| 1. |
- Bhuyan, Rahul, 1998, et al.
(författare)
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The Rise and Current Status of Polaritonic Photochemistry and Photophysics
- 2023
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Ingår i: Chemical Reviews. - 0009-2665 .- 1520-6890. ; 123:18, s. 10877-10919
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Forskningsöversikt (refereegranskat)abstract
- The interaction between molecular electronic transitions and electromagnetic fields can be enlarged to the point where distinct hybrid light-matter states, polaritons, emerge. The photonic contribution to these states results in increased complexity as well as an opening to modify the photophysics and photochemistry beyond what normally can be seen in organic molecules. It is today evident that polaritons offer opportunities for molecular photochemistry and photophysics, which has caused an ever-rising interest in the field. Focusing on the experimental landmarks, this review takes its reader from the advent of the field of polaritonic chemistry, over the split into polariton chemistry and photochemistry, to present day status within polaritonic photochemistry and photophysics. To introduce the field, the review starts with a general description of light-matter interactions, how to enhance these, and what characterizes the coupling strength. Then the photochemistry and photophysics of strongly coupled systems using Fabry-Perot and plasmonic cavities are described. This is followed by a description of room-temperature Bose-Einstein condensation/polariton lasing in polaritonic systems. The review ends with a discussion on the benefits, limitations, and future developments of strong exciton-photon coupling using organic molecules.
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| 2. |
- Hertzog, Manuel, 1989, et al.
(författare)
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Enhancing Vibrational Light-Matter Coupling Strength beyond the Molecular Concentration Limit Using Plasmonic Arrays
- 2021
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Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 21:3, s. 1320-1326
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Tidskriftsartikel (refereegranskat)abstract
- Vibrational strong coupling is emerging as a promising tool to modify molecular properties by making use of hybrid light-matter states known as polaritons. Fabry-Perot cavities filled with organic molecules are typically used, and the molecular concentration limits the maximum reachable coupling strength. Developing methods to increase the coupling strength beyond the molecular concentration limit are highly desirable. In this Letter, we investigate the effect of adding a gold nanorod array into a cavity containing pure organic molecules using FT-IR microscopy and numerical modeling. Incorporation of the plasmonic nanorod array that acts as artificial molecules leads to an order of magnitude increase in the total coupling strength for the cavity with matching resonant frequency filled with organic molecules. Additionally, we observe a significant narrowing of the plasmon line width inside the cavity. We anticipate that these results will be a step forward in exploring vibropolaritonic chemistry and may be used in plasmon based biosensors.
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| 3. |
- Yang, Yizhou, 1992, et al.
(författare)
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A Highly Conductive All-Carbon Linked 3D Covalent Organic Framework Film
- 2021
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Ingår i: Small. - : Wiley. - 1613-6810 .- 1613-6829. ; 17:40
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Tidskriftsartikel (refereegranskat)abstract
- Here an all-carbon linked 3D covalent organic framework (COF) is introduced by employing a templated surface reaction in a continuous flow (TSRCF). The presented method of synthesis provides spatial control over the reaction chemistry and allows for the creation of ultrasmooth COF films of desired thickness and significant crystallinity. The films show high electrical conductivity (approximate to 3.4 S m(-1)) after being doped with tetracyanoquinodimethane (TCNQ), setting a new record for 3D COF materials. The concurrence of 3D nanosized channels and high conductivity opens up for a number of hitherto unexplored applications for this class of materials, such as high surface area electrodes, electrochemical transistors, and for electronic sensing.
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| 4. |
- Yang, Yizhou, 1992, et al.
(författare)
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A self-standing three-dimensional covalent organic framework film
- 2023
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 14:1
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Tidskriftsartikel (refereegranskat)abstract
- Covalent crystals such as diamonds are a class of fascinating materials that are challenging to fabricate in the form of thin films. This is because spatial kinetic control of bond formation is required to create covalently bonded crystal films. Directional crystal growth is commonly achieved by chemical vapor deposition, an approach that is hampered by technical complexity and associated high cost. Here we report on a liquid-liquid interfacial approach based on physical-organic considerations to synthesize an ultrathin covalent crystal film. By distributing reactants into separate phases using hydrophobicity, the chemical reaction is confined to an interface that orients the crystal growth. A molecular-smooth interface combined with in-plane isotropic conditions enables the synthesis of films on a centimeter size scale with a uniform thickness of 13 nm. The film exhibits considerable mechanical robustness enabling a free-standing length of 37 µm, as well as a clearly anisotropic chemical structure and crystal lattice alignment.
