(Invited) Area-Selective Atomic-Molecular Layer Deposition of Photoluminescent Europium-Organic Thin Films on Graphene Activated by Direct Laser Writing

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Area-selective atomic layer deposition (AS-ALD) is a promising technique for advanced nanofabrication processes. This allows for the simple bottom-up creation of intricate nanostructures essential for advanced optoelectronic and sensor applications. 1 Due to the flexibility of ALD, the method can be used alongside its organic counterpart, molecular layer deposition (MLD). 2 The combined atomic/molecular layer deposition (ALD/MLD) enables tuning of material properties by incorporating organic linkers into the film while maintaining the nanoscale control. 3 Area-selective ALD and MLD separately have been demonstrated previously, but these processes typically rely on utilization of inhibitors and lithography steps to achieve the area-selectivity, which complicates the process. 4,5 While there are examples of AS-ALD being used on two-dimensional materials (2DM), AS-MLD on them is still mostly unexplored. Due to the inherent 2D nature, the surface of 2DM does not provide sufficient reactive sites for the chemisorption of ALD/MLD precursors compared with traditional microelectronics. Surface functionalization can provide the selective 3D growth of desired materials. Recently, we have overcome the chemical inertness of graphene to ALD precursors by local activation using direct femtosecond laser two-photon oxidation (TPO) 6 for selective ZnO deposition. 7 In this study, we guided the growth of Europium-terephthalate thin films on top of single-layer graphene via TPO. 8 We achieved high homogeneity and more than 90% selectivity in locally activated predefined regions for thicknesses up to 11 nm. The deposited thin films exhibited intriguing photoluminescent properties, broadening the material's characteristic excitation wavelength from ultraviolet to the visible light range. The work function, Raman spectroscopy, and fluorescence lifetime imaging data confirmed electronic interactions and n-type doping of TPO graphene after ALD/MLD. The demonstrated approach provides a path forward for integrating 2DM-based heterostructures into optoelectronic, photonic, and energy-harvesting devices. Sub-micron precision achieved in this work expands the design possibilities for multifunctional devices on a single chip. References Parsons G. N., Clark R. D., Chemistry of Materials . 2020 , Volume 32, Issue 12, Multia J., Karppinen M., Advanced Materials Interfaces. 2022 , Volume 9, Issue 15, Safdar M., Ghazy A., Tuomisto M., Lastusaari M, Karppinen M., Journal of Materials Science. 2021 , Volume 56 , 12634. Mackus A. J. M., Bol A. A., Kessles W. M. M., 2014 , Volume 6, Issue 9, 10941. Prasittichai C., Zhou H., Bent S. F., ACS Applied Materials & Interfaces. 2013 , Volume 5, Issue 24, Aumanen, A. Johansson, J. Koivistoinen, P. Myllyperkiö, M. Pettersson, Nanoscale 7 , 2851 (2015). K. Mentel, A. V. Emelianov, A. Philip, A. Johansson, M. Karppinen, M. Pettersson, Adv. Mater. Interfaces 9 , 2201110 (2022). A. V. Emelianov, K. K. Mentel, A. Ghazy, Yu-H. Wang, A. Johansson, M. Karppinen, M. Pettersson, submitted (2025). DOI: 10.26434/chemrxiv-2024-81qv0

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