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The tunability of the optical properties of lead halide perovskite nanocrystals makes them highly appealing for applications. Both, halide anion exchange and quantum confinement pave the way for tailoring their band gap energy. For spintronics applications, the Land\'e g-factors of electrons and hole are of great importance. By means of the empirical tight-binding and $\textbf{k}\cdot\textbf{p}$ methods, we calculate them for nanocrystals of the class of all-inorganic lead halide perovskites CsPb$X_3$ ($X = \text{I},\,\text{Br},\,\text{Cl}$). The hole g-factor as function of the band gap follows the universal dependence found for bulk perovskites, while for the electrons a considerable modification is predicted. Based on the $\textbf{k}\cdot\textbf{p}$ analysis we conclude that this difference arises from the interaction of the bottom conduction band with the spin-orbit split electron states. The model predictions are confirmed by experimental data for the electron and hole g-factors in CsPbI3 nanocrystals placed in a glass matrix, measured by time-resolved Faraday ellipticity in a magnetic field at cryogenic temperatures.

The photovoltaic and optoelectronic properties of lead halide perovskite semiconductors are controlled by excitons, so that investigation of their fundamental properties is of critical importance. The exciton Land\'e or g-factor g_X is the key parameter, determining the exciton Zeeman spin splitting in magnetic fields. The exciton, electron and hole carrier g-factors provide information on the band structure, including its anisotropy, and the parameters contributing to the electron and hole effective masses. We measure g_X by reflectivity in magnetic fields up to 60 T for lead halide perovskite crystals. The materials band gap energies at a liquid helium temperature vary widely across the visible spectral range from 1.520 up to 3.213 eV in hybrid organic-inorganic and fully inorganic perovskites with different cations and halogens: FA_{0.9}Cs_{0.1}PbI_{2.8}Br_{0.2], MAPbI_{3}, FAPbBr_{3}, CsPbBr_{3}, and MAPb(Br_{0.05}Cl_{0.95})_{3}. We find the exciton g-factors to be nearly constant, ranging from +2.3 to +2.7. Thus, the strong dependences of the electron and hole g-factors on the band gap roughly compensate each other when combining to the exciton g-factor. The same is true for the anisotropies of the carrier g-factors, resulting in a nearly isotropic exciton g-factor. The experimental data are compared favorably with model calculation results.

Coherent many-body states are highly promising for robust and scalable quantum information processing. While far-reaching theoretical predictions have been made for various implementations, direct experimental evidence of their appealing properties can be challenging. Here, we demonstrate coherent optical manipulation of the nuclear spin ensemble in the lead halide perovskite semiconductor FAPbBr$_3$ (FA=formamidinium), targeting a long-postulated collective dark state that is insensitive to optical pumping. Via optical orientation of localized hole spins we drive the nuclear many-body system into an entangled state, requiring a weak magnetic field of only a few Millitesla strength at cryogenic temperatures. During its fast build-up, the nuclear polarization along the optical axis remains small, while the transverse nuclear spin fluctuations are strongly reduced, corresponding to spin squeezing as evidenced by a strong violation of the generalized nuclear squeezing-inequality with $\xi_s < 0.3$. The dark state evidenced in this process corresponds to an approximately 750-body entanglement between the nuclei. Dark nuclear spin states can be exploited to store quantum information benefiting from their long-lived many-body coherence and to perform quantum measurements with a precision beyond the standard limit.

The spin physics of perovskite nanocrystals with confined electrons or holes is attracting increasing attention, both for fundamental studies and spintronic applications. Here, stable CsPb(Cl$_{0.5}$Br$_{0.5}$)$_3$ lead halide perovskite nanocrystals embedded in a fluorophosphate glass matrix are studied by time-resolved optical spectroscopy to unravel the coherent spin dynamics of holes and their interaction with nuclear spins of the $^{207}$Pb isotope. We demonstrate the spin mode locking effect provided by the synchronization of the Larmor precession of single hole spins in each nanocrystal in the ensemble that are excited periodically by a laser in an external magnetic field. The mode locking is enhanced by nuclei-induced frequency focusing. An ensemble spin dephasing time $T_2^*$ of a nanosecond and a single hole spin coherence time of $T_2=13\,$ns are measured. The developed theoretical model accounting for the mode locking and nuclear focusing for randomly oriented nanocrystals with perovskite band structure describes the experimental data very well., Comment: Main paper of 9 pages and 3 figures. Supplementary material of 16 pages and 12 figures

