Photonics / Fotonik
Permanent URI for this collectionhttps://hdl.handle.net/11147/2590
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Article Citation - WoS: 7Citation - Scopus: 7Breaking the Boundaries of the Goldschmidt Tolerance Factor With Ethylammonium Lead Iodide Perovskite Nanocrystals(American Chemical Society, 2024) Güvenç, Çetin Meriç; Toso, Stefano; Ivanov, Yurii P.; Saleh, Gabriele; Balcı, Sinan; Divitini, Giorgio; Manna, LiberatoWe report the synthesis of ethylammonium lead iodide (EAPbI3) colloidal nanocrystals as another member of the lead halide perovskites family. The insertion of an unusually large A-cation (274 pm in diameter) in the perovskite structure, hitherto considered unlikely due to the unfavorable Goldschmidt tolerance factor, results in a significantly larger lattice parameter compared to the Cs-, methylammonium- and formamidinium-based lead halide perovskite homologues. As a consequence, EAPbI3 nanocrystals are highly unstable, evolving to a nonperovskite delta-EAPbI3 polymorph within 1 day. Also, EAPbI3 nanocrystals are very sensitive to electron irradiation and quickly degrade to PbI2 upon exposure to the electron beam, following a mechanism similar to that of other hybrid lead iodide perovskites (although degradation can be reduced by partially replacing the EA+ ions with Cs+ ions). Interestingly, in some cases during this degradation the formation of an epitaxial interface between (EA x Cs1-x )PbI3 and PbI2 is observed. The photoluminescence emission of the EAPbI3 perovskite nanocrystals, albeit being characterized by a low quantum yield (similar to 1%), can be tuned in the 664-690 nm range by regulating their size during the synthesis. The emission efficiency can be improved upon partial alloying at the A site with Cs+ or formamidinium cations. Furthermore, the morphology of the EAPbI3 nanocrystals can be chosen to be either nanocube or nanoplatelet, depending on the synthesis conditions.Article Citation - WoS: 9Citation - Scopus: 9Non-Hermitian Hamiltonians for Linear and Nonlinear Optical Response: a Model for Plexcitons(AIP Publishing LLC, 2023) Finkelstein-Shapiro, Daniel; Mante, Pierre-Adrien; Balcı, Sinan; Zigmantas, Donatas; Pullerits, TonuIn polaritons, the properties of matter are modified by mixing the molecular transitions with light modes inside a cavity. Resultant hybrid light-matter states exhibit energy level shifts, are delocalized over many molecular units, and have a different excited-state potential energy landscape, which leads to modified exciton dynamics. Previously, non-Hermitian Hamiltonians have been derived to describe the excited states of molecules coupled to surface plasmons (i.e., plexcitons), and these operators have been successfully used in the description of linear and third order optical response. In this article, we rigorously derive non-Hermitian Hamiltonians in the response function formalism of nonlinear spectroscopy by means of Feshbach operators and apply them to explore spectroscopic signatures of plexcitons. In particular, we analyze the optical response below and above the exceptional point that arises for matching transition energies for plasmon and molecular components and study their decomposition using double-sided Feynman diagrams. We find a clear distinction between interference and Rabi splitting in linear spectroscopy and a qualitative change in the symmetry of the line shape of the nonlinear signal when crossing the exceptional point. This change corresponds to one in the symmetry of the eigenvalues of the Hamiltonian. Our work presents an approach for simulating the optical response of sublevels within an electronic system and opens new applications of nonlinear spectroscopy to examine the different regimes of the spectrum of non-Hermitian Hamiltonians.Article Citation - WoS: 17Citation - Scopus: 19Strong Coupling of Carbon Quantum Dots in Liquid Crystals(American Chemical Society, 2022) Sarısözen, Sema; Polat, Nahit; Mert Balcı, Fadime; Güvenç, Çetin Meriç; Kocabaş, Çoşkun; Yağlıoğlu, Halime Gül; Balcı, SinanCarbon quantum dots (CDs) have recently received a tremendous amount of interest owing to their attractive optical properties. However, CDs have broad absorption and emission spectra limiting their application ranges. We herein, for the first time, show synthesis of water-soluble red emissive CDs with a very narrow line width (∼75 meV) spectral absorbance and hence demonstrate strong coupling of CDs and plasmon polaritons in liquid crystalline mesophases. The excited state dynamics of CDs has been studied by ultrafast transient absorption spectroscopy, and CDs display very stable and strong photoluminescence emission with a quantum yield of 35.4% and a lifetime of ∼2 ns. More importantly, we compare J-aggregate dyes with CDs in terms of their absorption line width, photostability, and ability to do strong coupling, and we conclude that highly fluorescent CDs have a bright future in the mixed light-matter states for emerging applications in future quantum technologies.Article Citation - WoS: 35Citation - Scopus: 36Understanding Radiative Transitions and Relaxation Pathways in Plexcitons(Cell Press, 