We show that in cubic crystals with anisotropic impurity centers the sum of squares of the magnetic resonance [electron paramagnetic resonance (EPR)] frequencies is invariant with respect to the magnetic field direction. The connection between such an invariant and the g-tensor components of the impurity is derived for different types of centers. The established regularity is confirmed experimentally for the spin-noise spectra of a cubic CaF2-Nd3+ crystal. We show how this property of the EPR spectra can be efficiently used for the assignment of paramagnetic centers in cubic crystals. © 2022 American Physical Society.

Qubits based on crystal defect centers have been shown to exhibit long spin coherence times, up to seconds at room temperature. However, they are typically characterized by a comparatively slow initialization timescale. Here, fluorine implantation into ZnSe epilayers is used to induce defect states that are identified as zinc vacancies. We study the carrier spin relaxation in these samples using various pump-probe measurement methods, assessing phenomena such as resonant spin amplification, polarization recovery, and spin inertia in transverse or longitudinal magnetic field. The spin dynamics in isotopically natural ZnSe show a significant influence of the nuclear spin bath. Removing this source of relaxation by using isotopic purification, we isolate the anisotropic exchange interaction as the main spin dephasing mechanism and find spin coherence times of 100 ns at room temperature, with the possibility of fast optical access on the picosecond time scales through excitonic transitions of ZnSe. © 2021, The Author(s).

The spin-noise spectroscopy (SNS) method implies high efficiency of conversion of the spin-system magnetization to the Faraday rotation angle. Generally, this efficiency cannot be estimated using the characteristics of the regular magnetooptical activity of a paramagnet. However, it may be drastically enhanced in systems with strong inhomogeneous broadening of the optical transitions. This enhancement leads to the giant spin-noise gain effect and previously allowed one to apply the SNS to rare-earth activated crystals. We show that the nonlinear resonant Faraday effect can be used to measure the homogeneous width of the inhomogeneously broadened transition and, thus, to estimate the applicability of the SNS to this type of paramagnet. We present the theoretical description of the effect and perform measurements on intraconfigurational (4f-4f) transitions of the trivalent rare-earth ions of neodymium and ytterbium in fluorite-based crystals. The proposed experimental approach establishes new links between the effects of nonlinear optics and spin-noise characteristics of crystals with paramagnetic impurities and offers new methods of research in the physics of impurity crystals. © 2021 American Physical Society.

We demonstrate the realization of the resonant spin amplification (RSA) effect in Faraday geometry where a magnetic field is applied parallel to the optically induced spin polarization so that no RSA is expected. However, model considerations predict that it can be realized for a central spin interacting with a fluctuating spin environment. As a demonstrator, we choose an ensemble of singly-charged (In,Ga)As/GaAs quantum dots, where the resident electron spins interact with the surrounding nuclear spins. The observation of RSA in Faraday geometry requires intense pump pulses with a high repetition rate and can be enhanced by means of the spin-inertia effect. Potentially, it provides the most direct and reliable tool to measure the longitudinal g factor of the charge carriers. © 2021 American Physical Society.

The dynamics of the coupled electron-nuclear spin system is studied in an ensemble of singly charged (In,Ga)As/GaAs quantum dots (QDs) using periodic optical excitation at 1 GHz repetition rate. In combination with the electron-nuclei interaction, the highly repetitive excitation allows us to lock the electron spins into magnetic resonance in a transverse external magnetic field. Sweeping the field to higher values, the locking leads to an effective "diamagnetic"response of significant strength due to dynamic nuclear polarization, which shields the QD electrons at least partly from the external field and can even keep the internal magnetic field constant up to 1.3 T field variation. We model the effect through a magnetic field-dependent polarization rate of the nuclei, from which we suggest a strategy for adjusting the nuclear polarization through the detuning between optical excitation and electronic transition, in addition to tuning the magnetic field. © 2021 American Physical Society.

The coherent electron spin dynamics of an ensemble of singly charged (In,Ga)As/GaAs quantum dots in a transverse magnetic field is driven by periodic optical excitation at 1 GHz repetition frequency. Despite the strong inhomogeneity of the electron g factor, the spectral spread of optical transitions, and the broad distribution of nuclear spin fluctuations, we are able to push the whole ensemble of excited spins into a single Larmor precession mode that is commensurate with the laser repetition frequency. Furthermore, we demonstrate that an optical detuning of the pump pulses from the probed optical transitions induces a directed dynamic nuclear polarization and leads to a discretization of the total magnetic field acting on the electron ensemble. Finally, we show that the highly periodic optical excitation can be used as universal tool for strongly reducing the nuclear spin fluctuations and preparation of a robust nuclear environment for subsequent manipulation of the electron spins, also at varying operation frequencies. © 2021, The Author(s).

Fundamental properties of the spin-noise signal formation in a quantum-dot microcavity are studied by measuring the angular characteristics of the scattered light intensity. A distributed Bragg reflector microcavity was used to enhance the light-matter interaction with an ensemble of n-doped (In,Ga)As/GaAs quantum dots, which allowed us to study subtle effects of coherent scattering at the quantum dot ensemble. Detecting the scattered light outside of the aperture of the transmitted light, we measured the basic electron spin properties, such as g factor and spin dephasing time. Further, we investigated the influence of the microcavity on the scattering distribution and possibilities of signal amplification by additional resonant excitation. © 2020 American Physical Society.

