Automatic Chemical Design Using a Data-Driven Continuous Representation of Molecules.

We report a method to convert discrete representations of molecules to and from a multidimensional continuous representation. This model allows us to generate new molecules for efficient exploration and optimization through open-ended spaces of chemical compounds. A deep neural network was trained on hundreds of thousands of existing chemical structures to construct three coupled functions: an encoder, a decoder, and a predictor.

An Alternative Host Material for Long-Lifespan Blue Organic Light-Emitting Diodes Using Thermally Activated Delayed Fluorescence.

It has been challenging to find stable blue organic light emitting diodes (OLEDs) that rely on thermally activated delayed fluorescence (TADF). Lack of stable host materials well-fitted to the TADF emitters is one of the critical reasons. The most popular host for blue TADF, bis[2-(diphenylphosphino)phenyl] ether oxide (DPEPO), leads to unrealistically high maximum external quantum efficiency.

Design of efficient molecular organic light-emitting diodes by a high-throughput virtual screening and experimental approach.

Virtual screening is becoming a ground-breaking tool for molecular discovery due to the exponential growth of available computer time and constant improvement of simulation and machine learning techniques. We report an integrated organic functional material design process that incorporates theoretical insight, quantum chemistry, cheminformatics, machine learning, industrial expertise, organic synthesis, molecular characterization, device fabrication and optoelectronic testing. After exploring a search space of 1.

A kinetic and thermochemical database for organic sulfur and oxygen compounds.

Potential energy surfaces and reaction kinetics were calculated for 40 reactions involving sulfur and oxygen. This includes 11 H2O addition, 8 H2S addition, 11 hydrogen abstraction, 7 beta scission, and 3 elementary tautomerization reactions, which are potentially relevant in the combustion and desulfurization of sulfur compounds found in various fuel sources. Geometry optimizations and frequencies were calculated for reactants and transition states using B3LYP/CBSB7, and potential energies were calculated using CBS-QB3 and CCSD(T)-F12a/VTZ-F12.

Reaction of phenyl radical with propylene as a possible source of indene and other polycyclic aromatic hydrocarbons: an ab initio/RRKM-ME study.

Ab initio G3(MP2,CC)//B3LYP/6-311G** calculations have been performed to investigate the potential energy surface (PES) and mechanism of the reaction of phenyl radical with propylene followed by kinetic RRKM-ME calculations of rate constants and product branching ratios at various temperatures and pressures. The reaction can proceed either by direct hydrogen abstraction producing benzene and three C(3)H(5) radicals [1-propenyl (CH(3)CHCH), 2-propenyl (CH(3)CCH(2)), and allyl (CH(2)CHCH(2))] or by addition of phenyl to the CH or CH(2) units of propylene followed by rearrangements on the C(9)H(11) PES producing nine different products after H or CH(3) losses. The H abstraction channels are found to be kinetically preferable at temperatures relevant to combustion and to contribute 55-75% to the total product yield in the 1000-2000 K temperature range, with the allyl radical being the major product (~45%).

Crossed beam reaction of phenyl and D5-phenyl radicals with propene and deuterated counterparts--competing atomic hydrogen and methyl loss pathways.

We conducted the crossed molecular beams reactions of the phenyl and D5-phenyl radicals with propylene together with its partially deuterated reactants at collision energies of ~45 kJ mol(-1) under single collision conditions. The scattering dynamics were found to be indirect and were mainly dictated by an addition of the phenyl radical to the sterically accessible CH(2) unit of the propylene reactant. The resulting doublet radical isomerized to multiple C(9)H(11) intermediates, which were found to be long-lived, decomposing in competing methyl group loss and atomic hydrogen loss pathways with the methyl group loss leading to styrene (C(6)H(5)C(2)H(3)) and the atomic hydrogen loss forming C(9)H(10) isomers cis/trans 1-phenylpropene (CH(3)CHCHC(6)H(5)) and 3-phenylpropene (C(6)H(5)CH(2)C(2)H(3)).

Accurate coupled cluster calculations of the reaction barrier heights of two CH3* + CH4 reactions.

We have computed barrier heights of 71.8 +/- 2.0 and 216.

Accurate benchmark calculation of the reaction barrier height for hydrogen abstraction by the hydroperoxyl radical from methane. Implications for C(n)H(2n+2) where n = 2 --> 4.

The CH4 + HO2(*) reaction is studied by using explicitly correlated coupled-cluster theory with singles and doubles (CCSD-R12) in a large 19s14p8d6f4g3h basis (9s6p4d3f for H) to approach the basis-set limit at the coupled-cluster singles-doubles level. A correction for connected triple excitations is obtained from the conventional CCSD(T) coupled-cluster approach in the correlation-consistent quintuple-zeta basis (cc-pV5Z). The highly accurate results for the methane reaction are used to calibrate the calculations of the hydroperoxyl-radical hydrogen abstraction from other alkanes.

Density Functional Theory Study of the Formation of Naphthalene and Phenanthrene from Reactions of Phenyl with Vinyl- and Phenylacetylene.

Reaction pathways for polycyclic aromatic hydrocarbon growth from reactions of either vinyl- or phenylacetylene with a phenyl radical are proposed and investigated using density functional theory (DFT). B3LYP/TZVP calculations are performed to obtain structures of minima and saddle points as well as kinetic data, supplemented with BMK/TZVP single-point energy calculations. The pathways include a cis-trans isomerization via a radicalic four-membered ring intermediate, which has so far not been considered in the literature.