Abstract

A site-selective spectroscopy study of Ag nanoclusters dispersed in oxyfluoride glass hosts has been carried out. The nano- to millisecond, essentially non-exponential, luminescence kinetics of Ag nanoclusters has been detected in the spectral range from 450 to 1000 nm, when excited at discrete wavelengths in the range 250 to 450 nm. Based on these experimental observations, the energy level configuration coordinate diagram for the involved ground and excited singlet/triplet states of the Ag nanoclusters has been proposed and confirmed by the density functional theory (DFT). The sites for the Ag nanoclusters are argued to be multiple. The structure/geometry of the involved Ag nanoclusters has been suggested to involve spin-paired dimers Ag2+, or tetramers Ag42+, with a varying elongation/distortion along the tetramer diagonals.

© 2012 OSA

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2012 (2)

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

2011 (2)

I. Díez and R. H. A. Ras, “Fluorescent silver nanoclusters,” Nanoscale 3(5), 1963–1970 (2011).
[CrossRef] [PubMed]

M. T. Colvin, A. L. Smeigh, E. M. Giacobbe, S. M. M. Conron, A. B. Ricks, and M. R. Wasielewski, “Ultrafast intersystem crossing and spin dynamics of zinc meso-tetraphenylporphyrin covalently bound to stable radicals,” J. Phys. Chem. A 115(26), 7538–7549 (2011).
[CrossRef] [PubMed]

2010 (2)

V. D. Rodríguez, V. K. Tikhomirov, J. Mendez-Ramos, A. C. Yanes, and V. V. Moshchalkov, “Towards broad range and highly efficient down-conversion of solar spectrum by Er3+-Yb3+ co-doped nano-structured glass-ceramics,” Sol. Energy Mater. Sol. Cells 94(10), 1612–1617 (2010).
[CrossRef]

V. K. Tikhomirov, V. D. Rodríguez, A. Kuznetsov, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Preparation and luminescence of bulk oxyfluoride glasses doped with Ag nanoclusters,” Opt. Express 18(21), 22032–22040 (2010).
[CrossRef] [PubMed]

2009 (2)

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

L. Maretti, P. S. Billone, Y. Liu, and J. C. Scaiano, “Facile photochemical synthesis and characterization of highly fluorescent silver nanoparticles,” J. Am. Chem. Soc. 131(39), 13972–13980 (2009).
[CrossRef] [PubMed]

2008 (1)

P. Frantsuzov, M. Kuno, B. Janko, and R. A. Marcus, “Universal emission intermittency in quantum dots, nanorods, and nanowires,” Nat. Phys. 4(5), 519–522 (2008).
[CrossRef]

2007 (1)

Z. Shen, H. Duan, and H. Frey, “Water-soluble fluorescent Ag nanoclusters obtained from multiarm star poly(akrilic) acid as molecular hydrogel templates,” Adv. Mater. 19(3), 349–352 (2007).
[CrossRef]

2006 (1)

K. Driesen, V. K. Tikhomirov, C. Gorller-Walrand, V. D. Rodriguez, and A. B. Seddon, “Transparent Ho3+-doped nano-glass-ceramics for efficient infrared emission,” Appl. Phys. Lett. 88(7), 073111 (2006).
[CrossRef]

2005 (1)

J. Tang and R. A. Marcus, “Mechanisms of fluorescence blinking in semiconductor nanocrystal quantum dots,” J. Chem. Phys. 123(5), 054704 (2005).
[CrossRef] [PubMed]

2004 (2)

A. C. Yanes, J. Del Castillo, M. Torres, J. Peraza, V. D. Rodríguez, and J. Méndez-Ramos, “Nanocrystal-size selective spectroscopy in SnO2: Eu3+ semiconductor quantum dots,” Appl. Phys. Lett. 85(12), 2343–2345 (2004).
[CrossRef]

S. Hull, “Superionics: crystal structures and conduction processes,” Rep. Prog. Phys. 67(7), 1233–1314 (2004).
[CrossRef]

2003 (1)

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

2002 (2)

W. Chen, A. G. Joly, and J. Roark, “Photostimulated luminescence and dynamics of AgI and Ag nanoclusters in zeolites,” Phys. Rev. B 65(24), 245404 (2002).
[CrossRef]

