1. |
- Gözen, Irep, 1980, et al.
(author)
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Protocells: Milestones and Recent Advances
- 2022
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In: Small. - : Wiley. - 1613-6810 .- 1613-6829. ; 18:18
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Research review (peer-reviewed)abstract
- The origin of life is still one of humankind's great mysteries. At the transition between nonliving and living matter, protocells, initially featureless aggregates of abiotic matter, gain the structure and functions necessary to fulfill the criteria of life. Research addressing protocells as a central element in this transition is diverse and increasingly interdisciplinary. The authors review current protocell concepts and research directions, address milestones, challenges and existing hypotheses in the context of conditions on the early Earth, and provide a concise overview of current protocell research methods.
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2. |
- Katke, C., et al.
(author)
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Colony-like Protocell Superstructures
- 2023
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In: Acs Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 17:4, s. 3368-3382
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Journal article (peer-reviewed)abstract
- We report the formation, growth, and dynamics of model protocell superstructures on solid surfaces, resembling single cell colonies. These structures, consisting of several layers of lipidic compartments enveloped in a dome-shaped outer lipid bilayer, emerged as a result of spontaneous shape transformation of lipid agglomerates deposited on thin film aluminum surfaces. Collective protocell structures were observed to be mechanically more stable compared to isolated spherical compartments. We show that the model colonies encapsulate DNA and accommodate nonenzymatic, strand displacement DNA reactions. The membrane envelope is able to disassemble and expose individual daughter protocells, which can migrate and attach via nano tethers to distant surface locations, while maintaining their encapsulated contents. Some colonies feature "exocompartments", which spontaneously extend out of the enveloping bilayer, internalize DNA, and merge again with the superstructure. A continuum elastohydrodynamic theory that we developed suggests that a plausible driving force behind subcompartment formation is attractive van der Waals (vdW) interactions between the membrane and surface. The balance between membrane bending and vdW interactions yields a critical length scale of 236 nm, above which the membrane invaginations can form subcompartments. The findings support our hypotheses that in extension of the "lipid world hypothesis", protocells may have existed in the form of colonies, potentially benefiting from the increased mechanical stability provided by a superstructure.
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3. |
- Kuttruff, Joel, et al.
(author)
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Broadband tuning of the magneto-optical response of hybrid metal-insulator nanoparticles enabled by hyperbolic electric and magnetic modes
- 2021
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Conference paper (peer-reviewed)abstract
- In the framework of magneto-photonics, the optical properties of a material can controlled by an external magnetic field, providing active functionalities for applications, such as sensing and nonreciprocal optical isolation. For noble metals in particular, the inherently weak magnetooptical coupling of the bulk material can be greatly enhanced via excitation of localized surface plasmons (LSP) in nanostructured samples. Hyperbolic metamaterials therein provide the ideal platform to tune the plasmonic properties via careful design of the effective permittivity tensor. Here, we report on the magnetic circular dichroism of electric and magnetic dipole modes of a type II hyperbolic metasurface. Disk-shaped nanoparticles consist in stacks of alternating dielectric and metallic layers. Using an effective medium theory, we show that the optical properties of the system can be perfectly described by an anisotropic homogenized permittivity. Magnetic circular dichroism spectroscopy experiments are compared with plain gold disk samples and reveal a broadband magneto-optical response across the visible and near infrared spectral range. In particular, derivative-like spectral signatures at the resonances of the nanoparticles prove the induced dichroism for the two modes of the system. Results are interpreted in terms of magnetically induced spatial confinement/broadening of circular currents in the nanoparticles and are compared with a comprehensive numerical model based on the finite elements method using the real dimensions of the nanostructure. Spherical particles are employed as an analytical model system, allowing to generalize the contribution of electric and magnetic modes to the total magneto-optical response. More in detail, interaction cross sections are calculated as a weighted sum of the corresponding Mie coefficients. Utilizing a perturbative approach, we describe the magneto-optical effect in terms of linear changes in the cyclotron frequency of free charge carriers in the metal. By comparing our analytical model with full-wave numerical results, we can identify the contribution of electric and magnetic dipole modes to the spectrum and reproduce the spectral line shape we observe in the experiments for the hyperbolic nanoparticles.
