Temperature dependence of hole spin relaxation in ultrathin InAs monolayers

The temperature dependence of hole spin relaxation time in both neutral and n-doped ultrathin InAs monolayers has been investigated. It has been suggested that D'yakonov-Perel (DP) mechanism dominates the spin relaxation process at both low and high temperature regimes. The appearance of a peak in temperature dependent spin relaxation time reveals the important contribution of Coulomb scatterings between carriers to the spin kinetics at low temperature, though electron-phonon scattering becomes dominant at higher temperatures. Increased electron screening effect in the n-doped sample has been suggested to account for the shortened spin relaxation time compared with the undoped one. The results suggest that hole spins are also promising for building solid-state qubits.

Hole Spin Relaxation in an Ultrathin InAs Monolayer

We investigate the spin relaxation time of holes in an ultrathin neutral InAs monolayer (1.5 ML) and compare with that of electrons, using polarization-dependent time-resolved photoluminescence (TRPL) experiments. With excitation energies above the GaAs gap, we observe a rather slow relaxation of holes (tau(1h) = 196 +/- 17 ps) that is in the magnitude similar to electrons (tau(1e) = 354 +/- 32 ps) in this ultrathin sample. The results are in good agreement with earlier theoretical prediction, and the phonon scattering due to spin-orbit coupling is realized to play a dominant role in the carrier spin kinetics.

Effect of electron-hole spatial correlation on spin relaxation dynamics in InAs submonolayer

Using time-resolved photoluminescence and time-resolved Kerr rotation spectroscopy, we explore the unique electron spin behavior in an InAs submonolayer sandwiched in a GaAs matrix, which shows very different spin characteristics under resonant and non-resonant excitations. While a very long spin relaxation lifetime of a few nanoseconds at low temperature is observed under non-resonant excitation, it decreases dramatically under resonant excitation. These interesting results are attributed to the difference in electron-hole interactions caused by non-geminate or geminate capture of photo-generated electron-hole pairs in the two excitation cases, and provide a direct verification of the electron-hole spatial correlation effect on electron spin relaxation. (c) 2007 Elsevier Ltd. All rights reserved.

Electron spin relaxation by nuclei and holes in single InAs quantum dots

Electron spin relaxation of charged excitons X+ and X2+ are investigated by time-resolved and polarization-resolved photoluminescence spectroscopy. For X+ configuration, the electron spin relaxation shows a typical decay curve induced by hyperfine interaction with nuclei, whereas for X2+ state the electron spin relaxation is affected not only by nuclei but also by electron-hole exchange interaction, leading to a power-law time dependence.

Spin Relaxation of Electrons in Single InAs Quantum Dots

By using polarization-resolved photoluminescence spectra, we study the electron spin relaxation in single InAs quantum dots (QDs) with the configuration of positively charged excitons X+ (one electron, two holes). The spin relaxation rate of the hot electrons increases with the increasing energy of exciting photons. For electrons localized in QDs the spin relaxation is induced by hyperfine interaction with the nuclei. A rapid decrease of polarization degree with increasing temperature suggests that the spin relaxation mechanisms are mainly changed from the hyperfine interaction with nuclei into an electron-hole exchange interaction.

Spin relaxation dynamics in InAs monolayer and submonolayer

By using time-resolved photoluminescence and time-resolved Kerr rotation, we have studied the unique electron spin dynamics in InAs monolayer (ML) and submonolayer (SML), which were sandwiched in GaAs matrix. Under non-resonant excitation, the spin relaxation lifetimes of 3.4 ns and 0.48 ns were observed for 1/3 ML and I ML InAs samples, respectively. More interestingly, the spin lifetime of the 1/3 ML InAs decreased dramatically under resonant excitation, down to 70 ps, while the spin lifetime of the 1 ML sample did not vary much, changing only from 400 to 340 ps. These interesting results come from the different electron-hole interactions caused by different spatial electron-hole correlation, and they provide a direct evidence of the dominant spin relaxation process, i.e. the BAP mechanism. Furthermore, these new results may provide a valuable enlightenment in controlling the spin relaxation and in seeking new material systems for spintronics application.

