β-sheet-encoded anionic and cationic dendritic peptide amphiphiles form supramolecular copolymers when self-assembled in a 1:1 feed ratio of the monomers. These ampholytic materials have been designed for on-off polymerization response to pH triggers. The cooperative self-assembly process is switched on at physiologically relevant value can be off by increasing or decreasing value.

Modern computational chemistry has reached a stage at which massive exploration into chemical reaction space with unprecedented resolution respect to the number of potentially relevant molecular structures become possible. Various algorithmic advances have shown that such structural screenings must and can be automated routinely carried out. This will replace standard approach manually studying selected restricted for mechanism. The complexity task led many different approaches. However, all...

Fueled by advances in hardware and algorithm design, large-scale automated explorations of chemical reaction space have become possible. Here, we present our approach to an open-source, extensible framework for mechanisms based on the first principles quantum mechanics. It is intended facilitate network diverse problems with a wide range goals such as mechanism elucidation, path optimization, retrosynthetic validation, reagent microkinetic modeling. The stringent first-principles basis all...

The software for chemical interaction networks (SCINE) project aims at pushing the frontier of quantum calculations on molecular structures to a new level. While individual as well simple relations between them have become routine in chemistry, developments pushed field high-throughput calculations. Chemical may be created by search specific properties design attempt, or they can defined set elementary reaction steps that form network. modules SCINE been designed facilitate such studies....

We present the new quantum chemistry program Serenity. It implements a wide variety of functionalities with focus on subsystem methodology. The modular code structure in combination publicly available external tools and particular design concepts ensures extensibility robustness needs program. Several important features are exemplified sample calculations density-functional theory, potential reconstruction techniques, projection-based embedding approach combinations thereof geometry...

Quantum chemical calculations on atomistic systems have evolved into a standard approach to studying molecular matter. These often involve significant amount of manual input and expertise, although most this effort could be automated, which would alleviate the need for expertise in software hardware accessibility. Here, we present AutoRXN workflow, an automated workflow exploratory high-throughput electronic structure systems, (i) density functional theory methods are exploited deliver...

ConspectusQuantum mechanical methods have been well-established for the elucidation of reaction paths chemical processes and explicit dynamics molecular systems. While they are usually deployed in routine manual calculations on reactions which some insights already available (typically from experiment), new algorithms continuously increasing capabilities modern computer hardware allow exploratory open-ended computational campaigns that unbiased therefore enable unexpected discoveries. Highly...

Abstract SERENITY [J Comput Chem . 2018;39:788–798] is an open‐source quantum chemistry software that provides extensive development platform focused on quantum‐mechanical multilevel and embedding approaches. In this study, we give overview over the developments done in Serenity since its original publication 2018. This includes efficient electronic‐structure methods for ground states such as domain‐based local pair natural orbital coupled cluster Møller–Plesset perturbation theory well...

We demonstrate and discuss the feasibility of autonomous first-principles mechanistic explorations for providing quantum chemical data to enhance confidence data-driven retrosynthetic synthesis design based on molecular transformers.

The software for chemical interaction networks (SCINE) project aims at pushing the frontier of quantum calculations on molecular structures to a new level. While individual as well simple relations between them e.g., given by an intrinsic reaction coordinate) have become routine in chemistry, developments pushed field high-throughput calculations. Chemical may be created search specific properties design attempt or they can defined set elementary steps that form network. modules SCINE been...

For many chemical processes the accurate description of solvent effects are vitally important. Here, we describe a hybrid ansatz for explicit quantum mechanical solute-solvent and solvent-solvent interactions based on subsystem density functional theory continuum solvation schemes. Since molecules may compromise scalability model transferability predicted effect, aim to retain both, different solutes as well solvents. The key is consistent decomposition solute solvent. performance DFT...

In this article we report the preparation and characterization of a peptide-based hydrogel, which possesses characteristic rheological properties, is pH responsive can be functionalized at its thiol function. The tripeptide N-(fluorenyl-9-methoxycarbonyl)-L-Cys(acetamidomethyl)-L-His-L-Cys-OH 1 forms stable supramolecular aggregates in water leading to hydrogels above 1.5 wt%. Rheological analysis hydrogel revealed visco-elastic shear thinning properties samples containing wt% peptide 1....

Autonomously exploring chemical reaction networks with first-principles methods can generate vast data. Especially autonomous explorations without tight constraints risk getting trapped in regions of that are not interest. In many cases, these the only exited once fully searched. Consequently, required human time for analysis and computer data generation make investigations unfeasible. Here, we show how simple templates facilitate transfer knowledge from expert input or existing into new...

Recent reports on the necessity of using externally orthogonal orbitals in subsystem density-functional theory (SDFT) [Annu. Rep. Comput. Chem., 8, 2012, 53; J. Phys. Chem. A, 118, 2014, 9182] are re-investigated. We show that basis-set limit, supermolecular Kohn-Sham-DFT (KS-DFT) densities can exactly be represented as a sum densities, even if not orthogonal. This is illustrated both an analytical example and free numerical calculations for atomic test case. further with finite basis sets,...

Automated and high-throughput quantum chemical investigations into processes have become feasible in great detail broad scope. This results an increase complexity of the tasks amount generated data. An efficient intuitive way for operator to interact with these data steer virtual experiments is required. Here, we introduce Heron, a graphical user interface that allows advanced human-machine interactions exploration campaigns molecular structure reactivity. Heron offers access interactive...

Density functional theory (DFT) is used to calculate the relative free energies of deprotonation isomers iron-group hydride complexes MHXL4 where M = Fe, Ru, Os, L4 (CO)4 or (PMe2CH2CH2PMe2)2 for a wide range anionic ligands X. The most stable are pKa values Ka refers acid dissociation constant equilibrium → [MXL4]- + H+. These test proposal that given metal complex in THF can be simply calculated by adding contributions total value from each ligand L; these called acidity constants (LAC) AL...

Quantum chemical calculations on atomistic systems have evolved into a standard approach to study molecular matter. These often involve significant amount of manual input and expertise although most this effort could be automated, which would alleviate the need for in software hardware accessibility. Here, we present AutoRXN workflow, an automated workflow exploratory high-throughput lectronic structure systems, (i) density functional theory methods are exploited deliver minimum...

Automated and high-throughput quantum chemical investigations into processes have become feasible in great detail broad scope. This results an increase complexity of the tasks amount generated data. An efficient intuitive way for operator to interact with these data steer virtual experiments is required. Here, we introduce Heron, a graphical user interface that allows advanced human-machine interactions exploration campaigns molecular structure reactivity. Heron offers access interactive...

The autonomous exploration of chemical reaction networks with first-principles methods generates vast amounts data. Especially explorations that explore autonomously and without tight constraints run the risk exploring regions space are not interest. Consequently, required human time for analysis computer data generation can make these unfeasible. Here, we show how an automated extraction templates facilitate transfer knowledge from existing This process significantly accelerates network...

Autonomously exploring chemical reaction networks with first-principles methods can generate vast data. Especially autonomous explorations without tight constraints risk getting trapped in regions of that are not interest. In many cases, these the only exited once fully searched. Consequently, required human time for analysis and computer data generation make investigations unfeasible. Here, we show how simple templates facilitate transfer knowledge from expert input or existing into new...

Data-driven synthesis planning has seen remarkable successes in recent years by virtue of modern approaches artificial intelligence that efficiently exploit vast databases with experimental data on chemical reactions. However, this success story is intimately connected to the availability existing data. It may well occur retrosynthetic and design tasks predictions individual steps a reaction cascade are affected large uncertainties. In such cases, it will, general, not be easily possible...