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Sharma, H.

Publications and source records attributed to Sharma, H..

Application of advanced causal analyses to identify processes governing secondary organic aerosols

Abstract Understanding how different physical and chemical atmospheric processes affect the formation of fine particles has been a persistent challenge. Inferring causal relations between the various measured features affecting the formation of secondary organic aerosol (SOA) particles is complicated since correlations between variables do not necessarily imply causality. Here, we apply a state-of-the-art information transfer measure coupled with the Koopman operator framework to infer causal relations between isoprene epoxydiol SOA (IEPOX-SOA) and different chemistry and meteorological variables derived from detailed regional model predictions over the Amazon rainforest. IEPOX-SOA represents one of the most complex SOA formation pathways and is formed by the interactions between natural biogenic isoprene emissions and anthropogenic emissions affecting sulfate, acidity and particle water. Since the regional model captures the known relations of IEPOX-SOA with different chemistry and meteorological features, their simulated time series implicitly include their causal relations. We show that our causal model successfully infers the known major causal relations between total particle phase 2-methyl tetrols (the dominant component of IEPOX-SOA over the Amazon) and input features. We provide the first proof of concept that the application of our causal model better identifies causal relations compared to correlation and random forest analyses performed over the same dataset. Our work has tremendous implications, as our methodology of causal discovery could be used to identify unknown processes and features affecting fine particles and atmospheric chemistry in the Earth’s atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-Energy Coherent X-Ray Dffraction Microscopy of Polycrystal Grains: First Steps Towards a Multi-Scale Approach

Here, we present proof-of-concept imaging measurements of a polycrystalline material that integrate the elements of conventional high-energy x-ray diffraction microscopy with coherent diffraction-imaging techniques, and that can enable in situ strain-sensitive imaging of lattice structure in ensembles of deeply embedded crystals over five decades of length scale upon full realization. We demonstrate that the combination of these two characterization methods enables a more complete picture of the crystal-lattice strain than either method is capable of providing individually. Such complementary imaging capabilities are critical to addressing questions in a variety of research areas such as materials science and engineering, chemistry, and solid-state physics. Towards this eventual goal, the following key aspects are demonstrated: (1) high-energy Bragg coherent diffraction imaging (HE BCDI) of submicron-scale crystallites at 52 keV at current third-generation synchrotron light sources, (2) HE BCDI performed in conjunction with far-field high-energy diffraction microscopy (FF HEDM) on the grains of a polycrystalline sample in a smoothly integrated manner, and (3) the orientation information of an ensemble of grains obtained via FF HEDM used to perform complementary HE BCDI on multiple Bragg reflections of a single targeted grain. The imaged structures are seen to be 477 ± 50 nm or smaller in size, with an estimated strain resolution of 2.5 x 10 -4 . These steps lay the foundation for integration of HE BCDI, which typically provides a spatial resolution tens of nanometers, into a broad suite of well-established HEDM methods, extending HEDM beyond the few-micrometer resolution bound and into the nanoscale, and positioning the approach to take full advantage of the orders-of-magnitude improvement of x-ray coherence expected at fourth-generation light sources presently being built and commissioned worldwide.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Preferential nucleation during polymorphic transformations

Polymorphism is the ability of a solid material to exist in more than one phase or crystal structure. Polymorphism may occur in metals, alloys, ceramics, minerals, polymers, and pharmaceutical substances. Unresolved are the conditions for preferential nucleation during polymorphic transformations in which structural relationships or special crystallographic orientation relationships (OR’s) form between the nucleus and surrounding matrix grains. We measured in-situ and simultaneously the nucleation rates of grains that have zero, one, two, three and four special OR’s with the surrounding parent grains. These experiments show a trend in which the activation energy for nucleation becomes smaller – and therefore nucleation more probable - with increasing number of special OR’s. As a result, these insights contribute to steering the processing of polymorphic materials with tailored properties, since preferential nucleation affects which crystal structure forms, the average grain size and texture of the material, and thereby - to a large extent - the final properties of the material.

36 MATERIALS SCIENCE↗