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

1998 (1)

I. Rabin, W. Schulze, and G. J. Ertl, “Light emission during the agglomeration of silver clusters in noble gas matrices,” J. Chem. Phys. 108(12), 5137–5142 (1998).
[CrossRef]

1996 (4)

J. P. Perdew, K. Burke, and M. Ernzerhof, “Generalized gradient approximation made simple,” Phys. Rev. Lett. 77(18), 3865–3868 (1996).
[CrossRef] [PubMed]

R. Bauernschmitt and R. Ahlrichs, “Treatment of electronic excitations within the adiabatic approximation of time dependent density functional theory,” Chem. Phys. Lett. 256(4-5), 454–464 (1996).
[CrossRef]

L. Konig, I. Rabin, W. Schulze, and G. Ertl, “Chemiluminescence in the agglomeration of metal clusters,” Science 274(5291), 1353–1355 (1996).
[CrossRef] [PubMed]

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

1993 (1)

A. Stesmans, “Structural relaxation of Pb defects at the (111)Si/SiO2 interface as a function of oxidation temperature: The Pb-generation-stress relationship,” Phys. Rev. B Condens. Matter 48(4), 2418–2435 (1993).
[CrossRef] [PubMed]

1991 (1)

S. R. Elliott, “Medium-range structural order in covalent amorphous solids,” Nature 354(6353), 445–452 (1991).
[CrossRef]

1985 (1)

P. J. Hay and W. R. Wadt, “Ab initio effective core potentials for molecular calculations. Potentials for the transition metal atoms Sc to Hg,” J. Chem. Phys. 82(1), 270–283 (1985).
[CrossRef]

Ahlrichs, R.

R. Bauernschmitt and R. Ahlrichs, “Treatment of electronic excitations within the adiabatic approximation of time dependent density functional theory,” Chem. Phys. Lett. 256(4-5), 454–464 (1996).
[CrossRef]

Almeida, R. M.

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

Bauernschmitt, R.

R. Bauernschmitt and R. Ahlrichs, “Treatment of electronic excitations within the adiabatic approximation of time dependent density functional theory,” Chem. Phys. Lett. 256(4-5), 454–464 (1996).
[CrossRef]

Bawendi, M. G.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

Beggiora, M.

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Billone, P. S.

L. Maretti, P. S. Billone, Y. Liu, and J. C. Scaiano, “Facile photochemical synthesis and characterization of highly fluorescent silver nanoparticles,” J. Am. Chem. Soc. 131(39), 13972–13980 (2009).
[CrossRef] [PubMed]

Brus, L. E.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

Burke, K.

J. P. Perdew, K. Burke, and M. Ernzerhof, “Generalized gradient approximation made simple,” Phys. Rev. Lett. 77(18), 3865–3868 (1996).
[CrossRef] [PubMed]

Chen, W.

W. Chen, A. G. Joly, and J. Roark, “Photostimulated luminescence and dynamics of AgI and Ag nanoclusters in zeolites,” Phys. Rev. B 65(24), 245404 (2002).
[CrossRef]

Chibotaru, L. F.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Colvin, M. T.

M. T. Colvin, A. L. Smeigh, E. M. Giacobbe, S. M. M. Conron, A. B. Ricks, and M. R. Wasielewski, “Ultrafast intersystem crossing and spin dynamics of zinc meso-tetraphenylporphyrin covalently bound to stable radicals,” J. Phys. Chem. A 115(26), 7538–7549 (2011).
[CrossRef] [PubMed]

Conron, S. M. M.

M. T. Colvin, A. L. Smeigh, E. M. Giacobbe, S. M. M. Conron, A. B. Ricks, and M. R. Wasielewski, “Ultrafast intersystem crossing and spin dynamics of zinc meso-tetraphenylporphyrin covalently bound to stable radicals,” J. Phys. Chem. A 115(26), 7538–7549 (2011).
[CrossRef] [PubMed]

Cuong, N. T.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Dabbousi, B. O.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

Del Castillo, J.

