Proton exchange within water molecule

The exchange by quantum states between nuclear spins of two water molecule protons is considered. It is shown that such an intramolecular exchange does not break spin isomers of the molecule and does not cause quantum transitions between singlet and triplet states of the molecule spin system.     

Singlet–triplet oscillations and far-infrared spectrum of four-minima quantum-dot molecule

We study ground states and far-infrared spectra (FIR) of two electrons in four-minima quantum-dot molecule in magnetic field by exact diagonalization. Ground states consist of altering singlet and triplet states, whose frequency, as a function of magnetic field, increases with increasing dot–dot separation. When the Zeeman energy is included, only the two first singlet states remain as ground states. In the FIR spectra, we observe discontinuities due to crossing ground states. Non-circular symmetry induces anticrossings, and also an additional mode above ω₊ in the spin-triplet spectrum. In particular, we conclude that electron–electron interactions cause only minor changes to the FIR spectra and deviations from the Kohn modes result from the low-symmetry confinement potential.     

Stability of singlet and triplet trions in carbon nanotubes

We investigate singlet and triplet trion states in semiconducting carbon nanotubes using a one-dimensional model. It is concluded that singlet trion states in bind up to 13.6% stronger than exciton states, and that they lower the optical transition energy with up to 50% of the tight binding band gap energy.     

Dynamic model of ortho-para conversion of water molecules

A quantum model of mutual conversion of spin isomers of the water molecule, involving a proton of a neighboring water molecule, is proposed. Molecules interact due to magnetic dipole-dipole forces which give rise to flip-flop processes. An additional adsorption energy different in magnitude and sign for singlets and triplets arises from a fast exchange of spin states within an acceptor molecule. A slower flip-flop process controls the simultaneous evolution of all three protons, which results in the transition between singlet and triplet states. Based on the developed model, experimental data on ortho-para-water are discussed.     

Electron spin polarization in a rotating triplet

The triplet model of electron spin polarization in fluid media is evaluated. The model consists of an initial singlet molecule rotating in a static, externally applied magnetic field. Intersystem crossing into different zero-field states is represented by a rate matrix diagonal in the molecular frame, and this matrix is expressed as an effective spin operator. The triplet rotates, and the motion affects the polarization in the laboratory frame, and also causes spin relaxation in the triplet manifold. The triplet is chemically quenched, and the polarization appears in the doublet fragments. The model is treated in a density matrix formalism and on the basis of anisotropic rotational diffusion of the triplet molecule. Explicit expressions are obtained in terms of the molecular parameters, the various rate constants, and the rotational correlation time.     

Ultrafast solvent-induced spin-flip and nonadiabatic coupling: ClF in argon solids

Femtosecond pump-probe spectra show direct evidence for ultrafast solvent-induced spin flip in photodissociation-recombination events of ClF, a light diatomic molecule, for which the spin-orbit coupling is weak. The bound triplet states ((3)Pi) of ClF are probed and the dynamics for excitation to the singlet state ((1)Pi(1)) is compared with excitation to the triplet state B((3)Pi(0)). The population initially excited to the singlet state (1)Pi(1) is transferred to the bound triplet states (3)Pi within tau(f)=0.5 ps. Oscillations in the spectra indicate wave packet dynamics with the triplet state period of 300 to 400 fs in both cases. According to simulations of F(2)/Ar, most of the initially excited singlet state population is converted to repulsive and weakly bound triplet states within approximately 60 fs. In the first ps, 40% of the triplet population accumulates in the weakly bound (3)Pi states, in good accord with the experiment.     

A Realization of Yangian and Its Applications to the Bi-spin System in an External Magnetic Field

Yangian Y(sl(2)) is realized in the bi-spin system coupled with a time-dependent external magnetic field. It is shown that Y(sl(2)) generators can describe the transitions between the "spin triplet" and the "spin singlet" that evolve with time. Furthermore, new transition operators between the states with Berry phase factor and those between the states of nuclear magnetic resonance are presented.     

Mixed state of spin moments of two protons in the water molecule and stability of its spin isomers

It is shown that the para-to-ortho water ratio most abundant in the nature is the water molecule existence form most stable to external influences. The assumptions, which are implicitly adopted when singlet and triplet states of the quantum system of two spin moments are independently considered, are discussed.     

HighT c superconductivity in the itinerant Ising model II. Spin triplet pairing

We study the spin triplet pairing superconducting states of the itinerant Ising model. The spin and spatial symmetries of the states are explored. We find that only a restricted set of spin symmetry states are allowed, while an infinite number of spatial symmetry states exist. The spin triplet pairing states can either be gapless or have finite energy gaps, but all spin triplet pairing states have the sameT _c .The free energies of spin triplet and spin singlet pairing states are calculated and compared.     

