Bright bichromatic entanglement and quantum dynamics of sum frequency generation

We investigate the quantum properties of the well-known process of sum frequency generation, showing that it is potentially a very useful source of non-classical states of the electromagnetic field, some of which are not possible with the more common techniques. We show that it can produce quadrature squeezed light, bright bichromatic entangled states and symmetric and asymmetric demonstrations of the Einstein-Podolsky-Rosen paradox. We also show that the semiclassical equations totally fail to describe the mean-field dynamics when the cavity is strongly pumped

Quantum ultra-cold atomtronics

It is known that a semi-classical analysis is not always adequate for atomtronics devices, but that a fully quantum analysis is often necessary to make reliable predictions. While small numbers of atoms at a small number of sites are tractable using the density matrix, a fully quantum analysis is often not straightforward as the system becomes larger. We show that the fully quantum positive-P representation is then a viable calculational tool. We postulate an atomtronic phase-gate consisting of four wells in a Bose-Hubbard configuration, for which the semi-classical dynamics are controllable using the phase of the atomic mode in one of the wells. We show that the quantum predictions of the positive-P representation for the performance of this device have little relation to those found semi-classically, and that the performance depends markedly on the actual quantum states of the initially occupied modes. We find that initial coherent states lead to closest to classical dynamics, but that initial Fock states give results that are quite different. A fully quantum analysis also opens the door for deeply quantum atomtronics, in which properties such as entanglement and EPR (Einstein-Podolsky-Rosen) steering become valuable technical properties of a device.Comment: 12 pages, 6 figures, submitted to Phys. Rev

A quantum correlated twin atom laser from a Bose-Hubbard system

We propose and evaluate a method to construct a quantum correlated twin atom laser using a pumped and damped Bose-Hubbard inline trimer which can operate in a stationary regime. With pumping via a source condensate filling the middle well and damping using either an electron beam or optical means at the two end wells, we show that bipartite quantum correlations build up between the ends of the chain, and that these can be measured either in situ or in the outcoupled beams. While nothing similar to our system has yet been achieved experimentally, recent advances mean that it should be practically realisable in the near future.Comment: 15 pages, 8 figures, theory. Typos fixed and material added to introductio

Self-Assembly of Globular Protein Block Copolymers

Protein-based materials show a great deal of potential as catalysts, sensors, and optoelectronics, where the unique efficiency, selectivity, or activity of enzymes can be captured to improve the performance of these devices. However, careful control over the structure and orientation of the protein in three dimensions is required to improve transport through the devices, increase the density of active sites, and optimize the stability of the protein. We demonstrate self-assembly of globular protein-polymer conjugates into nanostructured phases as an elegant and simple method for structural control in bioelectronics. These conjugates may be conceptualized as deblock copolymers, where the first block is the globular protein and the second block is the synthetic polymer. In order to fundamentally investigate self-assembly in these complex block copolymer systems, a mutant of the red fluorescent protein mCherry was expressed in E. coli and site-specifically conjugated to a low polydispersity poly(N-isopropyl acrylamide) (PNIPAM) block using thiol-maleimide coupling to form a well-defined model globular protein-polymer diblock copolymer. Functional protein materials are obtained by solvent evaporation in order to access different pathways toward self-assembly using polymer-selective, non-selective, and protein-selective solvents. Similarly, solvent annealing using these different conditions is exploited as a means to both improve ordering and explore the thermodynamic stability of the ascast nanostructures. Small angle X-ray scattering and transmission electron microscopy are used to explore the dependence of nanostructure formation on processing conditions and the molecular weight of the PNIPAM block. Wide angle X-ray scattering demonstrates that diblock copolymer self-assembly results in a noncrystalline structure within the protein nanodomains. Circular dichroism, UV/Vis spectroscopy, and Fourier transform infra-red (FTIR) spectroscopy show that a large fraction of the protein remains in its folded and active state after conjugation. The effect of coil fraction and hydrogen bonding additives on maintaining protein activity within nanostructured phases is also explored, demonstrating methods for fabricating structures with both a high protein density and a high fraction of active protein. The effect of plasticizing additives on thermal and chemical stability was also explored, illustrating the ability of these materials to dramatically enhance the stability of proteins in polymeric materials. Phase diagrams for these materials have been prepared as a function of coil fraction and water content in the materials, providing insight into the type of self-assembled nanostructures that may be formed. Small-angle light scattering allows quantitative measurement of solvent-mediated interactions between the different components of the diblock copolymers, enabling a fundamental understanding of the relationship between molecular interactions and self-assembly. In addition, comparison of mCherry-b-PNIPAM diblocks with diblocks that incorporate green fluorescent protein (GFP-b-PNIPAM) enables the effects of protein shape and protein-protein interactions in these systems to be understood. Together, these results begin to lay a foundation for understanding the general principles of self-assembly in block copolymers containing globular proteins

