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Title: Magnetic memory from site isolated Dy(III) on silica materials

Abstract

Achieving magnetic remanence at single isolated metal sites dispersed at the surface of a solid matrix has been envisioned as a key step toward information storage and processing in the smallest unit of matter. Here, we show that isolated Dy(III) sites distributed at the surface of silica nanoparticles, prepared with a simple and scalable two-step process, show magnetic remanence and display a hysteresis loop open at liquid 4He temperature, in contrast to the molecular precursor which does not display any magnetic memory. This singular behavior is achieved through the controlled grafting of a tailored Dy(III) siloxide complex on partially dehydroxylated silica nanoparticles followed by thermal annealing. This approach allows control of the density and the structure of isolated, “bare” Dy(III) sites bound to the silica surface. Throughout the process, all organic fragments are removed, leaving the surface as the sole ligand, promoting magnetic remanence.

Authors:
 [1];  [1];  [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [4]; ORCiD logo [5];  [6];  [4]; ORCiD logo [1]
  1. ETH Zurich, Zurich (Switzerland)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. Lyon, Lyon Cedex (France)
  4. Univ. de Rennes, Rennes Cedex (France)
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  6. Univ. Pierre et Marie Curie, Paris Cedex (France)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1344432
Alternate Identifier(s):
OSTI ID: 1352052; OSTI ID: 1436623
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515; FP7-PEOPLE-2012-ITN N?317127
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 3; Journal Issue: 3; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Allouche, Florian, Lapadula, Giuseppe, Siddiqi, Georges, Lukens, Wayne W., Maury, Olivier, Le Guennic, Boris, Pointillart, Fabrice, Dreiser, Jan, Mougel, Victor, Cador, Olivier, and Copéret, Christophe. Magnetic memory from site isolated Dy(III) on silica materials. United States: N. p., 2017. Web. doi:10.1021/acscentsci.7b00035.
Allouche, Florian, Lapadula, Giuseppe, Siddiqi, Georges, Lukens, Wayne W., Maury, Olivier, Le Guennic, Boris, Pointillart, Fabrice, Dreiser, Jan, Mougel, Victor, Cador, Olivier, & Copéret, Christophe. Magnetic memory from site isolated Dy(III) on silica materials. United States. doi:10.1021/acscentsci.7b00035.
Allouche, Florian, Lapadula, Giuseppe, Siddiqi, Georges, Lukens, Wayne W., Maury, Olivier, Le Guennic, Boris, Pointillart, Fabrice, Dreiser, Jan, Mougel, Victor, Cador, Olivier, and Copéret, Christophe. Wed . "Magnetic memory from site isolated Dy(III) on silica materials". United States. doi:10.1021/acscentsci.7b00035.
@article{osti_1344432,
title = {Magnetic memory from site isolated Dy(III) on silica materials},
author = {Allouche, Florian and Lapadula, Giuseppe and Siddiqi, Georges and Lukens, Wayne W. and Maury, Olivier and Le Guennic, Boris and Pointillart, Fabrice and Dreiser, Jan and Mougel, Victor and Cador, Olivier and Copéret, Christophe},
abstractNote = {Achieving magnetic remanence at single isolated metal sites dispersed at the surface of a solid matrix has been envisioned as a key step toward information storage and processing in the smallest unit of matter. Here, we show that isolated Dy(III) sites distributed at the surface of silica nanoparticles, prepared with a simple and scalable two-step process, show magnetic remanence and display a hysteresis loop open at liquid 4He temperature, in contrast to the molecular precursor which does not display any magnetic memory. This singular behavior is achieved through the controlled grafting of a tailored Dy(III) siloxide complex on partially dehydroxylated silica nanoparticles followed by thermal annealing. This approach allows control of the density and the structure of isolated, “bare” Dy(III) sites bound to the silica surface. Throughout the process, all organic fragments are removed, leaving the surface as the sole ligand, promoting magnetic remanence.},
doi = {10.1021/acscentsci.7b00035},
journal = {ACS Central Science},
number = 3,
volume = 3,
place = {United States},
year = {Wed Feb 22 00:00:00 EST 2017},
month = {Wed Feb 22 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acscentsci.7b00035