A. C. Yanes, J. Del Castillo, M. Torres, J. Peraza, V. D. Rodríguez, and J. Méndez-Ramos, “Nanocrystal-size selective spectroscopy in SnO2: Eu3+ semiconductor quantum dots,” Appl. Phys. Lett. 85(12), 2343–2345 (2004).
[CrossRef]

Díez, I.

I. Díez and R. H. A. Ras, “Fluorescent silver nanoclusters,” Nanoscale 3(5), 1963–1970 (2011).
[CrossRef] [PubMed]

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Driesen, K.

K. Driesen, V. K. Tikhomirov, C. Gorller-Walrand, V. D. Rodriguez, and A. B. Seddon, “Transparent Ho3+-doped nano-glass-ceramics for efficient infrared emission,” Appl. Phys. Lett. 88(7), 073111 (2006).
[CrossRef]

Duan, H.

Z. Shen, H. Duan, and H. Frey, “Water-soluble fluorescent Ag nanoclusters obtained from multiarm star poly(akrilic) acid as molecular hydrogel templates,” Adv. Mater. 19(3), 349–352 (2007).
[CrossRef]

Elliott, S. R.

S. R. Elliott, “Medium-range structural order in covalent amorphous solids,” Nature 354(6353), 445–452 (1991).
[CrossRef]

Ernzerhof, M.

J. P. Perdew, K. Burke, and M. Ernzerhof, “Generalized gradient approximation made simple,” Phys. Rev. Lett. 77(18), 3865–3868 (1996).
[CrossRef] [PubMed]

Ertl, G.

L. Konig, I. Rabin, W. Schulze, and G. Ertl, “Chemiluminescence in the agglomeration of metal clusters,” Science 274(5291), 1353–1355 (1996).
[CrossRef] [PubMed]

Ertl, G. J.

I. Rabin, W. Schulze, and G. J. Ertl, “Light emission during the agglomeration of silver clusters in noble gas matrices,” J. Chem. Phys. 108(12), 5137–5142 (1998).
[CrossRef]

Ferrari, M.

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Frantsuzov, P.

P. Frantsuzov, M. Kuno, B. Janko, and R. A. Marcus, “Universal emission intermittency in quantum dots, nanorods, and nanowires,” Nat. Phys. 4(5), 519–522 (2008).
[CrossRef]

Frey, H.

Z. Shen, H. Duan, and H. Frey, “Water-soluble fluorescent Ag nanoclusters obtained from multiarm star poly(akrilic) acid as molecular hydrogel templates,” Adv. Mater. 19(3), 349–352 (2007).
[CrossRef]

Fron, E.

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

Furniss, D.

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Giacobbe, E. M.

M. T. Colvin, A. L. Smeigh, E. M. Giacobbe, S. M. M. Conron, A. B. Ricks, and M. R. Wasielewski, “Ultrafast intersystem crossing and spin dynamics of zinc meso-tetraphenylporphyrin covalently bound to stable radicals,” J. Phys. Chem. A 115(26), 7538–7549 (2011).
[CrossRef] [PubMed]

Goldmann, A. S.

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Gorller-Walrand, C.

K. Driesen, V. K. Tikhomirov, C. Gorller-Walrand, V. D. Rodriguez, and A. B. Seddon, “Transparent Ho3+-doped nano-glass-ceramics for efficient infrared emission,” Appl. Phys. Lett. 88(7), 073111 (2006).
[CrossRef]

Harris, T. D.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

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P. J. Hay and W. R. Wadt, “Ab initio effective core potentials for molecular calculations. Potentials for the transition metal atoms Sc to Hg,” J. Chem. Phys. 82(1), 270–283 (1985).
[CrossRef]

Hofkens, J.

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

Hull, S.

S. Hull, “Superionics: crystal structures and conduction processes,” Rep. Prog. Phys. 67(7), 1233–1314 (2004).
[CrossRef]

Ikkala, O.

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Janko, B.

P. Frantsuzov, M. Kuno, B. Janko, and R. A. Marcus, “Universal emission intermittency in quantum dots, nanorods, and nanowires,” Nat. Phys. 4(5), 519–522 (2008).
[CrossRef]

Jiang, H.

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Jivanescu, M.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

Joly, A. G.