Oxidation at the Si/SiO2 interface: influence of the spin degree of freedom

We show, using first-principles spin-polarized total-energy calculations, that depending on the spin configuration of the system, the reaction of an O2 molecule with a Si-Si bond in a suboxidized region might result either in a peroxy linkage defect (for a singlet spin state) or in a perfect Si-O-Si bond plus an interstitial O atom (for a triplet spin state). Even though the singlet has a lower energy than the triplet configuration, we find a rather small probability for triplet to singlet conversion. Therefore, as the O2 in an SiO2 interstitial site has a triplet configuration, this reaction spin dependence may have a strong influence on the high quality of the Si/SiO2 interface.     

Controlling and detecting spin correlations of ultracold atoms in optical lattices

We report on the controlled creation of a valence bond state of delocalized effective-spin singlet and triplet dimers by means of a bichromatic optical superlattice. We demonstrate a coherent coupling between the singlet and triplet states and show how the superlattice can be employed to measure the singlet-fraction employing a spin-blockade effect. Our method provides a reliable way to detect and control nearest-neighbor spin correlations in many-body systems of ultracold atoms. Being able to measure these correlations is an important ingredient in studying quantum magnetism in optical lattices. We furthermore employ a SWAP operation between atoms which are part of different triplets, thus effectively increasing their bond-length. Such a SWAP operation provides an important step towards the massively parallel creation of a multiparticle entangled state in the lattice.     

EPR of photo-excited triplet states: A personal account

A sketch is presented of the path that has led from Zavoisky’s pioneering experiments to modern investigations by electron paramagnetic resonance (EPR) of the phosphorescent (S = 1) triplet state of polyatomic molecules or ions. The group-theoretical method first introduced by Wigner in his analysis of the multiplets of atomic spectroscopy, likewise provides a key for understanding the zero-field splitting and selection rules for radiative decay of the phosphorescent triplet state. Examples to illustrate the progress made through EPR experiments are selected from three fields. (i) Conformational instability on excitation. Both the zero-field splitting and the electron spin density distribution provide unique fingerprints of a triplet state’s geometry — structural information of a kind that is nonexistent for singlet states! Illustrations are provided by benzene C₆H₆ and fullerene C₆₀. (ii) The optical pumping cycle. The spin selectivity of singlet-to-triplet intersystem crossing and radiative decay of the individual spin components of the triplet state is discussed. In practice this selectivity is put to advantage by performing EPR on triplet states in zero-field by means of optical detection. In turn, such experiments have led to a detailed insight into the spin-orbit coupling mechanisms responsible for the spin selectivity of the above processes. The high sensitivity attainable with optical detection has recently culminated in EPR experiments on single molecules. (iii) Quantum interference. In a triplet state of low symmetry two of the spin sublevels may decay to the ground state by the emission of photons of a common polarization (i.e., out of plane for an aromatic hydrocarbon). In such a situation quantum interference between the two decay channels can be induced by an appropriate preparation of the excited state. An example is shown where flash-excitation in the singlet manifold followed by rapid intersystem crossing causes theS = 1 spin angular momentum to be created in a spin state which is not an eigenstate of the zero-field splitting tensor. This nonstationary character of the initial triplet state, which reflects the spin-orbit coupling pathway, is observed through the detection of a spontaneous microwave signal following the 25 ps laser flash.     

Adiabatic passage schemes in coupled semiconductor nanostructures

Adiabatic passage schemes in coupled semiconductor quantum dots are discussed. For optical control, a doped double-dot molecule is proposed as a qubit realization. The quantum information is encoded in the carrier spin, and the flexibility of the molecular structure allows to map the spin degrees of freedom onto the orbital ones and vice versa, which opens the possibility for high-finesse quantum gates by means of stimulated Raman adiabatic passage. For tunnel-coupled dots, adiabatic passage of two correlated electrons in three coupled quantum dots is shown to provide a robust and controlled way of distilling, transporting and detecting spin entanglement, as well as of measuring the rate of spin disentanglement. Employing tunable interdot coupling the scheme creates, from an unentangled two-electron state, a superposition of spatially separated singlet and triplet states, which can be discriminated through a single measurement. Finally, we discuss phonon-assisted dephasing in quantum dots, and present control strategies to suppress such genuine solid-state decoherence losses.     