Anisotropy of spin relaxation of water protons in cartilage and tendon

Transverse spin relaxation rates of water protons in articular cartilage and tendon depend on the orientation of the tissue relative to the applied static magnetic field. This complicates the interpretation of magnetic resonance images of these tissues. At the same time, relaxation data can provide information about their organisation and microstructure. We present a theoretical analysis of the anisotropy of spin relaxation of water protons observed in fully hydrated cartilage. We demonstrate that the anisotropy of transverse relaxation is due almost entirely to intramolecular dipolar coupling modulated by a specific mode of slow molecular motion: the diffusion of water molecules in the hydration shell of a collagen fibre around the fibre, such that the molecular director remains perpendicular to the fibre. The theoretical anisotropy arising from this mechanism follows the “magic-angle” dependence observed in magnetic-resonance measurements of cartilage and tendon and is in good agreement with the available experimental results. We discuss the implications of the theoretical findings for MRI of ordered collagenous tissues.

Effect of partial H2O-D2O replacement on the anisotropy of transverse proton spin relaxation in bovine articular cartilage

Anisotropy of transverse proton spin relaxation in collagen-rich tissues like cartilage and tendon is a well-known phenomenon that manifests itself as the "magic-angle" effect in magnetic resonance images of these tissues. It is usually attributed to the non-zero averaging of intra-molecular dipolar interactions in water molecules bound to oriented collagen fibers. One way to manipulate the contributions of these interactions to spin relaxation is by partially replacing the water in the cartilage sample with deuterium oxide. It is known that dipolar interactions in deuterated solutions are weaker, resulting in a decrease in proton relaxation rates. In this work, we investigate the effects of deuteration on the longitudinal and the isotropic and anisotropic contributions to transverse relaxation of water protons in bovine articular cartilage. We demonstrate that the anisotropy of transverse proton spin relaxation in articular cartilage is independent of the degree of deuteration, bringing into question some of the assumptions currently held over the origins of relaxation anisotropy in oriented tissues.

The hole spin model for oxides

A model of mobile 0-holes hybrized with Cu-spins on a square lattice is examined. A variational groundstate wavefunction which interpolates smoothly between n.n. RVB and Néel limits gives a Néellike minimum. A hole in an AF lattice polarizes it locally and becomes quite mobile. Two n.n. holes attract. Finally we speculate how holes can stabilize a spin liquid state.

I. Electron spin relaxation studies of manganese(II) complexes in acetonitrile. II. Nuclear spin relaxation studies of bromine in tetrabromomanganese(II) in acetonitrile

Magnetic resonance techniques have given us a powerful means for investigating dynamical processes in gases, liquids and solids. Dynamical effects manifest themselves in both resonance line shifts and linewidths, and, accordingly, require detailed analyses to extract desired information. The success of a magnetic resonance experiment depends critically on relaxation mechanisms to maintain thermal equilibrium between spin states. Consequently, there must be an interaction between the excited spin states and their immediate molecular environment which promote changes in spin orientation while excess magnetic energy is coupled into other degrees of freedom by non-radiative processes. This is well known as spin-lattice relaxation. Certain dynamical processes cause fluctuations in the spin state energy levels leading to spin-spin relaxation and, here again, the environment at the molecular level plays a significant role in the magnitude of interaction. Relatively few electron spin relaxation studies of solutions have been conducted and the present work is addressed toward the extension of our knowledge in this area and the retrieval of dynamical information from line shape analyses on a time scale comparable to diffusion controlled phenomena.

Specifically, the electron spin relaxation of three Mn⁺²3d⁵ complexes, Mn(CH₃CN)₆⁺², MnCl₄^-2 in acetonitrile has been studied in considerable detail. The effective spin Hamiltonian constants were carefully evaluated under a wide range of experimental conditions. Resonance widths of these Mn⁺² complexes were studied in the presence of various excess ligand ions and as a function of concentration, viscosity, temperature and frequency (X-band, ~9.5 Ԍ Hz and K-band, ~35 Ԍ Hz).

A number of interesting conclusions were drawn from these studies. For the Et₄NCl-₄^-2 system several relaxation mechanisms leading to resonance broadening were observed. One source appears to arise through spin-orbit interactions caused by modulation of the ligand field resulting from transient distortions of the complex imparted by solvent fluctuations in the immediate surroundings of the paramagnetic ion. An additional spin relaxation was assigned to the formation of ion pairs [Et₄N⁺…MnCl₄^-2] and it was possible to estimate the dissociation constant for this specie in acetonitrile.

