Laughlin anyon complexes with Bose properties.

Two-dimensional electron systems in a quantizing magnetic field are regarded as of exceptional interest, considering the possible role of anyons-quasiparticles with non-boson and non-fermion statistics-in applied physics. To this day, essentially none but the fractional states of the quantum Hall effect (FQHE) have been experimentally realized as a system with anyonic statistics. In determining the thermodynamic properties of anyon matter, it is crucial to gain insight into the physics of its neutral excitations. We form a macroscopic quasi-equilibrium ensemble of neutral excitations - spin one anyon complexes in the Laughlin state ν = 1/3, experimentally, where ν is the electron filling factor. The ensemble is found to have such a long lifetime that it can be considered the new state of anyon matter. The properties of this state are investigated by optical techniques to reveal its Bose properties.

Geminate recombination in organic photovoltaic blend PCDTBT/PC71BM studied by out-of-phase electron spin echo spectroscopy.

The key process in organic solar cell operation is charge separation under light illumination. Due to the low dielectric constant of organic materials, the Coulomb attraction energy within the interfacial charge-transfer state (CTS) is larger than the thermal energy. Understanding the mechanism of charge separation at the organic donor/acceptor interface still remains a challenge and requires knowledge of the CTS temporal evolution. To address this problem, the CTS in the benchmark photovoltaic blend PCDTBT/PC71BM was studied by the out-of-phase Electron Spin Echo (ESE). The protocol for determining the CTS geminate recombination rate for certain electron-hole distances was developed. Simulating the out-of-phase ESE trace for the CTS in the PCDTBT/PC71BM blend allows precise determination of the electron-hole distance distribution function and its evolution with the increase in the delay after the laser flash. Distances of charge separation up to 6 nm were detected upon thermalization at a temperature of 20 K. Assuming the exponential decay of the recombination rate, the attenuation factor ß = 0.08 Å-1 is estimated for the PCDTBT/PC71BM blend. Such a low attenuation factor is probably caused by a high degree of hole delocalization along the PCDTBT chain.

Investigation of spin stiffness in spin-depolarized states of two-dimensional electron systems with time-resolved Kerr rotation.

An experimental technique based on time-resolved Kerr rotation allows a comparison of the spin stiffnesses of different spin-polarized and depolarized states in a two-dimensional electron system. With this technique, a new spin-correlated phase that has no known analogues was discovered. The new spin-depolarized phase is characterized by high spin stiffness equal to that of a spin-polarized quantum Hall ferromagnet.

Author Correction: Long-range non-diffusive spin transfer in a Hall insulator.

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Long-range non-diffusive spin transfer in a Hall insulator.

We report on optical visualization of spin propagation more than 100 µm. We present an electronic system in a new state of aggregation, the magnetofermionic condensate, in which the lowest-energy spin excitations - photoexcited spin-triplet magnetoexcitons - freely propagate over long distances, in the order of a millimeter, which implies non-diffusion spin transport. Our results open up a completely new system suitable for spintronic devices.

Spin dynamics of light-induced charge separation in composites of semiconducting polymers and PC60BM revealed using Q-band pulse EPR.

Light-induced processes in composites of semiconducting polymers and fullerene derivatives have been widely studied due to their usage as active layers of organic solar cells. However the process of charge separation under light illumination - the key process of an organic solar cell is not well understood yet. Here we report a Q-band pulse electron paramagnetic resonance study of composites of the fullerene derivative PC60BM ([6,6]-phenyl-C61-butyric acid methyl ester) with different p-type semiconducting polymers regioregular and regiorandom P3HT (poly(3-hexylthiophene-2,5-diyl), MEH-PPV (poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene]), PCDTBT (poly[N-9'-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)]), PTB7 (poly({4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl}{3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl}))), resulting in a detailed description of the in-phase laser flash-induced electron spin echo (ESE) signal. We found that in organic donor-acceptor composites the laser flash simultaneously induces species of two types: a polymer˙+/fullerene˙- spin-correlated polaron pair (SCPP) with an initial singlet spin state and (nearly) free polymer˙+ and fullerene˙- species with non-equilibrium spin polarization. Species of the first type (SCPP) are well-known for polymer/fullerene blends and are usually associated with a charge-separated state. Also, spin polarization of long-living free species (polarons in deep traps) is affected by the laser flash, which is the third contribution to the flash-induced ESE signal. A protocol for extracting the in-phase ESE signal of the SCPP based on the dependence of the microwave nutation frequency on the strength of the spin coupling within the polaron pair was developed. Nutation experiments revealed an unusual pattern of the SCPP in RR-P3HT/PC60BM composites, from which the strength of the exchange interaction between the polymer˙+ and fullerene˙- was extracted. In composites with low-efficient polymers the contribution of the SCPP to the in-phase ESE signal is high, while in composites with high-efficient polymers it is low. This finding can be used as a selection criterion of charge separation efficiency in the polymer/fullerene composites.

