Multiple-quantum dynamics of one-dimensional nuclear spin systems in solids

Multiple-quantum spin dynamics is studied using analytic and numerical methods for one-dimensional finite linear chains and rings of nuclear spins 1/2 coupled by dipole-dipole interactions. An approximation of dipole-dipole interaction between nearest neighbors having the same constants is used to obtain exact expressions for the intensities of the multiple-quantum coherences in the spin systems studied, which are initially in thermal equilibrium and whose evolution is described by a two-spin two-quantum Hamiltonian. An approximation of nearest neighbors with arbitrary dipole-dipole interaction constants is used to establish a simple relationship between the multiple-quantum dynamics and the dynamics of spin systems with an XY Hamiltonian. Numerical methods are developed to calculate the intensities of multiple-quantum coherences in multiple-quantum NMR spectroscopy. The integral of motion is obtained to expand the matrix of the two-spin two-quantum Hamiltonian into two independent blocks. Using the nearest-neighbor approximation the Hamiltonian is factorized according to different values of the projection operator of the total spin momentum on the direction of the external magnetic field. Results of calculations of the multiple-quantum dynamics in linear chains of seven and eight nuclear spins and a six-spin ring are presented. It is shown that the evolution of the intensities of the lowest-order multiple-quantum coherences in linear chains is accurately described allowing for dipole-dipole interaction of nearest and next-nearest neighbors only. Numerical calculations are used to compare the contributions of nearest and remote spins to the intensities of the multiple-quantum coherences.     

A Manifestation of two-quantum transitions in the ODEPR spectra of the spin-correlated radical pairs in micelles

Optically detected electron paramagnetic resonance spectra of the spin-correlated radical pairs diffusing inside a spherical region are numerically simulated taking into account an exchange interaction between partners of the pairs. It is shown that these spectra contain the lines induced by the two-quantum transitions. The shape and the width of this two-quantum transition line are analyzed as depending on magnetic resonance parameters, on molecular kinetic parameters and chemical reactivity of radicals.     

Electric-Wiggler-Enhanced Three-Quantum Scattering and the Output Power Affected by this Scattering in a Free-Electron Laser

We derive the cross section of scattering through the three-quantum interaction of an electron with the incident laser field, the emitted photon, and an axial electrostatic field produced by the magnetic wiggler in the magnetic wiggler acting as the sole zeroth-order perturbing classical field in the first free-electron laser （FEL）. In the derivation, we apply quantum-wiggler electrodynamics （QWD）. We find that this scattering predominates the usual two-quantum scattering. The output power of spontaneous free-electron two-quantum Stark emission driven by the above electrostatic field attenuated by the three-quantum scattering agrees within a factor of 10 with the measured power in the case of the first FEL.     

Vibrational dynamics of biological molecules: Multi-quantum contributions

High-resolution X-ray measurements near a nuclear resonance reveal the complete vibrational spectrum of the probe nucleus. Because of this, nuclear resonance vibrational spectroscopy (NRVS) is a uniquely quantitative probe of the vibrational dynamics of reactive iron sites in proteins and other complex molecules. Our measurements of vibrational fundamentals have revealed both frequencies and amplitudes of ⁵⁷Fe vibrations in proteins and model compounds. Information on the direction of Fe motion has also been obtained from measurements on oriented single crystals, and provides an essential test of normal mode predictions. Here, we report the observation of weaker two-quantum vibrational excitations (overtones and combinations) for compounds that mimic the active site of heme proteins. The predicted intensities depend strongly on the direction of Fe motion. We compare the observed features with predictions based on the observed fundamentals, using information on the direction of Fe motion obtained either from DFT predictions or from single crystal measurements. Two-quantum excitations may become a useful tool to identify the directions of the Fe oscillations when single crystals are not available.     

Two-quantum photoemission yield spectrum of silicon

We report the first two-quantum photoemission yield spectrum on silicon (111). Its general behaviour and characteristic features are discussed with reference to one-photon photoemission processes and linear optical properties.     

