The Future of Collaborative Human-Artificial Intelligence Decision-Making for Mission Planning.

In an increasingly complex military operating environment, next generation wargaming platforms can reduce risk, decrease operating costs, and improve overall outcomes. Novel Artificial Intelligence (AI) enabled wargaming approaches, based on software platforms with multimodal interaction and visualization capacity, are essential to provide the decision-making flexibility and adaptability required to meet current and emerging realities of warfighting. We highlight three areas of development for future warfighter-machine interfaces: AI-directed decisional guidance, computationally informed decision-making, and realistic representations of decision spaces.

Heuristic Global Optimization in Chemical Compound Space.

We report developments in combinatorial optimization under constraints in chemical space. We considered random functions, which serve as a baseline to measure performance, and constrained optimizations over two databases of electrochromic molecules (∼5000 and 10, respectively). These problems were optimized using sequential heuristic next-neighbor search (HNNS) (introduced in Elward and Rinderspacher 2015, 17, 24322 and Elward and Rinderspacher 2018, 3, 485) and kernel-based efficient global optimization (EGO) with two reordering strategies.

Theory of wavelet-based coarse-graining hierarchies for molecular dynamics.

We present a multiresolution approach to compressing the degrees of freedom and potentials associated with molecular dynamics, such as the bond potentials. The approach suggests a systematic way to accelerate large-scale molecular simulations with more than two levels of coarse graining, particularly applications of polymeric materials. In particular, we derive explicit models for (arbitrarily large) linear (homo)polymers and iterative methods to compute large-scale wavelet decompositions from fragment solutions.

Smooth heuristic optimization on a complex chemical subspace.

Several algorithms for optimizing a combinatorial subspace of chemical compound space with constraints are compared. The test system is a library of organic chromophores for electro-optic applications. The constraints on the optimization include the maximization of the candidate structure hyperpolarizability while keeping the absorption within acceptable limits in the range of 400-700 nm.

Nonlinear mechanics of thermoreversibly associating dendrimer glasses.

We model the mechanics of associating trivalent dendrimer network glasses with a focus on their energy dissipation properties. Various combinations of sticky bond (SB) strength and kinetics are employed. The toughness (work to fracture) of these systems displays a surprising deformation-protocol dependence; different association parameters optimize different properties.

Discrete Optimization of Electronic Hyperpolarizabilities in a Chemical Subspace.

We introduce a general optimization algorithm based on an interpolation of property values on a hypercube. Each vertex of the hypercube represents a molecule, while the interior of the interpolation represents a virtual superposition ("alchemical" mutation) of molecules. The resultant algorithm is similar to branch-and-bound/tree-search methods.

Performance of DFT Methods in the Calculation of Optical Spectra of TCF-Chromophores.

We present electronic structure calculations of the ultraviolet/visible (UV-vis) spectra of highly active push-pull chromophores containing the tricyanofuran (TCF) acceptor group. In particular, we have applied the recently developed long-range corrected Baer-Neuhauser-Livshits (BNL) exchange-correlation functional. The performance of this functional compares favorably with other density functional theory (DFT) approaches, including the CAM-B3LYP functional.

The geometry and electronic topology of higher-order charged Möbius annulenes.

Higher-order aromatic charged Möbius-type annulenes have been L(k) realized computationally. These charged species are based on strips with more than one electronic half-twist, as defined by their linking numbers. The B3LYP/6-311+G(d,p) optimized structures and properties of annulene rings with such multiple half-twists (C(12)H(12)(2+), C(12)H(12)(2-), C(14)H(14), C(18)H(18)(2+), C(18)H(18)(2-), C(21)H(21)(+), C(24)H(24)(2-), C(28)H(28)(2+), and C(28)H(28)(2-)) have the nearly equal C-C bond lengths, small dihedral angles around the circuits, stabilization energies, and nucleus-independent chemical shift values associated with aromaticity.

Syntheses and properties of enantiomerically pure higher (n > or = 7) [n-2]triangulanedimethanols and sigma-[n]helicenes.

(P)-(+)-Hexaspiro[2.0.0.

An Aufbau Ansatz for geminal functional theory.

We generalize antisymmetric geminal products to more than just one generating geminal using an Aufbau Ansatz similar to the Hartree-Fock theory. Investigation of Li-, Be, B+, LiH, BeH+, and He2 shows a very high recovery of electron-correlation energy using this Aufbau Ansatz. The method is inherently multideterminantal and insensitive to symmetry problems.

Bullvalene trisepoxide and its stereospecific rearrangement to 2,8,12-trioxahexacyclo[8.3.0.0(3,9)0(4,6)0(5,13)0(7,11)]tridecane: two new C3-symmetrical oligocycles with propeller chirality.

Epoxidation of bullvalene (1) with a neutralized solution of Oxone gave racemic trisepoxide rac-6 in 93 % isolated yield. Its structure was examined by X-ray crystallography. The two enantiomers of 6 were separated by preparative HPLC and exhibited specific rotations of [alpha](25)(D)= +160, [alpha](25)(365)= +567 (c=0.