Artificially Constructed Plasmarons and Plasmon-Exciton Molecules in 2D Metals.

Resonant optical excitation was used to create a macroscopic nonequilibrium ensemble of "dark" excitons with an unprecedented long lifetime in a two-dimensional electron system placed in a quantizing magnetic field. Exotic three-particle and four-particle states, plasmarons and plasmon-exciton molecules, coupled with the surrounding electrons through the collective plasma oscillations are engineered. Plasmarons and plasmon-exciton molecules are manifested as new features in the recombination spectra of nonequilibrium systems.

Magnetofermionic condensate in two dimensions.

Coherent condensate states of particles obeying either Bose or Fermi statistics are in the focus of interest in modern physics. Here we report on condensation of collective excitations with Bose statistics, cyclotron magnetoexcitons, in a high-mobility two-dimensional electron system in a magnetic field. At low temperatures, the dense non-equilibrium ensemble of long-lived triplet magnetoexcitons exhibits both a drastic reduction in the viscosity and a steep enhancement in the response to the external electromagnetic field. The observed effects are related to formation of a super-absorbing state interacting coherently with the electromagnetic field. Simultaneously, the electrons below the Fermi level form a super-emitting state. The effects are explicable from the viewpoint of a coherent condensate phase in a non-equilibrium system of two-dimensional fermions with a fully quantized energy spectrum. The condensation occurs in the space of vectors of magnetic translations, a property providing a completely new landscape for future physical investigations.

Super-long life time for 2D cyclotron spin-flip excitons.

An experimental technique for the indirect manipulation and detection of electron spins entangled in two-dimensional magnetoexcitons has been developed. The kinetics of the spin relaxation has been investigated. Photoexcited spin-magnetoexcitons were found to exhibit extremely slow relaxation in specific quantum Hall systems, fabricated in high mobility GaAs/AlGaAs structures; namely, the relaxation time reaches values over one hundred microseconds. A qualitative explanation of this spin-relaxation kinetics is presented. Its temperature and magnetic field dependencies are discussed within the available theoretical framework.

Extra spin-wave mode in quantum Hall systems: beyond the Skyrmion limit.

We report on the observation of a new spin mode in a quantum Hall system in the vicinity of odd electron filling factors under experimental conditions excluding the possibility of Skyrmion excitations. The new mode having presumably zero energy at odd filling factors emerges at small deviations from odd filling factors and couples to the spin exciton. The existence of an extra spin mode assumes a nontrivial magnetic order at partial fillings of Landau levels surrounding quantum Hall ferromagnets other then the Skyrmion crystal.

Electron-nuclear double resonance study of molecular librations of nitroxides in molecular glasses: quantum effects at low temperatures, comparison with low-frequency Raman scattering.

Pulsed electron-nuclear double resonance applied to 15N nitroxide spin probes in molecular glasses is shown to be very sensitive to measurement of the A(XX) principal value of the hyperfine interaction tensor. For molecules experiencing fast restricted orientational motions (molecular librations), this provides a precise tool to determine the motion-averaged value. For nitroxides in glycerol and o-terphenyl glasses, the observed temperature dependence below 40 K may be readily interpreted as arising from quantum effects in librations, when the thermal energy of a librating molecule becomes comparable with the elementary quantum of the oscillator. The estimated elementary quanta for nitroxide librations, approximately 60 cm(-1) in glycerol and approximately 90 cm(-1) in o-terphenyl, are found to match the characteristic frequencies of the vibrational spectral densities seen in low-frequency Raman scattering for these glasses. Above approximately 80 K in glycerol and above approximately 120 K in o-terphenyl, the temperature dependences manifest a kink with a slightly smaller slope than at lower temperatures.

Cyclotron spin-flip excitations in a nu = 1/3 quantum Hall ferromagnet.

Inelastic light scattering spectroscopy discloses a novel type of cyclotron spin-flip excitation in a quantum Hall system around the nu = 1/3 filling. The excitation energy follows qualitatively the degree of electron spin polarization, reaching a maximum value at nu = 1/3. This characterizes the new excitation as a nu = 1/3 ferromagnet eigenmode. The mode energy exceeds drastically the theoretical prediction obtained within the renowned single-mode approximation. We develop a new theoretical approach where the basis set is extended by adding a double-exciton component representing the cyclotron magnetoplasmon and spin wave coupled together. This double-mode approximation, inferred to be responsible for substantially reducing the gap between theoretical and experimental results, shows that the cyclotron spin-flip excitation is effectively a four-particle state.

Low-magnetic-field divergence of the electronic g factor obtained from the cyclotron spin-flip mode of the nu=1 quantum Hall ferromagnet.

We report an inelastic light scattering study of the cyclotron spin-flip mode in the two-dimensional electron system at filling nu=1. The energy of this mode can serve as a probe of the many-body exchange interaction on short length scales. Its magnetic field dependence is compared with predictions based on Hartree-Fock theory. They agree well when including the nonzero width of the electron system. From the measured energies, the exchange enhanced g factor is extracted. It diverges at small fields and differs largely from g factors obtained via transport activation studies.

