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N. E. Kopteva

Publications and source records attributed to N. E. Kopteva.

18 recordsLinked to original sources

Spin dynamics of excitons and carriers in mixed-cation MA$_{x}$FA$_{1-x}$PbI$_{3}$ perovskite crystals: alloy fluctuations probed by optical orientation

Optical spin orientation measured by time-resolved photoluminescence provides a powerful tool to probe the spin dynamics of excitons and charge carriers in perovskite semiconductors. The impact of alloy fluctuations on the spin dynamics of mixed-cation \MAFAPI{} perovskite single crystals is studied here experimentally. The optical orientation is measured under nonresonant excitation for crystals with $x = 0.1$, $0.4$, and $0.8$ at cryogenic temperatures and compared with data on \MAPI{} crystals. The high degree of exciton optical orientation of $75-80$\% for $x = 0.1$ and $0.8$ reduces to about 60\% for $x = 0.4$. A similar trend is observed for the carrier spin optical orientation. This behavior is attributed to enhanced scattering of free excitons and carriers in the alloys with increased compositional and structural disorder. From the Larmor spin precession measured from spin dynamics in an external magnetic field applied in the Voigt geometry, the electron and hole $g$-factors are evaluated. Their dependence on the band gap energy in \MAFAPI{} crystals follows the universal trend previously established for lead halide perovskites.

cond-mat.mtrl-sci

Optical cooling of nuclear spins in GaAs/(Al,Ga)As quantum wells at subkelvin temperatures: Evidence of the dynamic self-polarization of nuclear spins

We investigate the dynamic polarization of nuclear spins in a nominally undoped GaAs/Al$_{0.35}$Ga$_{0.65}$As quantum well using two complementary experimental approaches: time-resolved Kerr rotation and optical orientation measurements of photoluminescence. Using the first technique, we measure a remarkably large Overhauser field of 3.1 T in a geometry close to the Faraday configuration for a 19.7 nm wide quantum well at a temperature of 1.6 K. A nuclear spin temperature of 6.4 $μ$K is measured at an external magnetic field of 0.006 T following an adiabatic sweep from 0.6 T. Despite the quadrupole-induced nuclear spin splitting inherent to nanostructures, the nuclear spin system is found to follow the predictions of spin temperature theory. Using the optical orientation of the photoluminescence, we investigated nuclear spin dynamics at millikelvin temperatures down to 300 mK. At a temperature of 500 mK, an Overhauser field of 160 mT is generated in an oblique but nearly Voigt magnetic field using low optical power to avoid heating. The nuclear polarization build-up time is of 150 s, consistent with earlier reports at higher temperatures, where hyperfine scattering on free photoexcited electrons governs relaxation. At 500 mK, the onset of dynamic self-polarization of nuclear spins is observed, which becomes more pronounced as the lattice temperature is further reduced to 300 mK. The estimated nuclear spin temperature in the dynamic self-polarization regime can be as low as 200 nK.

cond-mat.mes-hall

Hole spin coherence in InAs/InAlGaAs self-assembled quantum dots emitting at telecom wavelengths

We report measurements of the longitudinal and transverse spin relaxation times of holes in an ensemble of self-assembled InAs/InAlGaAs quantum dots (QDs), emitting in the telecom spectral range. The spin coherence of a single carrier is determined using spin mode-locking in the inhomogeneous ensemble of QDs. Modeling the signal allows us to extract the hole spin coherence time to be in the range of T$_2 = 0.02-0.4$ $μ$s. The longitudinal spin relaxation time T$_1 = 0.5$ $μ$s is measured using the spin inertia method.

cond-mat.mes-hall

Continuous time crystal in an electron-nuclear spin system: stability and melting of periodic auto-oscillations