W. Chen, A. G. Joly, and J. Roark, “Photostimulated luminescence and dynamics of AgI and Ag nanoclusters in zeolites,” Phys. Rev. B 65(24), 245404 (2002).
[CrossRef]

Kirilenko, D.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

V. K. Tikhomirov, V. D. Rodríguez, A. Kuznetsov, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Preparation and luminescence of bulk oxyfluoride glasses doped with Ag nanoclusters,” Opt. Express 18(21), 22032–22040 (2010).
[CrossRef] [PubMed]

Konig, L.

L. Konig, I. Rabin, W. Schulze, and G. Ertl, “Chemiluminescence in the agglomeration of metal clusters,” Science 274(5291), 1353–1355 (1996).
[CrossRef] [PubMed]

Kulmala, S.

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Kuno, M.

P. Frantsuzov, M. Kuno, B. Janko, and R. A. Marcus, “Universal emission intermittency in quantum dots, nanorods, and nanowires,” Nat. Phys. 4(5), 519–522 (2008).
[CrossRef]

Kuznetsov, A.

Kuznetsov, A. S.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

Liu, Y.

L. Maretti, P. S. Billone, Y. Liu, and J. C. Scaiano, “Facile photochemical synthesis and characterization of highly fluorescent silver nanoparticles,” J. Am. Chem. Soc. 131(39), 13972–13980 (2009).
[CrossRef] [PubMed]

Macklin, J. J.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

Marcus, R. A.

P. Frantsuzov, M. Kuno, B. Janko, and R. A. Marcus, “Universal emission intermittency in quantum dots, nanorods, and nanowires,” Nat. Phys. 4(5), 519–522 (2008).
[CrossRef]

J. Tang and R. A. Marcus, “Mechanisms of fluorescence blinking in semiconductor nanocrystal quantum dots,” J. Chem. Phys. 123(5), 054704 (2005).
[CrossRef] [PubMed]

Maretti, L.

L. Maretti, P. S. Billone, Y. Liu, and J. C. Scaiano, “Facile photochemical synthesis and characterization of highly fluorescent silver nanoparticles,” J. Am. Chem. Soc. 131(39), 13972–13980 (2009).
[CrossRef] [PubMed]

Mendez-Ramos, J.

V. D. Rodríguez, V. K. Tikhomirov, J. Mendez-Ramos, A. C. Yanes, and V. V. Moshchalkov, “Towards broad range and highly efficient down-conversion of solar spectrum by Er3+-Yb3+ co-doped nano-structured glass-ceramics,” Sol. Energy Mater. Sol. Cells 94(10), 1612–1617 (2010).
[CrossRef]

Méndez-Ramos, J.

A. C. Yanes, J. Del Castillo, M. Torres, J. Peraza, V. D. Rodríguez, and J. Méndez-Ramos, “Nanocrystal-size selective spectroscopy in SnO2: Eu3+ semiconductor quantum dots,” Appl. Phys. Lett. 85(12), 2343–2345 (2004).
[CrossRef]

Montagna, M.

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Moshchalkov, V. V.

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

V. K. Tikhomirov, V. D. Rodríguez, A. Kuznetsov, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Preparation and luminescence of bulk oxyfluoride glasses doped with Ag nanoclusters,” Opt. Express 18(21), 22032–22040 (2010).
[CrossRef] [PubMed]

V. D. Rodríguez, V. K. Tikhomirov, J. Mendez-Ramos, A. C. Yanes, and V. V. Moshchalkov, “Towards broad range and highly efficient down-conversion of solar spectrum by Er3+-Yb3+ co-doped nano-structured glass-ceramics,” Sol. Energy Mater. Sol. Cells 94(10), 1612–1617 (2010).
[CrossRef]

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Müller, A. H. E.

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Nguyen, M. T.

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Nirmal, M.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

Peraza, J.

A. C. Yanes, J. Del Castillo, M. Torres, J. Peraza, V. D. Rodríguez, and J. Méndez-Ramos, “Nanocrystal-size selective spectroscopy in SnO2: Eu3+ semiconductor quantum dots,” Appl. Phys. Lett. 85(12), 2343–2345 (2004).
[CrossRef]

Perdew, J. P.