We report on theoretical and experimental study of the spin polarization recovery and Hanle effect for the charge carriers interacting with the fluctuating nuclear spins in the semiconductor structures. We start the theoretical description from the simplest model of static and isotropic nuclear spin fluctuations. Then we describe the modification of the polarization recovery and Hanle curves due to the anisotropy of the hyperfine interaction, finite nuclear spin correlation time, and the strong pulsed spin excitation. For the latter case, we predict the appearance of the resonant spin amplification in the Faraday geometry and of the quantum Zeno effect. The set of the experimental results for various structures and experimental conditions is chosen to highlight the specific effects predicted theoretically. We show that the joint analysis of the spin polarization recovery and the Hanle effect is a very valuable tool for addressing carrier spin dynamics in semiconductors and their nanostructures. © 2020 American Physical Society.

Nuclear spin coherence and relaxation dynamics of all constituent isotopes of an n-doped CdTe/(Cd,Mg)Te quantum well structure are studied employing optically detected nuclear magnetic resonance. Using time-resolved pump-probe Faraday ellipticity, we generate and detect the coherent spin dynamics of the resident electrons. The photogenerated electron spin polarization is transferred into the nuclear spin system, which becomes polarized and acts back on the electron spins as the Overhauser field. Under the influence of resonant radio frequency pulses, we trace the coherent spin dynamics of the nuclear isotopes Cd111, Cd113, and Te125. We measure nuclear Rabi oscillations, the inhomogeneous dephasing time T2∗, the spin coherence time T2, and the longitudinal relaxation time T1. Furthermore, we investigate the influence of the laser excitation and the corresponding electron spin polarization on the nuclear spin relaxation time and find a weak extension of this time induced by interaction with the electron spins. © 2019 American Physical Society.

The coherent spin dynamics of resident electrons and holes in an isotopically purified ZnSe/(Zn,Mg)Se single quantum well is investigated in different regimes, requiring corresponding adaption of the applied time-resolved pump-probe Kerr rotation technique. The purification of the Zn and Se atom species in the crystal to the isotopes with zero nuclear spin is expected to lead to an extension of the spin dephasing times of resident carriers, due to the suppression of their interaction with the nuclear spins. Indeed, we find no indication of carrier-nuclear interaction in this sample and link the observed carrier spin relaxation to the spin-orbit interaction. Theoretical considerations support the experimental results. © 2019 American Physical Society.

In spin noise spectroscopy, the magnetic susceptibility spectrum is known to be provided by the spin-system untouched by any external perturbation, or, better to say, disturbed only by its thermal bath. We propose a new version of spin noise spectroscopy, with the detected magnetization (Faraday-rotation) noise being "stimulated" by an external fluctuating magnetic field with a quasiwhite spectrum. An experimental study of the stimulated spin noise performed on a BaF 2: U 3 + crystal in a longitudinal magnetic field has revealed specific features of this approach and allowed us to identify the Van-Vleck and population-related contributions to the AC susceptibility of the system and to discover unusual magnetic-field dependence of the longitudinal spin relaxation rate in low magnetic fields. It is shown that spectra of the stimulated and spontaneous spin noise, being both closely related to the spin-system magnetic susceptibility, are still essentially different. Distinctions between the two types of the spin-noise spectra and two approaches to spin noise spectroscopy are discussed. © 2019 Author(s).

This work is devoted to a theoretical analysis of the effect of nuclear-induced field (Overhauser field) on the Larmor frequencies of electron spins under the periodic pulsed excitation. To describe the dynamical nuclear spin polarization, we use the model where the optically induced Stark field determines the magnitude and direction of the Overhauser field. The Stark field strongly depends on the detuning between the photon energy of excitation and the optical transition energy in the quantum system. Detailed calculations which show that the precession frequencies of fluorine donor-bound electron spins in ZnSe deviate from the linear dependence of the Larmor frequencies on the external magnetic field have been performed. A similar effect is observed for the (In,Ga)As/GaAs quantum dots, where it has been shown that the Overhauser field strongly changes the spectrum of the electron spin precession frequencies. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

The periodic optical orientation of electron spins in (In,Ga)As/GaAs quantum dots leads to the formation of electron spin precession modes about an external magnetic field which are resonant with the pumping periodicity. As the electron spin is localized within a nuclear spin bath, its polarization imprints onto the spin polarization of the bath. The latter acts back on the electron spin polarization. We implement a pulse protocol where a train of laser pulses is followed by a long, dark gap. It allows us to obtain a high-resolution precession mode spectrum from the free evolution of the electron spin polarization. Additionally, we vary the number of pump pulses in a train to investigate the buildup of the precession modes. To separate out nuclear effects, we suppress the nuclear polarization by using a radio-frequency field. We find that a long-living nuclear spin polarization imprinted by the periodic excitation significantly speeds up the buildup of the electron spin polarization and induces the formation of additional electron spin precession modes. To interpret these findings, we extend an established dynamical nuclear polarization model to take into account optically detuned quantum dots for which nuclear spins activate additional electron spin precession modes. © 2018 American Physical Society.

