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1.
Chemphyschem ; 23(18): e202200280, 2022 09 16.
Article in English | MEDLINE | ID: mdl-35686692

ABSTRACT

The complicated photophysics of wide variety of defects existing in silica (SiO2 ) layer of nanometer thickness determines widespread photoluminescence bands of Si/SiO2 based system as well as SiO2 nanoparticles (NPs) for their applications in photovoltaic and optoelectronic devices. This review attempts to summarize different photophysical processes in pure SiO2 NPs. Moreover, these NPs also act as scaffolds for various guest molecules to perform their specific functions. Guest fluorophore molecules when trapped inside pores of SiO2 NPs exhibit a different photodynamics than free state, which opens up several important applications of hybrid SiO2 NPs in artificial photosynthesis, sensing, biology and optical fiber.


Subject(s)
Nanoparticles , Nanostructures , Fluorescent Dyes/chemistry , Nanoparticles/chemistry , Nanostructures/chemistry , Silicon Dioxide/chemistry
2.
Adv Mater ; 30(46): e1804450, 2018 Nov.
Article in English | MEDLINE | ID: mdl-30295967

ABSTRACT

The sensitive detection of X-rays embodies an important research area, being motivated by a common desire to minimize the radiation doses required for detection. Among metal halide perovskites, the double-perovskite Cs2 AgBiBr6 system has emerged as a promising candidate for the detection of X-rays, capable of high X-ray stability and sensitivity (105 µC Gy-1 cm-2 ). Herein, the important photophysical pathways in single-crystal Cs2 AgBiBr6 are detailed at both room (RT) and liquid-nitrogen (LN2 T) temperatures, with emphasis made toward understanding the carrier dynamics that influence X-ray sensitivity. This study draws upon several optical probes and an RT excitation model is developed which is far from optimal, being plagued by a large trap density and fast free-carrier recombination pathways. Substantially improved operating conditions are revealed at 77 K, with a long fundamental carrier lifetime (>1.5 µs) and a marked depopulation of parasitic recombination pathways. The temperature dependence of a single-crystal Cs2 AgBiBr6 X-ray detecting device is characterized and a strong and monotonic enhancement to the X-ray sensitivity upon cooling is demonstrated, moving from 316 µC Gy-1 cm-2 at RT to 988 µC Gy-1 cm-2 near LN2 T. It is concluded that even modest cooling-via a Peltier device-will facilitate a substantial enhancement in device performance, ultimately lowering the radiation doses required.

3.
ACS Nano ; 12(8): 8081-8090, 2018 Aug 28.
Article in English | MEDLINE | ID: mdl-30086242

ABSTRACT

The room-temperature charge carrier mobility and excitation-emission properties of metal halide perovskites are governed by their electronic band structures and intrinsic lattice phonon scattering mechanisms. Establishing how charge carriers interact within this scenario will have far-reaching consequences for developing high-efficiency materials for optoelectronic applications. Herein we evaluate the charge carrier scattering properties and conduction band environment of the double perovskite Cs2AgBiBr6 via a combinatorial approach; single crystal X-ray diffraction, optical excitation and temperature-dependent emission spectroscopy, resonant and nonresonant Raman scattering, further supported by first-principles calculations. We identify deep conduction band energy levels and that scattering from longitudinal optical phonons- via the Fröhlich interaction-dominates electron scattering at room temperature, manifesting within the nominally nonresonant Raman spectrum as multiphonon processes up to the fourth order. A Fröhlich coupling constant nearing 230 meV is inferred from a temperature-dependent emission line width analysis and is found to be extremely large compared to popular lead halide perovskites (between 40 and 60 meV), highlighting the fundamentally different nature of the two "single" and "double" perovskite materials branches.

4.
Small ; 14(24): e1704439, 2018 06.
Article in English | MEDLINE | ID: mdl-29770576

ABSTRACT

The Zn2+ stored in the secretory vesicles of glutamatergic neurons is coreleased with glutamate upon stimulation, resulting in the elevation of extracellular Zn2+ concentration (CZn2+ex). This elevation of CZn2+ex regulates the neurotransmission and facilitates the fibrilization of amyloid-ß (Aß). However, the exact CZn2+ex surrounding neurons under (patho)physiological conditions is not clear and the connection between CZn2+ex and the Aß fibrilization remains obscure. Here, a silicon nanowire field-effect transistor (SiNW-FET) with the Zn2+ -sensitive fluorophore, FluoZin-3 (FZ-3), to quantify the CZn2+ex in real time is modified. This FZ-3/SiNW-FET device has a dissociation constant of ≈12 × 10-9 m against Zn2+ . By placing a coverslip seeded with cultured embryonic cortical neurons atop an FZ-3/SiNW-FET, the CZn2+ex elevated to ≈110 × 10-9 m upon stimulation with α-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid (AMPA). Blockers against the AMPA receptor or exocytosis greatly suppress this elevation, indicating that the Zn2+ stored in the synaptic vesicles is the major source responsible for this elevation of CZn2+ex. In addition, a SiNW-FET modified with Aß could bind Zn2+ with a dissociation constant of ≈633 × 10-9 m and respond to the Zn2+ released from AMPA-stimulated neurons. Therefore, the CZn2+ex can reach a level high enough to bind Aß and the Zn2+ homeostasis can be a therapeutic strategy to prevent neurodegeneration.


