High-Precision Laser Printing of Nanoparticle Metasurfaces for Light Control, Sensors, and Nanolasers
Final Report Abstract
Spherical metal and dielectric nanoparticles with strong electric and magnetic resonances in the visible spectral range are promising candidates for serving as building blocks of optical metamaterials and metasurfaces for light control at nano- and microscales. In this project, generation, precise positioning, shape-, size-, and morphology-control of such nanoparticles by illumination of material surfaces with short and ultrashort laser pulses have been investigated. The donor materials have locally been melted by laser radiation, and the ejected nanoparticles have been captured on thin receiver glass substrates within a distance of several micrometers. Using this laser-induced transfer (LIT), spherical nanoparticles have been generated from different bulk and thin-film material samples. For bulk or thin-film samples of highly thermally conducting metals, e.g. gold, silver, copper, nano-jet formation has been observed, leading to ejection of single particles. However, semiconductors (silicon, germanium, gallium arsenide) have an anomalous density increase, leading to ejection of multiple particles, even for ultrafast heating by fs-laser pulses. This problem has been overcome by use of thin-film samples. The local ultrafast heating leads to melting of a small volume of material, being determined by focal spot size, pulse energy, and material film thickness. When the molten material contracts into a sphere it acquires momentum which drives the particle against the receiver substrate where it is adhered. Theoretical modelling of the laser melting process has been performed, in good agreement with experimental results. With LIT nanoparticles of 100 nm – 500 nm diameter have been printed from materials like aluminum, iron, titanium, silicon, germanium, and silicon-germanium alloy. By varying the distance between donor and receiver surfaces in the range from 5 µm to 50 µm different morphology states from amorphous to polycrystalline have been found for semiconductor nanoparticles. In first experiments, second harmonic generation (SHG) of ultrashort pulse radiation at a central wavelength of 1050 nm from LIT printed silicon particles has been investigated, and the yield of second harmonic radiation in dependence of particle morphology and particle diameter has been studied. High efficiencies of SHG have been found for polycrystalline particles driven in the magnetic dipole resonance. Due to temporal non-availability of the femtosecond laser system used for particle printing and the subsequent corona-restrictions, investigations of wavelength dependencies of second and third harmonic generation from pump wavelength up to 2 µm could not be performed. However, corresponding experiments will be conducted in future work. As alternative laser systems, also picosecond laser systems have been tested for particle printing. With these longer pulses it is necessary to use pre-structured thin-film samples for single-particle printing. Disc-shaped material islands, predominantly from gold, have been realized by different lithographic methods, using anisotropic evaporation and lift-off as processing steps after illumination and development of commercial positive-tone photoresists. The laser molten material is directly captured in PDMS films placed in close contact to the donor substrate. With this approach different highly-ordered nanoparticle arrays with Fano-type resonances have been produced. Comparison of transmission measurements with numerical simulations reveals that the particles are up to 75% inside the PDMS. Nevertheless, the particles remain exactly in the prescribed positions. Laser direct writing and e-beam lithography for island-templated production has enabled realization of highly ordered nanoparticle arrays of square, rectangular, and hexagonal geometries and particle diameters down to 100 nm. Using microscope projection lithography, metasurfaces with focusing properties, consisting of gold particles with 160 nm diameter, having a focal length of 15 µm for a metalens diameter of 40 µm have been demonstrated, in perfect agreement with theoretical simulations. Corresponding simulations of metalens structures from silicon nanoparticle have been performed, where wavelength dependencies of the lens have been studied and different lens structures for various focal lengths have been optimized. Further, highly-ordered particle arrays covering areas of square-centimeters have been realized by multi beam interference lithography (experiments in cooperation with J. Schilling, S. Krause, and P. Miclea, Martin-Luther- Universität Halle-Wittenberg). Sharp Fano resonances have been revealed within arrays of varying particle distances between 300 nm to 800 nm, using transmission measurements in the range between 400 nm to 2500 nm. The huge potential of these metasurfaces for sensing applications has been demonstrated in SERS of 4MBA molecules. Due to the long-term corona restrictions not all intended experiments using LIT-nanoparticle metasurface could have been performed within the project period. In future experiments, metasurface enhanced coherent light generation and amplification effects will be investigated. In conclusion, laser induced transfer and printing of spherical nanoparticles with pronounced electric and magnetic resonances has been demonstrated as a powerful tool for accurately positioning individual particles as well as generating nanoparticle metasurfaces for light control, sensing applications, and nonlinear coherent light sources. The here presented technologies will open new possibilities for the realization of functional and low-cost photonic devices based on LIT-nanoparticles.