Mesoscopic dynamical differences from quantum state preparation in a Bose-Hubbard trimer

Conventional wisdom is that quantum effects will tend to disappear as the number of quanta in a system increases, and the evolution of a system will become closer to that described by mean field classical equations. In this letter we combine newly developed experimental techniques to propose and analyse an experiment using a Bose-Hubbard trimer where the opposite is the case. We find that differences in the preparation of a centrally evacuated trimer can lead to readily observable differences in the subsequent dynamics which increase with system size. Importantly, these differences can be detected by the simple measurements of atomic number.Comment: 5 pages, 4 figures, theor

Tripartite entanglement from interlinked χ(2)\chi^{(2)} parametric interactions

We examine the tripartite entanglement properties of an optical system using interlinked $\chi^{(2)}$ interactions, recently studied experimentally in terms of its phase-matching properties by Bondani et al [M. Bondani, A. Allevi, E. Gevinti, A. Agliati, and A. Andreoni, arXiv:quant-ph/0604002.]. We show that the system does produce output modes which are genuinely tripartite entangled and that detection of this entanglement depends crucially on the correlation functions which are measured, with a three-mode Einstein-Podolsky-Rosen inequality being the most sensitive.Comment: 15 pages, 5 figure

Bright tripartite entanglement in triply concurrent parametric oscillation

We show that a novel optical parametric oscillator, based on concurrent $\chi^{(2)}$ nonlinearities, can produce, above threshold, bright output beams of macroscopic intensities which exhibit strong tripartite continuous-variable entanglement. We also show that there are {\em two} ways that the system can exhibit a new three-mode form of the Einstein-Podolsky-Rosen paradox, and calculate the extra-cavity fluctuation spectra that may be measured to verify our predictions.Comment: title change, expanded intro and discussion of experimental aspects, 1 new figure. Conclusions unaltere

Phase-space analysis of bosonic spontaneous emission

We present phase-space techniques for the modelling of spontaneous emission in two-level bosonic atoms. The positive-P representation is shown to give a full and complete description and can be further developed to give exact treatments of the interaction of degenerate bosons with the electromagnetic field in a given experimental situation. The Wigner representation, even when truncated at second order, is shown to need a doubling of the phase-space to allow for a positive-definite diffusion matrix in the appropriate Fokker-Planck equation and still fails to agree with the full quantum results of the positive-P representation. We show that quantum statistics and correlations between the ground and excited states affect the dynamics of the emission process, so that it is in general non-exponential.Comment: 16 pages, 6 figure

Efficient Synthesis of Narrowly Dispersed Brush Copolymers and Study of Their Assemblies: The Importance of Side Chain Arrangement

Efficient, one-pot preparation of synthetically challenging, high molecular weight (MW), narrowly dispersed brush block copolymers and random copolymers in high conversions was achieved by ring-opening metathesis (co)polymerization (ROMP) of various macromonomers (MMs) using the highly active, fast-initiating ruthenium olefin metathesis catalyst (H_2IMes)(pyr)_2(Cl)_2RuCHPh. A series of random and block copolymers were prepared from a pair of MMs containing polylactide (PLA) and poly(n-butyl acrylate) (PnBA) side chains at similar MWs. Their self-assembly in the melt state was studied by small-angle X-ray scattering (SAXS) and atomic force microscopy (AFM). In brush random copolymers containing approximately equal volume fractions of PLA and PnBA, the side chains segregate into lamellae with domain spacing of 14 nm as measured by SAXS, which was in good agreement with the lamellar thickness measured by AFM. The domain spacings and order−disorder transition temperatures of brush random copolymers were insensitive to the backbone length. In contrast, brush block copolymers containing approximately equal volume fractions of these MMs self-assembled into highly ordered lamellae with domain spacing over 100 nm. Their assemblies suggested that the brush block copolymer backbone adopted an extended conformation in the ordered state