The coherent spin dynamics of fluorine donor-bound electrons in ZnSe induced by pulsed optical excitation is studied in a perpendicular applied magnetic field. The Larmor precession frequency serves as a measure for the total magnetic field exerted onto the electron spins and, surprisingly, does not increase linearly with the applied field, but shows a step-like behavior with pronounced plateaus, given by multiples of the laser repetition rate. This discretization occurs by a feedback mechanism in which the electron spins polarize the nuclear spins, which in turn generate a local Overhauser field adjusting the total magnetic field accordingly. Varying the optical excitation power, we can control the plateaus, in agreement with our theoretical model. From this model, we trace the observed discretization to the optically induced Stark field, which causes the dynamic nuclear polarization. © 2018 The Author(s).

We implement the homodyne detection scheme for an increase in the polarimetric sensitivity in spin noise spectroscopy. Controlling the laser intensity of the local oscillator, which is guided around the sample and does not perturb the measured spin system, we are able to improve the signal-to-noise ratio. The opportunity for additional amplification of the measured signal strength allows us to reduce the probe laser intensity incident on the sample and therefore to approach the nonperturbative regime. The efficiency of this scheme with signal enhancement by more than a factor of 3 at low probe powers is demonstrated on bulk n-doped GaAs, where the reduced electron-spin relaxation rate is shown experimentally. Additionally, the control of the optical phase provides us with the possibility to switch between measuring Faraday rotation and ellipticity without changes in the optical setup. © 2018 American Physical Society.

Periodic laser pulsing of singly charged semiconductor quantum dots in an external magnetic field leads to a synchronization of the spin dynamics with the optical excitation. The pumped electron spins partially rephase prior to each laser pulse, causing a revival of electron spin polarization with its maximum at the incidence time of a laser pulse. The amplitude of this revival is amplified by the frequency focusing of the surrounding nuclear spins. Two complementary theoretical approaches for simulating up to 20 million laser pulses are developed and employed that are able to bridge between 11 orders of magnitude in time: a fully quantum mechanical description limited to small nuclear bath sizes and a technique based on the classical equations of motion applicable for a large number of nuclear spins. We present experimental data of the nonmonotonic revival amplitude as function of the magnetic field applied perpendicular to the optical axis. The dependence of the revival amplitude on the external field with a profound minimum at 4T is reproduced by both of our theoretical approaches and is ascribed to the nuclear Zeeman effect. Since the nuclear Larmor precession determines the electronic resonance condition, it also defines the number of electron spin revolutions between pump pulses, the orientation of the electron spin at the incidence time of a pump pulse, and the resulting revival amplitude. The magnetic field of 4T, for example, corresponds to half a revolution of nuclear spins between two laser pulses. © 2018 American Physical Society.

We present an investigation of the electron spin dynamics in an ensemble of singly charged semiconductor quantum dots subject to an external magnetic field and laser pumping with circularly polarized light. The spectral laser width is tailored such that ensembles with an increasing number of quantum dots are coherently pumped. Surprisingly, the dephasing time T∗ of the electron spin polarization depends only weakly on the laser spectral width. These findings can be consistently explained by a cluster theory of coupled quantum dots with a long-range electronic spin-spin interaction. We present a numerical simulation of the spin dynamics based on the central spin model that includes a quantum mechanical description of the laser pulses as well as a time-independent Heisenberg interaction between each pair of electron spins. We discuss the individual dephasing contributions stemming from the Overhauser field, the distribution of the electron g factors, and the electronic spin-spin interaction as well as the spectral width of the laser pulse. This analysis reveals counterbalancing effects on the total dephasing time when increasing the spectral laser width. On one hand, the increasing deviations of the electron g factors reduce the dephasing time. On the other hand, more electron spins are coherently pumped and synchronize due to the electronic spin-spin interaction which extends the dephasing time. We find an excellent agreement between the experimental data and the dephasing time in the simulation using an exponential distribution of Heisenberg couplings with a mean value J≈0.26μeV. © 2018 American Physical Society.

The spin dynamics in a broad range of systems can be studied using circularly polarized optical excitation with alternating helicity. The dependence of spin polarization on the frequency of helicity alternation, known as the spin inertia effect, is used here to study the spin dynamics in singly charged (In,Ga)As/GaAs quantum dots (QDs), providing insight into spin generation and accumulation processes. We demonstrate that the dependence of spin polarization in n- and p-type QDs on the external magnetic field has a characteristic V- and M-like shape, respectively. This difference is related to different microscopic mechanisms of the resident carriers' spin orientation. It allows us to determine the parameters of the spin dynamics both for the ground and excited states of singly charged QDs. © 2018 American Physical Society.

The spin inertia measurement is a recently emerged tool to study slow spin dynamics, which is based on the excitation of the system by a train of circularly polarized pulses with alternating helicity. Motivated by the experimental results reported by Zhukov et al. [Phys. Rev. B 98, 121304(R) (2018)10.1103/PhysRevB.98.121304], we develop the general theory of spin inertia of localized charge carriers. We demonstrate that the spin inertia measurement in longitudinal magnetic field allows one to determine the parameters of the spin dynamics of resident charge carriers and of photoexcited trions, such as the spin relaxation times, longitudinal g factors, parameters of hyperfine interaction, and nuclear spin correlation times. © 2018 American Physical Society.