The Bu₄NBr-MnBr₄^-2 study was considerably more interesting. As in the former case, solvent fluctuations and ion-pairing of the paramagnetic complex [Bu₄N⁺…MnBr₄^-2] provide significant relaxation for the electronic spin system. Most interesting, without doubt, is the onset of a new relaxation mechanism leading to resonance broadening which is best interpreted as chemical exchange. Thus, assuming that resonance widths were simply governed by electron spin state lifetimes, we were able to extract dynamical information from an interaction in which the initial and final states are the same

MnBr₄^-2 + Br^- = MnBr₄^-2 + Br^-.

The bimolecular rate constants were obtained at six different temperatures and their magnitudes suggested that the exchange is probably diffusion controlled with essentially a zero energy of activation. The most important source of spin relaxation in this system stems directly from dipolar interactions between the manganese 3d⁵ electrons. Moreover, the dipolar broadening is strongly frequency dependent indicating a deviation between the transverse and longitudinal relaxation times. We are led to the conclusion that the 3d⁵ spin states of ion-paired MnBr₄^-2 are significantly correlated so that dynamical processes are also entering the picture. It was possible to estimate the correlation time, ^Td, characterizing this dynamical process.

In Part II we study nuclear magnetic relaxation of bromine ions in the MnBr4-2-Bu4NBr-acetonitrile system. Essentially we monitor the 79Br and 81Br linewidths in response to the [MnBr4-2]/[Br-] ratio with the express purpose of supporting our contention that exchange is occurring between "free" bromine ions in the solvent and bromine in the first coordination sphere of the paramagnetic anion. The complexity of the system elicited a two-part study: (1) the linewidth behavior of Bu4NBr in anhydrous CH3CN in the absence of MnBr4-2 and (2) in the presence of MnBr4-2. It was concluded in study (1) that dynamical association, Bu4NBr k1= Bu4N+ + Br-, was modulating field-gradient interactions at frequencies high enough to provide an estimation of the unimolecular rate constant, k1. A comparison of the two isotopic bromine linewidth-mole fraction results led to the conclusion that quadrupole interactions provided the dominant relaxation mechanism. In study (2) the "residual" bromine linewidths for both 79Br and 81Br are clearly controlled by quadrupole interactions which appear to be modulated by very rapid dynamical processes other than molecular reorientation. We conclude that the "residual" linewidth has its origin in chemical exchange and that bromine nuclei exchange rapidly between a "free" solvated ion and the paramagnetic complex, MnBr4-2.

I. Proton magnetic resonance of polynucleotides and transfer RNA. II. Electron spin relaxation studies of manganese (II) complexes in acetonitrile

Part I. Proton Magnetic Resonance of Polynucleotides and Transfer RNA.

Proton magnetic resonance was used to follow the temperature dependent intramolecular stacking of the bases in the polynucleotides of adenine and cytosine. Analysis of the results on the basis of a two state stacked-unstacked model yielded values of -4.5 kcal/mole and -9.5 kcal/mole for the enthalpies of stacking in polyadenylic and polycytidylic acid, respectively.

The interaction of purine with these molecules was also studied by pmr. Analysis of these results and the comparison of the thermal unstacking of polynucleotides and short chain nucleotides indicates that the bases contained in stacks within the long chain poly nucleotides are, on the average, closer together than the bases contained in stacks in the short chain nucleotides.

Temperature and purine studies were also carried out with an aqueous solution of formylmethionine transfer ribonucleic acid. Comparison of these results with the results of similar experiments with the homopolynucleotides of adenine, cytosine and uracil indicate that the purine is probably intercalating into loop regions of the molecule.

The solvent denaturation of phenylalanine transfer ribonucleic acid was followed by pmr. In a solvent mixture containing 83 volume per cent dimethylsulf oxide and 17 per cent deuterium oxide, the tRNA molecule is rendered quite flexible. It is possible to resolve resonances of protons on the common bases and on certain modified bases.

Part II. Electron Spin Relaxation Studies of Manganese (II) Complexes in Acetonitrile.