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4. |
- Kuttruff, Joel, et al.
(author)
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Magneto-Optical Activity in Nonmagnetic Hyperbolic Nanoparticles
- 2021
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In: Physical Review Letters. - : American Physical Society. - 0031-9007 .- 1079-7114. ; 127
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Journal article (peer-reviewed)abstract
- Active nanophotonics can be realized by controlling the optical properties of materials with external magnetic fields. Here, we explore the influence of optical anisotropy on the magneto-optical activity in nonmagnetic hyperbolic nanoparticles. We demonstrate that the magneto-optical response is driven by the hyperbolic dispersion via the coupling of metallic-induced electric and dielectric-induced magnetic dipolar optical modes with static magnetic fields. Magnetic circular dichroism experiments confirm the theoretical predictions and reveal tunable magneto-optical activity across the visible and near infrared spectral range.
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5. |
- Kuttruff, Joel, et al.
(author)
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Magneto-Optical Activity in Nonmagnetic Hyperbolic Nanoparticles
- 2021
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In: Physical Review Letters. - : American Physical Society. - 0031-9007 .- 1079-7114. ; 127:21
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Journal article (peer-reviewed)abstract
- Active nanophotonics can be realized by controlling the optical properties of materials with external magnetic fields. Here, we explore the influence of optical anisotropy on the magneto-optical activity in nonmagnetic hyperbolic nanoparticles. We demonstrate that the magneto-optical response is driven by the hyperbolic dispersion via the coupling of metallic-induced electric and dielectric-induced magnetic dipolar optical modes with static magnetic fields. Magnetic circular dichroism experiments confirm the theoretical predictions and reveal tunable magneto-optical activity across the visible and near infrared spectral range.
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6. |
- Kuttruff, Joel, et al.
(author)
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Magneto-optics in hyperbolic nanomaterials
- 2021
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Conference paper (peer-reviewed)abstract
- Hyperbolic nanoparticles provide a versatile platform to widely tune light-matter interactions. Active nanophotonics can be realized by controlling the optical properties of materials with external magnetic fields. Here, we explore the influence of optical anisotropy on the magneto-optical response of hyperbolic nanoparticles across the visible and near infrared spectral range. By using a perturbative approach, we establish a model where the magneto-optical activity of the system is described in terms of the coupling of fundamental electric and magnetic dipole modes, which are induced by the hyperbolic dispersion, with a static magnetic field. Finally, an analytical model is established in the framework of Mie theory to describe the magneto-optical response and identify the contribution of electric and magnetic modes to the total spectrum.
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7. |
- Kuttruff, Joel, et al.
(author)
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Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas
- 2023
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In: Nature Communications. - : Springer Nature. - 2041-1723 .- 2041-1723. ; 14:1
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Journal article (peer-reviewed)abstract
- Molecular polaritons are hybrid light-matter states that emerge when a molecular transition strongly interacts with photons in a resonator. At optical frequencies, this interaction unlocks a way to explore and control new chemical phenomena at the nanoscale. Achieving such control at ultrafast timescales, however, is an outstanding challenge, as it requires a deep understanding of the dynamics of the collectively coupled molecular excitation and the light modes. Here, we investigate the dynamics of collective polariton states, realized by coupling molecular photoswitches to optically anisotropic plasmonic nanoantennas. Pump-probe experiments reveal an ultrafast collapse of polaritons to pure molecular transition triggered by femtosecond-pulse excitation at room temperature. Through a synergistic combination of experiments and quantum mechanical modelling, we show that the response of the system is governed by intramolecular dynamics, occurring one order of magnitude faster with respect to the uncoupled excited molecule relaxation to the ground state.
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8. |
- Kuttruff, Joel, et al.
(author)
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Ultrafast Dynamics of Molecular Polaritons in Photoswitch Nanoantennas
- 2023
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In: 2023 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2023. - : Institute of Electrical and Electronics Engineers (IEEE). - 9798350345995
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Conference paper (peer-reviewed)abstract
- We study ultrafast dynamics of photocromic molecules both weakly and strongly coupled to plasmonic nanoantennas. Experiments, verified by quantum modelling, reveal subps collapse of molecular polaritons to intramolecular dynamics induced by interaction with the plasmons.
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