| 1. |
- Chaudhary, Shilpi, et al.
(författare)
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Adsorption of 3-(triethoxysilyl)propionitrile on a rutile TiO2(110) surface : An X-ray photoelectron spectroscopy study
- 2020
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Ingår i: DAE Solid State Physics Symposium 2019. - : AIP Publishing. - 1551-7616 .- 0094-243X. - 9780735420250 ; 2265
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Konferensbidrag (refereegranskat)abstract
- The adsorption of 3-(triethoxysilyl)propionitrile (TESP) on a reduced rutile TiO2(110) surface has been investigated using synchrotron-based X-ray photoelectron spectroscopy in ultrahigh vacuum (UHV). We have studied TESP adsorption on two surface preparation of rutile TiO2 (110) to explore the role of surface defects. In the first preparation, the adsorption of TESP was studied on reduced TiO2 (110) surface at room temperature. In the second experiment TESP was adsorbed on the oxygen-treated TiO2 surface to quench the oxygen vacancies generated by UHVannealing of the TiO2 crystal. The molecular footprints of the TESP molecules confirms the adsorption on both types of TiO2(110) surfaces. In the case of the reduced surface, temperature-dependent XPS measurements show the thermal stability of TESP molecules up to 600 °C. The comparison of the nitrogen and carbon lineshapes for both preparations suggests different adsorption geometries on the reduced and oxygen-dosed surfaces. To the best of our knowledge, the UHV preparations and measurements of TESP adsorption on rutile TiO2 (110) in the present study are reported for the first time.
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| 2. |
- Chaudhary, Shilpi, et al.
(författare)
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Controlled short-linkage assembly of functional nano-objects
- 2014
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Ingår i: Applied Surface Science. - : Elsevier BV. - 1873-5584 .- 0169-4332. ; 300, s. 22-28
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Tidskriftsartikel (refereegranskat)abstract
- In this work, we report a method that allows the deterministic, photo-controlled covalent assembly of nanoparticles directly on surface. As a model system, we study the conjugation of molecularly imprinted polymer (MIP) nanoparticles on a glass surface and confirm that the immobilized nanoparticles maintain their molecular recognition functionality. The glass slide was first modified with perfluorophenylazide and then used to bind MIP nanoparticles under UV irradiation. After each step the surface was analyzed by water contact angle measurement, fluorescence microscopy, scanning electron microscopy, and/or synchrotron-based X-ray photoelectron spectroscopy. The MIP nanoparticles immobilized on the glass surface remained stable and maintained specific binding for the template molecule, propranolol. The method developed in this work allows MIP nanoparticles to be directly coupled to a flat surface, offering a straightforward means to construct robust chemical sensors. Using the reported photo conjugation method, it is possible to generate patterned assembly of nanoparticles using a photomask. Since perfluorophenylazide-based photochemistry works with all kinds of organic material, the method developed in this work is expected to enable immobilization of not only MIPs but also other kinds of organic and inorganic-organic core-shell particles for various applications involving photon or electron transfer. (C) 2014 The Authors. Published by Elsevier B.V. All rights reserved.
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| 3. |
- Chaudhary, Shilpi, et al.
(författare)
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Real-Time Study of CVD Growth of Silicon Oxide on Rutile TiO2(110) Using Tetraethyl Orthosilicate
- 2015
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 119:33, s. 19149-19161
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Tidskriftsartikel (refereegranskat)abstract
- The interaction of the ruffle TiO2(110) surface with tetraethyl orthosilicate (TEOS) in the pressure range from UHV to 1 mbar as well as the TEOS-based chemical vapor deposition of SiO2 on the TiO2(110) surface were monitored in real time using near-ambient pressure X-ray photoelectron spectroscopy. The experimental data and density functional theory calculations confirm the dissociative adsorption of TEOS on the surface already at room temperature. At elevated pressure, the ethoxy species formed in the adsorption process undergoes further surface reactions toward a carboxyl species not observed in the absence of a TEOS gas phase reservoir. Annealing of the adsorption layer leads to the formation of SiO2, and an intermediate oxygen species assigned to a mixed titanium/silicon oxide is identified. Atomic force microscopy confirms the morphological changes after silicon oxide formation.
