arXiv subjects

Dmitri R. Yakovlev

Publications and source records attributed to Dmitri R. Yakovlev.

At least 37 records · Page 2Linked to original sources

arXiv2025

Resonant spin amplification and accumulation in MAPbI$_3$ single crystals

Quantum technologic and spintronic applications require reliable semiconducting materials that enable a significant, long-living spin polarization of electronic excitations and offer the ability to manipulate it optically in an external field. Due to the specifics of band structure and remarkable spin-dependent properties, the lead halide perovskite semiconductors are suitable candidates for that. Here, the carrier spin dynamics in a MAPbI$_3$ (MA = methylammonium) perovskite single crystal with thickness of 20 $μ$m are studied by the time-resolved Kerr ellipticity technique at cryogenic temperatures. Long times of longitudinal electron spin relaxation $T_1 = 30$ ns and transverse electron spin dephasing $T_{2,e}^*=21$ ns are found. The spin dynamics lasting longer than the applied laser pulse repetition period give rise to spin accumulation effects. We exploit them through the resonant spin amplification, polarization recovery, and spin inertia techniques to study the electron and hole spin systems coupled with the nuclear spins. These results establish the lead halide perovskite semiconductors as suitable platform for quantum technologies relying on spin-dependent phenomena.

cond-mat.mtrl-sci↗

arXiv2025

Optical orientation of excitons and charged carriers in MAPbI$_3$ perovskite single crystals in the orthorhombic phase

Optical orientation of exciton and carrier spins by circularly polarized light is the basic phenomenon in the spin physics of semiconductors. Here, we investigate spin orientation in MAPbI3 lead halide perovskite crystals at the cryogenic temperature of 1.6 K, where the material has an orthorhombic crystal structure. The recombination and spin dynamics of excitons and carriers are measured by time-resolved photoluminescence after circularly polarized excitation. The optical orientation of excitons reaches 85\%, which persists within their lifetime of 15-80 ps. This high orientation is maintained for excitation laser detunings from the exciton resonance to higher energies by up to 0.3 eV, then decreases and vanishes above 1.5 eV detuning. This indicates that the Dyakonov-Perel spin relaxation mechanism based on inversion symmetry breaking is inactive in MAPbI3 crystals with orthorhombic symmetry. The optical orientation of localized and spatially-separated electrons and holes results in 40\% circular polarization of their emission. Their contributions can be identified from the complex spin beats dynamics in transverse magnetic field. The dynamics analysis gives values of the Landé g-factors of 2.83 for electrons and 0.54 for holes. Also, the magnetic-field-induced polarization of excitons and carriers is analyzed in magnetic fields up to 6 T, showing that their spin relaxation times are longer than their lifetimes. Namely, for the excitons, the spin relaxation time exceeds the lifetime by a factor of 6. We model the dynamics of optical orientation degree for cumulative contributions of excitons and carriers and show that the exciton recombination dynamics can control these dynamics. The polarized emission of excitons and localized carriers, produced by their polarization on Zeeman-split levels in magnetic fields, is modeled.

cond-mat.mes-hall↗

arXiv2025

Coherent spin dynamics of electrons and holes photogenerated with large kinetic energy in lead halide perovskite crystals

The coherent spin dynamics of electrons and holes are studied in a FA0.9Cs0.1PbI2.8Br0.2 perovskite bulk crystal, using time-resolved Kerr ellipticity in a two-color pump-probe scheme. The probe photon energy is tuned to the exciton resonance, while the pump photon energy is detuned from it up to 0.75 eV to higher energies. The spin-oriented electrons and holes photogenerated with significant excess kinetic energy relax into states in vicinity of the band gap, where they undergo Larmor precession in an external magnetic field. At cryogenic temperatures down to 1.6 K, the spin dephasing time reaches the nanosecond range. During energy relaxation, the carrier spin relaxation is inefficient and only happens when the carriers become localized. In experiments with two pump pulses, all-optical control of the amplitudes and phases of the electron and hole spin signals is achieved in the additive regime by varying the intensities of the pump pulses and the time delay between them.

cond-mat.mes-hall↗

arXiv2024

Landé g-factors and spin dynamics of charge carriers in CuCl nanocrystals in a glass matrix

