Dassault Systèmes (United Kingdom)

Large Language Model agents capable of using software tools have recently surged in capability and popularity in the data science domain, but remain under-used in the physical sciences. We develop Agentic Pilot, a visual user interface built on LangGraph, to help fill this gap. Agentic Pilot enables the intuitive development of complex agentic workflows, allowing even small LLMs to perform industrially relevant tasks such as executing computational screening calculations or querying electronic lab notebook databases via natural language. In this work, we present Agentic Pilot and provide an industrial perspective on the future of LLM-based agentic workflows in chemistry.

The anhydrous di-iodyl carbonate (IO2)2[CO3] has been synthesized in a laser-heated diamondanvil cellat 30(2) GPa and 1600(200) K by a reaction of I2O5 with CO2. Its monoclinic crystal structure (C2/c with Z = 4) was determinedfrom synchrotron single crystal X-ray diffraction data. The experimentalstructural model was confirmed by density functional theory basedcalculations in combination with experimental Raman spectroscopy.(IO2)2[CO3]-C2/c belongs to the family of sp2-carbonates, andits crystal structure is characterized by the presence of nearly trigonal-planar[CO3]2– groups. In contrast to otheriodide-containing carbonates, in this structure the iodine atoms arepresent as small and highly oxidized I5+-cations and notas large I–-anions. The I5+-cations arecoordinated by seven oxygen atoms. The successful synthesis of (IO2)2[CO3]-C2/c represents a significant enlargement of the crystal chemistryof carbonates, as this chemically simple carbonate demonstrates thatanhydrous carbonates with highly charged cations can be formed andthat sp2-carbonates hosting a positively charged halogenatom as the only cation can be synthesized.

The existence of polymeric carbonic acid (H2CO3) at elevated pressures has been predicted, but has not been investigated experimentally. Here, polymeric carbonic acid containing sp3-hybridized carbon was synthesized and characterized at ≈40 GPa. H2CO3 single crystals were obtained by laser-heating a H2O + CO2 mixture in a diamond anvil cell. The orthorhombic crystal structure (Cmc21 with Z = 4) was refined from synchrotron single crystal X-ray diffraction data and is in agreement with a structural model predicted earlier. The crystal structure of H2CO3-Cmc21 is characterized by {[{{rm{CO}}}_{4}]}^{4-} building blocks which are connected via corner sharing, forming chains along the c-axis. The combination of single crystal X-ray data with experimental Raman spectroscopy and DFT-calculations confirms that the structural model of H2CO3-Cmc21 is appropriate. The synthesis condition of polymeric carbonic acid points towards its potential existence in ice giants including the ones present in our solar system.

We synthesized CdC2O5 and a new high-pressure polymorph of CdCO3 by laser heating otavite, CdCO3, in CO2 at 43 GPa. The structure of CdC2O5 contains pyramidal [C4O10]4– building blocks formed by [CO4] tetrahedra, where the carbon is in 4-fold coordination. In addition, we found a new monoclinic (P21/c) high-pressure polymorph of CdCO3 with trigonal [CO3]2– groups. Both new structures were characterized by single-crystal X-ray diffraction, Raman spectroscopy, and DFT calculations.

Experimental and theoretical studies were carried out to investigate the ozonolysis of trans-2-methyl-2-pentenal. The experiments were conducted in atmospheric simulation chambers coupled to a Fourier transform infrared (FTIR) spectrometer and a gas chromatograph-mass spectrometer at room temperature and atmospheric pressure in the presence of an excess of cyclohexane in dry conditions (RH < 1%). The ozonolysis reaction was investigated theoretically from the results of accurate density functional (M06-2X) and ab initio [CCSD(T)] computations, employing the AVTZ basis set. The sequence of reaction steps was established, and the system of kinetics equations was modeled using MESMER. In the first step, a primary ozonide is formed, which then decomposes along two pathways. The principal ozonolysis products are propanal, methylglyoxal, ethylformate, and a secondary ozonide. An interesting competition between sequential reaction steps and well-skipping is found, which leads to an inversion of the expected methylglyoxal/propanal product ratio at temperatures below 210 K. The mechanism of the "hot ester" reaction channel of the Criegee intermediate was revisited. The computed ozonolysis rate constant and product branching ratio are in excellent agreement with the experimental data that are also reported in the present work.