@article{carroll_margavio_parsons_2024, title={"Dual-Tone" Area-Selective Deposition: Selectivity Inversion of Polymer on Patterned Si/SiO2 Starting Surfaces}, volume={2}, ISSN={["1520-5002"]}, url={https://doi.org/10.1021/acs.chemmater.3c03158}, DOI={10.1021/acs.chemmater.3c03158}, abstractNote={Area-selective deposition (ASD) has recently emerged as a promising augmentation of lithographic patterning of small device features. However, current ASD processes are restricted to predefined growth and nongrowth surfaces, limiting their flexibility in industrial processing. In this work, we define the concept of “dual-tone ASD,” where a patterned surface is tuned to enable ASD on one of two adjacent surfaces while avoiding growth on the other surface. For the example case in this work, starting with ASD of the poly(3,4-ethylenedioxythipohene) (PEDOT) conjugated polymer on SiO2 vs on hydrogen-terminated silicon (Si–H), we demonstrate a method to modify a patterned Si–H/SiO2 surface to invert the selectivity, enabling PEDOT to grow selectively on the modified Si region and not on the modified SiO2. The selectivity inversion was achieved by selective modification of the substrate surface energy via treatments with dilute hydrofluoric acid (DHF), (dimethylamino)trimethylsilane (DMATMS), and water. Versatile control over selectivity configurations during ASD has implications for deposition of lateral control layers to reduce overgrowth defects, blocking layers for nonselective deposition steps, and sacrificial layers for recently reported simultaneous deposition and etching processes. Through this study, we identify generalized requirements for selectivity inversion as a patterning strategy in the ASD toolbox and show how this strategy is consistent with previous reports of ASD on metal–dielectric patterned surfaces. Extension of these surface energy treatment strategies to other materials will provide additional opportunities for selectivity inversion, leading to flexible applications of ASD in manufacturing settings.}, journal={CHEMISTRY OF MATERIALS}, author={Carroll, Nicholas M. and Margavio, Hannah R. M. and Parsons, Gregory N.}, year={2024}, month={Feb} } @article{nedzbala_westbroek_margavio_yang_noh_magpantay_donley_kumbhar_parsons_mayer_2024, title={Photoelectrochemical Proton-Coupled Electron Transfer of TiO2 Thin Films on Silicon}, volume={4}, ISSN={["1520-5126"]}, url={https://doi.org/10.1021/jacs.4c00014}, DOI={10.1021/jacs.4c00014}, journal={JOURNAL OF THE AMERICAN CHEMICAL SOCIETY}, author={Nedzbala, Hannah S. and Westbroek, Dalaney and Margavio, Hannah R. M. and Yang, Hyuenwoo and Noh, Hyunho and Magpantay, Samantha V. and Donley, Carrie L. and Kumbhar, Amar S. and Parsons, Gregory N. and Mayer, James M.}, year={2024}, month={Apr} } @article{zhirnov_chen_malakoutian_margavio_pawliczak_reidy_yanez_younkin_2023, title={SRC-led materials research: 40 years ago, and now}, ISSN={["2059-8521"]}, DOI={10.1557/s43580-023-00665-4}, abstractNote={Today, we are living through a pivotal moment when the semiconductor industry is moving towards 3D-integration including the close integration of logic and memory, the tighter integration of mixed-signal circuits, spintronic, embedded memories, sensors, communications, and improved power management. It is expected that 3D monolithic and heterogeneous integration will result in a new, truly multi-functional platform that drives continued system progress in the coming decades. Thus, over the next 40 years, the semiconductor industry will require significant innovation. At the heart of that is the need for significant contributions from the materials ecosystem to drive materials from the laboratory to the factory. For this perspective article, a selected group of distinguished SRC Scholars have been invited to present their research in the context of the potential impact that their work will drive for the future of microelectronics.