Counting statistics of collective photon transmissions

We theoretically study cooperative effects in the steady-state transmission of photons through a medium of N radiators. Using methods from quantum transport, we find a cross-over in scaling from N to N² in the current and to even higher powers of N in the higher cumulants of the photon counting statistics as a function of the tunable source occupation. The effect should be observable for atoms confined within a nano-cell with a pumped optical cavity as photon source.     

Evidence for Quantum Beats generated by a photo-induced charge transfer reaction

Photo-initiated charge transfer reactions in solution proceed via a radical pair intermediate which in most cases will separate on a time scale of several nanoseconds. The non-adiabicity of this process is the source of coherences in the spin system. A quantitative discussion of the observability of the resulting quantum beats using Fourier-transform EPR is presented. We also show experimental evidence for the predicted quantum beats using the photo-initiated charge transfer reaction of Zn-Tetraphenylporphyrin and benzoquinone in 2-propanol. The analysis of the beat frequency leads to an estimate of the exchamge couplingJ≈2.6·10⁶ s^?1 of the Coulomb-coupled radical pair.     

Quantum size effects of CO reactivity on metallic quantum dots

We study the reactivity of a metallic quantum dot when exposed to a gas phase CO molecule. First, we perform a Newns-Anderson model calculation in which the valence electrons of the quantum dot are confined by a finite potential well and the molecule is characterized by its lowest unoccupied molecular orbital in the gas phase. A pronounced quantum size effect regarding the charge transfer between the quantum dot and molecule is observed. We then perform a first-principles calculation for a selected size interval. The quantum dot is described within the jellium model and the molecule by pseudopotentials. Our results show that the charge transfer between the quantum dot and the molecule depends critically on the size of the quantum dot, and that this dependence is intimately connected with the electronic structure. The key factor for charge transfer is the presence of states with the symmetry of the chemically active molecular orbital at the Fermi level.     

Global and Local Spin Squeezing in Coupled Quantum Kicked Tops Model

We investigate the global and the local spin squeezing in a weakly coupled quantum kicked tops system. Two different situations are considered: (i) N=1 and (ii) N=30 for each subsystem, corresponding to quantum and classical cases, respectively. In the first case, since the two subsystems have no spin squeezing, the global squeezing completely originates from quantum correlations. For the second one, the global spin squeezing is enhanced over the local one. Due to the chaotic nature of the system, the spin squeezing is sensitive to the initial state. In chaotic region, the squeezing vanished time is much shorter than that in the regular region.     

平行耦合双量子点分子A-B干涉仪的电荷及其自旋输运

利用非平衡格林函数方法,理论研究每臂中嵌有一个平行耦合双量子点分子的A-B干涉仪(平行耦合双量子点分子A-B干涉仪)的电荷及其自旋输运性质.无外磁场时,与每臂中嵌有一个量子点的A-B干涉仪相比较,平行耦合双量子点分子A-B干涉仪中电子隧穿变得更加容易发生.当平行耦合双量子点分子A-B干涉仪中引入外磁场时,能够在电导能谱中观察到一个Fano共振和一个反共振,这两种输运状态在磁场取适当数值时能够同时消失.此外,通过调节左右两电极间的偏压、磁通和Rashba自旋轨道相互作用,可以对体系自旋输运进行调控.     

Theoretical studies on the single proton transfer process in adenine base

The effect of metal ions (Mⁿ⁺ = Na⁺, K⁺, Mg²⁺, Ca²⁺, Zn²⁺ and hydrated Mg²⁺ ions) and water molecules on the tautomerism of adenine induced by single intramolecular proton transfer (SPT) have been investigated theoretically. Calculated results show that the single proton transfer process in adenine base is favored and even becomes thermodynamically spontaneous because of the presence of Mⁿ⁺ interacting at the N₃ position of adenine. On the contrary, if Mⁿ⁺ coordinated to N₇ site, the single proton transfer process will become unfavorable than that in the neutral system. The effects of metal ions on the SPT of adenine base are more pronounced if Lewis acidity of metal ion is increased. Water plays a more important role than metal ions during the SPT process. It is found that water can act not only as a solvent but also as a mediator which gives and accepts protons to promote SPT, playing a bridge role. As a result, inclusion of a water molecule drastically reduces the energy barrier for the SPT. Moreover, two water molecules can yield larger assisting effect on the SPTs compared with one water molecule. We can conclude that the tautomerism of DNA adenine base can be modulated by the metal ions and water molecules. Copyright © 2015 John Wiley & Sons, Ltd.     