J. P. Perdew, K. Burke, and M. Ernzerhof, “Generalized gradient approximation made simple,” Phys. Rev. Lett. 77(18), 3865–3868 (1996).
[CrossRef] [PubMed]

Pusa, M.

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Rabin, I.

I. Rabin, W. Schulze, and G. J. Ertl, “Light emission during the agglomeration of silver clusters in noble gas matrices,” J. Chem. Phys. 108(12), 5137–5142 (1998).
[CrossRef]

L. Konig, I. Rabin, W. Schulze, and G. Ertl, “Chemiluminescence in the agglomeration of metal clusters,” Science 274(5291), 1353–1355 (1996).
[CrossRef] [PubMed]

Ras, R. H. A.

I. Díez and R. H. A. Ras, “Fluorescent silver nanoclusters,” Nanoscale 3(5), 1963–1970 (2011).
[CrossRef] [PubMed]

I. Díez, M. Pusa, S. Kulmala, H. Jiang, A. Walther, A. S. Goldmann, A. H. E. Müller, O. Ikkala, and R. H. A. Ras, “Color tuneability and electrochemiluminescence of silver nanoclusters,” Angew. Chem. Int. Ed. 48(12), 2122–2125 (2009).
[CrossRef]

Reaney, I. M.

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Ricks, A. B.

M. T. Colvin, A. L. Smeigh, E. M. Giacobbe, S. M. M. Conron, A. B. Ricks, and M. R. Wasielewski, “Ultrafast intersystem crossing and spin dynamics of zinc meso-tetraphenylporphyrin covalently bound to stable radicals,” J. Phys. Chem. A 115(26), 7538–7549 (2011).
[CrossRef] [PubMed]

Roark, J.

W. Chen, A. G. Joly, and J. Roark, “Photostimulated luminescence and dynamics of AgI and Ag nanoclusters in zeolites,” Phys. Rev. B 65(24), 245404 (2002).
[CrossRef]

Rodriguez, V. D.

K. Driesen, V. K. Tikhomirov, C. Gorller-Walrand, V. D. Rodriguez, and A. B. Seddon, “Transparent Ho3+-doped nano-glass-ceramics for efficient infrared emission,” Appl. Phys. Lett. 88(7), 073111 (2006).
[CrossRef]

Rodríguez, V. D.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

V. K. Tikhomirov, V. D. Rodríguez, A. Kuznetsov, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Preparation and luminescence of bulk oxyfluoride glasses doped with Ag nanoclusters,” Opt. Express 18(21), 22032–22040 (2010).
[CrossRef] [PubMed]

V. D. Rodríguez, V. K. Tikhomirov, J. Mendez-Ramos, A. C. Yanes, and V. V. Moshchalkov, “Towards broad range and highly efficient down-conversion of solar spectrum by Er3+-Yb3+ co-doped nano-structured glass-ceramics,” Sol. Energy Mater. Sol. Cells 94(10), 1612–1617 (2010).
[CrossRef]

A. C. Yanes, J. Del Castillo, M. Torres, J. Peraza, V. D. Rodríguez, and J. Méndez-Ramos, “Nanocrystal-size selective spectroscopy in SnO2: Eu3+ semiconductor quantum dots,” Appl. Phys. Lett. 85(12), 2343–2345 (2004).
[CrossRef]

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Rolli, R.

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Santos, L. F.

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

Scaiano, J. C.

L. Maretti, P. S. Billone, Y. Liu, and J. C. Scaiano, “Facile photochemical synthesis and characterization of highly fluorescent silver nanoparticles,” J. Am. Chem. Soc. 131(39), 13972–13980 (2009).
[CrossRef] [PubMed]

Schulze, W.

I. Rabin, W. Schulze, and G. J. Ertl, “Light emission during the agglomeration of silver clusters in noble gas matrices,” J. Chem. Phys. 108(12), 5137–5142 (1998).
[CrossRef]

L. Konig, I. Rabin, W. Schulze, and G. Ertl, “Chemiluminescence in the agglomeration of metal clusters,” Science 274(5291), 1353–1355 (1996).
[CrossRef] [PubMed]

Seddon, A. B.

