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Bekir Turedi

Publications and source records attributed to Bekir Turedi.

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Resonant cooling of nuclear spins by optically-oriented holes in MAPbI$_3$ perovskite crystals

Resonant cooling of nuclear spins by photogenerated spin-oriented holes is demonstrated for MAPbI$_3$ perovskite crystals. It is evidenced by Hanle-effect measurements under helicity-modulated excitation with variable frequency. The resonance position in magnetic field shifts toward higher fields with increasing modulation frequency. The invariance of the Hanle curve upon in-plane sample rotation is consistent with the involvement of $^{207}$Pb nuclei with spin $I = 1/2$, which do not exhibit quadrupolar splitting. The shape of the resonance feature in the Hanle curve reveals that the nuclear spins are cooled by carriers with a negative $g$-factor, consistent with holes. The resonance fields associated with the modulation frequencies exceed the half-width of the weakly localized hole contribution to the Hanle curve, indicating that strongly localized holes are the primary carriers responsible for the nuclear spin cooling.

cond-mat.mes-hall

Millisecond spin relaxation times of distinct electron and hole subensembles in MA$_x$FA$_{1-x}$PbI$_3$ perovskite crystals

The unique combination of outstanding optical quality and attractive spin properties opens new avenues for optical spin control in hybrid organic-inorganic perovskite semiconductors. Using the optically detected magnetic resonance technique, we study the spins of electrons and holes in mixed-cation MA$_x$FA$_{1-x}$PbI$_3$ single crystals with $x = 0.4$ and 0.8. Multiple distinct spin subensembles with $g$-factors spanning from 2.9 to 3.6 for electrons and from 0.5 to 1.2 for holes are resolved, revealing diverse localization environments. We measure the longitudinal spin relaxation times, $T_1$, reaching 2 ms and remaining in the $\mu$s range even for weakly localized carriers at the cryogenic temperature of 1.6 K. The magnetic-field dependence of $T_1$ is dominated by the random nuclear (Overhauser) fields with strengths of $\sim 0.4-0.8$ mT for electrons and $\sim 4-12$ mT for holes, corresponding to $\mu$s-long correlation times of the hyperfine field determined by carrier hopping between shallow localization sites. The temperature dependence of $T_1$ reveals a weak localization potential of the charge carriers and shows a correlation between $T_1$ and the inhomogeneity of the spin ensemble. These results establish mixed-A-site perovskite single crystals as a promising solid-state platform with long-lived spin states for quantum information applications.

cond-mat.mes-hall

Hyperfine interaction of electrons and holes with nuclei probed by optical orientation in MAPbI$_3$ perovskite crystals

Optical orientation of electron and hole spins by circularly polarized light is investigated for MAPbI$_3$ single crystals. The Hanle and polarization recovery effects measured in transverse and longitudinal magnetic fields, respectively, evidence the hyperfine interaction with nuclear spins as the main factor determining the spin dynamics of charge carriers at cryogenic temperatures. The parameters of the nuclear spin fluctuations within the carrier localization volume are evaluated. Dynamic polarization of the nuclear spins is demonstrated by the Overhauser field reaching 5 mT for acting on the electrons and -30 mT for acting on the holes.

cond-mat.mes-hall

Millisecond spin coherence of electrons in semiconducting perovskites revealed by spin mode locking

Long spin coherence times of carriers are essential for implementing quantum technologies using semiconductor devices for which, however, a possible obstacle is spin relaxation. For the spin dynamics, decisive features are the band structure, crystal symmetry, and quantum confinement. Perovskite semiconductors recently have come into focus of studies of their spin states, notivated by efficient optical access and potentially long-living coherence. Here, we report an electron spin coherence time $T_2$ of the order of 1 ms, measured for a bulk FA$_{0.95}$Cs$_{0.05}$PbI$_3$ lead halide perovskite crystal. Using periodic laser pulses, we synchronize the electron spin Larmor precession about an external magnetic field in an inhomogeneous ensemble, the effect known as spin mode locking. It appears as a decay of the optically created ensemble spin polarization within the dephasing time $T_2^*$ of up to 20 ns and its revival during the spin coherence time $T_2$ reaching the millisecond range. This exceptionally long spin coherence time in a bulk crystal is complemented by millisecond-long longitudinal spin relaxation times $T_1$ for electrons and holes, measured by optically-detected magnetic resonance. These long-lasting spin dynamics highlight perovskites as promising platform for the quantum devices with all-optical control.

cond-mat.mtrl-sci

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

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