}, journal={MRS ADVANCES}, author={Zhirnov, Victor and Chen, Michelle E. and Malakoutian, Mohamadali and Margavio, Hannah R. M. and Pawliczak, Emma and Reidy, Kate and Yanez, Wilson and Younkin, Todd}, year={2023}, month={Nov} } @article{oh_kim_margavio_parsons_2023, title={Self-Aligned Nanopatterning and Controlled Lateral Growth by Dual-Material Orthogonal Area-Selective Deposition of Poly(3,4-ethylenedioxythiophene) and Tungsten}, volume={35}, ISSN={["1520-5002"]}, url={https://doi.org/10.1021/acs.chemmater.3c00530}, DOI={10.1021/acs.chemmater.3c00530}, abstractNote={Despite recent advances in area-selective deposition (ASD) processes, most studies have focused on single-material ASD. Multi-material ASD processes could provide additional flexibility for fabricating semiconductor devices. In this work, we identify process requirements to sequentially combine two intrinsic ASD processes: (1) poly(3,4-ethylenedioxythiophene) (PEDOT) ASD on SiO2 vs Si–H via oxidative chemical vapor deposition and (2) W ASD on Si–H vs SiO2 via atomic layer deposition. Using ex situ X-ray photoelectron spectroscopy, we show that a preferred orthogonal ASD sequence involves PEDOT ASD on SiO2 vs Si–H, followed by W ASD on Si–H vs PEDOT. We find that the properties of the individual PEDOT and W ASD materials, including resistivity, surface roughness, and growth rate, are affected by the ASD sequence. Furthermore, we successfully demonstrate that orthogonal ASD can be extended to nanoscale starting patterns. The cross-sectional scanning transmission electron microscopy (STEM) with energy-dispersive X-ray spectroscopy analysis shows that the resulting PEDOT thickness on SiO2 depends on feature geometry and dimension. Finally, we demonstrate the feasibility that the PEDOT layer can control the lateral growth of W onto the non-growth surface.}, number={11}, journal={CHEMISTRY OF MATERIALS}, author={Oh, Hwan and Kim, Jung-Sik and Margavio, Hannah R. M. and Parsons, Gregory N.}, year={2023}, month={May}, pages={4375–4384} } @article{song_kim_margavio_parsons_2021, title={Multimaterial Self-Aligned Nanopatterning by Simultaneous Adjacent Thin Film Deposition and Etching}, volume={15}, ISSN={["1936-086X"]}, url={https://doi.org/10.1021/acsnano.1c04086}, DOI={10.1021/acsnano.1c04086}, abstractNote={Printed component sizes in electronic circuits are approaching 10 nm, but inherent variability in feature alignment during photolithography poses a fundamental barrier for continued device scaling. Deposition-based self-aligned patterning is being introduced, but nuclei defects remain an overarching problem. This work introduces low-temperature chemically self-aligned film growth via simultaneous thin film deposition and etching in adjacent regions on a nanopatterned surface. During deposition, nucleation defects are avoided in nongrowth regions because deposition reactants are locally consumed via sacrificial etching. For a range of materials and process conditions, thermodynamic modeling confirms that deposition and etching are both energetically favorable. We demonstrate nanoscale patterning of tungsten at 220 °C with simultaneous etching of TiO2. Area selective deposition (ASD) of the sacrificial TiO2 layer produces an orthogonal sequence for self-aligned patterning of two materials on one starting pattern, i.e., TiO2 ASD on SiO2 followed by W ASD on Si-H. Experiments also show capacity for self-aligned dielectric patterning via favorable deposition of AlF3 on Al2O3 at 240 °C with simultaneous atomic layer etching of sacrificial ZnO. Simultaneous deposition and etching provides opportunities for low-temperature bottom-up self-aligned patterning for electronic and other nanoscale systems.}, number={7}, journal={ACS NANO}, publisher={American Chemical Society (ACS)}, author={Song, Seung Keun and Kim, Jung-Sik and Margavio, Hannah R. M. and Parsons, Gregory N.}, year={2021}, month={Jul}, pages={12276–12285} }