Electron spin dephasing in a singly charged semiconductor quantum dot can partially be suppressed by periodic laser pulsing. We propose a semiclassical approach describing the decoherence of the electron spin polarization governed by the hyperfine interaction with the nuclear spins as well as the probabilistic nature of the photon absorption. We use the steady-state Floquet condition to analytically derive two subclasses of resonance conditions excellently predicting the peak locations in the part of the Overhauser field distribution which is projected in the direction of the external magnetic field. As a consequence of the periodic pulsing, a nonequilibrium distribution develops as a function of time. The numerical simulation of the coupled dynamics reveals the influence of the hyperfine coupling constant distribution onto the evolution of the electron spin polarization before the next laser pulse. Experimental indications are provided for both subclasses of resonance conditions. © 2017 American Physical Society.

The spin noise in singly charged self-assembled quantum dots is studied theoretically and experimentally under the influence of a perturbation, provided by additional photoexcited charge carriers. The theoretical description takes into account generation and relaxation of charge carriers in the quantum dot system. The spin noise is measured under application of above barrier excitation for which the data are well reproduced by the developed model. Our analysis demonstrates a strong difference of the recharging dynamics for holes and electrons in quantum dots. © 2017 American Physical Society.

We synthesize heterofluorene monomers with Si, Ge, N, As, Se, and Te occupying the 9-position of the fluorene motif, which are then polymerized by Suzuki coupling. The optical properties of the obtained polymers are investigated in their solid state. We compare and elucidate effects in the materials absorption, emission, quantum yield (π), and fluorescence lifetime. Moreover, we determine the refractive indices n and absorption coefficient k by variable angle spectroscopic ellipsometry (VASE). We show that in addition to already known C, Si, and N containing polyfluorenes also Ge and As containing polymers exhibit amplified spontaneous emission. © 2017 American Chemical Society.

Spins in semiconductor quantum dots have been considered as prospective quantum bit excitations. Their coupling to the crystal environment manifests itself in a limitation of the spin coherence times to the microsecond range, both for electron and hole spins. This rather short-lived coherence compared to atomic states asks for manipulations on timescales as short as possible. Due to the huge dipole moment for transitions between the valence and conduction band, pulsed laser systems offer the possibility to perform manipulations within picoseconds or even faster. Here, we report on results that show the potential of optical spin manipulations with currently available pulsed laser systems. Using picosecond laser pulses, we demonstrate optically induced spin rotations of electron and hole spins. We further realize the optical decoupling of the hole spins from the nuclear surrounding at the nanosecond timescales and demonstrate an all-optical spin tomography for interacting electron spin sub-ensembles. © 2016, Springer-Verlag Berlin Heidelberg.

We study the dynamics of optically induced nuclear spin polarization in a fluorine-doped ZnSe epilayer via time-resolved Kerr rotation. The nuclear polarization in the vicinity of a fluorine donor is induced by interaction with coherently precessing electron spins in a magnetic field applied in the Voigt geometry. It is detected by nuclei-induced changes in the electron spin coherence signal. This all-optical technique allows us to measure the longitudinal spin relaxation time T1 of the Se77 isotope in a magnetic field range from 10 to 130 mT under illumination. We combine the optical technique with radio frequency methods to address the coherent spin dynamics of the nuclei and measure Rabi oscillations, Ramsey fringes, and the nuclear spin echo. The inhomogeneous spin dephasing time T2∗ and the spin coherence time T2 of the Se77 isotope are measured. While the T1 time is on the order of several milliseconds, the T2 time is several hundred microseconds. The experimentally determined condition T1T2 verifies the validity of the classical model of nuclear spin cooling for describing the optically induced nuclear spin polarization. © 2016 American Physical Society.

We develop an extended pump-probe Faraday rotation technique to study submicrosecond electron spin dynamics with picosecond time resolution in a wide range of magnetic fields. The electron spin dephasing time T2∗ and the longitudinal spin relaxation time T1, both approaching 250 ns in weak fields, are measured thereby in n-type bulk GaAs. By tailoring the pump pulse train through increasing the contained number of pulses, the buildup of resonant spin amplification is demonstrated for the electron spin polarization. The spin precession amplitude in high magnetic fields applied in the Voigt geometry shows a nonmonotonic dynamics deviating strongly from a monoexponential decay and revealing slow beatings. The beatings indicate a two spin component behavior with a g-factor difference of Δg∼4×10-4, much smaller than the Δg expected for free and donor-bound electrons. This g-factor variation indicates efficient, but incomplete spin exchange averaging. © 2016 American Physical Society.

The spin fluctuations of electron and hole doped self-assembled quantum dot ensembles are measured optically in the low-intensity limit of a probe laser for absence and presence of longitudinal or transverse magnetic fields. The experimental results are modeled by two complementary approaches based either on a semiclassical or quantum mechanical description. This allows us to characterize the hyperfine interaction of electron and hole spins with the surrounding bath of nuclei on time scales covering several orders of magnitude. Our results demonstrate (i) the intrinsic precession of the electron spin fluctuations around the effective Overhauser field caused by the host lattice nuclear spins, (ii) the comparably long time scales for electron and hole spin decoherence, as well as (iii) the dramatic enhancement of the spin lifetimes induced by a longitudinal magnetic field due to the decoupling of nuclear and charge carrier spins. © 2016 American Physical Society.