The spin properties of charge carriers confined in CuCl semiconductor nanocrystals (NCs) of different sizes (radius from 1.8 nm up to 28 nm) crystallized in a glass matrix are studied experimentally and theoretically. By means of photoluminescence, spin-flip Raman scattering, time-resolved Faraday ellipticity, and time-resolved differential transmission performed at temperatures in the range of $1.6 - 120$ K at magnetic fields up to 8 T, comprehensive information on the Landé $g$-factors as well as the population and spin dynamics is received. The spin signals are contributed by confined electrons with a $g$-factor close to 2, which shows a weak increase with decreasing NC size, i.e. increasing electron confinement energy. We revisit the theory of exciton confinement as a whole in spherical NCs within the six-band valence band model in order to describe the size dependence of the $Z_3$ and $Z_{1,2}$ exciton energies in CuCl NCs. We demonstrate theoretically that the stronger increase of the $Z_{1,2}$ energy transitions with decreasing radius can be explained by the strong absorption from the excited exciton state caused by strong heavy hole-light hole mixing in the exciton. The parameters of the six-band Hamiltonian describing both the exciton and hole kinetic energies are estimated from the comparison of the calculated and experimental size dependences of the exciton transitions. A theoretical model of the size-dependent Landé $g$-factors for electron and hole confined in spherical NCs of semiconductors with negative spin-orbit splitting of the valence band is developed.

cond-mat.mes-hall↗

arXiv2024

Effect of crystal symmetry of lead halide perovskites on the optical orientation of excitons

The great variety of lead halide perovskite semiconductors represents an outstanding platform for studying crystal symmetry effects on the spin-dependent properties. Access to them is granted through optical orientation of exciton and carrier spins by circularly polarized photons. Here, the exciton spin polarization is investigated at $1.6$\,K cryogenic temperature in four lead halide perovskite crystals with different symmetries: (almost) cubic in FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$ and FAPbBr$_3$, and orthorhombic in MAPbI$_3$ and CsPbBr$_3$. Giant optical orientation of 85\% is found for the excitons in FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$, MAPbI$_3$, and CsPbBr$_3$, while it amounts to 20\% in FAPbBr$_3$. For all studied crystals, the optical orientation is robust to detuning of the laser photon energy from the exciton resonance, remaining constant for high energy detunings up to 0.3~eV, above which it continuously decreases to zero for detunings exceeding 1~eV. No acceleration of the spin relaxation for excitons with large kinetic energy is found in the cubic and orthorhombic crystals. This evidences the absence of the Dyakonov-Perel spin relaxation mechanism, which is based on the Rashba-Dresselhaus splitting of spin states at finite $k$-vectors. This indicates that the spatial inversion symmetry is maintained in perovskite crystals, independent of the cubic or orthorhombic phase.

cond-mat.mtrl-sci↗

arXiv2024

Landé $g$-factors of electrons and holes strongly confined in CsPbI$_3$ perovskite nanocrystals in glass

The Landé $g$-factor of charge carriers is a key parameter in spin physics controlling spin polarization and spin dynamics. In turn, it delivers information of the electronic band structure in vicinity of the band gap and its modification in nanocrystals provided by strong carrier confinement. The coherent spin dynamics of electrons and holes are investigated in CsPbI$_3$ perovskite nanocrystals with sizes varied from 4 to 16 nm by means of time-resolved Faraday ellipticity at the temperature of 6 K. The Landé $g$-factors of the charge carriers are evaluated through the Larmor spin precession in magnetic fields up to 430 mT across the spectral range from 1.69 to 2.25 eV, provided by variation of the nanocrystal size. The spectral dependence of the electron $g$-factor follows the model predictions when accounting for the mixing of the electronic bands with increasing confinement resulting from a decrease of the nanocrystal size. The spectral dependence of the hole $g$-factor, changing from $-0.19$ to $+1.69$, is considerably stronger than expected from the model. We analyze several mechanisms and conclude that none of them can be responsible for this difference. The renormalizations of the electron and hole $g$-factors roughly compensate each other, providing spectral independence for the bright exciton $g$-factor with a value of about $+2.2$.

cond-mat.mes-hall↗

arXiv2024

Hole spin precession and dephasing induced by nuclear hyperfine fields in CsPbBr$_3$ and CsPb(Cl,Br)$_3$ nanocrystals in a glass matrix

