arXiv subjects

Ilya A. Akimov

Publications and source records attributed to Ilya A. Akimov.

17 recordsLinked to original sources

arXiv2026

Assessing the classicality of photon echo from excitons in lead halide perovskite nanocrystals

Photon echo (PE) spectroscopy is a powerful technique for probing decoherence mechanisms and charge carrier dynamics in semiconductor systems. Beyond traditional coherence measurements, characterizing the photon statistics of the echo signal is important for assessing its potential in quantum information applications and understanding the underlying quantum mechanical processes. Here, we study the photon statistics of PE signals generated by excitons in ensembles of lead halide perovskite CsPbI$_3$ nanocrystals at cryogenic temperature of 2 K using continuous-variable quantum state optical tomography based on homodyne detection. Pronounced Rabi oscillations of the PE amplitude allow us to evaluate the statistics for various pulse areas in the excitation sequence. The damping of the oscillations with increasing pulse area is attributed to spatial excitation inhomogeneity and excitation-induced dephasing. Despite the large ensemble of optically addressed excitons, the efficiency of generated PE signals is low which is attributed to the complex energy level structure of excitons and non-radiative recombination channels in CsPbI$_3$ nanocrystals. We analyze the statistical characteristics of PE via the second-order correlation function $g^{(2)}(0)$ and the characteristic function for different combinations of the areas of the excitation pulses. Our results show that $g^{(2)}(0) = 1$, and the characteristic function of the PE signal corresponds to classical behavior. The formation of photon echoes as well as $g^{(2)}(0) = 1$ at the echo time is reproduced by a quantized free-space multimode model. Despite the relatively low efficiency, the photon echo exhibits a high degree of coherence and minimal classical noise, consistent with Poissonian statistics.

cond-mat.mes-hall↗

arXiv2026

Bright-dark exciton splitting in lead halide perovskite crystals accessed via quantum beats in photon echoes

Understanding the fine structure of excitons is crucial for optoelectronic and quantum photonic applications of lead halide perovskites. It is demonstrated that polarization-sensitive photon echo spectroscopy in magnetic field provides a powerful method to access coherent exciton dynamics and reveal their energy level structure, which is hidden by inhomogeneous broadening. Exciton quantum beats observed in both Faraday and Voigt geometries offer a precise probe of the energy splittings among the four 1$s$ exciton states, enabling determination of the fine structure and bright-dark splittings. Application of this technique to bulk mixed halide perovskite crystals FA$_{0.9}$Cs$_{0.1}$PbI$_{2.8}$Br$_{0.2}$ reveals a bright-dark exciton splitting of $Δ_\mathrm{X}=0.46~$meV, along with electron and hole Landé $g$ factors $g_\mathrm{e}=3.38$ and $g_\mathrm{h}=-1.14$, respectively. The quantum beats persist on timescales of 20--50$~$ps, demonstrating remarkably robust spin and optical coherences at cryogenic temperature of 2$~$K. The decay of the quantum beats of the outer doublet is governed by dephasing due to dispersion of the bright-dark splitting of $\sim0.06~$meV caused by localization potential fluctuations, while dephasing in the bright exciton inner doublet originates from a small zero field splitting of $\sim0.035~$meV due to anisotropic potentials.

cond-mat.mes-hall↗

arXiv2026

Magnetic switching of exciton lifetime in CrSBr

Exciton dynamics in layered magnetic semiconductors provide a sensitive probe of the interplay between spin order and light-matter interaction. Here, we study thin CrSBr layers using time-resolved photoluminescence spectroscopy in an external magnetic field, revealing a step-like reduction in the exciton lifetime from 11 to 7 ps, during the magnetization flip from the antiferromagnetic to the ferromagnetic phase. The reduction of the exciton lifetime in the ferromagnetic phase persists below the Néel temperature, as evidenced by its strong magnetic-field dependence that disappears in the paramagnetic phase. Ab initio calculations reveal a one-dimensional nature of free excitons accompanied by a pronounced change in the oscillator strength across the magnetic phase transition predicting a shorter radiative lifetime of free excitons in the antiferromagnetic phase of CrSBr contradicting the experimental observations. This discrepancy is explained by strong localization of excitons at low tempature. We show both experimentally and theoretically that the observed magnetic switching of the exciton lifetime is attributed to a larger exciton localization volume leading to a larger oscillator strength in the ferromagnetic phase. The results show that disorder-induced localization effects play a key role in exciton dynamics in CrSBr.

cond-mat.mes-hall↗

arXiv2025

Exciton spin structure in lead halide perovskite semiconductors explored via the spin dynamics in magnetic field

