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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.

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., Comment: 6 pages, 4 figures

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 $\Gamma_2=2\hbar/T_2$ on the $\mu$eV scale. Through intensity-dependent measurements, we evaluate the increase of $\Gamma_2$ by 10~$\mu$eV at an exciton density of 10$^{17}$~cm$^{-3}$ being comparable with the intrinsic linewidth of 14$\,\mu$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.

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.

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$\mu$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.

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., Comment: Manuscript: 12 pages, 3 figures; Supplemental information: 7 pages; 4 figures, 3 tables

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.

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., Comment: 11 pages, 8 figures

We study the polarization dynamics of exciton-polaritons propagating in sub-mm thick (Cd,Zn)Te bulk crystals using polarimetric time-of-flight techniques. The application of a magnetic field in Faraday geometry leads to synchronous temporal oscillations of all Stokes parameters of an initially linearly or circularly polarized, spectrally broad optical pulse of 150 fs duration propagating through the crystal. Strong dispersion for photon energies close to the exciton resonance leads to stretching of the optical pulse to a duration of 200$-$300 ps and enhancement of magneto-optical effects such as the Faraday rotation and the non-reciprocal birefringence. The oscillation frequency of the exciton-polariton polarization increases with magnetic field $B$, reaching 10 GHz at $B\sim 5$T. Surprisingly, the relative contributions of Faraday rotation and non-reciprocal birefringence undergo strong changes with photon energy, which is attributed to a non-trivial spectral dependence of Faraday rotation in the vicinity of the exciton resonance. This leads to polarization nutation of the transmitted optical pulse in the time domain. The results are well explained by a model that accounts for Faraday rotation and magneto-spatial dispersion in zinc-blende crystals. We evaluate the exciton $g$-factor $|g_{\rm exc}|=0.2$ and the magneto-spatial constant $V= 5 \times 10^{-12}$ eVcm$\textup{T}^{-1}$., Comment: 11 pages, 6 figures

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 $\mu$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.

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., Comment: 5 pages, 4 figures

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 $g^{(1)}(\tau)$ 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 $g^{(1)}(\tau)$ 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 $g^{(2)}(\tau)$ measurements performed with a recently developed streak camera technique., Comment: 12 pages, 5 figures