The coherent spin dynamics of holes are investigated for CsPbBr$_3$ and CsPb(Cl,Br)$_3$ perovskite nanocrystals in a glass matrix using the time-resolved Faraday rotation/ellipticity techniques. In an external magnetic field, pronounced Larmor spin precession of the hole spins is detected across a wide temperature range from 5 to 300 K. The hole Landé $g$-factor varies in the range of $0.8-1.5$, in which it increases with increasing high energy shift of the exciton due to enhanced confinement in small nanocrystals. The hole spin dephasing time decreases from 1 ns to 50 ps in this temperature range. Nuclear spin fluctuations have a pronounced impact on the hole spin dynamics. The hyperfine interaction of the holes with nuclear spins modifies their spin polarization decay and induces their spin precession in zero external magnetic field. The results can be well described by the model developed in Ref. 41, from which the hyperfine interaction energy of a hole spin with the nuclear spin fluctuation in range of $2-5$ $μ$eV is evaluated.

cond-mat.mes-hall↗

arXiv2024

Temperature dependence of the electron and hole Landé g-factors in CsPbI3 nanocrystals in a glass matrix

The coherent spin dynamics of electrons and holes in CsPbI3 perovskite nanocrystals in a glass matrix are studied by the time-resolved Faraday ellipticity technique in magnetic fields up to 430 mT across a temperature range from 6 K up to 120 K. The Landé g-factors and spin dephasing times are evaluated from the observed Larmor precession of electron and hole spins. The nanocrystal size in the three studied samples varies from about 8 to 16 nm, resulting in exciton transition varying from 1.69 to 1.78 eV at the temperature of 6 K, allowing us to study the corresponding energy dependence of the g-factors. The electron g-factor decreases with increasing confinement energy in the NCs as result of NC size reduction, and also with increasing temperature. The hole g-factor shows the opposite trend. A model analysis shows that the variation of g-factors with NC size arises from the transition energy dependence of the g-factors, which becomes strongly renormalized by temperature.

cond-mat.mes-hall↗

arXiv2024

Bright-Dark Exciton Interplay Evidenced by Spin Polarization in CdSe/CdMnS Nanoplatelets

Diluted magnetic semiconductor (DMS) colloidal nanocrystals demonstrate remarkable magneto-optical properties. However, the behavior of circular polarization of their emission in high magnetic fields remains unclear. We measure magneto-optical properties of colloidal CdSe/CdMnS nanoplatelets in high magnetic fields up to 30 T and at cryogenic temperatures. The degree of circular polarization of photoluminescence demonstrates non-monotonous behavior in a magnetic field. In low magnetic fields, the polarization degree is positive, due to an exchange interaction of excitons with localized spins of magnetic Mn ions. The exchange interaction is strong enough to overcome the intrinsic Zeeman splitting, which provides negatively polarized emission in nonmagnetic CdSe/CdS nanoplatelets. After reaching a maximum the polarization degree starts to decrease and reverses the sign to negative in high magnetic fields. The critical magnetic field, in which the sign is reversed, increases when temperature is elevated. We develop a model, which explains this behavior by an interplay of bright and dark exciton recombination.

cond-mat.mes-hall↗

arXiv2024

Nuclear spin relaxation mediated by donor-bound and free electrons in wide CdTe quantum wells

The nuclear spin systems in CdTe/(Cd,Zn)Te and CdTe/(Cd,Mg)Te quantum wells (QW) are studied using a multistage technique combining optical pumping and Hanle effect-based detection. The samples demonstrate drastically different nuclear spin dynamics in zero and weak magnetic fields. In CdTe/(Cd,Zn)Te, the nuclear spin relaxation time is found to strongly increase with the magnetic field, growing from 3 s in zero field to tens of seconds in a field of 25 G. In CdTe/(Cd,Mg)Te the relaxation is an order of magnitude slower, and it is field-independent up to at least 70 G. The differences are attributed to the nuclear spin relaxation being mediated by different kinds of resident electrons in these QWs. In CdTe/(Cd,Mg)Te, a residual electron gas trapped in the QW largely determines the relaxation dynamics. In CdTe/(Cd,Zn)Te, the fast relaxation in zero field is due to interaction with localized donor-bound electrons. Nuclear spin diffusion barriers form around neutral donors when the external magnetic field exceeds the local nuclear field, which is about $B_L\approx$0.4 G in CdTe. This inhibits nuclear spin diffusion towards the donors, slowing down relaxation. These findings are supported by theoretical modeling. In particular, we show that the formation of the diffusion barrier is made possible by several features specific to CdTe: (i) the large donor binding energy (about 10 meV), (ii) the low abundance of magnetic isotopes (only $\approx$30 % of nuclei have nonzero spin), and (iii) the absence of nuclear quadrupole interactions between nuclei. The two latter properties are also favorable to nuclear spin cooling via optical pumping followed by adiabatic demagnetization. Under non-optimized conditions we have reached sub-microkelvin nuclear spin temperatures in both samples, lower than all previous results obtained in GaAs.