We theoretically investigate the spin structure and spin dynamics of excitons in bulk lead halide perovskite semiconductors with cubic, tetragonal, and orthorhombic crystal symmetry. The exciton spin structure and its modification by an external magnetic field are modeled for different regimes defined by the relative magnitude of the electron-hole exchange interaction (splitting between dark and bright states) and the Zeeman spin splitting. The effects of crystal symmetry and magnetic field orientation with respect to the crystal axes are considered for lead halide perovskite crystals with band gaps in the range 1.4 - 3.5 eV, having different ratios of electron and hole g-factors. For cubic symmetry, in a longitudinal magnetic field, our theory predicts quantum beats between the bright exciton states under linearly polarized excitation and detection, while the dark exciton remains optically inactive. In a transverse magnetic field, all exciton spin states become optically active and can be excited by circularly polarized light. Reduction of the crystal symmetry leads to a zero-field offset of the exciton Larmor precession frequencies, modifying the Zeeman splitting energy dependence on magnetic field. This theoretical framework allows for the extraction of the strength of the exchange interaction and the crystal symmetry. Experimentally, we measure the exciton spin coherence via time-resolved photoluminescence at a temperature of 1.6 K in longitudinal and transverse magnetic fields in orthorhombic MAPbI3 crystals. Polarization beats at the frequency of the bright exciton are observed in both configurations. Comparison with theory indicates that the excitons are in the strong exchange interaction regime, and the reduction of symmetry does not lead to a significant splitting of the exciton spin levels.

cond-mat.other↗

arXiv2025

Efficient launch of shear phonons in photostrictive halide perovskites

Optical generation of transverse coherent phonons by femtosecond light pulses is appealing for high-speed sub-THz active control of material properties. Lead-free double perovskite semiconductors, such as Cs2AgBiBr6, attract particular interest due to their cubic to tetragonal phase transition below room temperature and strong polaron effects from carrier-lattice coupling. Here, we reveal that the anisotropic photostriction in halide perovskites with tetragonal crystal structure represents an efficient non-thermal tool for generating transverse coherent phonons. In particular, we demonstrate that along with compressive strain, optical generation of photoexcited carriers leads to strong shear strain in Cs2AgBiBr6 below the phase transition temperature of 122 K. Using time-domain Brillouin spectroscopy, we observe coherent transverse and longitudinal acoustic phonons with comparable amplitudes in the tetragonal phase, while in the cubic phase only longitudinal phonons are generated. The polarization of the photoinduced transverse phonons is dictated by the projection of the c-axis on the surface plane, which leads to a prominent anisotropic polarization response in the detection. The generated strain pulses correspond to transverse acoustic soft eigenmodes with a strong temperature dependence of dispersion, which provides an additional degree of freedom for active hypersonic control.

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↗

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

Spin relaxation of localized electrons in monolayer MoSe$_2$: importance of random effective magnetic fields

We study the Hanle and spin polarization recovery effects on resident electrons in a monolayer MoSe$_2$ on EuS. We demonstrate that localized electrons provide the main contribution to the spin dynamics signal at low temperatures below 15~K for small magnetic fields of only a few mT. The spin relaxation of these electrons is determined by random effective magnetic fields due to a contact spin interaction, namely the hyperfine interaction with the nuclei in MoSe$_2$ or the exchange interaction with the magnetic ions of the EuS film. From the magnetic field angular dependence of the spin polarization we evaluate the anisotropy of the intervalley electron $g$-factor and the spin relaxation time. The non-zero in-plane $g$-factor $|g_x|\approx 0.1$, the value of which is comparable to its dispersion, is attributed to randomly localized electrons in the MoSe$_2$ layer.

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↗

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↗

arXiv2020

Resonant thermal energy transfer to magnons in a ferromagnetic nanolayer

Energy harvesting is a modern concept which makes dissipated heat useful by transferring thermal energy to other excitations. Most of the existing principles for energy harvesting are realized in systems which are heated continuously, for example generating DC voltage in thermoelectric devices. Here we present the concept of high-frequency energy harvesting where the dissipated heat in a sample excites resonant magnons in a 5-nm thick ferromagnetic metal layer. The sample is excited by femtosecond laser pulses with a repetition rate of 10 GHz which results in temperature modulation at the same frequency with amplitude ~0.1 K. The alternating temperature excites magnons in the ferromagnetic nanolayer which are detected by measuring the net magnetization precession. When the magnon frequency is brought onto resonance with the optical excitation, a 12-fold increase of the amplitude of precession indicates efficient resonant heat transfer from the lattice to coherent magnons. The demonstrated principle may be used for energy harvesting in various nanodevices operating at GHz and sub-THz frequency ranges.