K. Driesen, V. K. Tikhomirov, C. Gorller-Walrand, V. D. Rodriguez, and A. B. Seddon, “Transparent Ho3+-doped nano-glass-ceramics for efficient infrared emission,” Appl. Phys. Lett. 88(7), 073111 (2006).
[CrossRef]

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

Shen, Z.

Z. Shen, H. Duan, and H. Frey, “Water-soluble fluorescent Ag nanoclusters obtained from multiarm star poly(akrilic) acid as molecular hydrogel templates,” Adv. Mater. 19(3), 349–352 (2007).
[CrossRef]

Smeigh, A. L.

M. T. Colvin, A. L. Smeigh, E. M. Giacobbe, S. M. M. Conron, A. B. Ricks, and M. R. Wasielewski, “Ultrafast intersystem crossing and spin dynamics of zinc meso-tetraphenylporphyrin covalently bound to stable radicals,” J. Phys. Chem. A 115(26), 7538–7549 (2011).
[CrossRef] [PubMed]

Stesmans, A.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

A. Stesmans, “Structural relaxation of Pb defects at the (111)Si/SiO2 interface as a function of oxidation temperature: The Pb-generation-stress relationship,” Phys. Rev. B Condens. Matter 48(4), 2418–2435 (1993).
[CrossRef] [PubMed]

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Tang, J.

J. Tang and R. A. Marcus, “Mechanisms of fluorescence blinking in semiconductor nanocrystal quantum dots,” J. Chem. Phys. 123(5), 054704 (2005).
[CrossRef] [PubMed]

Tikhomirov, V. K.

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

V. K. Tikhomirov, V. D. Rodríguez, A. Kuznetsov, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Preparation and luminescence of bulk oxyfluoride glasses doped with Ag nanoclusters,” Opt. Express 18(21), 22032–22040 (2010).
[CrossRef] [PubMed]

V. D. Rodríguez, V. K. Tikhomirov, J. Mendez-Ramos, A. C. Yanes, and V. V. Moshchalkov, “Towards broad range and highly efficient down-conversion of solar spectrum by Er3+-Yb3+ co-doped nano-structured glass-ceramics,” Sol. Energy Mater. Sol. Cells 94(10), 1612–1617 (2010).
[CrossRef]

K. Driesen, V. K. Tikhomirov, C. Gorller-Walrand, V. D. Rodriguez, and A. B. Seddon, “Transparent Ho3+-doped nano-glass-ceramics for efficient infrared emission,” Appl. Phys. Lett. 88(7), 073111 (2006).
[CrossRef]

V. K. Tikhomirov, A. B. Seddon, M. Ferrari, M. Montagna, L. F. Santos, and R. M. Almeida, “The structure of Er3+-doped oxy-fluoride transparent glass-ceramics studied by Raman scattering,” Europhys. Lett. 64(4), 529–535 (2003).
[CrossRef]

V. K. Tikhomirov, D. Furniss, A. B. Seddon, I. M. Reaney, M. Beggiora, M. Ferrari, M. Montagna, and R. Rolli, “Fabrication and characterization of nanoscale, Er3+-doped, ultratransparent oxyfluoride glass-ceramics,” Appl. Phys. Lett. 81(11), 1937–1939 (2002).
[CrossRef]

N. T. Cuong, V. K. Tikhomirov, L. F. Chibotaru, A. Stesmans, V. D. Rodríguez, M. T. Nguyen, and V. V. Moshchalkov, “Experiment and theoretical modeling of the luminescence of silver nanoclusters dispersed in oxyfluoride glass,” J. Chem. Phys. (to be published).

Torres, M.

A. C. Yanes, J. Del Castillo, M. Torres, J. Peraza, V. D. Rodríguez, and J. Méndez-Ramos, “Nanocrystal-size selective spectroscopy in SnO2: Eu3+ semiconductor quantum dots,” Appl. Phys. Lett. 85(12), 2343–2345 (2004).
[CrossRef]

Trautman, J. K.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature 383(6603), 802–804 (1996).
[CrossRef]

Van der Auweraer, M.

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

Van Tendeloo, G.

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

V. K. Tikhomirov, V. D. Rodríguez, A. Kuznetsov, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Preparation and luminescence of bulk oxyfluoride glasses doped with Ag nanoclusters,” Opt. Express 18(21), 22032–22040 (2010).
[CrossRef] [PubMed]

Velázquez, J. J.