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| 4. |
- Forchheimer, Daniel, et al.
(författare)
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Molecularly imprinted nanostructures by nanoimprint lithography
- 2010
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Ingår i: Analyst. - : Royal Society of Chemistry (RSC). - 1364-5528. ; 135:6, s. 1219-1223
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Tidskriftsartikel (refereegranskat)abstract
- Simultaneous imprinting on two length scales (nanometer and ångström) delivers highly specific molecular recognition sites in polymer patterns.
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| 5. |
- Forchheimer, Daniel, et al.
(författare)
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Molecularly selective nanopatterns using nanoimprint lithography : A label-free sensor architecture
- 2011
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Ingår i: Journal of Vacuum Science and Technology B. - : AVS Science and Technology Society. - 2166-2746 .- 2166-2754. ; 29:1
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Tidskriftsartikel (refereegranskat)abstract
- Nanoimprint lithography (NIL) can generate well defined nanostructures with high efficiency and at very low cost. Molecular imprinting (MIP) is a "bottom-up" technique creating a polymer layer exhibiting structures with a molecular selectivity. Such polymer structures may be employed as molecular recognition sites for sensing applications. In this work, the authors combine NIL with MIP and they are able to obtain micro- and nanopatterns of polymer with features down to 100 nm that show high molecular selectivity.
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| 6. |
- Kamra, Tripta, et al.
(författare)
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Covalent immobilization of molecularly imprinted polymer nanoparticles on a gold surface using carbodiimide coupling for chemical sensing.
- 2016
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Ingår i: Journal of Colloid and Interface Science. - : Elsevier BV. - 1095-7103 .- 0021-9797. ; 461, s. 1-8
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Tidskriftsartikel (refereegranskat)abstract
- One challenging task in building (bio)chemical sensors is the efficient and stable immobilization of receptor on a suitable transducer. Herein, we report a method for covalent immobilization of molecularly imprinted core-shell nanoparticles for construction of robust chemical sensors. The imprinted nanoparticles with a core-shell structure have selective molecular binding sites in the core and multiple amino groups in the shell. The model Au transducer surface is first functionalized with a self-assembled monolayer of 11-mercaptoundecanoic acid. The 11-mercaptoundecanoic acid is activated by treatment with carbodiimide/N-hydroxysuccinimide and then reacted with the core-shell nanoparticles to form amide bonds. We have characterized the process by studying the treated surfaces after each preparation step using atomic force microscopy, scanning electron microscopy, fluorescence microscopy, contact angle measurements and X-ray photoelectron spectroscopy. The microscopy results show the successful immobilization of the imprinted nanoparticles on the surface. The photoelectron spectroscopy results further confirm the success of each functionalization step. Further, the amino groups on the MIP surface were activated by electrostatically adsorbing negatively charged Au colloids. The functionalized surface was shown to be active for surface enhanced Raman scattering detection of propranolol. The particle immobilization and surface enhanced Raman scattering approach described here has a general applicability for constructing chemical sensors in different formats.
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| 7. |
- Kamra, Tripta, et al.
(författare)
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Covalent immobilization of molecularly imprinted polymer nanoparticles using an epoxy silane.
