Quantum coherence and correlation dynamics of two-qubit system in spin bath environment

The quantum entanglement,discord,and coherence dynamics of two spins in the model of a spin coupled to a spin bath through an intermediate spin are studied.The effects of the important physical parameters including the coupling strength of two spins,the interaction strength between the intermediate spin and the spin bath,the number of bath spins and the temperature of the system on quantum coherence and correlation dynamics are discussed in different cases.The frozen quantum discord can be observed whereas coherence does not when the initial state is the Bell-diagonal state.At finite temperature,we find that coherence is more robust than quantum discord,which is better than entanglement,in terms of resisting the influence of environment.Therefore,quantum coherence is more tenacious than quantum correlation as an important resource.     

Light induced radical pair intermediates in photosynthetic reaction centres in contact with an observer spin label: spin dynamics and effects on transient EPR spectra

A novel strategy is discussed using site directed spin labelling to study the electron transfer process in photosynthetic reaction centres. An algorithm is presented for numerical simulations of the time resolved EPR spectra of radical pair states in the presence of an observer spin label. This algorithm accounts for spin dynamics, charge recombination and relaxation processes. It is shown that satisfactory agreement between experimental and simulated EPR spectra of the first stabilized radical pair state in photosystem I is achieved for various microwave frequencies. Transient EPR spectra for the radical pair state P^?+Q^?- in photosystem I were simulated for various distances and positions of the observer spin label with respect to the acceptor quinone molecule. It is shown that distances up to more than 20 Å give rise to observable changes in the transient EPR spectra. Both the additional spin-spin coupling between the quinone radical and the label and the polarization transfer processes contribute to the changes. Furthermore, the shape and intensity of the EPR spectrum of the spin label is altered by the coupling with the radical pair spins for distances up to 25 Å. Experiments on site directed spin labelled photosystem I are thus expected to provide valuable information on the dynamics of electron transfer in photosystem I.     

Dynamics of multiple quantum coherences in dipole-coupling spins in solid

A perturbation method deals with dipolar coupling spins in solids is presented. As example of application the method, the multiple-quantum coherence dynamics in clusters of a linear chain of four nuclear spins and a ring of six spins coupled by dipole-dipole interaction are considered. The calculated 0Q and 2Q intensities in a linear chain of four nuclear spins and 6Q intensity in a ring of six spins vs. the duration of the preparation period agree well with the exact solutions (for linear chain of four nuclear spins) and simulation data (for linear chain of four nuclear spins and a ring of six spin).     

Analytical polarization and coherence transfer functions for three dipolar coupled spins 12

Analytical polarization and coherence transfer functions are presented for a spin system consisting of three dipolar coupled homonuclear spins 12 under energy matched conditions. Based on these transfer functions, optimal durations of Hartmann-Hahn mixing periods can be determined for arbitrary dipolar coupling constants D(12), D(13), and D(23). In addition, the dependence of the transfer efficiency on the relative size of the dipolar coupling constants is illustrated.     

Entanglement Dynamics of Two Coupled Spins in a Spin Star Environment

We theoretically study the entanglement dynamics of two coupled spins in a spin star environment, whose elements are coupled to local bosonic baths. It is shown that the dynamics of the entanglement depends on the initial state of the system and the coupling strength between the two coupled central spins, the interactions between the central system and the environment, as well as interactions between the bath spin and the reservoir. We also investigate the effect of non-Markovian dynamics in contrast with the Markovian case. It is found that the non-Markovian dynamics has a significant effect on the disentanglement between the two central spins.     

