Adaptive Optimization of Chemical Reactions with Minimal Experimental Information

Optimizing reaction conditions depends on expert chemistry knowledge and laborious exploration of reaction parameters. To automate this task and augment chemical intuition, we here report a computational tool to navigate search spaces. Our approach (LabMate.ML) integrates random sampling of 0.03%–0.04% of all search space as input data with an interpretable, adaptive machine-learning algorithm. LabMate.ML can optimize many real-valued and categorical reaction parameters simultaneously, with minimal computational resources and time. In nine prospective proof-of-concept studies pursuing distinctive objectives, we demonstrate how LabMate.ML can identify optimal goal-oriented conditions for several different chemistries and substrates. Double-blind competitions and the conducted expert surveys reveal that its performance is competitive with that of human experts. LabMate.ML does not require specialized hardware, affords quantitative and interpretable reactivity insights, and autonomously formalizes chemical intuition, thereby providing an innovative framework for informed, automated experiment selection toward the democratization of synthetic chemistry.D.R. is a Swiss National Science Foundation Fellow (grant nos. P2EZP3_168827 and P300P2_177833). E.A.H. is supported by the Herchel Smith Fellowship awarded by Williams College. G.J.L.B. is a Royal Society URF (URF\R\180019). T.R. is an Investigador Auxiliar supported by FCT Portugal (CEECIND/00887/2017). T.R. acknowledges the H2020 (TWINN-2017 ACORN, grant no. 807281), FCT/FEDER (02/SAICT/2017, grant no. 28333). D.R. acknowledges the MIT-IBM Watson AI Lab and the MIT SenseTime coalition for funding. The authors are extremely grateful to several colleagues for suggesting Ugi reaction conditions, and to Prof. R. Langer and Prof. G. Traverso, who provided invaluable comments on the research and manuscript. The authors are indebted to Prof. R. Moreira for access to the CEM microwave reactor; Dr. F. Corzana for technical assistance with HRMS; and the 13 graduate students, 17 postdoctoral researchers, and eight principal investigators across Austria, Denmark, Portugal, Spain, the United Kingdom, and the United States who took part in the survey. We thank R. Rodrigues for help in producing Figure 1. The survey was approved by the iMM and MIT (COUHES protocol 1809514426). The authors also thank the four anonymous reviewers for their most insightful comments.info:eu-repo/semantics/publishedVersio

Nucleon-Nucleon Scattering under Spin-Isospin Reversal in Large-N_c QCD

The spin-flavor structure of certain nucleon-nucleon scattering observables derived from the large N_c limit of QCD in the kinematical regime where time-dependent mean-field theory is valid is discussed. In previous work, this regime was taken to be where the external momentum was of order N_c which precluded the study of differential cross sections in elastic scattering. Here it is shown that the regime extends down to order N_c^{1/2} which includes the higher end of the elastic regime. The prediction is that in the large N_c limit, observables describable via mean-field theory are unchanged when the spin and isospin of either nucleon are both flipped. This prediction is tested for proton-proton and neutron-proton elastic scattering data and found to fail badly. We argue that this failure can be traced to a lack of a clear separation of scales between momentum of order N_c^{1/2} and N_c^1 when N_c is as small as three. The situation is compounded by an anomalously low particle production threshold due to approximate chiral symmetry.Comment: 5 pages, 1 figur

Complete Analysis of Baryon Magnetic Moments in 1/N_c

We generate a complete basis of magnetic moment operators for the N_c = 3 ground-state baryons in the 1/N_c expansion, and compute and tabulate all associated matrix elements. We then compare to previous results derived in the literature and predict additional relations among baryon magnetic moments holding to subleading order in 1/N_c and flavor SU(3) breaking. Finally, we predict all unknown diagonal and transition magnetic moments to <= 0.15 mu_N accuracy, and suggest possible experimental measurements to improve the analysis even further.Comment: 28 pages (including 11 tables), ReVTeX. One reference and grant acknowledgment adde

