Inferring Chemical Reaction Patterns Using Rule Composition in Graph Grammars

Modeling molecules as undirected graphs and chemical reactions as graph rewriting operations is a natural and convenient approach tom odeling chemistry. Graph grammar rules are most naturally employed to model elementary reactions like merging, splitting, and isomerisation of molecules. It is often convenient, in particular in the analysis of larger systems, to summarize several subsequent reactions into a single composite chemical reaction. We use a generic approach for composing graph grammar rules to define a chemically useful rule compositions. We iteratively apply these rule compositions to elementary transformations in order to automatically infer complex transformation patterns. This is useful for instance to understand the net effect of complex catalytic cycles such as the Formose reaction. The automatically inferred graph grammar rule is a generic representative that also covers the overall reaction pattern of the Formose cycle, namely two carbonyl groups that can react with a bound glycolaldehyde to a second glycolaldehyde. Rule composition also can be used to study polymerization reactions as well as more complicated iterative reaction schemes. Terpenes and the polyketides, for instance, form two naturally occurring classes of compounds of utmost pharmaceutical interest that can be understood as "generalized polymers" consisting of five-carbon (isoprene) and two-carbon units, respectively

Generic Strategies for Chemical Space Exploration

Computational approaches to exploring "chemical universes", i.e., very large sets, potentially infinite sets of compounds that can be constructed by a prescribed collection of reaction mechanisms, in practice suffer from a combinatorial explosion. It quickly becomes impossible to test, for all pairs of compounds in a rapidly growing network, whether they can react with each other. More sophisticated and efficient strategies are therefore required to construct very large chemical reaction networks. Undirected labeled graphs and graph rewriting are natural models of chemical compounds and chemical reactions. Borrowing the idea of partial evaluation from functional programming, we introduce partial applications of rewrite rules. Binding substrate to rules increases the number of rules but drastically prunes the substrate sets to which it might match, resulting in dramatically reduced resource requirements. At the same time, exploration strategies can be guided, e.g. based on restrictions on the product molecules to avoid the explicit enumeration of very unlikely compounds. To this end we introduce here a generic framework for the specification of exploration strategies in graph-rewriting systems. Using key examples of complex chemical networks from sugar chemistry and the realm of metabolic networks we demonstrate the feasibility of a high-level strategy framework. The ideas presented here can not only be used for a strategy-based chemical space exploration that has close correspondence of experimental results, but are much more general. In particular, the framework can be used to emulate higher-level transformation models such as illustrated in a small puzzle game

Observation of spatial quantum correlations induced by multiple scattering of non-classical light

We present the experimental realization of spatial quantum correlations of photons that are induced by multiple scattering of squeezed light. The quantum correlation relates photons propagating along two different light trajectories through the random medium and is infinite in range. Both positive and negative spatial quantum correlations are observed when varying the quantum state incident to the multiple scattering medium, and the magnitude of the correlations is controlled by the number of photons. The experimental results are in excellent agreement with recent theoretical proposals by implementing the full quantum model of multiple scattering

Hybrid quantum information processing

The development of quantum information processing has traditionally followed two separate and not immediately connected lines of study. The main line has focused on the implementation of quantum bit (qubit) based protocols whereas the other line has been devoted to implementations based on high-dimensional Gaussian states (such as coherent and squeezed states). The separation has been driven by the experimental difficulty in interconnecting the standard technologies of the two lines. However, in recent years, there has been a significant experimental progress in refining and connecting the technologies of the two fields which has resulted in the development and experimental realization of numerous new hybrid protocols. In this Review, we summarize these recent efforts on hybridizing the two types of schemes based on discrete and continuous variables.Comment: 13 pages, 6 figure

Raman-induced limits to efficient squeezing in optical fibers

We report new experiments on polarization squeezing using ultrashort photonic pulses in a single pass of a birefringent fiber. We measure what is to our knowledge a record squeezing of -6.8 +/- 0.3 dB in optical fibers which when corrected for linear losses is -10.4 +/- 0.8 dB. The measured polarization squeezing as a function of optical pulse energy, which spans a wide range from 3.5-178.8 pJ, shows a very good agreement with the quantum simulations and for the first time we see the experimental proof that Raman effects limit and reduce squeezing at high pulse energy.Comment: 3 pages, 3 figure

Continuous-wave spatial quantum correlations of light induced by multiple scattering

We present theoretical and experimental results on spatial quantum correlations induced by multiple scattering of nonclassical light. A continuous mode quantum theory is derived that enables determining the spatial quantum correlation function from the fluctuations of the total transmittance and reflectance. Utilizing frequency-resolved quantum noise measurements, we observe that the strength of the spatial quantum correlation function can be controlled by changing the quantum state of an incident bright squeezed-light source. Our results are found to be in excellent agreement with the developed theory and form a basis for future research on, e.g., quantum interference of multiple quantum states in a multiple scattering medium.Comment: 8 pages, 6 figure