Crystals spontaneously break the continuous translation symmetry in space, despite the invariance of the underlying energy function. This has triggered suggestions of time crystals analogously lifting translational invariance in time. Originally suggested for closed thermodynamic systems in equilibrium, no-go theorems prevent the existence of time crystals. Proposals for open systems out of equilibrium led to the observation of discrete time crystals subject to external periodic driving to which they respond with a sub-harmonic response. A continuous time crystal is an autonomous system that develops periodic auto-oscillations when exposed to a continuous, time-independent driving, as recently demonstrated for the density in an atomic Bose-Einstein condensate with a crystal lifetime of a few ms. Here we demonstrate an ultra-robust continuous time crystal in the nonlinear electron-nuclear spin system of a tailored semiconductor with a coherence time exceeding hours. Varying the experimental parameters reveals huge stability ranges of this time crystal, but allows one also to enter chaotic regimes, where aperiodic behavior appears corresponding to melting of the crystal. This novel phase of matter opens the possibility to study systems with nonlinear interactions in an unprecedented way.

cond-mat.mes-hall

Spin-Flip Raman Scattering on Electrons and Holes in Two-Dimensional (PEA)$_2$PbI$_4$ Perovskites

The class of Ruddlesden-Popper type (PEA)$_2$PbI$_4$ perovskites comprises two-dimensional (2D) structures whose optical properties are determined by excitons with a large binding energy of about 260 meV. It complements the family of other 2D semiconductor materials by having the band structure typical for lead halide perovskites, that can be considered as inverted compared to conventional III-V and II-VI semiconductors. Accordingly, novel spin phenomena can be expected for them. Spin-flip Raman scattering is used here to measure the Zeeman splitting of electrons and holes in a magnetic field up to 10 T. From the recorded data, the electron and hole Landé factors ($g$-factors) are evaluated, their signs are determined, and their anisotropies are measured. The electron $g$-factor value changes from $+2.11$ out-of-plane to $+2.50$ in-plane, while the hole $g$-factor ranges between $-0.13$ and $-0.51$. The spin flips of the resident carriers are arranged via their interaction with photogenerated excitons. Also the double spin-flip process, where a resident electron and a resident hole interact with the same exciton, is observed showing a cumulative Raman shift. Dynamic nuclear spin polarization induced by spin-polarized holes is detected in corresponding changes of the hole Zeeman splitting. An Overhauser field of the polarized nuclei acting on the holes as large as $0.6$ T can be achieved.

cond-mat.mes-hall

Weak dispersion of exciton Landé factor with band gap energy in lead halide perovskites: Approximate compensation of the electron and hole dependences

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 Landé 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.

cond-mat.mes-hall

Evidencing the squeezed dark nuclear spin state in lead halide perovskites

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 $ξ_s < 0.3$. 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.

cond-mat.mtrl-sci

Mode locking of hole spin coherences in CsPb(Cl,Br)$_3$ perovskite nanocrystals

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.

cond-mat.mes-hall

The Landé factors of electrons and holes in lead halide perovskites: universal dependence on the band gap

The Landé 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 Landé 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 Landé 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.

cond-mat.mtrl-sci

Zeeman and Davydov splitting of Frenkel excitons in the antiferromagnet CuB$_2$O$_4$

The optical spectra of antiferromagnetic copper metaborate CuB$_2$O$_4$ are characterized by an exceptionally rich structure of narrow absorption lines due to electronic transitions within the magnetic Cu$^{2+}$ ions, but their unambiguous identification and behavior in magnetic field remain far from being fully understood. We studied the polarized magneto-absorption spectra of this tetragonal antiferromagnet with a high spectral resolution in the range of $1.4055-1.4065$ eV in magnetic fields up to 9.5 T and temperatures from 1.6 up to $T_N = 20$ K. We observed a set of eight absorption lines at $T=1.6$ K in magnetic fields exceeding 1.4 T which we identified as arising from Frenkel excitons related to the ground and the first excited state of Cu$^{2+}$ ions. The number of these excitons is defined by the presence of the four Cu$^{2+}$ ions with the doubly-degenerate spin state $S = 1/2$ at the 4$b$ positions in the crystallographic unit cell. The energies of these excitons are determined the exchange interaction of 0.5 meV of Cu$^{2+}$ ions in the excited state with surrounding ions and by the Davydov splitting of 0.12 meV. In large magnetic field the observed Zeeman splitting is controlled by the anisotropic $g$-factors of both the ground and excited states. We developed a theoretical model of Frenkel excitons in magnetic field that accounts for specific features of the spin structure and exchange interactions in CuB$_2$O$_4$. The model was used for fitting the experimental data and evaluation of Frenkel exciton parameters, such as the Davydov splitting, the molecular exchange energy, and the $g$-factors of the ground and excited states of the Cu$^{2+}$ ions.

