Details
| Original language | English |
|---|---|
| Pages (from-to) | 5412-5421 |
| Number of pages | 10 |
| Journal | NANOSCALE |
| Volume | 12 |
| Issue number | 9 |
| Publication status | Published - 2020 |
Abstract
Materials displaying novel magnetic ground states signify the most exciting prospects for nanoscopic devices for nanoelectronics and spintronics. Spin transition materials, e.g., spin liquids and spin glasses, are at the forefront of this pursuit; but the few synthesis routes available do not produce them at the nanoscale. Thus, it remains an open question if and how their spin transition nature persists at such small dimensions. Here we demonstrate a new route to synthesize nanoparticles of spin transition materials, gas-diffusion electrocrystallization (GDEx), wherein the reactive precipitation of soluble metal ions with the products of the oxygen reduction reaction (ORR), i.e., in situ produced H 2O 2, OH -, drives their formation at the electrochemical interface. Using mixtures of Cu 2+ and Zn 2+ as the metal precursors, we form spin transition materials of the herbertsmithite family-heralded as the first experimental material known to exhibit the properties of a quantum spin liquid (QSL). Single-crystal nanoparticles of ∼10-16 nm were produced by GDEx, with variable Cu/Zn stoichiometry at the interlayer sites of Zn xCu 4-x(OH) 6Cl 2. For x = 1 (herbertsmithite) the GDEx nanoparticles demonstrated a quasi-QSL behavior, whereas for x = 0.3 (0.3 < x < 1 for paratacamite) and x = 0 (clinoatacamite) a spin-glass behavior was evidenced. Finally, our discovery not only confirms redox reactions as the driving force to produce spin transition nanoparticles, but also proves a simple way to switch between these magnetic ground states within an electrochemical system, paving the way to further explore its reversibility and overarching implications.
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In: NANOSCALE, Vol. 12, No. 9, 2020, p. 5412-5421.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Spin transition nanoparticles made electrochemically
AU - Pozo, Guillermo
AU - Presa, Patricia de la
AU - Prato, Rafael
AU - Morales, Irene
AU - Marin, Pilar
AU - Fransaer, Jan
AU - Dominguez-Benetton, Xochitl
N1 - Publisher Copyright: © 2020 The Royal Society of Chemistry.
PY - 2020
Y1 - 2020
N2 - Materials displaying novel magnetic ground states signify the most exciting prospects for nanoscopic devices for nanoelectronics and spintronics. Spin transition materials, e.g., spin liquids and spin glasses, are at the forefront of this pursuit; but the few synthesis routes available do not produce them at the nanoscale. Thus, it remains an open question if and how their spin transition nature persists at such small dimensions. Here we demonstrate a new route to synthesize nanoparticles of spin transition materials, gas-diffusion electrocrystallization (GDEx), wherein the reactive precipitation of soluble metal ions with the products of the oxygen reduction reaction (ORR), i.e., in situ produced H 2O 2, OH -, drives their formation at the electrochemical interface. Using mixtures of Cu 2+ and Zn 2+ as the metal precursors, we form spin transition materials of the herbertsmithite family-heralded as the first experimental material known to exhibit the properties of a quantum spin liquid (QSL). Single-crystal nanoparticles of ∼10-16 nm were produced by GDEx, with variable Cu/Zn stoichiometry at the interlayer sites of Zn xCu 4-x(OH) 6Cl 2. For x = 1 (herbertsmithite) the GDEx nanoparticles demonstrated a quasi-QSL behavior, whereas for x = 0.3 (0.3 < x < 1 for paratacamite) and x = 0 (clinoatacamite) a spin-glass behavior was evidenced. Finally, our discovery not only confirms redox reactions as the driving force to produce spin transition nanoparticles, but also proves a simple way to switch between these magnetic ground states within an electrochemical system, paving the way to further explore its reversibility and overarching implications.
AB - Materials displaying novel magnetic ground states signify the most exciting prospects for nanoscopic devices for nanoelectronics and spintronics. Spin transition materials, e.g., spin liquids and spin glasses, are at the forefront of this pursuit; but the few synthesis routes available do not produce them at the nanoscale. Thus, it remains an open question if and how their spin transition nature persists at such small dimensions. Here we demonstrate a new route to synthesize nanoparticles of spin transition materials, gas-diffusion electrocrystallization (GDEx), wherein the reactive precipitation of soluble metal ions with the products of the oxygen reduction reaction (ORR), i.e., in situ produced H 2O 2, OH -, drives their formation at the electrochemical interface. Using mixtures of Cu 2+ and Zn 2+ as the metal precursors, we form spin transition materials of the herbertsmithite family-heralded as the first experimental material known to exhibit the properties of a quantum spin liquid (QSL). Single-crystal nanoparticles of ∼10-16 nm were produced by GDEx, with variable Cu/Zn stoichiometry at the interlayer sites of Zn xCu 4-x(OH) 6Cl 2. For x = 1 (herbertsmithite) the GDEx nanoparticles demonstrated a quasi-QSL behavior, whereas for x = 0.3 (0.3 < x < 1 for paratacamite) and x = 0 (clinoatacamite) a spin-glass behavior was evidenced. Finally, our discovery not only confirms redox reactions as the driving force to produce spin transition nanoparticles, but also proves a simple way to switch between these magnetic ground states within an electrochemical system, paving the way to further explore its reversibility and overarching implications.
UR - http://www.scopus.com/inward/record.url?scp=85081084165&partnerID=8YFLogxK
U2 - 10.1039/c9nr09884d
DO - 10.1039/c9nr09884d
M3 - Article
VL - 12
SP - 5412
EP - 5421
JO - NANOSCALE
JF - NANOSCALE
SN - 2040-3364
IS - 9
ER -