Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

Citation: Pullen, M. G., Wolter, B., Le, A. T., Baudisch, M., Sclafani, M., Pires, H., . . . Biegert, J. (2016). Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets. Nature Communications, 7, 6. doi:10.1038/ncomms11922The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as pi(g)) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O-2 and C2H2 molecules, with pi(g) and pi(u) symmetries, respectively, and where their ionization probabilities do not maximize along their molecular axes. While this removes a serious bottleneck for laser-induced diffraction imaging, we find unexpectedly strong backscattering contributions from low-Z atoms

Polyatomic Molecular Structure Retrieval using Laser-Induced Electron Diffraction

Laser-induced electron diffraction is a developing dynamical imaging technique that is already able to probe molecular dynamics at few-femtosecond temporal resolutions and has the potential to reach the sub-femtosecond level. Here we provide the recipe for the extension of the technique to polyatomic molecules and we demonstrate the method by extracting the structure of aligned and anti-aligned acetylene (C₂H₂). We show that multiple bond lengths can be simultaneously imaged at high accuracy including elusive hydrogen containing bonds. Our results open the door to the investigation of larger complex molecules and the realization of a true molecular movie

Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene

Visualizing chemical reactions as they occur requires atomic spatial and femtosecond temporal resolution. Here, we report imaging of the molecular structure of acetylene (C2H2) 9 femtoseconds after ionization. Using mid-infrared laser–induced electron diffraction (LIED), we obtained snapshots as a proton departs the [C2H2]2+ ion. By introducing an additional laser field, we also demonstrate control over the ultrafast dissociation process and resolve different bond dynamics for molecules oriented parallel versus perpendicular to the LIED field. These measurements are in excellent agreement with a quantum chemical description of field-dressed molecular dynamicsPostprint (author's final draft

Polyatomic Molecular Structure Retrieval using Laser-Induced Electron Diffraction

Laser-induced electron diffraction is a developing dynamical imaging technique that is already able to probe molecular dynamics at few-femtosecond temporal resolutions and has the potential to reach the sub-femtosecond level. Here we provide the recipe for the extension of the technique to polyatomic molecules and we demonstrate the method by extracting the structure of aligned and anti-aligned acetylene (C₂H₂). We show that multiple bond lengths can be simultaneously imaged at high accuracy including elusive hydrogen containing bonds. Our results open the door to the investigation of larger complex molecules and the realization of a true molecular movie

Towards a verified compiler prototype for the synchronous language SIGNAL

International audienceSIGNAL belongs to the synchronous languages family which are widely used in the design of safety-critical real-time systems such as avionics, space systems, and nuclear power plants. This paper reports a compiler prototype for SIGNAL. Compared with the existing SIGNAL compiler, we propose a new intermediate representation (named S-CGA, a variant of clocked guarded actions), to integrate more synchronous programs into our compiler prototype in the future. The front-end of the compiler, i.e., the translation from SIGNAL to S-CGA, is presented. As well, the proof of semantics preservation is mechanized in the theorem prover Coq. Moreover, we present the back-end of the compiler, including sequential code generation and multithreaded code generation with time-predictable properties. With the rising importance of multi-core processors in safety-critical embedded systems or cyber-physical systems (CPS), there is a growing need for model-driven generation of multithreaded code and thus mapping on multi-core. We propose a time-predictable multi-core architecture model in architecture analysis and design language (AADL), and map the multi-threaded code to this model

The maintenance gap: a new theoretical perspective on the evolution of aging

One of the prevailing theories of aging, the disposable soma theory, views aging as the result of the accumulation of damage through imperfect maintenance. Aging, then, is explained from an evolutionary perspective by asserting that this lack of maintenance exists because the required resources are better invested in reproduction. However, the amount of maintenance necessary to prevent aging, ‘maintenance requirement’ has so far been largely neglected and has certainly not been considered from an evolutionary perspective. To our knowledge we are the first to do so, and arrive at the conclusion that all maintenance requirement needs an evolutionary explanation. Increases in maintenance requirement can only be selected for if these are linked with either higher fecundity or better capabilities to cope with environmental challenges to the integrity of the organism. Several observations are suggestive of the latter kind of trade-off, the existence of which leads to the inevitable conclusion that the level of maintenance requirement is in principle unbound. Even the allocation of all available resources to maintenance could be unable to stop aging in some organisms. This has major implications for our understanding of the aging process on both the evolutionary and the mechanistic level. It means that the expected effect of measures to reallocate resources to maintenance from reproduction may be small in some species. We need to have an idea of how much maintenance is necessary in the first place. Our explorations of how natural selection is expected to act on the maintenance requirement provides the first step in understanding this

Model theory of finite and pseudofinite groups

This is a survey, intended both for group theorists and model theorists, concerning the structure of pseudofinite groups, that is, infinite models of the first-order theory of finite groups. The focus is on concepts from stability theory and generalisations in the context of pseudofinite groups, and on the information this might provide for finite group theory

The diversity of population responses to environmental change

This is the final version. Available from Wiley via the DOI in this record.Data available from the Dryad Digital Repository: https:// doi.org/10.5061/dryad.d5f54s7The current extinction and climate change crises pressure us to predict population dynamics with ever-greater accuracy. Although predictions rest on the well-advanced theory of age-structured populations, two key issues remain poorly explored. Specifically, how the age-dependency in demographic rates and the year-to-year interactions between survival and fecundity affect stochastic population growth rates. We use inference, simulations and mathematical derivations to explore how environmental perturbations determine population growth rates for populations with different age-specific demographic rates and when ages are reduced to stages. We find that stage- vs. age-based models can produce markedly divergent stochastic population growth rates. The differences are most pronounced when there are survival-fecundity-trade-offs, which reduce the variance in the population growth rate. Finally, the expected value and variance of the stochastic growth rates of populations with different age-specific demographic rates can diverge to the extent that, while some populations may thrive, others will inevitably go extinct.Max Planck Society, Marie Curie FellowshipERCGerman Research FoundationSwiss National Science FoundationNational Science FoundationNational Institute of AgingRamon y Cajal Research GrantWenner-Gren FoundationLeakey FoundationNational Geographic SocietyZoological Society of San DiegoUniversity of PennsylvaniaArgentinean National Council of Researc