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Crossover from equilibrium to nonequilibrium dynamics in a reentrant AuFe ferromagnet

P. Mitchler, R. Roshko, W. Ruan

To cite this version:

P. Mitchler, R. Roshko, W. Ruan. Crossover from equilibrium to nonequilibrium dynamics in a reentrant AuFe ferromagnet. Journal de Physique I, EDP Sciences, 1992, 2 (12), pp.2299-2309.

�10.1051/jp1:1992282�. �jpa-00246702�

(2)

Classification

Physics

Abstracts

75.508 75.50L 75.60L

Crossover from equilibrium to nonequilibrium dynamics in

a

reentrant Aufe ferromagnet

P.

Mitchler,

R. M. Roshko and W. Ruan

Department

of

Physics, University

of Manitoba,

Winnipeg,

Manitoba, Canada R3T 2N2

(Received 26 May 1992, accepted in

final

form Ii August 1992)

Abstract. Measurements of the

decay

of the low field thermoremanent

magnetization,

over four decades of observation time, 6 s

w t

w10~

s. as a function of temperature T and wait time t~, have been

performed

on two Aufe

alloys

located on either side of the multicritical

point

: a Au~ofejo

spin

glass and a

strongly

bond-disordered reentrant Au83Fej~ ferromagnet. The

spin glass

relaxation isotherms exhibit the canonical symptoms of

nonequilibrium

ordering below

Tso,

the isotherms are characterized by an inflection

point,

on a

logarithmic

time

perspective,

which is sensitive to the wait time t~,

display

a memory for a

history

of field reversals, and are all

compatible

with an

analytical representation

based on a stretched

exponential

function,

M~(i)=Mo+Miexp[- (i/r)~~"],

with r =t,~~ and a weakly temperature and wait time dependent exponent n m 0.7. The reentrant ferromagnet exhibits a

temperature-driven

crossover

between two distinct relaxation

regimes

a «

high

temperature»

regime

coincident with the

ferromagnetic

phase, characterized

by

an extremely

rapid

approach to

equilibrium, negligible

wait time effects, and a weak power law

decay, M~(t)

=

Mo

+

Mi

t~~, with a weakly temperature

dependent

exponent 0.04 w m w 0.08, consistent with the

predictions

of droplet fluctuation models of random

Ising ferromagnets,

and a « low temperature »

regime

coincident with the reentrant

phase,

with

nonequilibrium, age-dependent

dynamics which are virtually

indistinguishable

from those in the

« pure » spin glass

phase

and describable by the same stretched

exponential

relaxation function. This

study

represents the first

systematic comparison

of relaxation dynamics in the

reentrant and

ferromagnetic

phases of a system with

sequential

transitions, and

provides

compelling

evidence for the

equivalence

of the reentrant and

spin

glass phases.

1. Introduction.

Ferromagnets

with substantial

exchange

bond

disorder,

due to some forni of

quenched

structural

randomness, frequently exhibit,

upon

cooling, apparently sequential magnetic

transitions from paramagnet to

ferromagnet

to a low temperature

phase

with many of the elements

(strong irreversibility, displaced hysteresis loops) commonly

associated with

spin glass freezing.

The Aufe system, in

spite

of its well documented

metallurgical complexities [I],

is

widely recognized

as the

archetype

of such « reentrant » behaviour and exhibits the

classic

symptoms [2]

: the low

frequency dynamic

response first increases

rapidly

with

decreasing

temperature, then passes

through

a

typical ferromagnetic Hopkinson

maximum

(if

(3)

the

susceptibility

is not limited

by

the

demagnetizing factor)

followed

by

a

weakly

temperature

dependent

«

plateau

», and then

abruptly

decreases

(in

a manner reminiscent of a pure

spin glass

below its

freezing

temperature

Tso)

as the

ferromagnetic phase collapses

into the

« reentrant »

phase.

Infinite

ranged

vector

spin

models for

magnetic

systems with

competing

exchange

interactions

[3] interpret

the reentrant transition as the onset of transverse

spin glass freezing

in the presence of

longitudinal ferromagnet ordering

; while local

probes,

such as M6ssbauer spectroscopy

[4]

and inelastic neutron

scattering [5],

appear to support this

identification, they

do not indicate that this

phenomenon

is critical in the sense of a

genuine cooperative thermodynamic phase change,

nor has there been any

systematic attempt

to characterize the relaxation

dynamics

within the reentrant

phase,

which are

expected

to exhibit

nonequilibrium

behaviour similar to that which dominates the relaxation response of pure

spin glasses.