We extend the range of quantum dot (QD) emission energies where electron and hole g factors have been measured to the practically important telecom range. The spin dynamics in InAs/In0.53Al0.24Ga0.23As self-assembled QDs with emission wavelengths at about 1.6 μm grown on InP substrate is investigated by pump-probe Faraday rotation spectroscopy in a magnetic field. Pronounced oscillations on two different frequencies, corresponding to the QD electron and hole spin precessions about the field, are observed from which the corresponding g factors are determined. The electron g factor of about -1.9 has the largest negative value so far measured for III-V QDs by optical methods. This value, as well as the g factors reported for other III-V QDs, differ from those expected for bulk semiconductors at the same emission energies, and this difference increases significantly for decreasing energies. © 2015 American Physical Society.

We present a systematic experimental study along with theoretical modeling of the energy transfer in an ensemble of closely packed CdTe colloidal nanocrystals identified as the Förster resonant energy transfer (FRET). We prove that at low temperature of 4.2 K, mainly the ground dark exciton states in the initially excited small-size (donor) nanocrystals participate in the dipole-dipole FRET leading to additional excitation of the large-size (acceptor) nanocrystals. The FRET becomes possible due to the weak admixture of the bright exciton states to the dark states. The admixture takes place even in zero magnetic field and allows the radiative recombination of the dark excitons. An external magnetic field considerably enhances this admixture, thus increasing the energy transfer rate by a factor of 2-3 in a field of 15 T, as well as the radiative rates of the dark excitons in the donor and acceptor nanocrystals. The theoretical modeling allows us to determine the spectral dependence of the probability for the NC to serve as a donor for larger nanocrystals, to evaluate the energy transfer rates as well as to predict their dependencies on the magnetic field, to describe the spectral shift of the photoluminescence maximum due to the energy transfer, and to reproduce the experimentally observed spectral dependencies of the photoluminescence recombination dynamics in the magnetic field. © 2015 American Physical Society.

The real-time spin dynamics and the spin noise spectra are calculated for p and n-charged quantum dots within an anisotropic central spin model extended by additional nuclear electric quadrupolar interactions and augmented by experimental data. Using realistic estimates for the distribution of coupling constants including an anisotropy parameter, we show that the characteristic long time scale is of the same order for electron and hole spins strongly determined by the quadrupolar interactions even though the analytical form of the spin decay differs significantly consistent with our measurements. The low frequency part of the electron spin noise spectrum is approximately 1/3 smaller than those for hole spins as a consequence of the spectral sum rule and the different spectral shapes. This is confirmed by our experimental spectra measured on both types of quantum dot ensembles in the low power limit of the probe laser. © 2015 American Physical Society.

Optically induced nuclear spin polarization in a fluorine-doped ZnSe epilayer is studied by time-resolved Kerr rotation using resonant excitation of donor-bound excitons. Excitation with helicity-modulated laser pulses results in a transverse nuclear spin polarization, which is detected as a change of the Larmor precession frequency of the donor-bound electron spins. The frequency shift in dependence on the transverse magnetic field exhibits a pronounced dispersion-like shape with resonances at the fields of nuclear magnetic resonance of the constituent zinc and selenium isotopes. It is studied as a function of external parameters, particularly of constant and radio frequency external magnetic fields. The width of the resonance and its shape indicate a strong spatial inhomogeneity of the nuclear spin polarization in the vicinity of a fluorine donor. A mechanism of optically induced nuclear spin polarization is suggested based on the concept of resonant nuclear spin cooling driven by the inhomogeneous Knight field of the donor-bound electron. © 2015 American Physical Society.

The spin dynamics of strongly localized donor-bound electrons in fluorine-doped ZnSe epilayers is studied using pump-probe Kerr rotation techniques. A method exploiting the spin inertia is developed and used to measure the longitudinal spin relaxation time T1 in a wide range of magnetic fields, temperatures, and pump densities. The T1 time of the donor-bound electron spin of about 1.6 μs remains nearly constant for external magnetic fields varied from zero up to 2.5 T (Faraday geometry) and in a temperature range 1.8-45 K. These findings impose severe restrictions on possible spin relaxation mechanisms. In our opinion they allow us to rule out scattering between free and donor-bound electrons, jumping of electrons between different donor centers, scattering between phonons and donor-bound electrons, and with less certainty charge fluctuations in the environment of the donors caused by the 1.5 ps pulsed laser excitation. © 2015 American Physical Society.

We demonstrate the potential of a periodic laser-pulse protocol for dynamic decoupling of hole spins in (In,Ga)As quantum dots from surrounding baths. When doubling the repetition rate of inversion laser pulses between two reference pulses for orienting the spins, we find that the spin coherence time is increased by a factor of 2. © 2014 American Physical Society.

Resonant cooling of different nuclear isotopes manifested in optically induced nuclear magnetic resonances (NMR) is observed in n-doped CdTe/(Cd,Mg)Te and ZnSe/(Zn,Mg)Se quantum wells and for donor-bound electrons in ZnSe:F and GaAs epilayers. By time-resolved Kerr rotation used in the regime of resonant spin amplification, we can expand the range of magnetic fields where the effect can be observed up to nuclear Larmor frequencies of 170 kHz. The mechanism of the resonant cooling of the nuclear spin system is analyzed theoretically. The developed approach allows us to model the resonant spin amplification signals with NMR features. © 2014 American Physical Society.

