Coherent spin dynamics of electrons and holes in CsPbBr3_3 perovskite crystals

The lead halide perovskites demonstrate huge potential for optoelectronic applications, high energy radiation detectors, light emitting devices and solar energy harvesting. Those materials exhibit strong spin-orbit coupling enabling efficient optical orientation of carrier spins in perovskite-based devices with performance controlled by a magnetic field. Perovskites are promising for spintronics due to substantial bulk and structure inversion asymmetry, however, their spin properties are not studied in detail. Here we show that elaborated time-resolved spectroscopy involving strong magnetic fields can be successfully used for perovskites. We perform a comprehensive study of high-quality CsPbBr$_3$ crystals by measuring the exciton and charge carrier $g$-factors, spin relaxation times and hyperfine interaction of carrier and nuclear spins by means of coherent spin dynamics. Owing to their "inverted" band structure, perovskites represent appealing model systems for semiconductor spintronics exploiting the valence band hole spins, while in conventional semiconductors the conduction band electrons are considered for spin functionality.Comment: 8 pages, 3 figures + supplementary informatio

Systematic study of the influence of coherent phonon wave packets on the lasing properties of a quantum dot ensemble

Kohärente Phononen können die Licht-Materie-Wechselwirkung in Halbleiter Nanostrukturen stark ändern. Bei einem Ensemble von Quantenpunkten (QP) als aktivem Lasermedium sind Phononen im Stande, die Laserintensität deutlich zu verstärken oder abzuschwächen. Die Physik des gekoppelten Phonon-Exziton-Licht-Systems wird von verschiedenen Mechanismen dominiert, die im Experiment nicht eindeutig unterschieden werden können, da die komplizierte Probenstruktur zu einem komplexen Verspannungspuls führt, der auf das QP-Ensemble trifft. Hier zeigen wir durch eine umfassende theoretische Studie, wie die Laseremission durch Phononpulse verschiedener Form und QP-Ensembles verschiedener spektraler Verteilung beeinflusst wird. Dies erlaubt einen Einblick in die grundlegenden Wechselspiele des gekoppelten Gesamtsystems. Dadurch können wir zwischen zwei Mechanismen unterschieden: der adiabatischen Verschiebung des Ensembles und dem Schüttel-Effekt. Dies ebnet den Weg zu einer gezielten Kontrolle der Laser Emission durch kohärente Phononen.Coherent phonons can greatly vary light–matter interaction in semiconductor nanostructures placed inside an optical resonator on a picosecond time scale. For an ensemble of quantum dots (QDs) as active laser medium, phonons are able to induce a large enhancement or attenuation of the emission intensity, as has been recently demonstrated. The physics of this coupled phonon–exciton–light system consists of various effects, which in the experiment typically cannot be clearly separated, in particular, due to the complicated sample structure a rather complex strain pulse impinges on the QD ensemble. Here we present a comprehensive theoretical study how the laser emission is affected by phonon pulses of various shapes as well as by ensembles with different spectral distributions of the QDs. This gives insight into the fundamental interaction dynamics of the coupled phonon–exciton–light system, while it allows us to clearly discriminate between two prominent effects: the adiabatic shifting of the ensemble and the shaking effect. This paves the way to a tailored laser emission controlled by phonons.</p

Ultra-deep optical cooling of coupled nuclear spin-spin and quadrupole reservoirs in a GaAs/(Al,Ga)As quantum well

The physics of interacting nuclear spins in solids is well interpreted within the nuclear spin temperature concept. A common approach to cooling the nuclear spin system is adiabatic demagnetization of the initial, optically created, nuclear spin polarization. Here, the selective cooling of 75As spins by optical pumping followed by adiabatic demagnetization in the rotating frame is realized in a nominally undoped GaAs/(Al,Ga)As quantum well. The lowest nuclear spin temperature achieved is 0.54 μK. The rotation of 6 kG strong Overhauser field at the 75As Larmor frequency of 5.5 MHz is evidenced by the dynamic Hanle effect. Despite the presence of the quadrupole induced nuclear spin splitting, it is shown that the rotating 75As magnetization is uniquely determined by the spin temperature of coupled spin-spin and quadrupole reservoirs. The dependence of heat capacity of these reservoirs on the external magnetic field direction with respect to crystal and structure axes is investigated