Nuclear–nuclear correlation function from non-Born–Oppenheimer calculations of diatomic rovibrational states with total angular momentum equal to two (N = 2). Charge asymmetry in HD

The HD molecule in rovibrational states where the total angular momentum quantum number is equal to two (N = 2) is characterised with quantum mechanical calculations without assuming the Born–Oppenheimer (BO) approximation. Explicitly correlated all-particle Gaussian functions are used in the calculations. The convergence of the total non-BO energies of the considered states with the basis set size is analysed. The calculations of the averaged interparticle distances demonstrate the asymmetry of the electronic charge distribution. The algorithm to calculate the nuclear–nuclear correlation function for the N = 2 states is derived and implemented. Plots of this function for different rovibrational states provide a visual representation of the molecular structure.     

Electronic and spectral properties of ametal-organic super container molecule by single point DFT

ABSTRACT

Metal-organic super container (MOSC) molecules are ideal candidates for photocatalysis due to their construction with transition metal centres and tuneable cavity sizes that could house catalytic sites. The basic electronic structure for a model of extremely large size (more than 2000 ions) is explored by single point calculation using unrestricted density functional theory, and Perdue–Burke–Ernzerhof functional in Vienna ab initio simulation package software. The information obtained through these calculations (such as density of states, absorbance spectra, and charge density) will allow for analysis of a MOSC's catalytic ability. Electronic characteristics of the nanostructures (MOSCs and their building blocks) in the ground and photoexcited electronic configurations are examined. We explore if the presence of transition metal ions with open shells in such close proximity to one another may result in high spin configurations and show any arrangement into ferromagnetic ordering. Spin-unrestricted computation was applied to evaluate how optical properties could be affected by d–d transitions. A scan of a spin-polarisation parameter allows one to resolve spin configuration and obtain a connection between theory and experiment. Analysis of Kohn–Sham orbitals of interest provides insight into charge transfer mechanisms, which were found to contribute to multiple low-energy charge transfer states to the electronic structure.     

Correlation between quantum charge fluctuations and magnetic ordering in multiferroic LuFe<Subscript>2</Subscript>O<Subscript>4</Subscript>

We examine the interplay between quantum charge fluctuations and magnetic ordering in multiferroic LuFe₂O₄ and show that this can couple spin and charge degrees of freedom in a LuFe₂O₄ bilayer below the Neel temperature T _N . Our analysis supports the idea that the double exchange mechanism normally used in metallic systems can be applied to charge-ordered insulators. This causes ferrimagnetic spin order to reduce the transfer integrals between Fe²⁺ and Fe³⁺ in LuFe₂O₄, decreasing charge fluctuations and increasing the polarization in this system below T _N . This work thus provides a more detailed understanding of the mechanism for spin-charge coupling in LuFe₂O₄.     

Adsorption patterns of caffeic acid on titania: affinity,charge transfer and sunscreen applications

ABSTRACT

Several photo-induced processes contribute to titania-catalysed photodegradation of organic UV-absorbing compound, caffeic acid (CA), utilised as skin photoprotector in sunscreens containing titania. Optical transitions, channels of photoexcitations, and charge transfer state formation in anatase TiO₂ nanowire sensitised by CA are computed and analysed. Trends of charge transfer state formation are explored through modelling of non-adiabatic dynamics using reduced density matrix approach combined with density functional theory with Perdew–Burke–Ernzerhof functional, in the basis of plane waves, using Vienna Ab initio Simulation Package software. The electronic structure of the explored model shows signatures of quantum confinement of TiO₂ nanowire. A change of excitation energy provides control of either one of the possible channels for photoexcitations: (1) local excitation at either nanowire or CA-adsorbate or (2) photo-induced electron transfer from CA-adsorbate to titania. The conclusions obtained from this computational modelling deliver further understanding of the adsorption of catechol groups on the surface of titania nanowire that will help in designing titania-based materials least damaging to CA and skin.     

Heisenberg-Integrable Spin Systems

We investigate certain classes of integrable classical or quantum spin systems. The first class is characterized by the recursively defined property P saying that the spin system consists of a single spin or can be decomposed into two uniformly coupled or disjoint subsystems with property P. For these systems the time evolution can be explicitly calculated. The second class consists of spin systems where all non-zero coupling constants have the same strength (spin graphs) possessing N − 1 independent, commuting constants of motion of Heisenberg type. These systems are shown to have the above property P and can be characterized as spin graphs not containing chains of length four as vertex-induced sub-graphs. We completely enumerate and characterize all spin graphs up to N = 5 spins. Applications to the construction of symplectic numerical integrators for non-integrable spin systems are briefly discussed.      

