamagnetic coefficient in wurtzite/zincblende (WZ/ZB) crystal-phase quantum dots (QDs) realized in single InP nanowires. The WZ and ZB alternating axial sections in the NWs are identified by high-angle annular dark-field scanning transmission electron …
Single strain-induced quantum dots are isolated for optical experiments by selective removal of the inducing InP islands from the sample surface. Unpolarized emission of single, bi- and triexciton transitions are identified by power-dependent photoluminescence spectroscopy. Employing time-resolved experiments performed at different excitation powers we find a pronounced shift of the rise and decay times of these different transitions as expected from cascaded emission. Good agreement is found for a rate equation model for a three step cascade.