According

to a

phenomenological theory [6-8] developed by

Fisher and Huse for

Ising

systems with

short-range interactions,

the low

lying

excitations which dominate the

long-

distance and

long-time

correlations in the ordered

phase

of systems with discrete broken symmetry are

droplets (or domains)

of

coherently flipped spins

enclosed

by

a

single

wall.

Droplet

formation

requires

activation over energy barriers B which grow with

length

scale L as B

~L*, leading

to

droplet

lifetimes r

exp(flL*),

and hence to

logarithmic droplet growth, L(t)~ (Tlnt)~~~.

If a

spin glass

is

subjected

to an ideal

quench

from infinite

temperature to a temperature T ~

Ts~

in zero

magnetic

field,

then,

after a time t~ has

elapsed,

the system will consist of domains of

typical

linear dimension

L(t~)

within which the

spin

configuration

is

locally equivalent

to one of the two pure

equilibrium

states

[6]

characteristic of the

temperature T,

and two

temporal

relaxation

regimes

are

distinguishable [7]

: an «

early epoch

»

(In

t « In

t~)

where relaxation occurs on

length

scales L «

L(t~) through

activated

equilibrium droplet fluctuations,

and the correlations

C(t) decay

as

C(t)~L(t)~Y~

(In t)~Y~*,

and a « late

epoch

»

(In

t

»Int~)

where the

dynamics

are a consequence of

activated

nonequilibrium

domain

growth

and the

decay

is

govemed by

a

nonequilibrium

exponent A ~y which leads to a more

rapid logarithmic

power

law, C(t)~L(t)~~

(ln

t

)~

~~*. Thermoremanent relaxation measurements allow both

regimes

to be observed in the

same

experiment [9]:

the

sample

is cooled

rapidly

in a field H to a temperature

T~TS~,

and, after a time t~ has

elapsed,

the field is

abruptly

reduced

by

an amount

AH which is small

enough

that the

overlap length

between the

equilibrium

states

(T, H)

and

(T,

H

AH)

is much

larger

than the

typical (T, H)-domain

size

L(t~).

On a

logarithmic

time

perspective,

the relaxation curves exhibit an age

(t~ )-dependent

inflection

point [9],

which

represents

the crossover between the two relaxation

regimes,

and

which,

in

practice,

is often modelled

by

a stretched

exponential

function

M(t )

exp

[- (t/r

)~ ~

],

with

r = t,n~mt~. The theoretical

justification

for this choice is

provided by

the

mesoscopic

domain model of

Koper

and Hilhorst

[10]

which

postulates

that, if a

nonequilibrium spin glass

is located in a heat bath of constant temperature T and in a constant

magnetic

field

H

then,

for any

arbitrary

choice of

(Ti, Hi ),

the system will be

composed

of

(Tj, Hi )-domains

which are characterized

by

a

specific

set of

(Tj, Hi )-spin correlations,

and which will grow

with time but never exceed the

overlap length I (Tj T, Hi

H

),

which defines the maximum

length

scale over which the

spin

correlations for the two

thermodynamic equilibrium

states

(Ti, Hi )

and

(T, H)

are

indistinguishable.

The relaxation response function of a

spin

in a domain with a

time-varying

size

s(t)

is a

complicated

functional of

s(t)

and, as in the Fisher and Huse

approach,

this model features an

interplay

between two

lengths,

a characteristic size I

(t

for a

growing

domain and the

overlap length

I

(AT,

AH ). In a field

jump experiment

of the

type described

above,

where the system is

quenched

to

T~TS~

at t =0 in a field

Ho

which is

subsquently

turned off at t

= t~, the model

predicts that,

when AH

=

Ho

is

(4)

sufficiently

small that

I(t~)~i(0, AH),

the relaxation rate exhibits a maximum at r'w t t~ m t~,

signalling

a crossover between a slow

equilibrium decay

and a more

rapid nonequilibrium

stretched

exponential decay.

In this paper, we present a detailed

comparison

of thermoremanent relaxation in the

spin glass

and reentrant

ferromagnetic configurations

of

Aufe,

and we show that the reentrant

ferromagnet

is characterized

by

two distinct relaxation

regimes corresponding

to the two

sequential

ordered

phases

: a low temperature

nonequilibrium regime,

coincident with the reentrant

phase,

in which the relaxation

dynamics

are

essentially

identical to those in the pure

spin glass phase,

and a

high temperature equilibrium regime,

coincident with the

ferromagnetic phase,

with an

entirely

different functional

representation.