Density-functional study of CO adsorbed on RhN （N = 2-19） clusters

We investigate the structural, electronic and adsorption properties of one single CO molecule adsorbed on Rh_N (N = 2-19) clusters, using the density-functional theory in the spin-polarized generalized gradient approximation. It is found that the structural growth model of the Rh_N clusters transforms from double layers (N = 12-16) to three layers (N = 17-19). Three different adsorption types are the atop site adsorption for N = 6, 8, 9, 11, 12, the bridge site adsorption for N = 2-5, 7, 10, 13-15, 17 and the face adsorption for N = 16, 18, 19. The adsorption abilities of Rh_N clusters are related to C-O bond length, vibrational frequency, adsorption energy and the charge transfer between CO and Rh clusters as well as the electronic density of state. With the increase of Rh cluster size, the adsorption energy of CO adsorbed on Rh_N clusters tends to be 2.2 eV-2.3 eV, which is 0.2 eV-0.3 eV larger than the theoretical value (about 2.0 eV) of CO molecule adsorption on clean Rh (111) surface.     

Electron Spin Resonance Study on the Photoinduced Electron Transfer in Chlorophyll a in Reconstituted Lipid Bilayer Vesicles

Abstract  

The photoinduced electron transfer from chlorophyll a through the interface of positively charged dioctadecyltrimethylammonium chloride (DODAC), neutral dipalmitoylphosphatidylcholine (DPPC) and negatively charged dihexadecylphosphate (DHP) headgroup of the lipid bilayers was studied. The photoinduced radicals were identified by electron spin resonance (ESR) and radical yields of chlorophyll a were determined by double integration of the ESR spectra. The formation of vesicles was identified indirectly by measuring change of the λ _max value of optical absorption spectrophotometer from diethyl ether solution to vesicle solutions, and observed directly with scanning and transmission electron microscopic images. The interaction distance between chlorophyll a and interface water (D₂O) determined by deuterium modulation depth with electron spin echo modulation (ESEM) showed a decreasing order DODAC > DPPC > DHP. The interface charge of each vesicle was determined with zeta potential measurement. The interface charge of the lipid bilayers affected the radical yields of chlorophyll a more critically than the interaction distance between chlorophyll a and interface water.     

Magnetic field dependence of electronic structures in a single and double quantum dots by 3D-MHFKS calculation

The 3-dimensional Mesh-Hartree-Fock-Kohn-Sham (3D-MHFKS) calculation is applied to study the magnetic (B-) field dependence of the electronic structures of circular-shaped vertical quantum dot (Q-dot) with electron number (N) in double barrier structure (DBS) and also coupled double Q-dots in triple barrier structure (TBS). One of the advantageous points of the 3D-MHFKS calculation is that the strength of coupling between two dots are explicitly evaluated by introducing the realistic barrier in TBS as a straightforward extension of 3D-MHFKS calculation of the single Q-dot in DBS. The calculated chemical potentials represented in B-N phase diagram are consistently and systematically discussed by showing the B-field dependence of the occupied single particle energy levels from the view point how the electronic states transfer sequentially from Fock-Darwin (FD) to lowest Landau (LL) and from LL to the spin flip (SF) and from SF to spin-polarized maximum density droplet (MDD) domains as increasing B-field in the Q-dots.     

T型双量子点分子Aharonov-Bohm干涉仪的电输运

利用非平衡格林函数方法, 理论研究T型双量子点分子Aharonov-Bohm (A-B)干涉仪的电荷及其自旋输运性质. 通过控制T型双量子点分子内量子点间有无耦合, 能够实现在同一电子能级位置处分别出现共振和反共振状态, 根据此性质, 能将体系设计成量子开关器件. 当将两个完全相同的T型双量子点分子分别嵌入A-B干涉仪两臂中时, 磁通取适当数值, 能够出现完全的量子相消干涉. 通过调节量子点能级、左右两电极间的偏压和Rashba自旋轨道相互作用强度, 可对体系自旋流进行调控. 关键词： 非平衡格林函数 T型双量子点分子 Aharonov-Bohm干涉仪 自旋输运     

Coherent spin dynamics of electrons and excitons in nanostructures (a review)

The studies of spin phenomena in semiconductor low-dimensional systems have grown into the rapidly developing area of the condensed matter physics: spintronics. The most urgent problems in this area, both fundamental and applied, are the creation of charge carrier spin polarization and its detection, as well as electron spin control by nonmagnetic methods. Here, we present a review of recent achievements in the studies of spin dynamics of electrons, holes, and their complexes in the pump-probe method. The microscopic mechanisms of spin orientation of charge carriers and their complexes by short circularly polarized optical pulses and the formation processes of the spin signals of Faraday and Kerr rotation of the probe pulse polarization plane as well as induced ellipticity are discussed. A special attention is paid to the comparison of theoretical concepts with experimental data obtained on the n-type quantum well and quantum dot array samples.     