2021) Finkelstein-Shapiro, Daniel; Mante, Pierre-Adrien; Sarısözen, Sema; Wittenbecher, Lukas; Minda, Iulia; Balcı, Sinan; Pullerits, TonuMolecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.Article Citation - WoS: 192Citation - Scopus: 194Multispectral Graphene-Based Electro-Optical Surfaces With Reversible Tunability From Visible To Microwave Wavelengths(Nature Research, 2021) Ergoktas, M. Said; Bakan, Gökhan; Kovalska, Evgeniya; Le Fevre, Lewis W.; Fields, Richard P.; Steiner, Pietro; Yu, Xiaoxiao; Balcı, SinanOptical materials with colour changing abilities have been explored for use in display devices(1), smart windows(2,3) or in the modulation of visual appearance(4-6). The efficiency of these materials, however, has strong wavelength dependence, which limits their functionality to a specific spectral range. Here, we report graphene-based electro-optical devices with unprecedented optical tunability covering the entire electromagnetic spectrum from the visible to microwave. We achieve this non-volatile and reversible tunability by electro-intercalation of lithium into graphene layers in an optically accessible device structure. The unique colour changing capability, together with area-selective intercalation, inspires the fabrication of new multispectral devices, including display devices and electro-optical camouflage coating. We anticipate that these results provide realistic approaches for programmable smart optical surfaces with a potential utility in many scientific and engineering fields such as active plasmonics and adaptive thermal management.Article Citation - WoS: 12Citation - Scopus: 14Laser Assisted Synthesis of Anisotropic Metal Nanocrystals and Strong Light-Matter Coupling in Decahedral Bimetallic Nanocrystals(Royal Society of Chemistry, 2021) Mert Balcı, Fadime; Sarısözen, Sema; Polat, Nahit; Güvenç, Çetin Meriç; Karadeniz, Uğur; Tertemiz, Necip Ayhan; Balcı, SinanThe advances in colloid chemistry and nanofabrication allowed us to synthesize noble monometallic and bimetallic nanocrystals with tunable optical properties in the visible and near infrared region of the electromagnetic spectrum. In the strong coupling regime, surface plasmon polaritons (SPPs) of metal nanoparticles interact with excitons of quantum dots or organic dyes and plasmon-exciton hybrid states called plexcitons are formed. Until now, various shaped metal nanoparticles such as nanorods, core-shell nanoparticles, hollow nanoparticles, nanoprisms, nanodisks, nanorings, and nanobipyramids have been synthesized to generate plasmon-exciton mixed states. However, in order to boost plasmon-exciton interaction at nanoscale dimensions and expand the application of plexcitonic nanocrystals in a variety of fields such as solar cells, light emitting diodes, and nanolasers, new plexcitonic nanocrystals with outstanding optical and chemical properties remain a key goal and challenge. Here we report laser-assisted synthesis of decahedral shaped noble metal nanocrystals, tuning optical properties of the decahedral shaped nanocrystals by galvanic replacement reactions, colloidal synthesis of bimetallic decahedral shaped plexcitonic nanocrystals, and strong plasmon-plasmon interaction in bimetallic decahedral shaped noble metal nanocrystals near a metal film. We photochemically synthesize decahedral Ag nanoparticles from spherical silver nanoparticles by using a 488 nm laser. The laser assisted synthesis of silver nanoparticles yields decahedral (bicolored) and prism (monocolored) shaped silver nanocrystals. The decahedral shaped nanoparticles were selectively separated from prism shaped nanoparticles by centrifugation. The optical properties of decahedral nanocrystals were tuned by the galvanic replacement reaction between gold ions and silver atoms. Excitons of J-aggregate dyes and SPPs of decahedral bimetallic nanoparticles strongly couple and hence decahedral shaped plexcitonic nanoparticles are prepared. In addition, localized SPPs of decahedral shaped bimetallic nanocrystals interact strongly with the propagating SPPs of a flat silver film and hence new hybrid plasmonic modes (plasmonic nanocavities) are generated. The experimental results are further fully corroborated by theoretical calculations including decahedral shaped plexcitonic nanoparticles and decahedral nanoparticles coupled to flat metal films.Article Citation - WoS: 13Citation - Scopus: 15Hybrid J-aggregate-graphene phototransistor(American Chemical Society, 2020) Yakar, Ozan; Balcı, Osman; Uzlu, Burkay; Polat, Nahit; Arı, Ozan; Tunç, İlknur; Balcı, SinanJ-aggregates are fantastic self-assembled chromophores with a very narrow and extremely sharp absorbance band in the visible and near-infrared spectrum, and hence they have found many exciting applications in nonlinear optics, sensing, optical devices, photography, and lasing. In silver halide photography, for example, they have enormously improved the spectral sensitivity of photographic process due to their fast and coherent energy migration ability. On the other hand, graphene, consisting of single layer of carbon atoms forming a hexagonal lattice, has a very low absorption coefficient. Inspired by the fact that J-aggregates have carried the role to sense the incident light in silver halide photography, we would like to