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Journal of Magnetism and Magnetic Materials
journal homepage: www.elsevier.com/locate/jmmm
Path dependent magnetic states and evidence of kinetically arrested states
in Nd doped LaFe
11.5
Al
1.5
Pallab Bag, R. Nath
⁎
School of Physics, Indian Institute of Science Education and Research, Thiruvananthapuram 695016, India
ARTICLE INFO
Keywords:
Rare-earth metal
First order phase transition
Phase coexistence
Magnetic glass
Kinetic arrest
Specific heat
ABSTRACT
First order antiferromagnetic to ferromagnetic transition and path dependent magnetic states in
La
1-x
Nd
x
Fe
11.5
Al
1.5
for x∼0.1 are studied at low temperatures via powder x-ray diffraction, magnetization,
and specific heat measurements. X-ray diffraction measurements suggest that around 8% of high temperature
antiferromagnetic phase is converted to ferromagnetic phase at low temperatures in zero field cooling. A
systematic study of temperature and magnetic field dependent magnetization measurements show a non-
monotonic variation of upper critical field and re-entrant antiferromagnetic-ferromagnetic-antiferromagnetic
transition while warming at an applied magnetic field under zero-field-cooled condition. This has been
interpreted in the framework of kinetic arrest model for first order magnetic transition. It is also found that the
antiferromagnetic phase is in the non-equilibrium state and behaves as a glass-like magnetic state at low
temperatures. The specific heat in field-temperature space is studied and found to have a lower electronic
contribution for the non-equilibrium antiferromagnetic state, compared to the equilibrium ferromagnetic state
in this compound.
1. Introduction
Recent magnetic studies of the doped itinerant electron metamag-
netic LaFe
13
compound have revealed wide varieties of interesting
properties such as giant magnetocaloric effect [1–22], giant barocaloric
effect [8,10,23], giant magnetostriction [24,25] etc due to the onset of a
first order magnetic transition. Though LaFe
13
does not exist as it is,
but substitution of Al or Si at the Fe site, stabilizes in a NaZn
13
-type
cubic structure [24]. For LaFe
13-x
Al
x
, the ground state is antiferro-
magnetic (AFM) in the range x 1.04 ≤ < 1.82, soft ferromagnetic (FM)
for x 1.82 ≤ < 4.94, and a mictomagnetic state for x 4.94 < < 7.02 [24].
The ground state of LaFe
13-x
Al
x
for the above x-ranges can be tuned
from AFM to FM by substituting rare earth elements like Ce/Pr/Nd at
the La site [11,12,15,20,22,26,27], Si at the Al site, Co/Mn at the Fe
site [5,13,14,19,22,23,28] and with interstitial addition of H/C/N/B
atoms [2,4,6,15,16,21,22,29–32]. With increasing temperature, the
compounds having FM ground state show a first order FM-AFM
transition followed by a second order AFM to paramagnetic (PM)
transition or only a first order FM-PM transition depending on the
doping concentration [3,6,7,12,15,16,19,21,22,24–27,31–34]. The
first order magnetic transition in these systems are accompanied by
around 1% iso-structural change in volume where the low temperature
FM state has the higher volume than the high temperature AFM (or
PM) state [24,35,36]. Moreover, the FM state has the higher electronic
contribution or the lower resistivity than that for the AFM state
[12,24,27,28,32].
The first order magnetic transition in this series can be explained on
the basis of the itinerant electron magnetism model, which basically
depends on the Fe-Fe distance and its coordination number
[24,25,36,37]. The magnetism in these systems arise due to Fe, which
have two crystallographically inequivalent sites 8b [Fe(1)] and 96i
[Fe(2)] [24,37]. Neutron diffraction measurements suggest that the FM
clusters/icosahedra composed of twelve Fe(2) and one Fe(1) sites are
coupled ferromagnetically in the (100) plane and antiferromagnetically
between the planes [35,37]. The first order magnetic transition is also
strongly dependent on external perturbations such as magnetic field
and external pressure [3,8,13,15,16,21,24,26,31,33,34,38].
It is reported that the ground state of LaFe
11.5
Al
1.5
is AFM and it
shows a field induced FM state at low temperatures [12,16,21]. With
Nd doping (at the La site), the FM state is stabilized when Nd
concentration exceeds 20%. Below this concentration, there exists a
strong AFM – FM competition, as inferred from the anomalous
temperature and field-dependent magnetic behaviour [11,12,22,26].
The magnetization data in zero-field-cooled cycle measured while
warming at an applied field (ZFCW) shows two transitions (namely
AFM to FM followed by FM to AFM) whereas, the field-cooled-cooling
http://dx.doi.org/10.1016/j.jmmm.2016.11.129
Received 30 September 2016; Received in revised form 28 November 2016; Accepted 28 November 2016
⁎
Corresponding author.
E-mail address: rnath@iisertvm.ac.in (R. Nath).
Journal of Magnetism and Magnetic Materials 426 (2017) 525–529
0304-8853/ © 2016 Published by Elsevier B.V.
Available online 30 November 2016
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