Optical orientation of carrier spins by circularly polarized light is the basic concept and tool of spin physics in semiconductors. We study the optical orientation of electrons and holes in a crystal of the FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$ lead halide perovskite by means of polarized photoluminescence, time-resolved differential reflectivity, and time-resolved Kerr rotation. At the cryogenic temperature of 1.6 K the optical orientation degree measured for continuous-wave excitaton reaches 6% for localized electrons and 2\% for localized holes. Their contributions are distinguished from each other and from exciton optical orientation through the pronounced Hanle effect in transverse magnetic fields and the polarization recovery effect in longitudinal magnetic fields. The optical orientation degree is highly stable against detuning of the laser photon energy from the band gap by up to 0.25 eV, showing then a gradual decrease for detunings up to 0.9 eV. This evidences the inefficiency of spin relaxation mechanisms for free carriers during their energy relaxation. Spin relaxation for localized electrons and holes is provided by the hyperfine interaction with the nuclear spins. Dynamic polarization of nuclear spins is demonstrated by the Overhauser field reaching 4 mT acting on the electrons and $-76$ mT acting on the holes. This confirms the specifics of lead halide perovskite semiconductors, where the hole hyperfine interaction with the nuclei considerably exceeds that of the electron.

Measurements of the longitudinal and transverse spin relaxation times of holes in an ensemble of vertically tunnel‐coupled self‐assembled InAs/InAlGaAs quantum dots (QDs), emitting in the telecom spectral range, are reported. The spin coherence is determined using the spin mode‐locking method in the inhomogeneous ensemble of QDs. Modeling the signal allows us to extract the hole spin coherence time to be in the range of μs. The longitudinal spin relaxation time μs is measured using the spin inertia method. The parameters investigated allow us to suggest that the main relaxation mechanism at low magnetic fields is related to the electron–hole spin exchange.

Quantum measurement back action is fundamentally unavoidable when manipulating electron spins. Here we demonstrate that this back action can be efficiently exploited to tune the spin relaxation of localized electrons induced by the hyperfine interaction. In optical pump-probe experiments, powerful probe pulses suppress the spin relaxation of electrons on Si donors in an InGaAs epilayer due to the quantum Zeno effect. By contrast, an increase of the probe power leads to a speed up of the spin relaxation for electrons in InGaAs quantum dots due to the quantum anti-Zeno effect. The microscopic description shows that the transition between the two regimes occurs when the spin dephasing time is comparable to the probe pulse repetition period.

The coherent spin dynamics of electrons in CdSe nanocrystals embedded in a glass matrix with diameters from 3.3 up to 6.1 nm are investigated by time-resolved Faraday ellipticity at room and cryogenic temperatures. Only one Larmor precession frequency is detected, which corresponds to the larger of the two precession frequencies and thus g-factor values found in the typical signal from solution-grown colloidal CdSe nanocrystals. We identify this frequency accordingly as associated with the spin precession of resident electrons localized in the nanocrystals in the vicinity of the surface. We provide a detailed theoretical analysis of the exciton level spin structure in the magnetic field and model the spin dynamics in CdSe nanocrystals of different symmetries. This allows us to exclude the exciton as the origin of the experimentally observed oscillating signal. At a cryogenic temperature of 6 K, an additional nonoscillating component emerges in the spin dynamics. We consider several possible origins of this signal and conclude that it is related to the hole spin polarization.

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.

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.

The outstanding optical quality of lead halide perovskites inspires studies of their potential for the optical control of carrier spins as pursued in other materials. Entering largely uncharted territory, time-resolved pump-probe Kerr rotation is used to explore the coherent spin dynamics of electrons and holes in bulk formamidinium caesium lead iodine bromide (FA0.9 Cs0.1 PbI2.8 Br0.2 ) and to determine key parameters characterizing interactions of their spins, such as the g-factors and relaxation times. The demonstrated long spin dynamics and narrow g-factor distribution prove the perovskites as promising competitors for conventional semiconductors in spintronics. The dynamic nuclear polarization via spin-oriented holes is realized and the identification of the lead (207 Pb) isotope in optically detected nuclear magnetic resonance proves that the hole-nuclei interaction is dominated by the lead ions. A detailed theoretical analysis accounting for the specifics of the lead halide perovskite materials allows the evaluation of the underlying hyperfine interaction constants, both for electrons and holes. Recombination and spin dynamics evidence that at low temperatures, photogenerated electrons and holes are localized at different regions of the perovskite crystal, resulting in their long lifetimes up to 44 μs. The findings form the base for the tailored development of spin-optoelectronic applications for the large family of lead halide perovskites and their nanostructures.

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.

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 ^111Cd, ^113Cd, and ^125Te. We measure nuclear Rabi oscillations, the inhomogeneous dephasing time T_2^*, the spin coherence time T_2, and the longitudinal relaxation time T_1. 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.

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.

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 4 T 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 4 T, for example, corresponds to half a revolution of nuclear spins between two laser pulses.

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.

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) over bar approximate to 0.26 mu eV.

The spin relaxation dynamics of Ce3+ ions in heavily cerium-dopedYAGcrystals is studied using pulse-electron paramagnetic resonance and time-resolved pump-probe Faraday rotation. Both techniques address the 4f ground state, while pump-probe Faraday rotation also provides access to the excited 5d state. We measure a millisecond spin-lattice relaxation time T-1, a microsecond spin coherence time T-2, and a similar to 10 ns inhomogeneous spin dephasing time T-2* for the Ce3+ ground state at low temperatures. The spin-lattice relaxation of Ce3+ ions is due to modified Raman processes involving the optical phonon mode at similar to 125 cm(-1). The relaxation at higher temperature goes through a first excited level of the 2F52 term at about h omega approximate to 228 cm(-1). Effects provided by the hyperfine interaction of the Ce3+ with the Al-27 nuclei are observed.

Electron spin dephasing in a singly charged semiconductor quantum dot can partially be suppressed by periodic laser pulsing. We propose a semi-classical 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 non-equilibrium 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 polarisation before the next laser pulse. Experimental indications are provided for both subclasses of resonance conditions.

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 T-2* and the longitudinal spin relaxation time T-1, 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 Delta g similar to 4 x 10(-4), much smaller than the Delta g expected for free and donor-bound electrons. This g-factor variation indicates efficient, but incomplete spin exchange averaging.

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.

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.