cond-mat.mes-hall↗

arXiv2024

Spin-dependent exciton-exciton interactions in a mixed lead halide perovskite crystal

We investigate the two-pulse photon echo response of excitons in the mixed lead halide perovskite crystal \sample in dependence on the excitation intensity and polarization of the incident laser pulses. Using spectrally narrow picosecond laser pulses, we address localized excitons with long coherence times $T_2 \approx 100\,$ps. This approach offers high sensitivity for the observation of excitation-induced changes in the homogeneous linewidth $Γ_2=2\hbar/T_2$ on the $μ$eV scale. Through intensity-dependent measurements, we evaluate the increase of $Γ_2$ by 10~$μ$eV at an exciton density of 10$^{17}$~cm$^{-3}$ being comparable with the intrinsic linewidth of 14$\,μ$eV. We observe that the decay of the photon echo and its power dependence are sensitive to the polarization configuration of the excitation pulses, which indicates that spin-dependent exciton-exciton interactions contribute to excitation-induced dephasing. In cross-linear polarization, the decay is faster and its dependence on exciton density is stronger as compared to the co-polarized configuration. Using a two-exciton model accounting for different spin configurations we are able to reproduce the experimental results.

cond-mat.mes-hall↗

arXiv2024

Optical spin orientation of localized electrons and holes interacting with nuclei in an FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$ perovskite crystal

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.

cond-mat.mes-hall↗

arXiv2024

Temperature-dependent photoluminescence dynamics of CsPbBr$_3$ and CsPb(Cl,Br)$_3$ perovskite nanocrystals in a glass matrix

Lead halide perovskite nanocrystals (NCs) in a glass matrix combine excellent optical properties and stability against environment. The spectral and temporal characteristics of photoluminescence from CsPbBr$_3$ and CsPb(Cl,Br)$_3$ nanocrystals (NCs) in a fluorophosphate glass matrix are measured in a temperature range from 6 to 270 K in order to reveal factors that determine their quantum yield and recombination dynamics. At low temperatures, the recombination dynamics is characterized by three decay components with time scales on the order of 1 ns, 10 ns, and 1 $μ$s. The relative contributions of the corresponding processes and their characteristic times are strongly temperature dependent. The emission intensity decreases with growing temperature. This effect is stronger in smaller NCs, which highlights the role of surface states. These experimental results are discussed on the basis of a model taking into account the NC energy structure and the presence of electron and hole surface trap states. The photoluminescence dynamics at low temperatures is dominated by charge-carrier radiative recombination and relaxation to shallow traps. At temperatures exceeding 100 K, the dynamics is affected by carrier activation to the excited states.

cond-mat.mtrl-sci↗

arXiv2023

Exciton-polaritons in CsPbBr$_3$ crystals revealed by optical reflectivity in high magnetic fields and two-photon spectroscopy

Cesium lead bromide (CsPbBr$_3$) is a representative material of the emerging class of lead halide perovskite semiconductors that possess remarkable optoelectronic properties. Its optical properties in the vicinity of the band gap energy are greatly contributed by excitons, which form exciton-polaritons due to strong light-matter interactions. We examine exciton-polaritons in solution-grown CsPbBr$_3$ crystals by means of circularly-polarized reflection spectroscopy measured in high magnetic fields up to 60 T. The excited 2P exciton state is measured by two-photon absorption. Comprehensive modeling and analysis provides detailed quantitative information about the exciton-polariton parameters: exciton binding energy of 32.5 meV, oscillator strength characterized by longitudinal-tranverse splitting of 5.3 meV, damping of 6.7 meV, reduced exciton mass of $0.18 m_0$, exciton diamagnetic shift of 1.6 $μ$eV/T$^2$, and exciton Landé factor $g_X=+2.35$. We show that the exciton states can be well described within a hydrogen-like model with an effective dielectric constant of 8.7. From the measured exciton longitudinal-transverse splitting we evaluate the Kane energy of $E_p=15$ eV, which is in reasonable agreement with values of $11.8-12.5$ eV derived from the carrier effective masses.