Quantum Speed Limit for Dynamics of Central Spin Model with Initial System-Bath Correlations

We investigate the quantum speed limit (QSL) time of an electronic spin coupled to a bath of nuclear spins. We consider three types of initial states with different correlations between the system and bath, i.e., quantum correlation, classical correlation, and no any correlation. Interestingly, we show that the QSL times of the central spin for these three types of initial correlations are identical when the couplings are homogeneous. However, it is remarkable different for inhomogenous couplings. The QSL time of the central spin is sensitive to the initial states, the average coupling strength, the distribution of the couplings between the system and bath and the number of the nuclear spins in the bath. Furthermore, we find that the coherence in the initial state has significant influences on the QSL time of the system, and can lead to the increase of QSL time for homogeneous couplings.     

Direct observation of quantum coherence in single-molecule magnets

Direct evidence of quantum coherence in a single-molecule magnet in a frozen solution is reported with coherence times as long as T{2}=630+/-30 ns. We can strongly increase the coherence time by modifying the matrix in which the single-molecule magnets are embedded. The electron spins are coupled to the proton nuclear spins of both the molecule itself and, interestingly, also to those of the solvent. The clear observation of Rabi oscillations indicates that we can manipulate the spin coherently, an essential prerequisite for performing quantum computations.     

Steady state and transient Overhauser effect in systems of three spins

The rate equations describing spin polarization in a system of three spins are derived and solved for the case of a free radical dissolved in a solvent containing two nuclear spins. Triple irradiation experiments indicate that a nuclear spin A can be effectively coupled to an electron spin C via a second nuclear spin B and measurements of both the steady state and transient Overhauser effects are in accord with the theoretical predictions for a three-spin system. The ‘three spin effect’ is found to operate only in dilute solutions of free radicals in which case the probabilities for transitions between different nuclear or electronic energy levels can be determined. It was found to be effective for fluorine nuclei—in the presence of both protons and a free radical and for carbon [13] nuclei in the presence of either protons or fluorine nuclei and a free radical. Detailed measurements have been performed for CHFCl₂, para-difluorobenzene, and meta-fluorotoluene containing the tritertiary butyl phenoxyl radical.     

Quantum coherence dynamics of spin pairs in many-spin cluster

We consider the dynamics of a quantum coherence of two chosen spins in systems of dipolar coupled nuclear spins s=1/2 in solid. With the purpose to study this coherence we suggest two different methods. One of them uses the partial trace technique and reduced density matrix. The second method is based on the calculation the intensity of multiple quantum coherences using two-spin operator and the density matrix of the whole spin system. Results of calculations of the multiple-quantum dynamics in spin clusters of various dimensionalities are presented. It is shown that the whole density matrix method is more informative than the method based on the reduced density matrix.     

Coherent Polarization Transfer Effects Are Crucial for Interpreting Low-Field CIDNP Data

In this work we demonstrate that low-field chemically induced dynamic nuclear polarization (CIDNP) is strongly affected by re-distribution of polarization, which is formed in the course of spin evolution in transient radical pairs, in diamagnetic reaction products. This phenomenon is of importance when the spins of the reaction product are coupled strongly meaning that spin–spin interactions between them are comparable to the differences in their Zeeman interactions with the external magnetic field. In this case, polarization transfer relies on a coherent mechanism; as a consequence, spins can acquire significant polarization even when they have no hyperfine coupling to the electron spins in the radical pairs, i.e., cannot be polarized directly by CIDNP. This is demonstrated by taking CIDNP of n-butylamine as an example: in this case only the α-CH₂ protons are polarized directly, which is confirmed by high-field CIDNP, whereas the β-CH₂, γ-CH₂ and δ-CH₃ protons get polarized only indirectly due to the transfer of polarization from the α-CH₂ protons. These results show that low-field CIDNP data should be interpreted with care to discriminate between the effects of spin evolution in transient radical pairs and in diamagnetic reaction products.     

