401 research outputs found
Chemputation and the standardization of chemical informatics
The explosion in the use of machine learning for automated chemical reaction optimization is gathering pace. However, the lack of a standard architecture that connects the concept of chemical transformations universally to software and hardware provides a barrier to using the results of these optimizations and could cause the loss of relevant data and prevent reactions from being reproducible or unexpected findings verifiable or explainable. In this Perspective, we describe how the development of the field of digital chemistry or chemputation, that is the universal code-enabled control of chemical reactions using a standard language and ontology, will remove these barriers allowing users to focus on the chemistry and plug in algorithms according to the problem space to be explored or unit function to be optimized. We describe a standard hardware (the chemical processing programming architectureâthe ChemPU) to encompass all chemical synthesis, an approach which unifies all chemistry automation strategies, from solid-phase peptide synthesis, to HTE flow chemistry platforms, while at the same time establishing a publication standard so that researchers can exchange chemical code (ĎDL) to ensure reproducibility and interoperability. Not only can a vast range of different chemistries be plugged into the hardware, but the ever-expanding developments in software and algorithms can also be accommodated. These technologies, when combined will allow chemistry, or chemputation, to follow computationâthat is the running of code across many different types of capable hardware to get the same result every time with a low error rate
Radiation MHD modeling of a proposed dynamic hohlraum
In this paper we report 2D radiation magnetohydrodynamic simulations of a dynamic hohlraum target designed to be driven by the Z accelerator at Sandia National Laboratory, Albuquerque New Mexico. Z generates currents up 20 MA with a rise time of 100 ns and peak electrical power of 40 TW. In this design we attempt to reduce the effects of magneto-Rayleigh Taylor (RT) modes by using a distributed initial density profile. Earlier work showed that ``tailoring`` the initial density profile could reduce the sheath acceleration and the number of e-foldings that the RT instability grows during the implosion . As the sheath moves in radially, fresh material is swept up or ``snow plowed``, providing a back pressure that counters the J x B force. A special profile can be found in which the unstable outer surface of the sheath implodes at constant velocity, reducing the classical growth rate to zero, although residual Richtmeyer-Meshkov type instability (instability of the snow-plow shock front) may be present. In practice, it is hard to create tailored initial density profiles due to the difficulty of machining and otherwise manipulating very low density materials. It becomes easier to manufacture these complex targets as the current, energy and load mass increase with large drivers. Z is the first fast pulse power device with enough energy to consider loads of this type
An autonomous electrochemical discovery robot that utilises probabilistic algorithms: probing the redox behaviour of inorganic materials
The discovery of new electroactive materials is slow due to the large combinatorial chemical space of possible experiments. Efficient exploration of redoxâactive chemical space requires a machine learning assisted robotic platform with realâtime feedback. Here, we developed a closedâloop robotic platform which is capable of synthesis and electrochemical characterisation controlled using a probabilistic algorithm. This was used to probe the redox behaviour of different polyoxometalates (POMs) precursors and explore the formation of redoxâactive coordination complexes. The system can run accurate analytical electrochemical measurements whilst maintaining the performance and accuracy of both the working and reference electrodes. The platform successfully ran and analysed 336 coordination chemistry reactions by performing ca. 2500 cyclic voltammetry (CV) scans for analysis and electrode cleaning. Overall, the platform carried out over 9900 operations in 350 hours at a rate of 28 operations per hour, and we identified 24 complex solutions which showed significantly different redox activity. Experiments were performed using a universal chemical synthesis language (ĎDL) with variable inputs. The platform was used autonomously to investigate a range of POM precursor materials demonstrating 45 % increase in capacitance. The experiments ran for 36 hours with more than 6400 operations during which we analysed 200 POM precursor solutions
Bailing Out the Milky Way: Variation in the Properties of Massive Dwarfs Among Galaxy-Sized Systems
Recent kinematical constraints on the internal densities of the Milky Way's
dwarf satellites have revealed a discrepancy with the subhalo populations of
simulated Galaxy-scale halos in the standard CDM model of hierarchical
structure formation. This has been dubbed the "too big to fail" problem, with
reference to the improbability of large and invisible companions existing in
the Galactic environment. In this paper, we argue that both the Milky Way
observations and simulated subhalos are consistent with the predictions of the
standard model for structure formation. Specifically, we show that there is
significant variation in the properties of subhalos among distinct host halos
of fixed mass and suggest that this can reasonably account for the deficit of
dense satellites in the Milky Way. We exploit well-tested analytic techniques
to predict the properties in a large sample of distinct host halos with a
variety of masses spanning the range expected of the Galactic halo. The
analytic model produces subhalo populations consistent with both Via Lactea II
and Aquarius, and our results suggest that natural variation in subhalo
properties suffices to explain the discrepancy between Milky Way satellite
kinematics and these numerical simulations. At least ~10% of Milky Way-sized
halos host subhalo populations for which there is no "too big to fail" problem,
even when the host halo mass is as large as M_host = 10^12.2 h^-1 M_sun.
Follow-up studies consisting of high-resolution simulations of a large number
of Milky Way-sized hosts are necessary to confirm our predictions. In the
absence of such efforts, the "too big to fail" problem does not appear to be a
significant challenge to the standard model of hierarchical formation.