use Jaggregates to increase spectral sensitivity of graphene in the visible spectrum. Nevertheless, it has been an outstanding challenge to place isolated J-aggregate films on graphene to extensively study interaction between them. We herein noncovalently fabricate isolated J-aggregate thin films on graphene by using a thin film fabrication technique we termed here membrane casting (MC). MC significantly simplifies thin film formation of water-soluble substances on any surface via porous polymer membrane. Therefore, we reversibly modulate the Dirac point of graphene in the J-aggregate/graphene van der Waals (vdW) heterostructure and demonstrate an all-carbon phototransistor gated by visible light. Owing to the hole transfer from excited excitonic thin film to graphene layer, graphene is hole-doped. In addition, spectral and power responses of the all-carbon phototransistor have been measured by using a tunable laser in the visible spectrum. The first integration of J-aggregates with graphene in a transistor structure enables one to reversibly write and erase charge doping in graphene with visible light that paves the way for using J-aggregate/graphene vdW heterostructures in optoelectronic applications.Article Citation - WoS: 5Citation - Scopus: 5Large Rabi Splitting of Mixed Plasmon-Exciton States in Small Plasmonic Moire Cavities(The Optical Society, 2020) Ateş, Simge; Karademir, Ertuğrul; Balcı, Sinan; Kocabaş, Coşkun; Aydınlı, Atilla; Ateş, Simge; Ateş, Simge; Karademir, Ertuğrul; Karademir, Ertuğrul; Balcı, Sinan; Balcı, Sinan; Kocabaş, Coşkun; Kocabaş, Coşkun; Aydınlı, Atilla; Aydınlı, AtillaWe report on exciton-plasmon coupling in metallic moire cavities, both numerically and experimentally. Moire cavities fabricated using double exposure laser interference lithography were filled with a molecular dye, J-aggregate. Polarization-dependent spectroscopic reflection measurements supported by simulations reveal strong coupling of organic dye excitons with cavity modes of the plasmonic moire cavities. An anti-crossing at zero detuning, a clear indication of strong coupling, has been observed when the excitonic absorption band resonates with the cavity mode. LargeRabi splitting energies owing to the strong coupling of plasmons and excitons are clearly observed. (C) 2020 Optical Society of AmericaArticle Citation - WoS: 13Citation - Scopus: 14Strong Plasmon-Exciton Coupling in Colloidal Halide Perovskite Nanocrystals Near a Metal Film(Royal Society of Chemistry, 2020) Güvenç, Çetin Meriç; Polat, Nahit; Balcı, SinanAll inorganic colloidal halide perovskite nanoplatelets and nanowires are highly anisotropic shaped semiconductor nanocrystals with highly tunable optical properties in the visible spectrum. These nanocrystals have large exciton binding energies and high oscillator strengths due to their strongly quantum confined natures. The optical properties of the halide perovskites are tunable by variation of halide composition and morphology of the nanocrystals. We herein demonstrate that colloidal perovskite nanocrystals (NCs) placed in close proximity to chemically functionalized metal films show mixed plasmon-exciton formation, plexciton formation, in the strong coupling regime. The optical properties of all-inorganic lead halide perovskite NCs were controlled by colloidally synthesizing NCs with different morphologies such as nanowires and nanoplatelets or by controlling the composition of the halides in the NCs. The experimentally observed Rabi splitting energies are around 90 meV, 70 meV, and 55 meV for CsPbI3 nanoplatelets, CsPbI3 nanowires, and CsPb(Br/I)(3) nanoplatelets, respectively. In addition, the numerical simulations are in good agreement with the experimentally obtained data. The results show that colloidal all-inorganic halide perovskite NCs are promising and strong candidates for studying light-matter interaction at nanoscale dimension.Article Citation - WoS: 9Citation - Scopus: 9Fourier Transform Plasmon Resonance Spectrometer Using Nanoslit-Nanowire Pair(American Institute of Physics, 2019) Uulu, Doolos Aibek; Ashirov, Timur; Polat, Nahit; Yakar, Ozan; Balcı, Sinan; Kocabaş, CoşkunIn this paper, we present a nanoscale Fourier transform spectrometer using a plasmonic interferometer consisting of a tilt subwavelength slit-nanowire pair on a metallic surface fabricated by the focused ion beam microfabrication technique. The incident broadband light strongly couples with the surface plasmons on the gold surface, and thus, surface plasmon polaritons (SPPs) are generated. The launched SPPs interfere with the incident light and generate high contrast interference fringes in the nanoslit. The transmitted SPPs through the metal nanoslit can decouple into free space and are collected by an objective in the far field. The spectroscopic information of the incidence light is obtained by fast Fourier transform of the fringe pattern of the SPPs. In our design, there is no need for a bulky dispersive spectrometer or dispersive optical elements. The dimension of the spectrometer is around 200 mu m length. Our design is based on inherent coherence of the SPP waves propagating through the subwavelength metal nanoslit structures etched into an opaque gold film.