Subject(s)
Amyloid beta-Peptides/metabolism , Extracellular Space/chemistry , Nanowires/chemistry , Neurons/metabolism , Transistors, Electronic , Zinc/pharmacology , Animals , Female , Ions , Neurons/drug effects , Neurotransmitter Agents/metabolism , Rats, Sprague-Dawley , alpha-Amino-3-hydroxy-5-methyl-4-isoxazolepropionic Acid/pharmacology
5.
Small ; 12(40): 5524-5529, 2016 Oct.
Article in English | MEDLINE | ID: mdl-27551968

ABSTRACT

Silicon nanowire field-effect transistors modified with specific aptamers can directly detect the minute dopamine and neuropeptide Y released from cells. The binding of these molecules to the aptamers results in a conductance change of the transistor biosensor and illustrates the differential releasing mechanisms of these molecules stored in various vesicle pools.


Subject(s)
Aptamers, Peptide/chemistry , Dopamine/analysis , Histamine/pharmacology , Nanowires/chemistry , Neuropeptide Y/analysis , Transistors, Electronic , Animals , PC12 Cells , Rats , Silicon/chemistry
6.
Analyst ; 137(12): 2871-5, 2012 Jun 21.
Article in English | MEDLINE | ID: mdl-22576100

ABSTRACT

A di-triazole based peptide has been synthesised by copper catalyzed Huisgen cycloaddition. Fluorescence intensity is enhanced selectively in the presence of Zn(2+), which is ascribed to reversal of photoelectron transfer. Compound 7 was found to self-assemble in the presence of Zn(ClO(4))(2) in an exclusive 2:1 ratio, which is supported by (1)H NMR titration and mass spectral data. The fluorescence intensity of 7 shows a subsequent ON-OFF phenomenon upon repetitive and alternate addition of Zn(ClO(4))(2) and HClO(4).


Subject(s)
Chemistry Techniques, Analytical/instrumentation , Peptides/chemistry , Spectrometry, Fluorescence/methods , Triazoles/chemistry , Zinc/analysis , Catalysis , Copper/chemistry , Limit of Detection , Peptides/chemical synthesis , Zinc/chemistry
7.
Langmuir ; 26(2): 1172-6, 2010 Jan 19.
Article in English | MEDLINE | ID: mdl-20067315

ABSTRACT

The reverse micelle sol-gel method was used earlier to prepare silica nanotubes, in aerosol OT/n-heptane/water microemulsions containing FeCl(3). The present communication reports the remarkable effect of the amount of water in the microemulsions on the shape, size, and spectral properties of the silica nanostructures formed. Nanotubes are formed, as expected, at lower water contents. However, for higher water contents, nanodisks form in predominance. This rather surprising observation indicates the formation of flat, disklike water pools in this medium. Notably, a phase separation occurs at higher water contents, and this appears to be essential for the formation of the disklike nanostructures. Hence, we propose that flat water pools form at the interface of the two liquid phases. The nanotubes and nanodisks exhibit blue photoluminescence. The photoluminescence of the nanotubes is more susceptible to quenching by moisture than that of the nanodisks. Luminescence is restored by heating or purging nitrogen or oxygen. Time-resolved photoluminescence studies conform to a model in which the luminescence is ascribed to a particular kind of defect center, with some contribution from surface-associated defects.

8.
Chem Commun (Camb) ; (33): 4982-4, 2009 Sep 07.
Article in English | MEDLINE | ID: mdl-19668823

ABSTRACT

Attachment of three different fluorophores to an aza-oxa cryptand (L) gives a transition-metal ion induced two-step fluorescence resonance energy transfer system.


Subject(s)
Ethers, Cyclic/chemistry , Fluorescence Resonance Energy Transfer , Fluorescent Dyes/chemistry , Schiff Bases/chemistry , Transition Elements/chemistry , Quantum Theory , Spectrometry, Fluorescence , Spectrophotometry, Ultraviolet
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