Citation Metrics:
Cited by: 5works
Citation information provided by
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  • Achieving magnetic remanence at single isolated metal sites dispersed at the surface of a solid matrix has been envisioned as a key step toward information storage and processing in the smallest unit of matter. Here, we show that isolated Dy(III) sites distributed at the surface of silica nanoparticles, prepared with a simple and scalable two-step process, show magnetic remanence and display a hysteresis loop open at liquid 4He temperature, in contrast to the molecular precursor which does not display any magnetic memory. This singular behavior is achieved through the controlled grafting of a tailored Dy(III) siloxide complex on partially dehydroxylatedmore » silica nanoparticles followed by thermal annealing. This approach allows control of the density and the structure of isolated, “bare” Dy(III) sites bound to the silica surface. Throughout the process, all organic fragments are removed, leaving the surface as the sole ligand, promoting magnetic remanence.« less
  • © 2017 American Chemical Society. Achieving magnetic remanence at single isolated metal sites dispersed at the surface of a solid matrix has been envisioned as a key step toward information storage and processing in the smallest unit of matter. Here, we show that isolated Dy(III) sites distributed at the surface of silica nanoparticles, prepared with a simple and scalable two-step process, show magnetic remanence and display a hysteresis loop open at liquid 4 He temperature, in contrast to the molecular precursor which does not display any magnetic memory. This singular behavior is achieved through the controlled grafting of a tailoredmore » Dy(III) siloxide complex on partially dehydroxylated silica nanoparticles followed by thermal annealing. This approach allows control of the density and the structure of isolated, bare Dy(III) sites bound to the silica surface. During the process, all organic fragments are removed, leaving the surface as the sole ligand, promoting magnetic remanence.« less
  • Well-defined, isolated, single-site organovanadium(III) catalyst on SiO 2 [(SiO 2)V(Mes)(THF)] were synthesized via surface organometallic chemistry, and fully characterized using a combination of analytical and spectroscopic techniques (EA, ICP, 1H NMR, TGA-MS, EPR, XPS, DR-UV/Vis, UV-Raman, DRIFTS, XAS). The catalysts exhibit unprecedented reactivity in liquid- and gas-phase alkene/alkyne hydrogenation. Catalyst poisoning experiments revealed that 100% of the V sites are active for hydrogenation.
  • The possibility to enrich paramagnetic dysprosium(III) ions in a magnetic field gradient is proved by means of interferometry, which may open the route for a magnetic separation of rare earth ions from aqueous solutions. The separation dynamics are studied for three different concentrations of DyCl{sub 3} and compared with those found recently in a sulphate solution of the 3d ion Mn(II). In view of the similar-sized hydration spheres for Dy(III) and Mn(II), the slower separation dynamics in DyCl{sub 3} is attributed to both a higher densification coefficient and the strong impact of Brownian motion due to the absence of ion-pairmore » clusters.« less
  • Bright nano objects emitting in the near infrared with a maximal cross section of 41.4 x 103 GM (Goppert Mayer), were prepared by implanting ca. 180 4,4 diethylaminostyryl 2,2 bipyridine (DEAS) Yb(III) complexes on the surface of 12 nm silica nanoparticles. The surface complexes ([DEAS Ln SiO2], Ln =Y,Yb) were characterized using IR, solid state NMR, UV Vis, EXAFS spectroscopies in combination with the preparation and characterization of similar molecular analogues by analytical techniques (IR, solution NMR, UV Vis, X ray crystallography) as well as DFT calculations. Starting from the partial dehydroxylation of the silica at 700 C on highmore » vacuum having 0.8 OH.nm 2, the grafting of Ln(N(SiMe3)2)3 generate ≤SiO Ln(N(SiMe3)2)2, which upon thermal step and coordination of the DEAS chromophore yields (≤SiO)3Ln(DEAS). Surface and molecular analogues display similar properties, in terms of DEAS binding constants absorption maxima and luminescence properties (intense emission band assigned to a ligand centered CT fluorescence and life time) in the solid state, consistent with the molecular nature of the surface species. The densely functionalized nanoparticles can be dispersed via ultra-sonication in small ca. 15-20 nm aggregates (1 to 6 elementary particles) that were detected using two photon microscopy imaging at 720 nm excitation, making them promising nano objects for bio imaging.« less