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Erik Kirstein

Publications and source records attributed to Erik Kirstein.

7 recordsLinked to original sources

Layer-dependent Landé $g$-factors of electrons, holes, and excitons in two-dimensional Ruddlesden-Popper lead halide perovskites

Two-dimensional Ruddlesden-Popper lead halide perovskites provide a valuable platform for tailoring charge and spin properties through quantum confinement and reduced symmetry. While the electron and hole Landé $g$-factors in bulk lead halide perovskites exhibit a universal dependence on the band gap energy, their evolution in two-dimensional perovskites has remained largely unexplored. Here, the Zeeman splittings of electrons and holes in (PEA)$_2$MA$_{n-1}$Pb$_n$I$_{3n+1}$ perovskites with the number of inorganic layers ovarying in the range $n=1,...,8$ are measured by means of the spin-flip Raman scattering and time-resolved Kerr rotation magneto-optical techniques. A systematic evolution of the electron and hole $g$-factors with decreasing layer thickness, which deviates from the universal bulk behavior and reveals confinement-driven trends similar to those observed in perovskite nanocrystals, is found. The experimental results are in good qualitative agreement with empirical tight-binding calculations. The exciton $g$-factors are evaluated from the Zeeman splittings of the exciton resonances in reflectivity measured in pulsed magnetic fields up to 55~T. These results provide comprehensive insight into the spin properties of two-dimensional lead halide perovskites and establish them as a tunable platform for engineering spin-dependent phenomena in quantum-confined semiconductors.

cond-mat.other↗

Tunable chiral and nematic states in the triple-Q antiferromagnet Co$_{1/3}$TaS$_2$

Complex spin configurations in magnetic materials, ranging from collinear single-Q to noncoplanar multi-Q states, exhibit rich symmetry and chiral properties. However, their detailed characterization is often hindered by the limited spatial resolution of neutron diffraction techniques. Here we employ magnetic circular dichroism (MCD) and magnetic linear dichroism (MLD) to investigate the triangular lattice antiferromagnet Co$_{1/3}$TaS$_2$, revealing three-state (Z3) nematicity and also spin chirality across its multi-Q magnetic phases. At intermediate temperatures, the presence of MLD identifies nematicity arising from a single-Q stripe phase, while at high magnetic fields and low temperatures, a phase characterized solely by MCD emerges, signifying a purely chiral non-coplanar triple-Q state. Notably, at low temperatures and small fields, we discover a unique phase where both chirality and nematicity coexist. A theoretical analysis based on a continuous multi-Q manifold captures the emergence of these distinct magnetic phases, as a result of the interplay between four-spin interactions and weak magnetic anisotropy. Additionally, MCD and MLD microscopy spatially resolves the chiral and nematic domains. Our findings establish Co$_{1/3}$TaS$_2$ as a rare platform hosting diverse multi-Q states with distinct combinations of spin chirality and nematicity while demonstrating the effectiveness of polarized optical techniques in characterizing complex magnetic textures.

cond-mat.str-el↗

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↗

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↗

Tailoring the electron and hole Landé 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 Landé 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.

cond-mat.mes-hall↗

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↗

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↗