2.

Experimental

details.

Two

alloys

of Aufe, one a

spin glass containing nominally

10 at. fGFe and the other a reentrant

ferromagnet containing nominally

17at.fGFe were

prepared by

arc

melting appropriate

amounts of 99. 99 fG pure Au wire and 99.99 9b pure Fe wire on the water cooled copper hearth

of a

titanium-gettered

argon arc fumace

using

a tungsten electrode. The choice of these

compositions

was based on the definitive

dynamic magnetic

characterizations of Sarkissian

II

], and,

as our static measurements

subsequently confirmed,

the

similarity

of the fabrication

and heat treatment

techniques ultimately

ensured very

comparable magnetic products.

Each

alloy

was

repeatedly

inverted and remelted in order to achieve a

homogeneous consistency,

and calculations based on total

melting

losses indicated that the true concentrations were

(at worst)

within ± 0.3 at.fG of the nominal

values,

in each case. Each of the

original ingots

was

cold rolled into a

sheet,

and one

sample

was

prepared

from each sheet: the reentrant

Au~3Fej~ ferromagnet

was a

thin, needle-shaped sample,

with dimensions 0.08 mm x 0.8 mm x10.4 mm, while the

Au~ofejo spin glass

was a

thicker, rod-shaped sample (for

enhanced

sensitivity),

with dimensions 0.9 mm x0.9 mm x5.2 mm. Each

sample

was

encapsulated

in a qualtz tube in an argon

atmosphere,

annealed for 3

days

at

900

°C,

and then

quenched rapidly

into water, in order to

generate

an

atomically

disordered state, and an EDAX

analysis

was consistent with a

high degree

of

homogeneity

and

negligible clustering.

The static

magnetization

and remanent relaxation measurements were

performed

with a variable temperature, variable

frequency SQUID

susceptometer,

operating

in the

magnetometer mode

(w

=

0),

as described in detail elsewhere in the literature

[12].

3. Data

analysis

and discussion.

Figure

I shows the temperature

dependence

of the low field static

magnetization

of the

Au~ofeio spin glass

and the reentrant

Au83Fej7 ferromagnet,

measured under both field

cooled

(PC)

and zero field cooled

(ZFC)

conditions. The

spin glass

exhibits the canonical

cusp-like

structure at

Ts~

=

32K,

indicative of random

spin freezing,

and the

gradual

bifurcation of the

M~c

and

Mz~c

curves below

Ts~ symptomatic

of

irreversibility

; the reentrant

ferromagnet

exhibits

multiple

structure

(identified by

the vertical arrows in

Fig. lb)

consistent with the

dynamic

measurements of

Sarkissian[11],

and thus with the formation of a

ferromagnetically

ordered state below about T~ m100

K,

which

subsequently collapses

near

T m 40 K into a low

temperature

reentrant

phase,

within which the temperature

dependence

of the PC and ZFC

magnetizations

mimic those in the pure

spin glass phase.

In order to

fully appreciate

the

significance

of the relaxation

dynamics

of the Aufe system in its reentrant

configuration,

it is first essential to characterize the thermoremanent

decay

within the pure

spin glass phase,

and

figure

2 summarizes the essential features of this

decay

at a

typical

measurement temperature

T~

=

22K. Each relaxation isotherm in

figure

2a was

obtained

by cooling

the

sample

in an

applied

field

H~

= 5.0 Oe from a reference

temperature

(5)

la)

Au~fe~~

Ha=500e 16)

Au~fe~~

Ha.05

/~

~OO~OOOOOO~

~

Fcoo°°

'

~

~o j

°~ ~

~i

°~°°~

~

~~

Cl

, j LO ,

f I '.

i

w O 'O ©

~ O*

2 ~

OO ~

*

°

' O

° O. ZFC ~~'

.' e

5o o ioo

T(K)

Fig. I. (al The temperature dependence of the field cooled (FC) and zero field cooled (ZFC) static

magnetization

of the

Au~ofejo spin

glass measured in an

applied

field H~ = 5.0 Oe. (b) The temperature

dependence

of the FC and ZFC static magnetization of the reentrant Au83Fe17

ferromagnet

measured in

an

applied

field H~ = 0.5 Oe. The vertical arrows

identify

the structural features which also characterize

the measurements of the

dynamic

response in reference [11].