The electron paramagnetic resonance spectra of three Mn⁺² complexes, [Mn(CH₃CN)₆]⁺², [MnCl₄]^-2, and [MnBr₄]^-2, in acetonitrile were studied in detail. The objective of this study was to relate changes in the effective spin Hamiltonian parameters and the resonance line widths to the structure of these molecular complexes as well as to dynamical processes in solution.

Of the three systems studied, the results obtained from the [Mn(CH₃CN)₆]⁺² system were the most straight-forward to interpret. Resonance broadening attributable to manganese spin-spin dipolar interactions was observed as the manganese concentration was increased.

In the [MnCl₄]^-2 system, solvent fluctuations and dynamical ion-pairing appear to be significant in determining electron spin relaxation.

In the [MnBr₄]^-2 system, solvent fluctuations, ion-pairing, and Br- ligand exchange provide the principal means of electron spin relaxation. It was also found that the spin relaxation in this system is dependent upon the field strength and is directly related to the manganese concentration. A relaxation theory based on a two state collisional model was developed to account for the observed behavior.

Hole-Phonon Relaxation and Photocatalytic Properties of Titanium Dioxide and Zinc Oxide: First-Principles Approach

First-principles calculations for the temporal characteristics of hole-phonon relaxation in the valence band of titanium dioxide and zinc oxide have been performed. A first-principles method for the calculations of the quasistationary distribution function of holes has been developed. The results show that the quasistationary distribution of the holes in TiO2 extends to an energy level approximately 1eV below the top of the valence band. This conclusion in turn helps to elucidate the origin of the spectral dependence of the photocatalytic activity of TiO2. Analysis of the analogous data for ZnO shows that in this material spectral dependence of photocatalytic activity in the oxidative reactions is unlikely.

Carrier spin relaxation in (Ga, Mn) As at room temperature

In this paper, the excitation energy density dependence of carrier spin relaxation is studied at room temperature for the as-grown and annealed (Ga, Mn) As samples using femtosecond time-resolved pump-probe Kerr spectroscopy. It is found that spin relaxation lifetime of electrons lengthens with increasing excitation energy density for both samples, and the annealed ( Ga, Mn) As has shorter carrier recombination and electron spin relaxation lifetimes as well as larger Kerr rotation angle than the as-grown ( Ga. Mn) As under the same excitation condition. which shows that DP mechanism is dominant in the spin relaxation process for ( Ga, Mn)As at room temperature. The enhanced ultrafast Kerr effect in the annealed (Ga,Mn)As shows the potential application of the annealed ( Ga, Mn) As in ultrafast all-optical spin switches, and also provides a further evidence for the p-d exchange mechanism of the ferromagnetic origin of (Ga, Mn) As.

Localized and free exciton spin relaxation dynamics in GaInNAs/GaAs quantum well

We have investigated the exciton spin relaxation in a GaInNAs/GaAs quantum well. The recombination from free and localized excitons is resolved on the basis of an analysis of the photoluminescence characteristics. The free exciton spin relaxation time is measured to be 192 ps at 10 K, while the localized exciton spin relaxation time is one order of magnitude longer than that of the free exciton. The dependence of the free exciton spin relaxation time on the temperature above 50 K suggests that both the D'yakonov-Perel' and the Elliot-Yafet effects dominate the spin relaxation process. The temperature independence below 50 K is considered to be due to the spin exchange interaction. The ultralong spin relaxation time of the localized excitons is explained to be due to the influence of nonradiative deep centers. (c) 2008 American Institute of Physics.

Spin relaxation in submonolayer and monolayer InAs structures grown in a GaAs matrix

Electron-spin dynamics in InAs/GaAs heterostructures consisting of a single layer of InAs (1/3-1 monolayer) embedded in (001) and (311)A GaAs matrix was studied by means of time-resolved Kerr rotation spectroscopy. The spin-relaxation time of the submonolayer InAs samples is significantly enhanced, compared with that of the monolayer InAs sample. The electron-spin-relaxation time and the effective g factor in submonolayer samples were found to be strongly dependent on the photogenerated carrier density. The contribution from both the D'yakonov-Perel' mechanism and Bir-Aronov-Pikus mechanism are discussed to interpret the temperature dependence of spin decoherence at various carrier densities.