Electron spin-lattice relaxation of the S0 state of the oxygen-evolving complex in photosystem II and of dinuclear manganese model complexes.

The temperature dependence of the electron spin-lattice relaxation time T1 was measured for the S0 state of the oxygen-evolving complex (OEC) in photosystem II and for two dinuclear manganese model complexes by pulse EPR using the inversion-recovery method. For [Mn(III)Mn(IV)(mu-O)2 bipy4]ClO4, the Raman relaxation process dominates at temperatures below 50 K. In contrast, Orbach type relaxation was found for [Mn(II)Mn(III)(mu-OH)(mu-piv)2(Me3 tacn)2](ClO4)2 between 4.3 and 9 K. For the latter complex, an energy separation of 24.7-28.0 cm(-1) between the ground and the first excited electronic state was determined. In the S0 state of photosystem II, the T1 relaxation times were measured in the range of 4.3-6.5 K. A comparison with the relaxation data (rate and pre-exponential factor) of the two model complexes and of the S2 state of photosystem II indicates that the Orbach relaxation process is dominant for the S0 state and that its first excited state lies 21.7 +/- 0.4 cm(-1) above its ground state. The results are discussed with respect to the structure of the OEC in photosystem II.

Restricted orientational motion of nitroxides in molecular glasses: direct estimation of the motional time scale basing on the comparative study of primary and stimulated electron spin echo decays.

A comparative study of anisotropic relaxation in two-pulse primary and three-pulse stimulated electron spin echo decays provides a direct way to distinguish fast (correlation time tau(c)<10(-6) s) and slow (tau(c)>10(-6) s) motions. Anisotropic relaxation is detected as a difference of the decay rates for different resonance field positions in anisotropic electron paramagnetic resonance spectra. For fast motion anisotropic relaxation influences the primary echo decay and does not influence the stimulated echo decay. For slow motion it is seen in both two-pulse echo and three-pulse stimulated echo decays. For nitroxide spin probes dissolved in glassy glycerol only fast motion was found below 200 K. Increase of temperature above 200 K results in the appearance of slow motion. Its amplitude increases rapidly with temperature increase. While in glycerol glass slow motion appears above glass transition temperature T(g), in ethanol glass it is observable below T(g). The scenario of motional dynamics in glasses is proposed which involves the broadening of the correlation time distribution with increasing temperature.

Selective excitation in pulsed EPR of a spin-correlated triplet-radical pair.

Experiments are described in which a low-amplitude microwave pulse excites only one out of three allowed transitions of the quinone radical (Q(A)(-)) in a spin-correlated triplet-radical pair 3PQ(A)(-) of the bacterial photosynthetic reaction center. A second high-amplitude pulse produces a FID whose temporal shape is strongly modulated with frequencies determined by electron-electron dipolar interaction in the pair. The FID is detected in both the in-phase and the out-of-phase channels. The out-of-phase FID is a result of switching off the magnetic dipolar interaction between 3P and Q(A)(-) due to decay of 3P during the time interval between the two pulses. Refocusing of FID by an additional non-selective pulse allows a dead-time free measurement of this modulation. The influence of the dead-time problem on the distance determination is discussed.

Electron dipole-dipole ESEEM in field-step ELDOR of nitroxide biradicals.

The use of a rapid stepping of the magnetic field for investigation of electron dipole-dipole ESEEM in pulsed X-band ELDOR is described. The magnetic field jump, synchronized with a microwave pumping pulse, is positioned between the second and the third pulses of the stimulated echo pulse sequence. This echo is measured as a function of the delay between the first and the second pulses. The data are analyzed for a Fourier transform resulting in a Pake resonance pattern. To remove the electron-nuclear contributions to ESEEM, time traces with pumping were divided by those without. This resulted in complete elimination of electron-nuclear contributions, which is seen from the absence of peaks at nuclear frequencies and the similarity of results for protonated and deuterated solvents. For increasing the electron-electron modulation depth, a scanning of the magnetic field during the microwave pumping is proposed. The interspin distances and their distribution are determined for two long-chained (ca. 2 nm) nitroxide biradicals in glassy toluene and in frozen nematic liquid crystal 4-cyano-4'-pentyl-biphenyl. For the latter solvent, the alignment of the axis connecting two nitroxides in biradicals is quantitatively analyzed.

Modification of the intersubband excitation spectrum in a two-dimensional electron system under a perpendicular magnetic field.

Under an external magnetic field, new branches of spin- and charge-density waves have been studied in a quasi-two-dimensional electron system whose ground state has more than one Landau level occupied by electrons. These collective excitations can be treated as manifestations of the multicomponent nature of the electron system in magnetic field, whereas the occupied Landau levels should be associated with degrees of freedom.