(~) T~= 22 K (bl

fl

6O ~

i

'

I

w Q~

7

9 _.~ 9

~~ .~ m

~

s

s

2 3 4 2 3 4

log t

Fig. 2. (a) The

decay

of the therrnoremanent

magnetization

of the Au~ofeio spin glass at a typical

measurement temperature

T~

= 22 K,

plotted

on a

logarithmic

time scale, for five different wait times

t~. The vertical arrows mark the locations of the inflection

points

as determined from the maxima in the relaxation rate S(t ), and the solid curves illustrate

typical

fits to

equation

(I ) for two extreme wait times.

(b) The

numerically

calculated relaxation rate S(t

w

am~lafn

t for four of the five relaxation curves in

figure

2a,

plotted

on a

logarithmic

time scale.

T~

=

60K in the

paramagnetic regime,

where relaxation effects were

negligible,

to the

measurement temperature

T~

=

22K

(the cooling procedure

was very

reproducible

and

yielded cooling

times

consistently

close to t~ = 500 s),

waiting

for a

predetermined

time t~ to

elapse

at constant temperature

T~,

then

abruptly removing

the

applied

field and

recording

(6)

the

decay

over four decades of observation time 6s

~ t

w10~s.

On

a

logarithmic

time

perspective,

the relaxation isotherms all exhibit well defined inflection

points

which coincide, within

experimental

error, with the effective age of the system, so that t,~~ = t~ + t~ this age

dependent

behaviour is a manifestation of the

nonequilibrium

nature of the

spin glass

state, and translates into a maximum in the relaxation rate

S(t)w %M~/%fn

t at t~ = t~ + t~ which propagates towards

longer

observation times with

increasing

t~, as shown in

figure

2b. The existence of

macroscopically long

relaxation times in the

Au~ofeio spin glass ultimately implies

that the

decay

of the thermoremanent

magnetization depends

on the

history

of the

sample

and should thus

display

a memory for past events. This is

vividly

illustrated in

figure 3,

which shows the time

dependence

of the thermoremanent

magnetization

measured at

T~

= 22 K

after

the

sample

was

subjected

to the sequence of field reversals

depicted

in the upper half of the

figure

; the oscillations observed in zero

applied

field are a manifestation of the

principal

of

superposition [13]

which assumes that the memory of a field

change

is not

erased

by

a

subsequent reversal,

and which describes the net relaxation response as the sum of

a sequence of

essentially independent

responses.

.

,' P~ i

~ ~ ~~

'~

,

m

°., ~/

~

2 3 4

log

Fig.3.-The

memory effect: the time

dependence

of the therrnoremanent

magnetization

of the

Au~ofeio spin glass

after the

sample

was cooled in zero field to the measurement temperature T~

= 22 K and then subjected to the sequence of field pulses shown in the upper half of the

figure.

In order to

permit quantitative comparisons

with the reentrant

data,

it was instructive to establish a functional

description

of the relaxation isotherms in

figure

2a. Of the various

empirical

and theoretical

representations proposed

in the

literature,

the

simplest

formulation which was

capable

of

consistently

and

accurately replicating

the

principal

structural features of the

experimental

data over

virtually

the entire observational time

window,

consisted of the

superposition

of a stretched

exponential

and a constant term

MR(t)

=

Mo

+

Mi

exp

i- (t/r

)~

~~i (I)

(It

should be mentioned here that double

logarithmic plots

of

M~(t)

as a function of

in

t, constructed to

verify

the Fisher and Huse

prediction

that

M~ (in t)~

Y, do not

yield

(7)

straight

lines over any extended

temporal interval,

but rather exhibit continuous curvature with

a

monotonically increasing negative slope, although

the

systematic

trend towards

larger

values of y with

increasing

observation time is

generally

consistent with the crossover from slower to

faster

dynamics expected

within the

droplet

fluctuation

formalism.)

Table I presents a

comprehensive

list of the best fit values of the

parameters Mo,

n, and r,

along

with a number of other relevant

experimental

parameters, for a sequence of relaxation isotherms

(including

those in

Fig. 2)

with measurement temperatures

T~ spanning

much of the

spin glass phase,

and the solid curves in

figures

2a illustrate

typical

fits for two extreme wait times. For wait times t~ w 240 s,

equation (I) provides

a

complete description

of the measured isotherms over the entire

experimental

time interval

(6

s ~ t w

10~ s),

and the characteristic time r agrees, within

experimental

error, with the location of the inflection

point

t~n~ deduced from the maxima in the relaxation rate S

(t ).