A note on the error analysis of classical Gram-Schmidt

An error analysis result is given for classical Gram--Schmidt factorization of a full rank matrix $A$ into $A=QR$ where $Q$ is left orthogonal (has orthonormal columns) and $R$ is upper triangular. The work presented here shows that the computed $R$ satisfies \normal{R}=\normal{A}+E where $E$ is an appropriately small backward error, but only if the diagonals of $R$ are computed in a manner similar to Cholesky factorization of the normal equations matrix. A similar result is stated in [Giraud at al, Numer. Math. 101(1):87--100,2005]. However, for that result to hold, the diagonals of $R$ must be computed in the manner recommended in this work.Comment: 12 pages This v2. v1 (from 2006) has not the biliographical reference set (at all). This is the only modification between v1 and v2. If you want to quote this paper, please quote the version published in Numerische Mathemati

On the origin and application of the Bruggeman Correlation for analysing transport phenomena in electrochemical systems

The widely used Bruggeman equations correlate tortuosity factors of porous media with their porosity. Finding diverse application from optics to bubble formation, it received considerable attention in fuel cell and battery research, recently. The ability to estimate tortuous mass transport resistance based on porosity alone is attractive, because direct access to the tortuosity factors is notoriously difficult. The correlation, however, has limitations, which are not widely appreciated owing to the limited accessibility of the original manuscript. We retrace Bruggemans derivation, together with its initial assumptions, and comment on validity and limitations apparent from the original work to offer some guidance on its use.<br/

Acceptance test report for the mobile color camera system

The purpose of this report is to present test data recorded during acceptance testing of the Mobile Color Camera System (MCCS)

Tank 241-B-108, cores 172 and 173 analytical results for the final report

The Data Summary Table (Table 3) included in this report compiles analytical results in compliance with all applicable DQOS. Liquid subsamples that were prepared for analysis by an acid adjustment of the direct subsample are indicated by a `D` in the A column in Table 3. Solid subsamples that were prepared for analysis by performing a fusion digest are indicated by an `F` in the A column in Table 3. Solid subsamples that were prepared for analysis by performing a water digest are indicated by a I.wl. or an `I` in the A column of Table 3. Due to poor precision and accuracy in original analysis of both Lower Half Segment 2 of Core 173 and the core composite of Core 173, fusion and water digests were performed for a second time. Precision and accuracy improved with the repreparation of Core 173 Composite. Analyses with the repreparation of Lower Half Segment 2 of Core 173 did not show improvement and suggest sample heterogeneity. Results from both preparations are included in Table 3

Phenomenology of Mirror Fermions in the Littlest Higgs Model with T-Parity

Little Higgs models are an interesting alternative to explain electroweak symmetry breaking without fine-tuning. Supplemented with a discrete symmetry (T-parity) constraints from electroweak precision data are naturally evaded and also a viable dark matter candidate is obtained. T-parity implies the existence of new (mirror) fermions in addition to the heavy gauge bosons of the little Higgs models. In this paper we consider the effects of the mirror fermions on the phenomenology of the littlest Higgs model with T-parity at the LHC. We study the most promising production channels and decay chains for the new particles. We find that the mirror fermions have a large impact on the magnitude of signal rates and on the new physics signatures. Realistic background estimates are given.Comment: 13 p

An AER to CAN Bridge for Spike-Based Robot Control

Address-Event-Representation (AER) is a bio-inspired communication protocol between chips. A set of AER sensors (retina and cochleas), processors (convolvers, WTA, mappers, …) and actuators can be found in the literature that have been specifically designed for mimicking the communication principle in the brain: spikes. The problem when developing complex robots based on AER (or spikes) is to command actuators (motors) directly with spikes. Commercial robots are usually based on commercial standards (CAN) that do not allow powering actuators directly with spikes. This paper presents a co-design FPGA and embedded computer system that implements a bridge between these two protocols: CAN and AER. The bridge has been analyzed under the Spanish project VULCANO1 with an arm robot and a Shadow anthropomorphic hand.Ministerio de Ciencia e Innovación TEC2009-10639-C04-0

A variational analysis of Einstein-scalar field Lichnerowicz equations on compact Riemannian manifolds

We establish new existence and non-existence results for positive solutions of the Einstein-scalar field Lichnerowicz equation on compact manifolds. This equation arises from the Hamiltonian constraint equation for the Einstein-scalar field system in general relativity. Our analysis introduces variational techniques, in the form of the mountain pass lemma, to the analysis of the Hamiltonian constraint equation, which has been previously studied by other methods.Comment: 15 page