cond-mat.other

Shielding of external magnetic field by dynamic nuclear polarization in (In,Ga)As quantum dots

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.

cond-mat.mes-hall

Suppression of nuclear spin fluctuations in an InGaAs quantum dot ensemble by GHz-pulsed optical excitation

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.

cond-mat.mes-hall

Effect of electric current on optical orientation of electrons in AlGaAs/GaAs heterostructure

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.

cond-mat.mes-hall

Decay and revival of electron spin polarization in an ensemble of (In,Ga)As quantum dots

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 build-up 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.

cond-mat.mes-hall

Long-range p-d exchange interaction in a ferromagnet-semiconductor Co/CdMgTe/CdTe quantum well hybrid structure

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 $Δ_S$ on the external magnetic field $B$. We show that in strong magnetic field $Δ_S$ is a linear function of $B$ with an offset of $Δ_{pd} = 50-100~μ$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.

cond-mat.mtrl-sci

Inverse-phase Rabi oscillations in semiconductor microcavities

We study experimentally the oscillations of a non stationary transient signal of a semiconductor microcavity with embedded InGaAs quantum wells. The oscillations occur as a result of quantum beats between the upper and lower polariton modes due to the strong exciton-photon coupling in the microcavity sample (Rabi oscillations). The registration of spectrally resolved signal has allowed for separate observation of oscillations at the eigenfrequencies of two polariton modes. Surprisingly, the observed oscillations measured at the lower and upper polariton modes have opposite phases. We demonstrate theoretically that the opposite-phase oscillations are caused by the pump-induced modification of polariton Hopfield coefficients, which govern the ratio of exciton and photon components in each of the polartion modes. Such a behaviour is a fundamental feature of the quantum beats of coupled light-matter states. In contrast, the reference pump-probe experiment performed for the pure excitonic states in a quantum well heterostructure with no microcavity revealed the in-phase oscillations of the pump-probe signals measured at different excitonic levels.

cond-mat.mes-hall

Ultimate photo-induced Kerr rotation achieved in semiconductor microcavities

Photoinduced Kerr rotation by more than $π/2$ radians is demonstrated in planar quantum well microcavity in the strong coupling regime. This result is close to the predicted theoretical maximum of $π$. It is achieved by engineering microcavity parameters such that the optical impedance matching condition is reached at the smallest negative detuning between exciton resonance and the cavity mode. This ensures the optimum combination of the exciton induced optical non-linearity and the enhancement of the Kerr angle by the cavity. Comprehensive analysis of the polarization state of the light in this regime shows that both renormalization of the exciton energy and the saturation of the excitonic resonance contribute to the observed optical nonlinearities.

cond-mat.mes-hall

Optics of spin-noise-induced gyrotropy of asymmetric microcavity

The optical gyrotropy noise of a high-finesse semiconductor Bragg microcavity with an embedded quantum well (QW) is studied at different detunings of the photon mode and the QW exciton resonances. A strong suppression of the noise magnitude for the photon mode frequencies lying above exciton resonances is found. We show that such a critical behavior of the observed optical noise power is specific of asymmetric Fabry-Perot resonators. As follows from our analysis, at a certain level of intracavity loss, the reflectivity of the asymmetric resonator vanishes, while the polarimetric sensitivity to the gyrotropy changes dramatically when moving across the critical point. The results of model calculations are in a good agreement with our experimental data on the spin noise in a single-quantum-well microcavity and are confirmed also by the spectra of the photo-induced Kerr rotation in the pump-probe experiments.

cond-mat.mes-hall