RESUMO
Ice has been suggested to have played a significant role in the origin of life partly owing to its ability to concentrate organic molecules and promote reaction efficiency. However, the techniques for studying organic molecules in ice are absorption-based, which limits the sensitivity of measurements. Here we introduce an emission-based method to study organic molecules in water ice: the phosphorescence displays high sensitivity depending on the hydration state of an organic salt probe, acridinium iodide (ADI). The designed ADI aqueous system exhibits phosphorescence that can be severely perturbed when the temperature is higher than 110â K at a concentration of the order of 10-5â M, indicating changes in hydration for ADI. Using the ADI phosphorescent probe, it is found that the microstructures of water ice, i.e., crystalline vs. glassy, can be strongly dictated by a trace amount (as low as 10-5â M) of water-soluble organic molecules. Consistent with cryoSEM images and temperature-dependent Raman spectral data, the ADI is dehydrated in more crystalline ice and hydrated in more glassy ice. The current investigation serves as a starting point for using more sensitive spectroscopic techniques for studying water-organics interactions at a much lower concentration and wider temperature range.
RESUMO
Chiral recognition of amino acids is very important in both chemical and life sciences. Although chiral recognition with luminescence has many advantages such as being inexpensive, it is usually slow and lacks generality as the recognition module relies on structural complementarity. Here, we show that one single molecular-solid sensor, L-phenylalanine derived benzamide, can manifest the structural difference between the natural, left-handed amino acid and its right-handed counterpart via the difference of room-temperature phosphorescence (RTP) irrespective of the specific chemical structure. To realize rapid and reliable sensing, the doped samples are obtained as nanocrystals from evaporation of the tetrahydrofuran solutions, which allows for efficient triplet-triplet energy transfer to the chiral analytes generated in situ from chiral amino acids. The results show that L-analytes induce strong RTP, whereas the unnatural D-analytes produce barely any afterglow. The method expands the scope of luminescence chiral sensing by lessening the requirement for specific molecular structures.
Assuntos
Aminoácidos , Luminescência , Aminoácidos/química , Temperatura , Estrutura MolecularRESUMO
Label-free data mining can efficiently feed large amounts of data from the vast scientific literature into artificial intelligence (AI) processing systems. Here, we demonstrate an unsupervised syntactic distance analysis (SDA) approach that is capable of mining chemical substances, functions, properties, and operations without annotation. This SDA approach was evaluated in several areas of research from the physical sciences and achieved performance in information mining comparable to that of supervised learning, as shown by its satisfactory scores of 0.62-0.72, 0.60-0.82, and 0.86-0.95 in precision, recall, and accuracy, respectively. We also showcase how our approach can assist robotic chemists programmed to perform research focused on double-perovskite colloidal nanocrystals, gold colloidal nanocrystals, oxygen evolution reaction catalysts, and enzyme-like catalysts by designing materials, formulations, and synthesis parameters based on data mined from 1.1 million literature references.