Systematic Study of Amorphous ABC Heterostructures at the Atomic Scale as a Second-Order Nonlinear Optical Metamaterial
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arXiv
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| Main Authors: | , , , , , , , , , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866915731973603328 |
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| author | Mičulka, Martin Liu, Jinsong Beer, Sebastian Rafi, Raihan Sevriukov, Denys Yulin, Sergiy Roddatis, Vladimir Gierth, Stephan Nolte, Stefan Schröder, Sven Staude, Isabelle Tünnermann, Andreas Szeghalmi, Adriana |
| author_facet | Mičulka, Martin Liu, Jinsong Beer, Sebastian Rafi, Raihan Sevriukov, Denys Yulin, Sergiy Roddatis, Vladimir Gierth, Stephan Nolte, Stefan Schröder, Sven Staude, Isabelle Tünnermann, Andreas Szeghalmi, Adriana |
| contents | Systematic exploration of amorphous ABC heterostructures revealed that nanoscale morphological modifications markedly improved their artificial bulk second-order susceptibility. These amorphous birefringent heterostructures were fabricated through plasma-enhanced atomic layer deposition of three oxides, effectively breaking the centrosymmetry on the nanoscale. We observe a dependence of the optical nonlinearity on the thickness variation of three constituent materials, SiO$_2$, TiO$_2$, and Al$_2$O$_3$, ranging from tens of nanometers to the atomic scale, and these thin films exhibit second-order susceptibility at their interfaces. Our findings reveal that the enhancement of nonlinear optical properties is strongly correlated with a high density of layers and superior interface quality, where the interface second-order nonlinearity transitions to bulk-like second-harmonic generation. An effective bulk second-order susceptibility of $χ_{zzz} = 2.0 \pm 0.2$~pm/V at the wavelength of 1032~nm is achieved, comparable to typical values for conventional monocrystalline nonlinear materials. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2509_21583 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Systematic Study of Amorphous ABC Heterostructures at the Atomic Scale as a Second-Order Nonlinear Optical Metamaterial Mičulka, Martin Liu, Jinsong Beer, Sebastian Rafi, Raihan Sevriukov, Denys Yulin, Sergiy Roddatis, Vladimir Gierth, Stephan Nolte, Stefan Schröder, Sven Staude, Isabelle Tünnermann, Andreas Szeghalmi, Adriana Applied Physics Materials Science Optics Systematic exploration of amorphous ABC heterostructures revealed that nanoscale morphological modifications markedly improved their artificial bulk second-order susceptibility. These amorphous birefringent heterostructures were fabricated through plasma-enhanced atomic layer deposition of three oxides, effectively breaking the centrosymmetry on the nanoscale. We observe a dependence of the optical nonlinearity on the thickness variation of three constituent materials, SiO$_2$, TiO$_2$, and Al$_2$O$_3$, ranging from tens of nanometers to the atomic scale, and these thin films exhibit second-order susceptibility at their interfaces. Our findings reveal that the enhancement of nonlinear optical properties is strongly correlated with a high density of layers and superior interface quality, where the interface second-order nonlinearity transitions to bulk-like second-harmonic generation. An effective bulk second-order susceptibility of $χ_{zzz} = 2.0 \pm 0.2$~pm/V at the wavelength of 1032~nm is achieved, comparable to typical values for conventional monocrystalline nonlinear materials. |
| title | Systematic Study of Amorphous ABC Heterostructures at the Atomic Scale as a Second-Order Nonlinear Optical Metamaterial |
| topic | Applied Physics Materials Science Optics |
| url | https://arxiv.org/abs/2509.21583 |