Ab initio multi-reference configuration interaction of the low-lying states of the AsP molecule

Nine low-lying electronic states of the AsP molecule, including Σ , Ⅱ, and △ symmetries with singlet, triplet, and quintet spin multiplicities, are studied using multi-reference configuration interaction method.The potential energy curves and the spectroscopic constants of these nine states are determined, and compared with the experimental observed data as well as other theoretical works available at present.Three quintet states are reported for the first time.Furthermore, the analytical potential energy functions of these states are fitted using Murrell-Sorbie function and least square fitting method.     

Excitation of lowest electronic states of the uracil molecule by slow electrons

The excitation of lowest electronic states of the uracil molecule in the gas phase has been studied by electron energy loss spectroscopy. Along with excitation of lowest singlet states, excitation of two lowest triplet states at 3.75 and 4.76 eV (±0.05 eV) and vibrational excitation of the molecule in two resonant ranges (1?C2 and 3?C4 eV) have been observed for the first time. The peak of the excitation band related to the lowest singlet state (5.50 eV) is found to be blueshifted by 0.4 eV in comparison with the optical absorption spectroscopy data. The threshold excitation spectra have been measured for the first time, with detection of electrons inelastically scattered by an angle of 180°. These spectra exhibit clear separation of the 5.50-eV-wide band into two bands, which are due to the excitation of the triplet 1³ A?? and singlet 1¹ A?? states.     

Generalization of the Cooper pairing mechanism for spin-triplet in superconductors

A generalization of the Cooper pairing mechanism is proposed which allows for a triplet state of lower energy. This is achieved by incorporating spin into the canonical commutation relations and by modifying the δ potential contact interaction. The gap equation contain as solutions both singlet and triplet states. It is shown that the triplet state is lower in energy than the singlet state which may explain the spin-triplet superconductivity observed.     

The Bertlmann–Martin Inequality and Spin Degrees of Freedom

The Bertlmann–Martin inequality based on the dipole sum rule is revisited taking into account the spin degrees of freedom. We consider 1 and 2 particles of spin 1/2 in a mean field, adding a spin dependent interaction. The derivation of the inequality relies on the closure relation. We discuss the effect of the Pauli principle, and the restrictions it imposes on the use of the closure relation. The problem is exemplified by a simple model based on harmonic forces. Moreover, in the 2 particle case, the model we use is separable in the relative and centre of mass coordinates. In this case, we show that for operators connecting only singlet states, their sum rule can be calculated in the usual way, i.e. via the double commutator of this operator with the Hamiltonian. An upper bound can also be obtained by using the Bertlmann–Martin technique. This is not possible for operators involving a transition between singlet and triplet states.     

Transparent manganite films as hole injectors for organic light emitting diodes

Organic light-emitting diodes (OLEDs) are nowadays one of the most attractive devices based on organic semiconductors due to their successful application in the display technology. Electroluminescence in OLEDs is mainly governed by the fluorescence from excited singlet states, which have large transition probabilities providing the major radiative pathway. The “forbidden” triplet state emission can be activated by increasing spin–orbit coupling via dye doping. The singlet–triplet exciton formation statistics is usually given by 1:3 partition due to the quantum constrains.

Injection of carriers with finite spin polarisation should influence and modify the recombination statistics and can be used for tuning of the device efficiency. In this context, the development of a new class of electrodes able to guarantee both efficient charge and spin injection becomes of paramount importance. We show that strongly spin polarised colossal magnetoresistance manganite La_0.7Sr_0.3MnO₃ (LSMO) can successfully substitute conventional ITO electrodes in OLEDs. Highly transparent, metallic and ferromagnetic LSMO layers were used in combination with standard Al and spin polarised Co top electrodes. Electrical and optical characterisations of the OLEDs with spin polarised electrodes indicate the applicability of the new manganite electrodes for organic light-emitting devices.     

A theory of the collision-induced singlet to triplet transition of methylene

This paper begins with a survey and critique of past experimental and theoretical studies of the inert gas catalysed singlet to triplet transition of methylene. Next we develop a transition-state theory in which the process of activation consists of a collisional distortion of methylene to the extent that degeneracy occurs between adiabatic singlet and triplet vibronic states. Establishment of this collision induced degeneracy is followed by a spin-orbit coupled singlet to triplet transition which is then subsequently stabilized by the splitting of the degeneracy which accompanies the continued relative motion of catalyst and radical. This theory appears to be able to account for what is presently known about the bimolecular singlet to triplet reaction. It is capable of generating rate constants with the correct order of magnitude and of accounting for the experimentally observed isotope and catalytic dependence of these constants.