Researcher profile

Raymond R. Unocic

Raymond R. Unocic contributes to research discovery and scholarly infrastructure.

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Published work

4 published item(s)

preprint2026arXiv

Born-Qualified: An Autonomous Framework for Deploying Advanced Energy and Electronic Materials

Autonomous science is transforming how we discover materials and chemical systems for advanced energy technologies. However, many initially promising systems never reach deployment. This "valley of death" stems from optimization that prioritizes laboratory metrics over industrial viability. We propose a new strategy: "born-qualified" autonomous development, which embeds manufacturability, cost, and durability constraints from the outset. This approach is enabled by four pillars, including the development of multi-objective metrics, causal models, a modular infrastructure, and embedding manufacturing in the discovery loop. Realizing this vision will require sustained, community-wide commitment, but the potential return on that investment is commensurate with the scale of the challenge.

preprint2022arXiv

Probing electron beam induced transformations on a single defect level via automated scanning transmission electron microscopy

The robust approach for real-time analysis of the scanning transmission electron microscopy (STEM) data streams, based on the ensemble learning and iterative training (ELIT) of deep convolutional neural networks, is implemented on an operational microscope, enabling the exploration of the dynamics of specific atomic configurations under electron beam irradiation via an automated experiment in STEM. Combined with beam control, this approach allows studying beam effects on selected atomic groups and chemical bonds in a fully automated mode. Here, we demonstrate atomically precise engineering of single vacancy lines in transition metal dichalcogenides and the creation and identification of topological defects graphene. The ELIT-based approach opens the pathway toward the direct on-the-fly analysis of the STEM data and engendering real-time feedback schemes for probing electron beam chemistry, atomic manipulation, and atom by atom assembly.

preprint2020arXiv

Fluid Guided CVD Growth for Large-scale Monolayer Two-dimensional Materials

Atmospheric pressure chemical vapor deposition (APCVD) has been used extensively for synthesizing two-dimensional (2D) materials, due to its low cost and promise for high-quality monolayer crystal synthesis. However, the understanding of the reaction mechanism and the key parameters affecting the APCVD processes is still in its embryonic stage. Hence, the scalability of the APCVD method in achieving large scale continuous film remains very poor. Here, we use MoSe2 as a model system and present a fluid guided growth strategy for understanding and controlling the growth of 2D materials. Through the integration of experiment and computational fluid dynamics (CFD) analysis in the full-reactor scale, we identified three key parameters: precursor mixing, fluid velocity and shear stress, which play a critical role in the APCVD process. By modifying the geometry of the growth setup, to enhance precursor mixing and decrease nearby velocity shear rate and adjusting flow direction, we have successfully obtained inch-scale monolayer MoSe2. This unprecedented success of achieving scalable 2D materials through fluidic design lays the foundation for designing new CVD systems to achieve the scalable synthesis of nanomaterials.

preprint2020arXiv

Lattice strain measurement of core@shell electrocatalysts with 4D-STEM nanobeam electron diffraction

Strain engineering enables the direct modification of the atomic bonding and is currently an active area of research aimed at improving the electrocatalytic activity. However, directly measuring the lattice strain of individual catalyst nanoparticles is challenging, especially at the scale of a single unit cell. Here, we quantitatively map the strain present in rhodium@platinum (core@shell) nanocube electrocatalysts using conventional aberration-corrected scanning transmission electron microscopy (STEM) and the recently developed technique of 4D-STEM nanobeam electron diffraction. We demonstrate that 4D-STEM combined with data pre-conditioning allows for quantitative lattice strain mapping with sub-picometer precision without the influence of scan distortions. When combined with multivariate curve resolution, 4D-STEM allows us to distinguish the nanocube core from the shell and to quantify the unit cell size as a function of distance from the core-shell interface. Our results demonstrate that 4D-STEM has significant precision and accuracy advantages in strain metrology of catalyst materials compared to aberration-corrected STEM imaging and is beneficial for extracting information about the evolution of strain in catalyst nanoparticles.