Quantum statistics of degenerate four wave mixing

A microscopic model of degenerate four wave mixing including the quantisation of the atomic medium is analysed. In the limits of large detuning, low saturation and zero loss, ideal squeezing in the output field is possible. The effect of nonoptimal conditions is analysed.     

Mutually disjoint families of 0–1 sequences

Obtain a family of infinite binary sequences by fixing k positions each with 0 or 1 and allowing the nonfixed positions to vary over {0,1}. The object of this note is to find the maximum number of pairwise disjoint families and to determine the maximum possible number of distinct fixed positions. Extensions to n-ary infinite sequences will also be discussed.     

Incompatibility of macroscopic local realism with quantum mechanics in measurements with macroscopic uncertainties

We show that quantum mechanics predicts a contradiction with local hidden variable theories for photon number measurements which have limited resolving power, to the point of imposing an uncertainty in the photon number result which is macroscopic in absolute terms. We show how this can be interpreted as a failure of a new premise, macroscopic local realism.     

Continuous variable tripartite entanglement and Einstein-Podolsky-Rosen correlations from triple nonlinearities

We develop three-mode generalizations of the Einstein-Podolsky-Rosen paradox, allowing us to define inequalities which may be used to indicate continuous-variable tripartite entanglement. We use these inequalities and an appropriate version of the previously developed van Loock-Furusawa inequalities to theoretically compare the continuous-variable tripartite entanglement available from the use of three concurrent x ⁽²⁾ nonlinearities and from three independent squeezed states mixed on beamsplitters. The text was submitted by the authors in English.     

Monolithic optical parametric oscillator using chirped quasi-phase matching

We describe a highly efficient monolithic, Q-switched, nanosecond optical parametric oscillator based on a magnesium-oxide-doped periodically poled lithium niobate crystal and containing multiple quasi-phase-matched gratings. The crystal consisted of a single unchirped grating and five gratings containing progressively increasing amounts of longitudinal chirp. The monolithic design makes the device highly compact, stable, and robust, and it demonstrated a pump-to-signal conversion efficiency of around 50%, generating 50 microJ pulses at 1.55 microm with a spectral bandwidth of 20 nm. Sonogram traces are presented showing the effect of crystal chirp on the temporal and spectral performance.     

Electronic structure of adenine and thymine base pairs studied by femtosecond electron-ion coincidence spectroscopy

Femtosecond pump-probe spectroscopy was combined with photoelectron-photoion coincidence detection to investigate the electronic structure and dynamics of isolated adenine (A) and thymine (T) dimers and the adenine-thymine (AT) base pair. The photoelectron spectra show that pipi* and npi* states are only weakly perturbed in the hydrogen-bound dimers as compared to the monomers. For cationic base pairs with internal energies greater than 1 eV, we observed considerable cluster fragmentation into protonated monomers. This process selectively removed signals from the npi* --> n-1 ionization channel in all dimers. The photoelectron spectra are compared to time-resolved mass spectra and confirm the assignment of short-lived pipi* and npi* populations in the adenine, thymine, and mixed AT dimers.     

Identification of protein phosphorylation sites within Ser/Thr-rich cluster domains using site-directed mutagenesis and hybrid linear quadrupole ion trap Fourier transform ion cyclotron resonance mass spectrometry

We describe a method for the analysis of multi-site phosphorylation in serine/threonine (Ser/Thr)-rich protein sequences. Site-specific mutagenesis was used to introduce tryptic cleavage sites in the serine glutamine/threonine glutamine cluster domain (SCD) of the human checkpoint protein kinase (Chk2). The mutant proteins were shown to autophosphorylate on residues that are inducibly phosphorylated when mammalian cells are exposed to ionizing radiation (serine 33/35, serine 516, threonine 68 and threonine 432). Five Ser/Thr clusters within the SCD were flanked by arginine or lysine residues to produce tryptic peptides for nanospray liquid chromatography (nanoLC)/linear quadrupole ion trap Fourier transform ion cyclotron resonance mass spectrometry. Phosphorylation sites were assigned using accurate-mass-driven analysis and interpretation of low-energy collision-induced dissociation spectra acquired in the ion trap. In addition to verifying known phosphorylation sites, seventeen novel sites were identified within the SCD of Chk2. The approach should be applicable to other O-linked post-translational modifications that occur in proteins with Ser/Thr-rich sequences.     

Theory-guided design and synthesis of multichromophore dendrimers: an analysis of the electro-optic effect

Extensive experimental and theoretical study suggests that interchromophore electrostatic interactions are among the most severe impediments to the induction and stability of large electro-optic coefficients in electric-field-poled organic materials. In this report, multichromophore-containing dendritic materials have been investigated as a means to minimize unwanted attenuation of nonlinear optical (electro-optic) activity at high chromophore loading. The dendritic molecular architectures employed were designed to provide optimized molecular scaffolding for electric-field-induced molecular reorientation. Design parameters were based upon past experimental results in conjunction with statistical and quantum mechanical modeling. The electro-optic behavior of these materials was evaluated through experimental and theoretical analysis. Experimental data collected from the dendrimer structures depict a reasonably linear relationship between chromophore number density (N) and electro-optic activity (r(33)) demonstrating a deviation from the dipolar frustration that typically limits r(33) in conventional chromophore/polymer composite materials. The observed linear dependence holds at higher chromophore densities than those that have been found to be practical in systems of organic NLO chromophores dispersed in polymer hosts. Theoretical analysis of these results using Monte Carlo modeling reproduces the experimentally observed trends confirming linear dependence of electro-optic activity on N in the dendrimer materials. These results provide new insight into the ordering behavior of EO dendrimers and demonstrate that the frequently observed asymptotic dependence of electro-optic activity on chromophore number density may be overcome through rational design.     

Nonequilibrium versus equilibrium molecular dynamics studies of solvation dynamics after photoexcitation of OCIO

The results of our earlier work [C. Brooksby, O. V. Prezhdo, and P. J. Reid, J. Chem. Phys. 119, 9111 (2003)] rationalizing the surprisingly weak solvent dependence of the dynamics following photoexcitation of chlorine dioxide in water, chloroform, and cyclohexane are thoroughly tested. Comparisons are made between equilibrium and nonequilibrium solvent response, equilibrium response in the ground and excited electronic states, as well as the cumulant and direct evaluation of the optical response function. In general, the linear response and cumulant approximations are found to hold, although minor deviations are found with all solvents. The ground state, linear response, and cumulant data show best agreement with experiment, most likely due to the better tested ground-state force field and the robust behavior of the linear response and cumulant approximations. The main conclusion of our earlier work explaining the weak solvent dependence by the domination of the van der Waals interaction component remains intact within the more advanced treatments. However, the molecular origin of this surprising experimental observation is different in water and chloroform compared to cyclohexane.