cond-mat.mes-hall↗

arXiv2023

Giant optical orientation of exciton spins in lead halide perovskite crystals

Optical orientation of carrier spins by circularly polarized light is the basis of spin physics in semiconductors. Here, we demonstrate strong optical orientation of 85\%, approaching the ultimate limit of unity, for excitons in FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$ lead halide perovskite bulk crystals. Time-resolved photoluminescence allows us to distinguish excitons with 60~ps lifetime from electron-hole recombination in the spin dynamics detected via coherent spin quantum beats in magnetic field. We reveal electron-hole spin correlations through linear polarization beats after circularly polarized excitation. Detuning of the excitation energy from the exciton resonance up to 0.5~eV does not reduce the optical orientation, evidencing clean chiral selection rules in agreement with atomistic calculations, and suppressed spin relaxation of electrons and holes even with large kinetic energies.

cond-mat.mes-hall↗

arXiv2023

Long-lived exciton coherence in mixed-halide perovskite crystals

Compositional engineering of the optical properties of hybrid organic-inorganic lead halide perovskites is one of the cornerstones for the realization of efficient solar cells and tailored light-emitting devices. We study the effect of compositional disorder on coherent exciton dynamics in a mixed FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$ perovskite crystal using photon echo spectroscopy. We reveal that the homogeneous linewidth of excitons can be as narrow as 16$μ$eV at a temperature of 1.5K. The corresponding exciton coherence time of $T_2=83$ps is exceptionally long being attributed to the localization of excitons due to variation of composition at the scale of ten to hundreds of nanometers. From spectral and temperature dependences of the two- and three-pulse photon echo decay we conclude that for low-energy excitons, pure decoherence associated with elastic scattering on phonons is comparable with the exciton lifetime, while for excitons with higher energies, inelastic scattering to lower energy states via phonon emission dominates.

cond-mat.mes-hall↗

arXiv2022

Coherent Spin Dynamics of Electrons in Two-Dimensional (PEA)$_2$PbI$_4$ Perovskites

The versatile potential of lead halide perovskites and two-dimensional materials is merged in the Ruddlesen-Popper perovskites having outstanding optical properties. Here, the coherent spin dynamics in Ruddlesen-Popper (PEA)$_2$PbI$_4$ perovskites are investigated by picosecond pump-probe Kerr rotation in an external magnetic field. The Larmor spin precession of resident electrons with a spin dephasing time of 190~ps is identified. The longitudinal spin relaxation time in weak magnetic fields measured by the spin inertia method is as long as 25~$μ$s. A significant anisotropy of the electron $g$-factor with the in-plane value of $+2.45$ and out-of-plane value of $+2.05$ is found. The exciton out-of-plane $g$-factor is measured to be of $+1.6$ by magneto-reflectivity. This work contributes to the understanding of the spin-dependent properties of two-dimensional perovskites and their spin dynamics.

cond-mat.mtrl-sci↗

arXiv2021

Exchange interaction in the yellow exciton series of cuprous oxide

We experimentally and numerically investigate the exchange interaction of the yellow excitons in cuprous oxide. By varying the material parameters in the numerical calculations, we can interpret experimental findings and understand their origin in the complex band structure and central-cell corrections. In particular, we experimentally observe the reversal of the ortho- and paraexciton for the $2S$ yellow exciton, and explain this phenomenon by an avoided crossing with the green $1S$ orthoexciton in a detailed numerical analysis. Furthermore, we discuss the exchange splitting as a function of the principal quantum number $n$ and its deviation from the $n^{-3}$ behavior expected from a hydrogenlike model. We also explain why the observed exchange splitting of the green $1S$ exciton is more than twice the splitting of the yellow $1S$ state.

cond-mat.mtrl-sci↗