Electron transmission and quantum current distribution of C<Subscript>70</Subscript> molecule

The characteristics of electron transmission through C₇₀ molecule bridge in which two atomic chain leads are connected to long-axis carbon atoms are investigated theoretically by using tight-binding approach based on the Green’s function with only one π orbital electron per carbon atom. Electron transmission through C₇₀ molecule from the input to the output terminal is obtained. From the spectrum, the switching feature of the electron transmission through C₇₀ is found, and the oscillation property based on the quantized level is explained. The quantum current distributions inside C₇₀ molecule bridge are calculated and simulated by the quantum current density theory based on Fisher-Lee formula at the energy point E = −0.2 eV, where the transmission spectrum shows a peak. The maximum and the minimum bond quantum currents are presented, and the reason why the currents are distributed nonuniformly is explained by the phase difference of the atomic orbits. The result shows that the currents at each atomic site agree with Kirchhoff quantum current conservation law. Supported by the National Key Basic Research Development Project (Grant No. 2003CB716204), the International Corporation Project of the Education Department of China (Grant No. 20050360563), the Key Laboratory of Advanced Photonic and Electronic Materials of Jiangsu (Grant No. BM2003202) and the State Key Laboratory of Solid State Microstructures of Nanjing University     

Catalytic mechanism of human N-acetylserotonin methyltransferase: a theoretical investigation

The methyl-transfer mechanism of human N-acetylserotonin methyltransferase and the roles of several residues around the active sites are investigated by density function theory method. This enzyme will catalyse the conversion of N-acetylserotonin and S-adenosyl-L-methionine (SAM) into melatonin and S-asenosylhomocysteine, which is the terminal step in the melatonin (N-acetyl-5-methoxytryptamine) biosynthesis. The calculated results confirm that the methyl transfer and proton transfer will take place via a S_N2 step with a concerted mechanism, which is different from the experimental estimation via a water bridge. The residues H255, D256, E311, and R252 play an important role in reducing the barrier height and inducing methyl transfer. In addition, a full SAM molecule is considered in this work, which is never explored in previous reports. We find that some residues around the SAM in the centre of active site are essential factors to influence the mechanism and barrier height. So a truncated SAM model may not be suitable for all reactions.     

First excitations of the spin 1/2 Heisenberg antiferromagnet on the kagomé lattice

We study the exact low energy spectra of the spin 1/2 Heisenberg antiferromagnet on small samples of the kagomé lattice of up to N=36 sites. In agreement with the conclusions of previous authors, we find that these low energy spectra contradict the hypothesis of Néel type long range order. Certainly, the ground state of this system is a spin liquid, but its properties are rather unusual. The magnetic () excitations are separated from the ground state by a gap. However, this gap is filled with nonmagnetic () excitations. In the thermodynamic limit the spectrum of these nonmagnetic excitations will presumably develop into a gapless continuum adjacent to the ground state. Surprisingly, the eigenstates of samples with an odd number of sites, i.e. samples with an unsaturated spin, exhibit symmetries which could support long range chiral order. We do not know if these states will be true thermodynamic states or only metastable ones. In any case, the low energy properties of the spin 1/2 Heisenberg antiferromagnet on the kagomé lattice clearly distinguish this system from either a short range RVB spin liquid or a standard chiral spin liquid. Presumably they are facets of a generically new state of frustrated two-dimensional quantum antiferromagnets. Received: 27 November 1997 / Accepted: 29 January 1998     

Quantum pumping in helimagnet heterostructures

Spin-dependent diffraction occurs in helimagnet-related transport processes. In this work, we investigated quantum pumping properties in the normal-metal/helimagnet/normal-metal heterostructure driven by two out of phase time-dependent gate potentials. At the condition when one of the diffracted beams goes out of the horizon the pumped charge and spin currents demonstrate sharp dips and rises as a function of the helimagnet spiral wave vector q. At small and large q?s, the transmission and pumping properties approach the behaviors of a ferromagnet and an insulating barrier, respectively. For different helimagnet spiral periods, the diffracted angles are different. As a result, the pumped charge and spin currents demonstrate multiple maximal and minimal peaks as a function of q, hence, sensitively depend on the helimagnet spin configuration. All the pumping properties can be interpreted by the quantum gate-switching mechanisms.