Methylammonium lead triiodine (MAPbI$_3$) is a material representative of the hybrid organic-inorganic lead halide perovskites which attract currently great attention due to their photovoltaic efficiency and bright optoelectronic properties. Here, the coherent spin dynamics of charge carriers and spin dependent phenomena induced by the carrier interaction with nuclear spins are studied in MAPbI$_3$ single crystals, using time-resolved Kerr rotation at cryogenic temperatures in magnetic fields up to 3 T. Spin dephasing times up to a few nanoseconds and a longitudinal spin relaxation time of 37 ns are measured. The Larmor spin precession of both resident electrons and holes is identified in the Kerr rotation signals. The Land\'e factors ($g$-factors) in the orthorhombic crystal phase show a strong anisotropy, ranging for the holes from $-0.28$ to $-0.71$ and for the electrons from $+2.46$ to $+2.98$, while the $g$-factor dispersion of about 1% is rather small. An exciton $g$-factor of $+2.3$ is measured by magneto-reflectivity. A dynamic nuclear polarization by means of spin polarized electrons and holes is achieved in tilted magnetic fields giving access to the carrier-nuclei exchange interaction and the nuclei spin relaxation time exceeding 16 minutes.

The Land\'e or $g$-factors of charge carriers are decisive for the spin-dependent phenomena in solids and provide also information about the underlying electronic band structure. We present a comprehensive set of experimental data for values and anisotropies of the electron and hole Land\'e factors in hybrid organic-inorganic (MAPbI$_3$, MAPb(Br$_{0.5}$Cl$_{0.5}$)$_3$, MAPb(Br$_{0.05}$Cl$_{0.95}$)$_3$, FAPbBr$_3$, FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$) and all-inorganic (CsPbBr$_3$) lead halide perovskites, determined by pump-probe Kerr rotation and spin-flip Raman scattering in magnetic fields up to 10~T at cryogenic temperatures. Further, we use first-principles DFT calculations in combination with tight-binding and $\mathbf k \cdot \mathbf p$ approaches to calculate microscopically the Land\'e factors. The results demonstrate their universal dependence on the band gap energy across the different perovskite material classes, which can be summarized in a universal semi-phenomenological expression, in good agreement with experiment.

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., Comment: 7 pages including 4 figures; 8 pages supplement including 4 figures

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 describe the resonance spin amplification effect in the Faraday geometry and discuss the manifestations 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 spin polarization recovery is a very valuable tool for addressing carrier spin dynamics in semiconductors and their nanostructures., Comment: 16 pages, 15 figures

The effect of a lateral electric current on the photoluminescence H-band of an AlGaAs/GaAs heterostructure is investigated. The photoluminescence intensity and optical orientation of electrons contributing to the H-band are studied by means of continuous wave and time-resolved photoluminescence spectroscopy and time-resolved Kerr rotation. It is shown that the H-band is due to recombination of the heavy holes localized at the heterointerface with photoexcited electrons attracted to the heterointerface from the GaAs layer. Two lines with significantly different decay times constitute the H-band: a short-lived high-energy one and a long-lived low-energy one. The high-energy line originates from recombination of electrons freely moving along the structure plane, while the low-energy one is due to recombination of donor-bound electrons near the interface. Application of the lateral electric field of ~ 100-200 V/cm results in a quenching of both lines. This quenching is due to a decrease of electron concentration near the heterointerface as a result of a photocurrent-induced heating of electrons in the GaAs layer. On the contrary, electrons near the heterointerface are effectively cooled, so the donors near the interface are not completely empty up to ~ 100 V/cm, which is in stark contrast with the case of bulk materials. The optical spin polarization of the donor-bound electrons near the heterointerface weakly depends on the electric field. Their polarization kinetics is determined by the spin dephasing in the hyperfine fields of the lattice nuclei. The long spin memory time (> 40 ns) can be associated with suppression of the Bir-Aronov-Pikus mechanism of spin relaxation for electrons., Comment: 21 pages, 7 figures

Spin-dependent photon echoes in combination with pump-probe Kerr rotation are used to study the microscopic electron spin transport in a CdTe/(Cd,Mg)Te quantum well in the hopping regime. We demonstrate that independent of the particular spin relaxation mechanism, hopping of resident electrons leads to a shortening of the photon echo decay time, while the transverse spin relaxation time evaluated from pump-probe transients increases due to motional narrowing of spin dynamics in the fluctuating effective magnetic field of the lattice nuclei., Comment: 11 pages, 8 figures