J-ONLY-TOCSY: efficient suppression of RDC-induced transfer in homonuclear TOCSY experiments using JESTER-1-derived multiple pulse sequences

The main purpose of homonuclear Hartmann-Hahn or TOCSY experiments is the assignment of spin systems based on efficient coherence transfer via scalar couplings. In partially aligned samples, however, magnetization is also transferred via residual dipolar couplings (RDCs) and therefore through space correlations can be observed in COSY and TOCSY experiments that make the unambiguous assignment of covalently bound spins impossible. In this article, we show that the JESTER-1 multiple pulse sequence, originally designed for broadband heteronuclear isotropic Hartmann-Hahn transfer, efficiently suppresses the homonuclear dipolar coupling Hamiltonian. This suppression can be enhanced even further by variation of the supercycling scheme. The application of the resulting element in homonuclear TOCSY periods results in coherence transfer via J-couplings only. As a consequence, the assignment of scalar coupled spin systems is also possible in partially aligned samples. The bandwidth of coherence transfer for the JESTER-1-derived sequences is comparable to existing TOCSY multiple pulse sequences. Results are demonstrated in theory and experiment.     

Geometry of multiple-spin systems as reflected in 13C-{1H} dipolar spectra measured at Lee-Goldburg cross-polarization

Theoretical calculation and analysis of (13)C-{(1)H} dipolar spectra of small-size spin clusters is presented. Dipolar spectra simulated using the time-independent average Hamiltonian are compared with the dipolar profiles obtained by 2D and 3D (1)H-(13)C correlation experiments employing Lee-Goldburg off-resonance cross-polarization (LG-CP). It is demonstrated that the structural parameters such as interatomic distances as well as mutual orientation of internuclear vectors can be derived from the dipolar profiles of simple spin clusters. Simplified analysis of the dipolar spectra based on isolated-like spin-pair approach can be used only if interacting spin cluster is reduced to the three-spin system in which the angle between both internuclear vectors ranges from 45 degrees to 135 degrees . For other local arrangements of spin systems the produced dipolar spectra must be analyzed with high caution. Contributions of all interacting spins to dipolar evolution of (13)C magnetization are mutually mixed and cannot be easily separated. However, simplification of the dipolar spectra is achieved by selective excitation. Enhanced selectivity of LG-CP transfer due to the initial (1)H chemical-shift-evolution period makes it possible to construct the dipolar spectra from (1)H-(13)C cross-peak intensities for every detected (1)H-(13)C spin-pair. Consequently, isolated-like spin pair evolution of the detected (1)H-(13)C coherence dominates to the resulting dipolar profile, while the influence of other interacting spins is suppressed. However, this suppression is not quite complete and analysis of the selective dipolar spectra based on isolated-like spin-pair approach cannot be used generally. Especially evolution of long-range (1)H-(13)C coherence is still significantly affected by spin states of other coupled hydrogen atoms.     

Quantum bit commitment is weaker than quantum bit seals

We investigate the reduced dynamics of a central spin coupled to a spin environment with non-uniform coupling. Through using the method of time-dependent density-matrix renormalization group (t-DMRG), we nonperturbatively show the dissipative dynamics of the central spin beyond the case of uniform coupling between the central spin and the environment spins. It is shown that only when the system-environment coupling is weak enough, the central spin system shows Markovian effect and will finally reach the steady state; otherwise, the reduced dynamics is non-Markovian and exhibits a quasi-periodic oscillation. The frequency spectrum and the correlation between the central spin system and the environment are also studied to elucidate the dissipative dynamics of the central spin system for different coupling strengths.     

Second-order effects on the EPR spectra of exchange-coupled pairs of paramagnetic ions

The paper gives a spin-hamiltonian formalism for a pair of exchange-coupled paramagnetic ions, operating within the single S-multiplet of total spin and in which coupling among the different multiplets is taken into account with a second-order perturbative approximation. Arbitrary values of the coupled spins S₁ and S₂ are considered and a tensorial form for the various contributions to the pair energy is assumed, without restrictions on principal values and directions. That allows us to point out some new EPR aspects related principally to the role of local and exchange anisotropies.     