[abridged]Comment: 12 pages, 3 figures; accepted by JCAP. Replaced with published
versio
An integrated self-optimizing programmable chemical synthesis and reaction engine
Robotic platforms for chemistry are developing rapidly but most systems are not currently able to adapt to changing circumstances in real-time. We present a dynamically programmable system capable of making, optimizing, and discovering new molecules which utilizes seven sensors that continuously monitor the reaction. By developing a dynamic programming language, we demonstrate the 10-fold scale-up of a highly exothermic oxidation reaction, end point detection, as well as detecting critical hardware failures. We also show how the use of in-line spectroscopy such as HPLC, Raman, and NMR can be used for closed-loop optimization of reactions, exemplified using Van Leusen oxazole synthesis, a four-component Ugi condensation and manganese-catalysed epoxidation reactions, as well as two previously unreported reactions, discovered from a selected chemical space, providing up to 50% yield improvement over 25â50 iterations. Finally, we demonstrate an experimental pipeline to explore a trifluoromethylations reaction space, that discovers new molecules
Quantum dots coordinated with conjugated organic ligands: new nanomaterials with novel photophysics
CdSe quantum dots functionalized with oligo-(phenylene vinylene) (OPV) ligands (CdSe-OPV nanostructures) represent a new class of composite nanomaterials with significantly modified photophysics relative to bulk blends or isolated components. Single-molecule spectroscopy on these species have revealed novel photophysics such as enhanced energy transfer, spectral stability, and strongly modified excited state lifetimes and blinking statistics. Here, we review the role of ligands in quantum dot applications and summarize some of our recent efforts probing energy and charge transfer in hybrid CdSe-OPV composite nanostructures
Search for a W' boson decaying to a bottom quark and a top quark in pp collisions at sqrt(s) = 7 TeV
Results are presented from a search for a W' boson using a dataset
corresponding to 5.0 inverse femtobarns of integrated luminosity collected
during 2011 by the CMS experiment at the LHC in pp collisions at sqrt(s)=7 TeV.
The W' boson is modeled as a heavy W boson, but different scenarios for the
couplings to fermions are considered, involving both left-handed and
right-handed chiral projections of the fermions, as well as an arbitrary
mixture of the two. The search is performed in the decay channel W' to t b,
leading to a final state signature with a single lepton (e, mu), missing
transverse energy, and jets, at least one of which is tagged as a b-jet. A W'
boson that couples to fermions with the same coupling constant as the W, but to
the right-handed rather than left-handed chiral projections, is excluded for
masses below 1.85 TeV at the 95% confidence level. For the first time using LHC
data, constraints on the W' gauge coupling for a set of left- and right-handed
coupling combinations have been placed. These results represent a significant
improvement over previously published limits.Comment: Submitted to Physics Letters B. Replaced with version publishe
Search for the standard model Higgs boson decaying into two photons in pp collisions at sqrt(s)=7 TeV
A search for a Higgs boson decaying into two photons is described. The
analysis is performed using a dataset recorded by the CMS experiment at the LHC
from pp collisions at a centre-of-mass energy of 7 TeV, which corresponds to an
integrated luminosity of 4.8 inverse femtobarns. Limits are set on the cross
section of the standard model Higgs boson decaying to two photons. The expected
exclusion limit at 95% confidence level is between 1.4 and 2.4 times the
standard model cross section in the mass range between 110 and 150 GeV. The
analysis of the data excludes, at 95% confidence level, the standard model
Higgs boson decaying into two photons in the mass range 128 to 132 GeV. The
largest excess of events above the expected standard model background is
observed for a Higgs boson mass hypothesis of 124 GeV with a local significance
of 3.1 sigma. The global significance of observing an excess with a local
significance greater than 3.1 sigma anywhere in the search range 110-150 GeV is
estimated to be 1.8 sigma. More data are required to ascertain the origin of
this excess.Comment: Submitted to Physics Letters
Measurement of the Lambda(b) cross section and the anti-Lambda(b) to Lambda(b) ratio with Lambda(b) to J/Psi Lambda decays in pp collisions at sqrt(s) = 7 TeV
The Lambda(b) differential production cross section and the cross section
ratio anti-Lambda(b)/Lambda(b) are measured as functions of transverse momentum
pt(Lambda(b)) and rapidity abs(y(Lambda(b))) in pp collisions at sqrt(s) = 7
TeV using data collected by the CMS experiment at the LHC. The measurements are
based on Lambda(b) decays reconstructed in the exclusive final state J/Psi
Lambda, with the subsequent decays J/Psi to an opposite-sign muon pair and
Lambda to proton pion, using a data sample corresponding to an integrated
luminosity of 1.9 inverse femtobarns. The product of the cross section times
the branching ratio for Lambda(b) to J/Psi Lambda versus pt(Lambda(b)) falls
faster than that of b mesons. The measured value of the cross section times the
branching ratio for pt(Lambda(b)) > 10 GeV and abs(y(Lambda(b))) < 2.0 is 1.06
+/- 0.06 +/- 0.12 nb, and the integrated cross section ratio for
anti-Lambda(b)/Lambda(b) is 1.02 +/- 0.07 +/- 0.09, where the uncertainties are
statistical and systematic, respectively.Comment: Submitted to Physics Letters
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