Voltage control of ferromagnetism on the nanometer scale is highly appealing for the development of novel electronic devices. Here a key challenge is to implement and combine low power consumption, high operation speed, reliable reversibility and compatibility with semiconductor technology. Hybrid structures based on the assembly of ferromagnetic and semiconducting building blocks are attractive candidates in that respect as such systems bring together the properties of the isolated constituents: They are expected to show magnetic order as a ferromagnet and to be electrically tunable as a semiconductor. Here we demonstrate the electrical control of the exchange coupling in a hybrid consisting of a ferromagnetic Co layer and a semiconductor CdTe quantum well, separated by a thin non-magnetic (Cd,Mg)Te barrier. The effective magnetic field of the exchange interaction reaches up to 2.5 Tesla and can be turned on and off by application of 1 V bias across the heterostructure. The mechanism of this electric field control is essentially different from the conventional concept, in which wavefunctions are spatially redistributed to vary the exchange interaction, requiring high field strengths. Here we address instead control of the novel exchange mechanism that is mediated by elliptically polarized phonons emitted from the ferromagnet, i.e. the phononic ac Stark effect. An essential parameter of this coupling is the splitting between heavy and light hole states in the quantum well which can be varied by the electric field induced band bending. Thereby the splitting can be tuned with respect to the magnon-phonon resonance energy in the ferromagnet, leading to maximum coupling for flat band conditions. Our results demonstrate the feasibility of electrically controlled exchange coupling in hybrid semiconductor nanostructures at quite moderate electric field strengths., Comment: 25 pages, 5 figures, supplementary material

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 in E. A. Zhukov et al., arXiv:1806.11100 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., Comment: 11 pages, 7 figures. This is a joint submission with "Spin Inertia of Resident and Photoexcited Carriers in Singly-Charged Quantum Dots" by the same authors

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 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., Comment: 5 pages, 3 figures. This is a joint submission with "Theory of spin inertia in singly-charged quantum dots" by the same authors

The exchange interaction between magnetic ions and charge carriers in semiconductors is considered as prime tool for spin control. Here, we solve a long-standing problem by uniquely determining the magnitude of the long-range $p-d$ exchange interaction in a ferromagnet-semiconductor (FM-SC) hybrid structure where a 10~nm thick CdTe quantum well is separated from the FM Co layer by a CdMgTe barrier with a thickness on the order of 10~nm. The exchange interaction is manifested by the spin splitting of acceptor bound holes in the effective magnetic field induced by the FM. The exchange splitting is directly evaluated using spin-flip Raman scattering by analyzing the dependence of the Stokes shift $\Delta_S$ on the external magnetic field $B$. We show that in strong magnetic field $\Delta_S$ is a linear function of $B$ with an offset of $\Delta_{pd} = 50-100~\mu$eV at zero field from the FM induced effective exchange field. On the other hand, the $s-d$ exchange interaction between conduction band electrons and FM, as well as the $p-d$ contribution for free valence band holes, are negligible. The results are well described by the model of indirect exchange interaction between acceptor bound holes in the CdTe quantum well and the FM layer mediated by elliptically polarized phonons in the hybrid structure., Comment: 11 pages, 8 figures

The optically induced spin polarization in (Cd,Mn)Te/(Cd,Mn,Mg)Te diluted-magnetic-semiconductor quantum wells is investigated by means of picosecond pump-probe Kerr rotation. At 1.8 K temperature, additionally to the oscillatory signals from photoexcited electrons and Manganese spins precessing about an external magnetic field, a surprisingly long-lived (up to 60 ns) nonoscillating spin polarization is detected. This polarization is related to optical orientation of equilibrium magnetic polarons involving resident holes. The suggested mechanism for the optical orientation of the equilibrium magnetic polarons indicates that the detected polaron dynamics originates from unexcited magnetic polarons. The polaron spin dynamics is controlled by the anisotropic spin structure of the heavy-hole resulting in a freezing of the polaron magnetic moment in one of the two stable states oriented along the structure growth axis. Spin relaxation between these states is prohibited by a potential barrier, which depends on temperature and magnetic field. The magnetic polaron relaxation is accelerated with increasing temperature and in magnetic field., Comment: 9 Figures, 11 pages

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 $T_{1}$ of the $^{77}\text{Se}$ 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 $T_{2}^{*}$ and the spin coherence time $T_{2}$ of the $^{77}\text{Se}$ isotope are measured. While the $T_{1}$ time is on the order of several milliseconds, the $T_{2}$ time is several hundred microseconds. The experimentally determined condition $T_{1}\gg T_{2}$ verifies the validity of the classical model of nuclear spin cooling for describing the optically-induced nuclear spin polarization., Comment: 5 pages, 3 figures