Fast and accurate algorithm for the simulation of NMR spectra of large spin systems

The computational cost for the simulation of NMR spectra grows exponentially with the number of nuclei. Today, the memory available to store the Hamiltonian limits the size of the system that can be studied. Modern computers enable to tackle systems containing up to 13 spins [1], which obviously does not allow to study most molecules of interest in research. This issue can be addressed by identifying groups of spins or fragments that are not or only weakly interacting together, i.e., that only share weakly coupled spin pairs. Such a fragmentation is only permitted in the weak coupling regime, i.e., when the coupling interaction is weak compared to the difference in chemical shift of the coupled spins. Here, we propose a procedure that removes weak coupling interactions in order to split the spin system efficiently and to correct a posteriori for the effect of the neglected couplings. This approach yields accurate spectra when the adequate interactions are removed, i.e., between spins only involved in weak coupling interactions, but fails otherwise. As a result, the computational time for the simulation of 1D spectra grows linearly with the size of the spin system.     

Quantum counterpart of measure synchronization: A study on a pair of Harper systems

Measure synchronization is a well-known phenomenon in coupled classical Hamiltonian systems over last two decades. Here, synchronization in a pair of coupled Harper systems is investigated both in classical and quantum contexts. It seems that the concept of measure synchronization is restricted in the classical limit as it involves with the phase space. We show the quantum counterpart of the synchronization in a pair of coupled quantum kicked Harper chains. In the quantum context, the coupling occurs between two spins chains via a time and site dependent potential. We use the average interaction energy between the participating systems as an order parameter in both the contexts to establish a connection between the classical and the quantum scenarios. Besides, we also study the entanglement between the chains and difference between the average bare energies in the quantum context. Interestingly, all such indicators suggest a connection between the MS transition in classical maps and a phase transition in quantum spin chains.     

Transverse magnetization transfer under planar mixing conditions in spin systems consisting of three coupled spins 1/2

Polarization transfer under planar mixing conditions is a widely used tool in modern NMR-experiments. In the case of two coupled spins 1/2 or a chain of three or more spins 1/2 with only nearest neighbor couplings, it is only possible to transfer a single magnetization component (longitudinal magnetization in the principle axis system of the planar coupling tensors). However, if all couplings in a three-spin system are non-zero, it turns out that all magnetization components can be efficiently transferred even under strictly planar mixing conditions. In this article a detailed theoretical analysis is presented based on analytical transverse coherence transfer functions and on the underlying commutator algebra. In addition, transverse magnetization transfer is demonstrated experimentally. The results show that in highly coupled spin systems, as for example in the case of partially aligned samples with many residual dipolar couplings, special care has to be taken to avoid phase distortions if planar mixing steps are used.     

Multiple Quantum Coherences (MQ) NMR and Entanglement Dynamics in the Mixed-Three-Spin XXX Heisenberg Model with Single-Ion Anisotropy

We analytically investigate Multiple Quantum (MQ) NMR dynamics in a mixed-three-spin (1/2,1,1/2) system with XXX Heisenberg model at the front of an external homogeneous magnetic field B. A single-ion anisotropy property ζ is considered for the spin-1. The intensities dependence of MQ NMR coherences on their orders (zeroth and second orders) for two pairs of spins (1,1/2) and (1/2,1/2) of the favorite tripartite system are obtained. It is also investigated dynamics of the pairwise quantum entanglement for the bipartite (sub)systems (1,1/2) and (1/2,1/2) permanently coupled by, respectively, coupling constants J₁ and J₂, by means of concurrence and fidelity. Then, some straightforward comparisons are done between these quantities and the intensities of MQ NMR coherences and ultimately some interesting results are reported. We also show that the time evolution of MQ coherences based on the reduced density matrix of the pair spins (1,1/2) is closely connected with the dynamics of the pairwise entanglement. Finally, we prove that one can introduce MQ coherence of the zeroth order corresponds to the pair spins (1,1/2) as an entanglement witness at some special time intervals.