cond-mat.mtrl-sci↗

arXiv2017

Optical properties of opaline photonic crystals covered by phase-change material Ge$_2$Sb$_2$Te$_5$

The physical origin of resonant Wood's anomalies in the reflection spectra of three-dimensional (3D) opaline photonic crystals covered with Ge$_2$Sb$_2$Te$_5$ (GST225) is discussed. For this purpose, the optical reflection spectra are studied for different incident angles of light both experimentally and theoretically. The performed eigenmode analysis reveals that the Wood's anomalies originate from the quasiguided modes which appear in the GST225 capping layer. This conclusion is supported by the simulated electromagnetic near-field distributions of incident light at resonant frequencies. The experimental reflection spectra are in a good agreement with theoretical calculations performed by the Fourier modal method in the scattering matrix form.

physics.optics↗

arXiv2015

THz lattice vibrations for active plasmonics with light: Ultrafast optical response in gold/telluride hybrid plasmonic crystals

Excitation of coherent optical phonons in solids provides a pathway for ultrafast modulation of light on a sub-ps timescale. Here, we report on efficient 3.6 THz modulation of light reflected from hybrid metal/semiconductor plasmonic crystals caused by lattice vibrations in a few nm thick layer of elemental tellurium. We observe that surface plasmon polaritons contribute significantly to photoinduced formation of this thin layer at the interface between a telluride-based II-VI semiconductor, such as (Cd,Mg)Te or (Cd,Mn)Te, and a one-dimensional gold grating. The change in interface composition is monitored via the excitation and detection of coherent optical tellurium phonons of $A_1$ symmetry by femtosecond laser pulses in a pump-probe experiment. The patterning of a plasmonic grating onto the semiconductor enhances the transient signal which originates from the interface region. This allows monitoring the layer formation and observing the shift of the phonon frequency caused by confinement of the lattice vibrations in the nm-thick segregated layer. Efficient excitation and detection of coherent optical phonons by means of surface plasmon polaritons are evidenced by the dependence of the signal strength on polarization of pump and probe pulses and its spectral distribution.

cond-mat.mtrl-sci↗

arXiv2012

Correlation and dephasing effects on the non-radiative coherence between bright excitons in an InAs QD ensemble measured with 2D spectroscopy

Exchange-mediated fine-structure splitting of bright excitons in an ensemble of InAs quantum dots is studied using optical two-dimensional Fourier-transform spectroscopy. By monitoring the non-radiative coherence between the bright states, we find that the fine-structure splitting decreases with increasing exciton emission energy at a rate of 0.1 $μ$eV/meV. Dephasing rates are compared to population decay rates to reveal that pure dephasing causes the exciton optical coherences to decay faster than the radiative limit at low temperature, independent of excitation density. Fluctuations of the bright state transition energies are nearly perfectly-correlated, protecting the non-radiative coherence from interband dephasing mechanisms.

cond-mat.mes-hall↗

arXiv2012

Modulation of a surface plasmon-polariton resonance by sub-terahertz diffracted coherent phonons

Coherent sub-THz phonons incident on a gold grating that is deposited on a dielectric substrate undergo diffraction and thereby induce an alteration of the surface plasmon-polariton resonance. This results in efficient high-frequency modulation (up to 110 GHz) of the structure's reflectivity for visible light in the vicinity of the plasmon-polariton resonance. High modulation efficiency is achieved by designing a periodic nanostructure which provides both plasmon-polariton and phonon resonances. Our theoretical analysis shows that the dynamical alteration of the plasmon-polariton resonance is governed by modulation of the slit widths within the grating at the frequencies of higher-order phonon resonances.

cond-mat.mtrl-sci↗

arXiv2010

First- and second-order coherence properties of a quantum-dot micropillar laser

We present investigations on the coherence of the emission from the polarization split fundamental mode of an AlGaInAs/GaAs quantum-dot microcavity laser. Using polarization insensitive measurements of the first-order field-correlation function $g^{(1)}(τ)$ we determine the power-dependent degree of polarization. Whereas the orthogonally-polarized components of the fundamental mode exhibit comparable strength below the lasing threshold, a degree of linear polarization of 0.99 is observed in the coherent regime. This is also observed for increasing temperatures up to 77K. Furthermore, by measuring $g^{(1)}(τ)$ for both modes separately the stronger mode is found to reveal a record coherence time of 20ns. Finally, based on a theoretical model it is possible to fully characterize the cavity emission in terms of first- and second-order coherence using auxiliary data from $g^{(2)}(τ)$ measurements performed with a recently developed streak camera technique.

cond-mat.mes-hall↗