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| 5. |
- Albinsson, Bo, 1963, et al.
(författare)
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Functionalized DNA Nanostructures for Light Harvesting and Charge Separation
- 2012
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Ingår i: Coordination Chemistry Reviews. - : Elsevier BV. - 0010-8545. ; 256:21-22, s. 2399-2413
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Forskningsöversikt (refereegranskat)abstract
- Mimicking natural photosynthesis by covalently arranging antenna and charge separation units is a formidable task. Many such beautiful supramolecular complexes have been designed and synthesized with large efforts, some of which are presented in this special issue. The ability to predict relative position of and electronic coupling between the active components in covalent arrays is quite high but there are two obvious drawbacks with the covalent approach. Firstly, as the size grows the complexity of the organic synthesis increases and secondly, sensitivity to light-induced damage becomes a major issue if covalent bonds are broken. Self-assembly of the photoactive components should, in principle, provide a solution to both these issues but generally the ability to predict position and electronic coupling is too low to have the designed properties needed for a functional artificial photosynthetic complex. Here, we present an approach of using DNA as a template for arranging both charge separation units and antenna molecules that govern long-range energy transfer. Of particular interest is the ability of DNA to function as a scaffold for chromophores, either through covalent attachment, or through non-covalent association by means of intercalation or grove binding. Using controlled positioning of dyes, multichromophoric assemblies can be created, capable of long range communication through multi-step energy transfer. This facilitates creation of DNA-based photonic devices for both light harvesting and directed information transfer. The channeled excitation energy can be transformed site specifically to chemical energy by charge separation of DNA linked porphyrins. A two phase system is discussed, in which the DNA is located in buffered solution whereas the hydrophobic porphyrins, responsible for the charge separation reaction, are located in the lipid bilayer of liposomes or supported lipid bilayers.
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| 6. |
- Appelqvist, Hanna, et al.
(författare)
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Specific Imaging of Intracellular Lipid Droplets Using a Benzothiadiazole Derivative with Solvatochromic Properties
- 2017
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Ingår i: Bioconjugate Chemistry. - : American Chemical Society (ACS). - 1043-1802 .- 1520-4812. ; 28:5, s. 1363-1370
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Tidskriftsartikel (refereegranskat)abstract
- Altered lipid metabolism and extensive lipid storage in cells have been associated with various medical disorders, including cancer. The development of fluorescent probes that specifically accumulate in lipid deposits is therefore of great interest in order to study pathological processes that are linked to dysregulated lipogenesis. In the present study, we present a small fluorescent benzothiadiazole dye that specifically stains lipid droplets in living and fixated cells. The photophysical characterization of the probe revealed strong solvatochromic behavior, large Stokes shifts, and high fluorescent quantum yields in hydrophobic solvents. In addition, the fluorophore exhibits a nontoxic profile and a high signal-to-noise ratio in cells (i.e., lipid droplets vs cytosol), which make it an excellent candidate for studying lipid biology using confocal fluorescent microscopy.
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| 7. |
- Bahsoun, H., et al.
(författare)
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Electronic Light-Matter Strong Coupling in Nanofluidic Fabry-Pérot Cavities
- 2018
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Ingår i: ACS Photonics. - : American Chemical Society (ACS). - 2330-4022. ; 5:1, s. 225-232
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Tidskriftsartikel (refereegranskat)abstract
- Electronic light-matter strong coupling has been limited to solid molecular films due to the challenge of preparing optical cavities with nanoscale dimensions. Here we report a technique to fabricate such Fabry-Pérot nanocavities in which solutions can be introduced such that light-molecule interactions can be studied at will in the liquid phase. We illustrate the versatility of these cavities by studying the emission properties of Chlorin e6 solutions in both the weak and strong coupling regimes as a function of cavity detuning. Liquid nanocavities will broaden the investigation of strong coupling to many solution-based molecular processes. © 2017 American Chemical Society.