V. K. Tikhomirov, T. Vosch, E. Fron, V. D. Rodríguez, J. J. Velázquez, D. Kirilenko, G. Van Tendeloo, J. Hofkens, M. Van der Auweraer, and V. V. Moshchalkov, “Luminescence of oxyfluoride glasses co-doped with Ag nanoclusters and Yb3+ ions,” RCS Adv. 2(4), 1496–1501 (2012).

A. S. Kuznetsov, N. T. Cuong, V. K. Tikhomirov, M. Jivanescu, A. Stesmans, L. F. Chibotaru, J. J. Velázquez, V. D. Rodríguez, D. Kirilenko, G. Van Tendeloo, and V. V. Moshchalkov, “Effect of heat-treatment on luminescence and structure of Ag nanoclusters doped oxyfluoride glasses and implication for fiber drawing,” Opt. Mater. 34(4), 616–621 (2012).
[CrossRef]

Vosch, T.

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Figures (5)

Fig. 1
Fig. 1

Normalized emission and excitation spectra of the base oxyfluoride glass doped with 5 wt% AgNO3, the corresponding excitation and emission wavelengths are indicated.

Fig. 2
Fig. 2

Luminescence decays of the base oxyfluoride glass doped with 5 wt% AgNO3 after pulsed excitation into Ag nanoclusters absorption band at 355 (a) and 420 (b) nm, detected at the indicated wavelengths. The pump pulse duration was 10 ns, repetition rate 20 Hz. The red lines represent the optimized fits of the experimental kinetics according to Eq. (1).

Fig. 3
Fig. 3

Luminescence decays of the base oxyfluoride glass doped with 5 wt% AgNO3 after pulsed excitation in the Ag nanoclusters absorption band at 406 nm, detected at the indicated wavelengths. The pump pulse duration was 70 ps, repetition rate 1 MHz. The red lines represent optimized fits of the experimental kinetics according to Eq. (1).

Fig. 4
Fig. 4

(a) The Ag42+ tetramer embedded in the fluorite-type lattice MF2. The light blue balls represent the Ag+ which substitute the M2+ cations and dark blue balls represent Ag+ which occupy the nearby vacancies in the MF2 lattice network. The five chemical bonds in the tetramer are indicated by solid lines. (b) A fragment of the fluorite-type lattice including the Ag42+ tetramer with its first coordination sphere encompassing two nearby charge compensating F- vacancies. The hydrogen atoms are attached to the F- ions for saturation of their external bonds, resulting in [Ag4M4(HF)34]10+ nanocluster which was used for DFT calculation in this work.

Fig. 5
Fig. 5

(a) Three-dimensional energy configuration coordinate (CCD) diagram for the ground and several lowest excited states of the Ag42+ tetramer outlined in Fig. 4(b). (b) Two-dimensional energy configuration coordinate diagram (CCD) for the ground and several lowest excited states of the Ag42+ tetramer representing the cross-section of CCD from (a) viewed along d1. The up-headed and down-headed arrows indicate possible excitation and emission transitions, respectively. The wavy line represents an ultra-fast inter-system crossing process from the singlet, S1, to the triplet, T2, state.

Tables (2)

Tables Icon

Table 1 Fast (τfast) and slow (τslow) decay components of the Ag emission band in the base Ag-doped glass (5 wt% AgNO3) obtained after excitation at 355 (upper part) and 420 (lower part) nm and detected at 450, 500 and 800 nm as indicated in the respective column heading. Relative accuracy of the values is ± 10%. Duration of excitation pulses is 10 ns, repetition rate is 20 Hz.

Tables Icon

Table 2 Fast (τfast) and slow (τslow) decay components of the Ag emission band in Ag-doped glass (5 wt% AgNO3) obtained after excitation at 406 nm and detected at 450, 500, 600 and 700 nm as post-signed in the respective columns. Relative accuracy of the values is ± 10%. Duration of excitation pulses is 70 ps, repetition rate is 1 MHz.

Equations (1)

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I= I 1 e t τ fast + I 2 e t τ slow

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