We demonstrate the basic features of an all-optical spin tomography on picosecond time scale. The magnetization vector associated with a mode-locked electron spin ensemble in singly charged quantum dots is traced by ellipticity measurements using picosecond laser pulses. After optical orientation the spins precess about a perpendicular magnetic field. By comparing the dynamics of two interacting ensembles with the dynamics of a single ensemble we find buildup of a spin component along the magnetic field in the two-ensemble case. This component arises from a Heisenberg-like spin-spin interaction. © 2014 American Physical Society.

We exploit the flexibility offered by an (In,Ga)As/GaAs quantum dot spin ensemble to demonstrate that complex dynamic evolutions can be excited in the ensemble magnetization and accessed by tailored pulsed laser protocols. The modes for spin precession about a magnetic field are adapted to the periodic excitation protocol such that at specific times the magnetization can effectively be decomposed in two, three, or four equal components with angles of π,2π/3, or π/2 between them. Optical orientation of these components by an additional laser pulse leads to the generation of higher harmonics in the spin precession, as evidenced by time-resolved ellipticity measurements. © 2014 American Physical Society.

The recombination and spin dynamics of excitons in colloidal CdTe nanocrystals (NCs) are studied by time-resolved photoluminescence in high magnetic fields up to 15 T and at cryogenic temperatures. The recombination decay shows a nonexponential temporal behavior, with the longest component corresponding to the dark excitons having 260-ns decay time at zero magnetic field and 4.2-K temperature. This long component shortens to 150 ns at 15 T due to the magnetic-field-induced mixing of the bright- and dark-exciton states. The spin dynamics, assessed through the evolution of the magnetic-field-induced circular polarization degree of the photoluminescence, has a fast component shorter than 1 ns related to the bright excitons and a slow component of 5-10 ns associated with the dark excitons. The latter shortens with increasing magnetic field, which is characteristic for a phonon-assisted spin-relaxation mechanism. The relatively low saturation level of the associated magnetic-field-induced circular polarization degree of -30% is explained by a model that suggests the CdTe NCs to constitute an ensemble of prolate and oblate NCs, both having a structural quantization axis. The exciton g factor of 2.4-2.9 evaluated from fitting the experimental data in the frame of the suggested approach is in good agreement with the expected value for the dark excitons in CdTe NCs. © 2014 American Physical Society.

A comprehensive overview of coherent spin manipulation in (In, Ga)As quantum dots, singly charged with resident electrons or holes, is given, from orientation to rotation of the spins. These operations are performed by excitation of the charged exciton complex with laser pulses. The specifics of the approach is performing the manipulations on dot ensembles, potentially giving robustness to the coherent spin dynamics. In particular, we focus on the spin mode-locking regime, in which the precession of the spins about an external magnetic field is synchronized with the periodic pulsed laser excitation initiating the operations. The periodic excitation protocol introduces a frequency comb through which detrimental effects of the inhomogeneities in the spin system can be avoided. © 2014 The Authors. Phys. Status Solidi B is published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Per the fluctuation-dissipation theorem, the information obtained from spin fluctuation studies in thermal equilibrium is necessarily constrained by the system's linear response functions. However, by including weak radio frequency magnetic fields, we demonstrate that intrinsic and random spin fluctuations even in strictly unpolarized ensembles can reveal underlying patterns of correlation and coupling beyond linear response, and can be used to study nonequilibrium and even multiphoton coherent spin phenomena. We demonstrate this capability in a classical vapor of K41 alkali atoms, where spin fluctuations alone directly reveal Rabi splittings, the formation of Mollow triplets and Autler-Townes doublets, ac Zeeman shifts, and even nonlinear multiphoton coherences. © 2014 American Physical Society.

Compared to electrons, holes in InAs quantum dots have a significantly weaker hyperfine interaction that leads to less dephasing from nuclear spins. Thus many recent studies have suggested that nuclear spins are unimportant for hole-spin dynamics compared to electric-field fluctuations. We show that the hole hyperfine interaction can have a strong effect on hole-spin coherence measurements through a nuclear feedback effect. The nuclear polarization is generated through a unique process that is dependent on the anisotropy of the hole hyperfine interaction and the coherent precession of nuclear spins, giving rise to strong modulation at the nuclear precession frequency. © 2014 American Physical Society.

Spin noise spectroscopy is an optical technique for probing electron and hole spin dynamics that is based on detecting their intrinsic fluctuations while in thermal equilibrium. Here we show that fluctuation correlations can be further exploited in multi-probe noise studies to reveal information that in general cannot be accessed by conventional linear optical spectroscopy, such as the underlying homogeneous linewidths of individual constituents within inhomogeneously broadened systems. This is demonstrated in singly charged (In,Ga)As quantum-dot ensembles using two weak probe lasers: When the lasers have similar wavelengths, they probe the same quantum dots in the ensemble and show correlated spin fluctuations. In contrast, mutually detuned probe lasers measure different subsets of quantum dots, giving uncorrelated fluctuations. The noise correlation versus laser detuning directly reveals the quantum dot homogeneous linewidth even in the presence of a strong inhomogeneous broadening. Such noise-based correlation techniques are not limited to semiconductor spin systems, but are applicable to any system with measurable intrinsic fluctuations. © 2014 Macmillan Publishers Limited.