Vibrational dynamics of ions in glass from fifth-order two-dimensional infrared spectroscopy

The vibrational dynamics of the first four antisymmetric stretch vibrational levels of azide in an ionic glass have been measured and correlated using a heterodyned fifth-order two-dimensional infrared pulse sequence. By rephasing a two-quantum coherence, a process not possible with third-order spectroscopy, solvent effects on the frequencies and anharmonicities of the potential energy surface are measured. Fifth-order pulse sequences are another step towards precisely controlling vibrational coherence in analogy to the manipulation of spins in NMR but with ultrafast time resolution.     

Canonical dressing in the multimode two-quantum Jaynes-Cummings model

Based upon the hidden Lie SU(1,1) symmetry, we have constructed the unitary decoupling transformation which diagonalizes the multimode two-quantum Jaynes-Cummings model and provides us with an extremely convenient basis to gain a deeper understanding of the dressing processes present in the matter-field interaction. This canonical transformation approach is very simple and can be easily extended to other generalized Jaynes-Cummings models. Received: 5 July 1997 / Revised: 3 November 1997 / Accepted: 14 November 1997     

Searching for evolutions from pure states into mixed states with entangled neutral kaons

Entangled two-quantum states may be a sensitive probe for a loss of quantum coherence due to apparent violations of quantum mechanics, e.g. as caused by gravitation. We show that there exists a modest experiment sensitive to any one of the nine phenomenological parameters which describe decoherence in the neutral kaon system.Received: 14 March 2003, Published online: 26 November 2003     

Manifestations of the two-quantum photoeffect and photon statistics in the photoelectron multiplier pulse amplitude distribution

The contribution of the two-quantum photoeffect to the pulse amplitude distribution at the output of a photomultiplier is considered. An expression generalizing the Mandel formula is derived that takes into account the second-order photoeffect. The influence of a temporal and spatial coherency of the radiation field on the photomultiplier count statistics is studied. Possible applications of the obtained results to determining statistical characteristics of the optical fields are discussed.     

The possibility of generating and receiving gravitational beams

We consider the possibility of creating a super-radiative gravitational state and a nonradiative electromagnetic state in a system of N-particles with a discrete spectrum using laser techniques and the excitation of particles in a two-quantum regime.We estimate the parameters and explain the requirements for systems which can generate observable powers of coherent gravitational waves in optical and gamma frequencies.We also describe the basic diagram for a receiver of a coherent gravitational beam.     

Efficient propagation of polarization from laser photons to positrons through compton scattering and electron-positron pair creation

We have demonstrated for the first time the production of highly polarized short-pulse positrons with a finite energy spread in accordance with a new scheme that consists of two-quantum processes, such as inverse Compton scattering and electron-positron pair creation. Using a circularly polarized laser beam of 532 nm scattered off a high-quality, 1.28 GeV electron beam, we have obtained polarized positrons with an intensity of 2 x 10(4) e+ /bunch. The magnitude of positron polarization has been determined to be 73 +/- 15(stat) +/- 19(syst)% by means of a newly designed positron polarimeter.     

Identification of the Amplification Mechanism in the First Free-Electron Laser as Net Stimulated Free-Electron Two-Quantum Stark Emission

We find that the electron phase with respect to the incident laser radiation must be random in the first freeelectron laser （FEL） and, hence, the incident laser radiation works as a relaxation force to keep a Maxwellian distribution. We formulate the threshold laser intensity for amplification which agrees with the measured value in the order of magnitude in the first FEL. The magnetic wiggler must produce an electric wiggler whose period is the same as that of the magnetic wiggler. We find that net stimulated free-electron two-quantum Stark （FETQS） emission driven by this electric wiggler is the mechanism responsible for the measured gain and the measured laser intensity at the plateau in the first FEL.     

Quantum computation with vibrationally excited molecules

A new physical implementation for quantum computation is proposed. The vibrational modes of molecules are used to encode qubit systems. Global quantum logic gates are realized using shaped femtosecond laser pulses which are calculated applying optimal control theory. The scaling of the system is favorable; sources for decoherence can be eliminated. A complete set of one- and two-quantum gates is presented for a specific molecule. Detailed analysis regarding experimental realization shows that the structural resolution of today's pulse shapers is easily sufficient for pulse formation.     