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| 8. |
- Bharmoria, Pankaj, 1985, et al.
(författare)
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Recyclable optical bioplastics platform for solid state red light harvesting via triplet-triplet annihilation photon upconversion
- 2022
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7496 .- 2050-7488. ; 10:40, s. 21279-21290
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Tidskriftsartikel (refereegranskat)abstract
- Sustainable photonics applications of solid-state triplet-triplet annihilation photon upconversion (TTA-UC) are limited by a small UC spectral window, low UC efficiency in air, and non-recyclability of polymeric materials used. In a step to overcome these issues, we have developed new recyclable TTA-UC bioplastics by encapsulating TTA-UC chromophores liquid inside the semicrystalline gelatin films showing broad-spectrum upconversion (red/far-red to blue) with high UC efficiency in air. For this, we synthesized a new anionic annihilator, sodium-TIPS-anthracene-2-sulfonate (TIPS-AnS), that combined with red/far-red sensitizers (PdTPBP/Os(m-peptpy)(2)(TFSI)(2)), a liquid surfactant Triton X-100 reduced (TXr) and protein gelatin (G) formed red/far-red to blue TTA-UC bioplastic films just by air drying of their aqueous solutions. The G-TXr-TIPS-AnS-PdTPBP film showed record red to blue (633 to 478 nm) TTA-UC quantum yield of 8.5% in air. The high UC quantum yield has been obtained due to the fluidity of dispersed TXr containing chromophores and oxygen blockage by gelatin fibers that allowed efficient diffusion of triplet excited chromophores. Further, the G-TXr-TIPS-AnS-Os(m-peptpy)(2)(TFSI)(2) bioplastic film displayed far-red to blue (700-730 nm to 478 nm) TTA-UC, demonstrating broad-spectrum photon harvesting. Finally, we demonstrated the recycling of G-TXr-TIPS-AnS-PdTPBP bioplastics by developing a downstream approach that gives new directions for designing future recyclable photonics bioplastic materials.
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| 9. |
- Bhuyan, Rahul, 1998, et al.
(författare)
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The Effect of the Relative Size of the Exciton Reservoir on Polariton Photophysics
- 2024
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Ingår i: Advanced Optical Materials. - 2195-1071. ; 12:2
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Tidskriftsartikel (refereegranskat)abstract
- Strong interactions between excitons and photons lead to the formation of exciton-polaritons, which possess different properties compared to their constituents. Polaritons are created by incorporating a dye in an optical cavity where the electromagnetic field is tightly confined. The interest in the subject has exploded in recent years due to the ability to change (photo)chemistry, but still as simple a variable as the yield of emission varies between studies. For the field to progress, linking observables to system parameters is a dire need. Here, the study pairs emission yield to the size of the so-called exciton reservoir, which dictates polariton relaxation dynamics. To do this, a method is devised to experimentally control the relative size of the exciton reservoir and link it to the yield of emission. Thus, the results enable comparison of the photophysics of previous studies within the field and provide the tools to study the effect of the exciton reservoir on polariton photochemistry. Polaritons are created by incorporating a dye in an optical cavity. Here, the study pairs the emission yield to the size of the so-called exciton reservoir, which dictates polariton relaxation dynamics. To do this, a method is devised to experimentally control the relative size of the exciton reservoir and link it to the yield of emission.image
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| 10. |
- Börjesson, Karl, 1982, et al.
(författare)
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A Bioinspired Self Assembled Dimeric Porphyrin Pocket that Binds Electron Accepting Ligands
- 2012
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Ingår i: Chemical Communications. - : Royal Society of Chemistry (RSC). - 1364-548X .- 1359-7345. ; 48:12, s. 1793-1795
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Tidskriftsartikel (refereegranskat)abstract
- A binding pocket consisting of two zinc porphyrins self assembled by Watson-Crick base pairing is presented. The porphyrin binding pocket is located in the confined environment of a lipid membrane whereas the DNA is located in the water phase. Bidentate electron accepting ligands are shown to coordinate in-between the two porphyrins.
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