Two electron spins in quantum dots coupled through coherent tunneling are generally acknowledged to approximately obey Heisenberg isotropic exchange. This has not been established for two holes. Here we measure the spectra of two holes and of two electrons in two vertically stacked self-assembled InAs quantum dots using optical spectroscopy as a function of electric and magnetic fields. We find that the exchange is approximately isotropic for both systems, but that significant asymmetric contributions, arising from spin-orbit and Zeeman interactions combined with spatial asymmetries, are required to explain large anticrossings and fine-structure energy splittings in the spectra. Asymmetric contributions to the isotropic Hamiltonian for electrons are of the order of a few percent while those for holes are an order of magnitude larger. © 2013 American Physical Society.

Spontaneous fluctuations of the magnetization of a spin system in thermodynamic equilibrium (spin noise) manifest themselves as noise in the Faraday rotation of probe light. We show that the correlation properties of this noise over the optical spectrum can provide clear information about the composition of the spin system that is largely inaccessible for conventional linear optics. Such optical spectroscopy of spin noise, e.g., allows us to clearly distinguish between optical transitions associated with different spin subsystems, to resolve optical transitions that are unresolvable in the usual optical spectra, to unambiguously distinguish between homogeneously and inhomogeneously broadened optical bands, and to evaluate the degree of inhomogeneous broadening. These new possibilities are illustrated by theoretical calculations and by experiments on paramagnets with different degrees of inhomogeneous broadening of optical transitions [atomic vapors of K41 and singly charged (In,Ga)As quantum dots]. © 2013 American Physical Society.

We attract attention to the fact that the ultimate (shot-noise-limited) polarimetric sensitivity can be enhanced by orders of magnitude leaving the photon flux incident onto the photodetector on the same low level. This opportunity is of crucial importance for present-day spin noise spectroscopy, where a direct increase of sensitivity by increasing the probe beam power is strongly restricted by the admissible input power of the broadband photodetectors. The gain in sensitivity is achieved by replacing the 45° polarization geometry commonly used in conventional schemes with balanced detectors by geometries with stronger polarization extinction. The efficiency of these high-extinction polarization geometries with enhancement of the detected signal by more than an order of magnitude is demonstrated by measurements of the spin noise spectra of bulk n:GaAs in the spectral range 835-918 nm. It is shown that the inevitable growth of the probe beam power with the sensitivity gain makes spin noise spectroscopy much more perturbative, but, at the same time, opens up fresh opportunities for studying nonlinear interactions of strong light fields with spin ensembles. © 2013 American Physical Society.

We discuss advantages and limitations of the spin noise spectroscopy for characterization of interacting quantum dot systems on specific examples of individual singly and doubly charged quantum dot molecules (QDMs). It is shown that all the relevant parameters of the QDMs, including tunneling amplitudes with spin-conserving and spin-nonconserving interactions, decoherence rates, Coulomb repulsions, anisotropic g factors and the distance between the dots, can be determined by measuring properties of the spin noise power spectrum. © 2013 American Physical Society.

The temperature dependence of the coherence time of hole spins confined in self-assembled (In,Ga)As/GaAs quantum dots is studied by spin-mode-locking and spin-echo techniques. Coherence times limited to about a microsecond are measured for temperatures below 8 K. For higher temperatures, a fast drop occurs down to a few nanoseconds over a 10-K range. The hole-nuclear hyperfine interaction appears too weak to account for these limitations. We suggest that spin-orbit-related interactions are the decisive sources for hole spin decoherence. © 2013 American Physical Society.

Coherent collective phenomena of hole spins confined in an ensemble of (In,Ga)As quantum dots are studied by monitoring their Larmor precession about a magnetic field. Variation of the field strength drives the hole spins from a regime of resonant spin amplification, in which their precession frequency is a unique multiple of the laser repetition rate, to spin mode locking, in which several precession modes are commensurable with the laser repetition rate. In this regime the spin coherence time of individual holes is determined to be 0.7 μs. In contrast, electron spins in the quantum dots are always trapped in the mode-locking regime due to the strong hyperfine interaction with nuclear spins. © 2012 American Physical Society.

Two-color pump probe experiments reveal the possibility to use non-resonant pulsed laser excitation to create mode-locking of the ground state electron spin precessions in an ensemble of singly charged (In,Ga)As/GaAs quantum dots. The mode-locking shows a resonance for excitation into the first excited shell while for excitation into higher shells or barriers it disappears; however, spin coherence can still be induced. We conclude that the optically excited carriers relax spin-conserved from the p-shell into their ground states on a picosecond time scale, much shorter than the spin revolution period about the magnetic field. © 2012 American Institute of Physics.

The spin coherence of an ensemble of electrons bound to fluorine donors in epitaxially grown ZnSe layers is studied by time-resolved pump-probe Kerr rotation. Long-lived spin dephasing with decay times up to T2*=33 ns is found for a sample with a low fluorine concentration of 1×1015 cm -3 at cryogenic temperatures. The time is close to the limit set by nuclear-spin fluctuations, for which we measure a strength of 1.65 mT. We find T2* to be constant up to 40 K, with a strong drop for higher temperatures. The dephasing time also shortens with increasing fluorine concentration, indicating an interaction between the spins at different fluorine centers. © 2012 American Physical Society.