On determination of effective mass of the delocalized positronium in NaCl crystals

The angular correlation of the photons of two-quantum annihilation in NaCl crystal was measured at temperatures ranging from 77 to 500 K. The data obtained clearly showed a narrow peak which was earlier observed only at low temperatures. The positronium nature of this peak was examined by applying a magnetic field. The positronium effective mass was found to be (1.5±0.2)2 m₀.     

Two-quantum transitions between the fine-structure levels of a hydrogen-like atom

A study is made of the probability of two-quantum spontaneous transitions between fine-structure levels for fixed value of the principal quantum number (the radiation spectrum and the total transition probabilities are calculated) on the basis of the solution of the Dirac equation in a Coulomb field with arbitrary value of the charge of the nucleus.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 7, pp. 20–24, July, 1980.     

Theory of the line shape of gamma-photon transitions

There is a discussion of the line shape for the nuclear two-quantum transition due to the simultaneous absorption of a Mossbauer quantum and a quantum from a classical photon source. The problem is solved through the use of density-matrix equations, and an equation is derived for the intensity of absorbed gamma rays. In contrast with the case of the ordinary probabilistic approach, the equation for the intensity of gamma absorption reveals a dependence on the relaxation times within the ground and excited states. The line shape for gamma-photon transitions for low intensities of the incident radiation usually differs little from the shape of the Mossbauer line. However, at large irradiation intensities, a shift and a broadening of the resonant lines occur, proportional to the radiation power. These corrections must be taken into account in, e.g., gamma-magnetic resonance.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, Vol. 12, No. 7, pp. 24–30, July, 1969.     

Intracavity two-photon polarization spectroscopy on the basis of light-induced peaks of radiation power

A calculation of the selective losses of a spectrometer based on a broad-band laser with an anisotropic three-mirror ring resonator containing a two-photon-absorbing atomic gas medium with a light-induced resonance anisotropy has been performed. The conditions under which laser radiation power resonances appear in the output radiation spectrum and the contribution of different factors to their formation have been revealed. Possible ways of obtaining information on the polarization effects induced by a powerful light wave in a medium at the frequencies of two-quantum transitions were investigated. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 66, No. 1, pp. 48–53, January–February, 1999.     

Positron states in alkali-halide single crystals

Detailed consideration is given to the annihilatory decay of positron states in real alkali-halide single crystals of defective structure. Representations of the exciton-positron states in the matrix of the crystal and close to a lattice defect are analyzed. On the basis of these representations, expressions are derived for the yield of the three-quantum decay process and the intensities of the components contributing to two-quantum annihilation; the expressions agree with existing experimental data. It is shown that the greatest contribution to the three-quantum decay arises from an exciton-orthopositronium state located in the vicinity of the defect.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 10, pp. 76–79, October, 1974.     

Control of a Nonlocal Entanglement in the Micromaser via Two Quanta Non-Linear Processes Induced by?Dynamic Stark Shift

We show that, under certain conditions, the micromaser can act as an effective source of highly correlated atoms. It is possible to create an extended robust entanglement between two successive, initially unentangled atoms passing through a cavity filled with a nonlinear medium taking into consideration a slight level shift. Information is transfered from the cavity to the atoms in order to build up entanglement. The scheme has an advantage over conventional creation of entanglement if the two atoms (qubits) are so far apart that a direct interaction is difficult to achieve. The interaction of the atoms with the micromaser occurs under the influence of a two-quantum transition process. Interesting phenomena are observed, and an extended robust entangled state is obtained for different values of the system parameters. Illustrative variational calculations are performed to demonstrate the effect within an analytically tractable two-qubit model.     

Head-on collision of quantum ion-acoustic solitary waves in a dense electron-positron-ion plasma

The characteristics of the head-on collision between two-quantum ion-acoustic solitary waves (QIASWs) in a dense electron-positron-ion plasma are investigated. Using the extended Poincaré-Lighthill-Kuo (PLK) method, the Korteweg-de Vries (KdV) equations and the analytical phase shifts, after two QIASWs collision occurs, are derived. This study is a first attempt to illustrate the effects of both of the quantum diffraction corrections and the Fermi temperature ratio of positrons to electrons on the phase shifts. It is found that the electron-positron-ion plasma parameters modify significantly the phase shifts of the two colliding solitary waves.