Tailoring the electron and hole Land\'e factors in lead halide perovskite nanocrystals by quantum confinement and halide exchange

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

Hybrid coherent control of magnons in a ferromagnetic phononic resonator excited by laser pulses

We propose and demonstrate the concept of hybrid coherent control (CC) whereby a quantum or classical harmonic oscillator is excited by two excitations: one is quasiharmonic (i.e., harmonic with a finite lifetime) and the other is a pulsed broadband excitation. Depending on the phase relation between the two excitations, controlled by the detuning of the oscillator eigenfrequencies and the wave forms of the quasiharmonic and broadband excitations, it is possible to observe Fano-like spectra of the harmonic oscillator due to the interference of the two responses to the simultaneously acting excitations. Experimentally, as an example, the hybrid CC is implemented for magnons in a ferromagnetic grating where GHz coherent phonons act as the quasiharmonic excitation and the broadband impact arises from pulsed optical excitation followed by spin dynamics in the ferromagnetic nanostructure

Giant photoelasticity of polaritons for detection of coherent phonons in a superlattice with quantum sensitivity

The functionality of phonon-based quantum devices largely depends on the efficiency of interaction of phonons with other excitations. For phonon frequencies above 20 GHz, generation and detection of the phonon quanta can be monitored through photons. The photon-phonon interaction can be enormously strengthened by involving an intermediate resonant quasiparticle, e.g. an exciton, with which a photon forms a polariton. In this work, we discover a giant photoelasticity of exciton-polaritons in a short-period superlattice and exploit it for detecting propagating acoustic phonons. We demonstrate that 42 GHz coherent phonons can be detected with extremely high sensitivity in the time domain Brillouin oscillations by probing with photons in the spectral vicinity of the polariton resonance.Comment: 6 pages, 3 figures, Supplemental Material

Electron and hole g-factors and spin dynamics of negatively charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells

We address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions). Electron g-factor of 1.68 is measured and heavy-hole g-factor varying with increasing magnetic field from -0.4 to -0.7 is evaluated. Hole g-factors for two-dimensional structures are calculated for various hole confining potentials for cubic- and wurtzite lattice in CdSe core. These calculations are extended for various quantum dots and nanoplatelets based on II-VI semiconductors. We developed a magneto-optical technique for the quantitative evaluation of the nanoplatelets orientation in ensemble

On-chip phonon-magnon reservoir for neuromorphic computing

Reservoir computing is a concept involving mapping signals onto a high-dimensional phase space of a dynamical system called “reservoir” for subsequent recognition by an artificial neural network. We implement this concept in a nanodevice consisting of a sandwich of a semiconductor phonon waveguide and a patterned ferromagnetic layer. A pulsed write-laser encodes input signals into propagating phonon wavepackets, interacting with ferromagnetic magnons. The second laser reads the output signal reflecting a phase-sensitive mix of phonon and magnon modes, whose content is highly sensitive to the write- and read-laser positions. The reservoir efficiently separates the visual shapes drawn by the write-laser beam on the nanodevice surface in an area with a size comparable to a single pixel of a modern digital camera. Our finding suggests the phonon-magnon interaction as a promising hardware basis for realizing on-chip reservoir computing in future neuromorphic architectures

Addressing the exciton fine structure in colloidal nanocrystals: the case of CdSe nanoplatelets

We study the band-edge exciton fine structure and in particular its bright-dark splitting in colloidal semiconductor nanocrystals by four different optical methods based on fluorescence line narrowing and time-resolved measurements at various temperatures down to 2 K. We demonstrate that all these methods provide consistent splitting values and discuss their advances and limitations. Colloidal CdSe nanoplatelets with thicknesses of 3, 4 and 5 monolayers are chosen for experimental demonstrations. The bright-dark splitting of excitons varies from 3.2 to 6.0 meV and is inversely proportional to the nanoplatelet thickness. Good agreement between experimental and theoretically calculated size dependence of the bright-dark exciton slitting is achieved. The recombination rates of the bright and dark excitons and the bright to dark relaxation rate are measured by time-resolved techniques

Resonant thermal energy transfer to magnons in a ferromagnetic nanolayer

Energy harvesting is a concept which makes dissipated heat useful by transferring thermal energy to other excitations. Most of the existing principles are realized in systems which are heated continuously. We present the concept of high-frequency energy harvesting where the dissipated heat in a sample excites resonant magnons in a thin 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