Reversible photo-chem-electrotriggered three-state luminescence switching based on core-shell nanostructures.

Reversible three-state fluorescence switches triggered by light, electricity and chemical inputs based on "sponges" of Pyronin Y-doped silica nanoparticles (PYDS) and polyoxometalate K14[Na(H2O)P5W30O110] (Na-POMs) core-shell nanostructures were realized. Under one or two signal inputs, the system exhibited distinct three-state interconvertible automaton, achieving reversible "on" and "off" luminescence switches via the related luminescence quenching effect. The features of the system correspond to the equivalent circuitry of an IMPLICATION logic gate performing the Boolean operation by using potential and chemical as inputs. Such a multi-chromic device with novel structure possesses several advantages, such as relative low operation voltage, large reproducibility and reversibility, apparent fluorescence contrast, and long-time stability, which make it a suitable candidate for nonvolatile memory devices. In addition, the current protocol for the hybrid film fabrication can be easily extended from the polyoxometalate and organic dyes to other novel nanostructures matched multifunctional stimulus-responsive species and fluorescence materials in the future.

[1]  A. Credi,et al.  Photophysical, photochemical and electrochemical properties of a series of aromatic electron acceptors based on N-heterocycles , 2007 .

[2]  Bin Wang,et al.  An electroswitchable fluorescence thin-film based on a luminescent polyoxometalate cluster. , 2010, Chemical communications.

[3]  R. Mallavia,et al.  In situ electrochemical fluorescence studies of PPV. , 2006, The journal of physical chemistry. B.

[4]  Itamar Willner,et al.  Photochemically and electrochemically triggered Au nanoparticles "sponges". , 2011, Journal of the American Chemical Society.

[5]  T. Moore,et al.  1-(3′-amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells , 2009, Nanotechnology.

[6]  Alberto Credi,et al.  Photochemical switching of luminescence and singlet oxygen generation by chemical signal communication. , 2009, Chemical communications.

[7]  M. T. Pope,et al.  Rigid nonlabile polyoxometalate cryptates [ZP5W30O110](15-n)- that exhibit unprecedented selectivity for certain lanthanide and other multivalent cations , 1993 .

[8]  Zhiyong Tang,et al.  Reversible photoswitchable fluorescence in thin films of inorganic nanoparticle and polyoxometalate assemblies. , 2010, Journal of the American Chemical Society.

[9]  Lixin Wu,et al.  Electroswitchable fluorescent thin film controlled by polyoxometalate , 2011 .

[10]  J. Yao,et al.  Reversible Luminescent Switching in a [Eu(SiW10MoO39)2]13−‐Agarose Composite Film by Photosensitive Intramolecular Energy Transfer , 2009 .

[11]  Vânia F. Pais,et al.  OFF-ON-OFF Fluorescence Switch with T-Latch Function , 2011, Organic letters.

[12]  V. S. Lin,et al.  Light- and pH-responsive release of doxorubicin from a mesoporous silica-based nanocarrier. , 2011, Chemistry.

[13]  Gennaro J. Gama,et al.  The structures of europium(III)- and uranium(IV) derivatives of [P5w3oo110]15-: Evidence for “cryptohydration” , 1996 .

[14]  J. Yao,et al.  Transparent and flexible phosphomolybdate–agarose composite thin films with visible-light photochromism , 2010 .

[15]  Gregory F. Payne,et al.  Redox Capacitor to Establish Bio‐Device Redox‐Connectivity , 2012 .

[16]  E. Wang,et al.  Reversible electroswitchable luminescence in thin films of organic-inorganic hybrid assemblies. , 2012, Nanoscale.

[17]  Ming Zhou,et al.  Bioelectrochemical interface engineering: toward the fabrication of electrochemical biosensors, biofuel cells, and self-powered logic biosensors. , 2011, Accounts of chemical research.