Publications
- "Efficient second-harmonic generation in nanocrystalline silicon nanoparticles", Nano LettersS, Vol. 17, Art. no. 5 (2017)
S.V. Makarov, M. I. Petrov, U. Zywietz, V. Milichko, D. Zuev, N. Lopanitsyna, A. Kuksin, I. Mukhin, G. Zograf, E. Ubyivovk∥, D.A. Smirnova, S. Starikov, B.N. Chichkov, Y.S. Kivshar
(See online at https://doi.org/10.1021/acs.nanolett.7b00392) - "Femtosecond laser printing of single Ge and SiGe nanoparticles with electric and magnetic optical resonances" ACS Photonics, Vol. 5, Art. no. 3 (2018)
D.M. Zhigunov, A.B. Evlyukhin, A.S. Shalin, U. Zywietz, B.N. Chichkov
(See online at https://doi.org/10.1021/acsphotonics.7b01275) - "Resonant silicon nanoparticles with controllable crystalline states and nonlinear optical responses", Nanoscale Vol. 10, Art. no. 24 (2018)
S. Makarov, L. Kolotova, S. Starikov, U. Zywietz, B. Chichkov
(See online at https://doi.org/10.1039/C8NR02057D) - Laser Printing of Functional Materials: 3D Microfabrication, Electronics and Biomedicine, Chapter 11, pp. 251-268 (John Wiley & Sons, 2018)
K. U. Zywietz, T. Fischer, A. Evlyukhin, C. Reinhardt, and B. Chichkov
(See online at https://doi.org/10.1002/9783527805105.ch11) - “Experimental Demonstration of Surface Plasmon Polaritons Reflection and Transmission Effects”, Sensors, Vol. 19, Iss. 11, Art. No. 4633 (2019)
L. Zheng, U. Zywietz, A.B. Evlyukhin, B. Roth, L. Overmeyer, C. Reinhardt
(See online at https://doi.org/10.3390/s19214633) - “Nanofabrication of High- Resolution Periodic Structures with a Gap Size Below 100 nm by Two-Photon Polymerization”, Nanoscale Research Letters, Vol. 14, Art. No. 134 (2019)
L. Zhen, K. Kurselis, A. El-Tamer, U. Hinze, C. Reinhardt, L. Overmeyer, B.N. Chichkov
(See online at https://doi.org/10.1186/s11671-019-2955-5) - “Nanoscale Broadband Deep-Ultraviolet Light Source from Plasmonic Nanoholes”, ACS Photonics, Vol. 6, Iss. 4, pp. 858-863 (2019)
L.P.Shi, J.R.C. Andrade, J.M. Yi, M. Mariskas, C. Reinhardt, E. Almeida, U. Morgner, M. Kovacev
(See online at https://doi.org/10.1021/acsphotonics.9b00127) - “Omnidirectional Surface Plasmon Polaritons Concentration in 3D Metallic Structures”, Plasmonics, Vol. 14, Iss. 6, pp. 1547-1554 (2019)
L. Zheng, A.B. Evlyukhin, L. Overmeyer, C. Reinhardt
(See online at https://doi.org/10.1007/s11468-019-00942-9) - “Microscope Projection Photolithography of Polymeric Optical Micro- and Nanocomponents“,Proc. SPIE 112920Q (2020)
L. Zheng, C. Reinhardt, B. Roth
(See online at https://doi.org/10.1117/12.2546679) - “Progressive Self-Boosting Anapole-Enhanced Deep-Ultraviolet Third Harmonic During Few-Cycle Laser Radiation”, ACS Photonics, Vol. 7, Iss. 7, pp. 1655-1661 (2020)
L.P. Shi, A.B. Evlyukhin, C. Reinhardt, I. Babushkin, V.A. Zenin, S. Burger, R. Malureanu, B.N. Chichkov, U. Morgner, M. Kovacev
(See online at https://doi.org/10.1021/acsphotonics.0c00753) - “Laser printing of Au nanoparticles with sub-micron resolution for the fabrication of monochromatic reflectors on stretchable substrates“, Optics and Laser Technology, Vol. 135, Art. No. 1066660 (2021)
F. Zacharatos, M. Duderstadt, E. Almpanis, L.Patsiouras, K. Kurselis, D. Tsoukalas, C. Reinhardt, N. Papanikolaou, B.N. Chichkov, I. Zergioti
(See online at https://doi.org/10.1016/j.optlastec.2020.106660)