The g-factor tensors of electron and hole in self-assembled (In,Ga)As/GaAs quantum dots are studied by time-resolved ellipticity measurements in a three dimensional vector magnet system. Both g-factor tensors show considerable deviations from isotropy. These deviations are much more pronounced for the hole than for the electron and are described by different anisotropy factors, which can even have opposite signs. © 2011 American Institute of Physics.

Coherent interactions between spins in quantum dots are a key requirement for quantum gates. We have performed pump-probe experiments in which pulsed lasers emitting at different photon energies manipulate two distinct subsets of electron spins within an inhomogeneous InGaAs quantum dot ensemble. The spin dynamics are monitored through their precession about an external magnetic field. These measurements demonstrate spin precession phase shifts and modulations of the magnitude of one subset of oriented spins after optical orientation of the second subset. The observations are consistent with results from a model using a Heisenberg-like interaction with μeV strength. © 2011 American Physical Society.

A single hole spin in a semiconductor quantum dot has emerged as a quantum bit that is potentially superior to an electron spin. A key feature of holes is that they have a greatly reduced hyperfine interaction with nuclear spins, which is one of the biggest difficulties in working with an electron spin. It is now essential to show that holes are viable for quantum information processing by demonstrating fast quantum gates and scalability. To this end, we have developed InAs/GaAs quantum dots coupled through coherent tunnelling and charged with controlled numbers of holes. We report fast, single-qubit gates using a sequence of short laser pulses. We then take the important next step towards scalability of quantum information by optically controlling two interacting hole spins in separate dots. © 2011 Macmillan Publishers Limited. All rights reserved.

The interaction between two quantum bits enables the creation of entanglement, the two-particle correlations that are at the heart of quantum information science. In semiconductor quantum dots, much work has focused on demonstrating control over single spin qubits using optical techniques. However, optical control of two spin qubits remains a major challenge for scaling to a fully fledged quantum-information platform. Here, we combine advances in vertically stacked quantum dots with ultrafast laser techniques to achieve optical control of the entangled state of two electron spins. Each electron is in a separate InAs quantum dot, and the spins interact through tunnelling, where the tunnelling rate determines how rapidly entangling operations can be carried out. We achieve two-qubit gates with an interaction rate of 30 GHz, more than an order of magnitude faster than demonstrated in any other system so far. These results demonstrate the viability and advantages of optically controlled quantum-dot spins for multi-qubit systems. © 2011 Macmillan Publishers Limited. All rights reserved.

The spin state of holes confined in single InAs quantum dots have recently emerged as a promising system for the storage or manipulation of quantum information. These holes are often assumed to have no mixing between orthogonal heavy-hole-spin projections (in the absence of a transverse magnetic field). The same assumption has been applied to InAs quantum dot molecules formed by two stacked InAs quantum dots that are coupled by coherent tunneling of the hole between the two dots. We present experimental evidence of the existence of a hole-spin-mixing term obtained with magnetophotoluminescence spectroscopy on such InAs quantum dot molecules. We use a Luttinger spinor model to explain the physical origin of this hole-spin-mixing term: misalignment of the dots along the stacking direction breaks the angular symmetry and allows mixing of the heavy-hole components through the light-hole component of the spinor. We discuss how this spin-mixing mechanism may offer new spin manipulation opportunities that are unique to holes. © 2010 The American Physical Society.

We present three unique spin properties of holes in the delocalized states of coupled pairs of InAs quantum dots: resonant changes in the hole g factor, antisymmetric hole molecular ground states, and hole spin mixing. These three properties suggest new opportunities for spin control that are unique to holes and further support holes as a competitive candidate for the storage and manipulation of quantum information. © 2010 IOP Publishing Ltd.

The carrier spin dynamics in a n -doped (In,Ga)As/GaAs quantum well has been studied by time-resolved Faraday rotation and ellipticity techniques in the temperature range down to 430 milliKelvin. These techniques give data with very different spectral dependencies, from which nonetheless consistent information on the spin dynamics can be obtained, in agreement with theoretical predictions. The mechanisms of long-lived spin coherence generation are discussed for the cases of trion and exciton resonant excitation. We demonstrate that carrier localization leads to a saturation of spin relaxation times at 45 ns for electrons below 4.5 K and at 2 ns for holes below 2.3 K. The underlying spin relaxation mechanisms are discussed. © 2010 The American Physical Society.

We measure the frequency spectra of random spin fluctuations, or "spin noise," in ensembles of (In,Ga)As/GaAs quantum dots (QDs) at low temperatures. We employ a spin noise spectrometer based on a sensitive optical Faraday rotation magnetometer that is coupled to a digitizer and field-programmable gate array, to measure and average noise spectra from 0-1 GHz continuously in real time with subnanoradian/Hz sensitivity. Both electron and hole spin fluctuations generate distinct noise peaks, whose shift and broadening with magnetic field directly reveal their g factors and dephasing rates within the ensemble. A large, energy-dependent anisotropy of the in-plane hole g factor is clearly exposed, reflecting systematic variations in the average QD confinement potential. © 2010 The American Physical Society.