[18]  Xiao‐Peng He,et al.  Epimeric monosaccharide-quinone hybrids on gold electrodes toward the electrochemical probing of specific carbohydrate-protein recognitions. , 2011, Journal of the American Chemical Society.

[19]  David J. Williams,et al.  Simple Mechanical Molecular and Supramolecular Machines: Photochemical and Electrochemical Control of Switching Processes , 1997 .

[20]  Shaoqin Liu,et al.  A Thin-Film Electrochromic Device Based on a Polyoxometalate Cluster , 2002 .

[21]  Daeyeon Lee,et al.  pH-induced hysteretic gating of track-etched polycarbonate membranes: swelling/deswelling behavior of polyelectrolyte multilayers in confined geometry. , 2006, Journal of the American Chemical Society.

[22]  W. Heineman,et al.  Fluorescence spectroelectrochemical sensor for 1-hydroxypyrene. , 2010, Analytical chemistry.

[23]  T. Aartsma,et al.  Monitoring interfacial bioelectrochemistry using a FRET switch. , 2006, The journal of physical chemistry. B.

[24]  Shaoqin Liu,et al.  Functional Polyoxometalate Thin Films via Electrostatic Layer-by-Layer Self-Assembly , 2003 .

[25]  Z. Tang,et al.  Polyoxometalate-based functional nanostructured films: Current progress and future prospects , 2010 .

[26]  A. Knorr,et al.  New molecular systems for functional dye-based molecular switching of luminescence , 1996 .

[27]  Jason J. Davis,et al.  Reversible luminescence switching of a redox-active ferrocene-europium dyad. , 2011, Journal of the American Chemical Society.

[28]  Eunkyoung Kim,et al.  Tetrazine-based electrofluorochromic windows: Modulation of the fluorescence through applied potential , 2009 .

[29]  V. Yam,et al.  Photochromic and luminescence switching properties of a versatile diarylethene-containing 1,10-phenanthroline ligand and its rhenium(I) complex. , 2004, Journal of the American Chemical Society.

[30]  Lei Wang,et al.  Effects of morphology of nanostructured ZnO on direct electrochemistry and biosensing properties of glucose oxidase , 2011 .

[31]  S. Dong,et al.  Design of fluorescent assays for cyanide and hydrogen peroxide based on the inner filter effect of metal nanoparticles. , 2009, Analytical chemistry.

[32]  S. Dong,et al.  Sensitive turn-on fluorescent detection of cyanide based on the dissolution of fluorophore functionalized gold nanoparticles. , 2009, Chemical communications.

[33]  V. Tsukruk,et al.  Ultrathin Layer-by-Layer Hydrogels with Incorporated Gold Nanorods as pH-Sensitive Optical Materials , 2008 .

[34]  Jorge A. Fernández,et al.  Polyoxometalates with internal cavities: redox activity, basicity, and cation encapsulation in [Xn+P5W30O110](15-n)- Preyssler complexes, with X = Na+, Ca2+, Y3+, La3+, Ce3+, and Th4+. , 2007, Journal of the American Chemical Society.

[35]  F. Raymo,et al.  Luminescence quenching in supramolecular assemblies of quantum dots and bipyridinium dications , 2008 .

[36]  I. Willner,et al.  Control of bioelectrocatalytic transformations on DNA scaffolds. , 2009, Journal of the American Chemical Society.

[37]  Kemin Wang,et al.  Dye-doped nanoparticles for bioanalysis , 2007 .

[38]  Min Jae Lee,et al.  Photoswitchable fluorescent diarylethene in a turn-on mode for live cell imaging. , 2012, Chemical communications.

[39]  E. Wang,et al.  G-quadruplex DNAzyme based molecular catalytic beacon for label-free colorimetric logic gates. , 2011, Biomaterials.

[40]  Lehui Lu,et al.  Europium-based fluorescence nanoparticle sensor for rapid and ultrasensitive detection of an anthrax biomarker. , 2009, Angewandte Chemie.