A detailed study of the $g$-factor anisotropy of electrons and holes in InAs/In$_{0.53}$Al$_{0.24}$Ga$_{0.23}$As self-assembled quantum dots emitting in the telecom spectral range of $1.5-1.6$ $\mu$m (around 0.8 eV photon energy) is performed by time-resolved pump-probe ellipticity technique using a superconducting vector magnet. All components of the $g$-factor tensors are measured, including their spread in the quantum dot (QD) ensemble. Surprisingly, the electron $g$ factor shows a large anisotropy changing from $g_{\mathrm{e},x}= -1.63$ to $g_{\mathrm{e},z}= -2.52$ between directions perpendicular and parallel to the dot growth axis, respectively, at an energy of 0.82 eV. The hole $g$-factor anisotropy at this energy is even stronger: $|g_{\text{h},x}|= 0.64$ and $|g_{\text{h},z}|= 2.29$. On the other hand, the in-plane anisotropies of electron and hole $g$ factors are small. The pronounced out-of-plane anisotropy is also observed for the spread of the $g$ factors, determined from the spin dephasing time. The hole longitudinal $g$ factors are described with a theoretical model that allows us to estimate the QD parameters. We find that the QD height-to-diameter ratio increases while the indium composition decreases with increasing QD emission energy., Comment: 10 pages, 7 figures, 2 tables

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., Comment: 12 pages, 11 figures

The spin dynamics of the strongly localized, donor-bound electrons in fluorine-doped ZnSe epilayers is studied by pump-probe Kerr rotation techniques. A method exploiting the spin inertia is developed and used to measure the longitudinal spin relaxation time, $T_1$, in a wide range of magnetic fields, temperatures, and pump densities. The $T_1$ time of the donor-bound electron spin of about 1.6 $\mu$s 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. The inhomogeneous spin dephasing time, $T_2^*=8-33$ ns, is measured using the resonant spin amplification and Hanle effects under pulsed and steady-state pumping, respectively. These findings impose severe restrictions on possible spin relaxation mechanisms., Comment: 10 pages, 7 figures

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 resonances., Comment: 11 pages, 6 figures

Optical control of the spin coherence of quantum well electrons by short laser pulses with circular or linear polarization is studied experimentally and theoretically. For that purpose the coherent electron spin dynamics in a n-doped CdTe/(Cd,Mg)Te quantum well structure was measured by time-resolved pump-probe Kerr rotation, using resonant excitation of the negatively charged exciton (trion) state. The amplitude and phase shifts of the electron spin beat signal in an external magnetic field, that are induced by laser control pulses, depend on the pump-control delay and polarization of the control relative to the pump pulse. Additive and non-additive contributions to pump-induced signal due to the control are isolated experimentally. These contributions can be well described in the framework of a two-level model for the optical excitation of the resident electron to the trion., Comment: 15 pages, 18 figures

We study the electron spin dynamics in p-type GaAs doped with magnetic Mn acceptors by means of time-resolved pump-probe and photoluminescence techniques. Measurements in transverse magnetic fields show a long spin relaxation time of 20 ns that can be uniquely related to electrons. Application of weak longitudinal magnetic fields above 100 mT extends the spin relaxation times up to microseconds which is explained by suppression of the Bir-Aronov-Pikus spin relaxation for the electron on the Mn acceptor., Comment: 5 pages, 3 figures

Experimental and theoretical studies of all-optical spin pump and probe of resident electrons in CdTe/(Cd,Mg)Te semiconductor quantum wells are reported. A two-color Hanle-MOKE technique (based on continuous-wave excitation) and time-resolved Kerr rotation in the regime of resonant spin amplification (based on pulsed excitation) provide a complementary measure of electron spin relaxation time. Influence of electron localization on long-lived spin coherence is examined by means of spectral and temperature dependencies. Various scenarios of spin polarization generation (via the trion and exciton states) are analyzed and difference between continuous-wave and pulsed excitations is considered. Effects related to inhomogeneous distribution of $g$-factor and anisotropic spin relaxation time on measured quantities are discussed., Comment: 26 pages, 19 figures, submitted to special issue on Optical Orientation of Semiconductor Science and Technology

The mechanisms for generation of long-lived spin coherence in a two-dimensional electron gas (2DEG) have been studied experimentally by means of a picosecond pump-probe Kerr rotation technique. CdTe/(Cd,Mg)Te quantum wells with a diluted 2DEG were investigated. The strong Coulomb interaction between electrons and holes, which results in large binding energies of neutral excitons and negatively charged excitons (trions), allows one to address selectively the exciton or trion states by resonant optical excitation. Different scenarios of spin coherence generation were analyzed theoretically, among them the direct trion photocreation, the formation of trions from photogenerated excitons and the electron-exciton exchange scattering. Good agreement between experiment and theory is found., Comment: 18 pages, 20 figures

Electron spin coherence has been generated optically in n-type modulation doped (In,Ga)As/GaAs quantum dots (QDs) which contain on average a single electron per dot. The coherence arises from resonant excitation of the QDs by circularly-polarized laser pulses, creating a coherent superposition of an electron and a trion state. Time dependent Faraday rotation is used to probe the spin precession of the optically oriented electrons about a transverse magnetic field. Spin coherence generation can be controlled by pulse intensity, being most efficient for (2n+1)pi-pulses., Comment: 5 pages, 4 figures