Synthesis, structure, and properties of Ln{sub r}Ni{sub 3}O{sub 10{minus}{delta}} (Ln = La, Pr, Nd)
- Rutgers-The State Univ. of New Jersey, NJ (United States)
The Ruddlesden-Popper nickelates Ln{sub 4}Ni{sub 3}O{sub 10{minus}5}, with Ln = La, Pr, and Nd, have been synthesized by a precursor method. Power X-ray diffraction studies show orthorhombic symmetry with space group Fmmm for all three compounds; however, electron diffraction patterns of single crystals show that the space group symmetry is lower than F or C. The orthorhombic unit cell parameters decrease monotonically with decreasing effective ionic radius of the lanthanide ion. The distortion from ideal tetragonal symmetry and the orthorhombic strain increase with decreasing radius of the lanthanide ion; Nd was the smallest lanthanide for which Ln{sub 4}Ni{sub 3}O{sub 10{minus}5} could be stabilized. Pr{sub 4}Ni{sub 3}O{sub 10{minus}5} and Nd{sub 4}Ni{sub 3}O{sub 10{minus}5} are oxygen deficient ({delta} {approximately} 0.15), while La{sub 4}Ni{sub 3}O{sub 10} is nearly stoichiometric. The resistivity measurements indicate metallic temperature dependence for La{sub 4}Ni{sub 3}O{sub 10}, and a metal-to-metal transition for Pr{sub 4}Ni{sub 3}O{sub 10{minus}5} at 145 and 165 K, respectively. These anomalies are attributed to charge-density-wave driven instabilities and are confirmed by differential scanning calorimetry to coincide with first-order structural phase transitions. The magnetic susceptibility of metallic La{sub 4}Ni{sub 3}O{sub 10} is nearly temperature independent above 100 K, and shows paramagnetic behavior at lower temperatures. Pr{sub 4}Ni{sub 3}O{sub 10{minus}5} and Nd{sub 4}Ni{sub 3}O{sub 10{minus}5} and Nd{sub 4}Ni{sub 3}O{sub 10{minus}5} show paramagnetic behavior in the temperature range 4-300 K, due to the large magnetic contributions of the lanthanides to the total moment.
- Sponsoring Organization:
- USDOE
- OSTI ID:
- 146432
- Journal Information:
- Journal of Solid State Chemistry, Journal Name: Journal of Solid State Chemistry Journal Issue: 2 Vol. 117; ISSN 0022-4596; ISSN JSSCBI
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
CALORIMETRY
CHEMICAL PREPARATION
CRYSTAL STRUCTURE
ELECTRIC CONDUCTIVITY
LANTHANUM COMPOUNDS
MAGNETIC PROPERTIES
MAGNETIC SUSCEPTIBILITY
NEODYMIUM COMPOUNDS
NICKELATES
ORTHORHOMBIC LATTICES
PARAMAGNETISM
PHASE TRANSFORMATIONS
PRASEODYMIUM COMPOUNDS
TEMPERATURE DEPENDENCE
TEMPERATURE RANGE 0000-0013 K
TEMPERATURE RANGE 0013-0065 K
TEMPERATURE RANGE 0065-0273 K
TEMPERATURE RANGE 0273-0400 K