- 2015
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Ingår i: Journal of Colloid and Interface Science. - : Elsevier BV. - 1095-7103 .- 0021-9797. ; 445, s. 277-284
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Tidskriftsartikel (refereegranskat)abstract
- Molecularly imprinted polymers (MIPs) can be used as antibody mimics to develop robust chemical sensors. One challenging problem in using MIPs for sensor development is the lack of reliable conjugation chemistry that allows MIPs to be fixed on transducer surface. In this work, we study the use of epoxy silane to immobilize MIP nanoparticles on model transducer surfaces without impairing the function of the immobilized nanoparticles. The MIP nanoparticles with a core-shell structure have selective molecular binding sites in the core and multiple amino groups in the shell. The model transducer surface is functionalized with a self-assembled monolayer of epoxy silane, which reacts with the core-shell MIP particles to enable straightforward immobilization. The whole process is characterized by studying the treated surfaces after each preparation step using atomic force microscopy, scanning electron microscopy, fluorescence microscopy, contact angle measurements and X-ray photoelectron spectroscopy. The microscopy results show that the MIP particles are immobilized uniformly on surface. The photoelectron spectroscopy results further confirm the action of each functionalization step. The molecular selectivity of the MIP-functionalized surface is verified by radioligand binding analysis. The particle immobilization approach described here has a general applicability for constructing selective chemical sensors in different formats.
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| 8. |
- Kamra, Tripta, et al.
(författare)
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Implementation of Molecularly Imprinted Polymer Beads for Surface Enhanced Raman Detection
- 2015
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Ingår i: Analytical Chemistry. - : American Chemical Society (ACS). - 1520-6882 .- 0003-2700. ; 87:10, s. 5056-5061
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Tidskriftsartikel (refereegranskat)abstract
- Molecularly imprinted polymers (MIPs) have a predesigned molecular recognition capability that can be used to build robust chemical sensors. MIP-based chemical sensors allow label-free detection and are particularly interesting due to their simple operation. In this work we report the use of thiol-terminated MIP microspheres to construct surfaces for detection of a model organic analyte, nicotine, by surface enhanced Raman scattering (SERS). The nicotine-imprinted microspheres are synthesized by RAFT precipitation polymerization and converted into thiol-terminated microspheres through aminolysis. The thiol groups on the MIP surface allow the microspheres to be immobilized on a gold-coated substrate. Three different strategies are investigated to achieve surface enhanced Raman scattering in the vicinity of the imprinted sites: (1) direct sputtering of gold nanoparticles, (2) immobilization of gold colloids through the MIPs thiol groups, and (3) trapping of the MIP microspheres in a patterned SERS substrate. For the first time we show that large MIP microspheres can be turned into selective SERS surfaces through the three different approaches of assembly. The MIP-based sensing surfaces are used to detect nicotine to demonstrate the proof of concept. As synthesis and surface functionalization of MIP microspheres and nanoparticles are well established, the methods reported in this work are handy and efficient for constructing label-free chemical sensors, in particular for those based on SERS detection.
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| 9. |
- Kamra, Tripta, et al.
(författare)
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Photoconjugation of Molecularly Imprinted Polymer Nanoparticles for Surface-Enhanced Raman Detection of Propranolol
- 2015
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 7:49, s. 27479-27485
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Tidskriftsartikel (refereegranskat)abstract
- We report a simple and versatile method to covalently immobilize molecularly imprinted polymer (MIP) nanoparticles on a Raman active substrate (Klarite) using a disulfide-derivatized perfluorophenylazide (PFPA-disulfide). Gold-coated Klarite was functionalized with PFPA-disulfide via a gold sulfur bond. Upon light radiation, the available azido groups were converted to highly reactive singlet perfluorophenyl nitrene that undergoes a CH insertion reaction and form covalent bonds with the MIP nanoparticles. The resulting surfaces were characterized using scanning electron microscopy and surface enhanced Raman spectroscopy to study the morphology and template affinity of the surfaces, respectively. The Raman measurements clearly show a dose-responsive signal when propranolol binds to the MIP surface. Because the MIP particles were covalently attached to the Raman active substrate, the sensing surface was stable and could be reused after regeneration in acetic acid solution. The MIP-based Raman sensor was used successfully to detect propranolol in urine samples (7.7 X 10(-4) M). Our results show that the high selectivity of MLPs and the fingerprint Raman identification can be integrated into a compact sensing unit using high-efficiency photoconjugation. Thus, the method proposed is reliable, efficient and fast for fabricating label-free chemical sensors.
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