This

correspondence

continues to hold for

longer

wait times t~ ~ l 000 s,

although

the range of

validity

of the stretched

exponential

fit becomes

progressively

narrower,

with

systematic

deviations apparent at short observation times

(solid

curve for t~ =

3 600 s in

Fig. 2a).

Such behaviour is consistent with

previous investigations [14],

which suggest that the

applicability

of the stretched

exponential

is restricted to

experimental

time intervals in the immediate

vicinity

of the effective

experimental

age of the system, where the relaxation rate is dominated

by

the influence of the

aging

process, but that it is

incompatible

with the short time

(t

«

t~) equilibrium

response, which is

expected

to be a weak power law

decay [14].

The

magnitude

of the exponent n is

typical

of

spin glasses,

and exhibits a

slight

increase with

measurement temperature for

T~/Ts~

~

0.8,

as well as a weak inverse

dependence

on the wait time t~, which is

just resolvable, experimentally.

The introduction of the constant term

Mo

is difficult to

justify

on

physical grounds,

and is

probably symptomatic

of a further limitation inherent in the stretched

exponential representation,

which vanishes too

rapidly

to

provide

a proper

description

of the actual

long

term

decay

to zero

magnetization [9]

;

nevertheless,

such a term is an essential

ingredient

of other

empirical representations [9, 15]

of

spin glass relaxation,

even those

[15]

which do not

explicitly

invoke a stretched

exponential

component, and exhibits similar temperature

dependent systematics [9].

Table I.

Au~ofejo spin glass

parameters.

Tel) ~(s) ~(8) n (s)

13 60 640 600+200 730+10 0.68+0.01 1.63+0.01 6-10'

20 60 610 600+200 630+8 0.71+0.01 1.16+0.01 6-10'

22 60 610 360+100 440+6 0.67+0.01 0.96+0.01 6-10'

22 240 720 700+100 690+8 0.67+0.01 0.93+0.01 6-10'

22 1200 1680 2000+600 2050+60 0.65+0.01 0.88+0.02 10-10~

22 1800 2280 3000+600 2060+70 0.62+0.01 0.98+0.02 20-10'

22 3600 4050 4000+1000 4006+240 0.69+0.01 0.98+0.04 160'-10'

24 60 570 250+100 290+3 0.70+0.01 0.70+0.01 6-10'

26 60 780 350+100 330+4 0.72+0.01 0A7+0.01 6-10'

28 60 630 250+100 185+3 0.73+0.01 0.30+0.01 6-10'

The characterization of the thermoremanent relaxation in the reentrant

Au~~fei~ ferromagnet proceeded by adapting

the

experimental

and

analytical techniques developed

for the

Au~ofejo spin glass.

The

tendency

for residual relaxation effects to

persist

well above the

peak

in the ZFC

magnetization (see Fig. lb)

necessitated the choice of a

comparatively high

(8)

reference

temperature T~

= 140 K for

establishing

the zero level of

magnetization,

so that the

reentrant

study

was

severely

constrained

by

the

anomalously large cooling

intervals

T~-T~ (~100K

for the reentrant

phase)

and

correspondingly long cooling

times t~

(typically

l 000

s),

which allowed the

cooling

process to assume a dominant role in

defining

the age of the system.

Figure

4 summarizes the

thermorenianent decay

for

a sequence of

representative

measurement temperatures

T~ spanning virtually

the entire ordered

phase (15

Km

T~w100K),

with all isotherms

corresponding

to an identical

cooling

field

H~

= 2 Oe and wait time t~ =

60 s. While the structure of these isotherms

(particularly

at the lower

temperatures)

is much broader and

considerably

more subtle than that associated with

« pure »

spin glass

relaxation

(undoubtedly

a consequence of the

comparatively

slow

cooling rates),

there is nevertheless an

unmistakable, progressive change

in curvature

throughout figure 4,

from concave down to concave up with

increasing

measurement temperature

T~. Furthermore, quantitative analysis

of the isotherms reveals that there are nvo distinct types

of relaxation

behaviour, corresponding

to two distinct

temperature regimes

each of which coincides with one of the two ordered

phases

which characterize the reentrant sequence, and the isotherms in

figure

4 have been

grouped accordingly

in order to reflect this

dichotomy

:

(a)

a low temperature (« reentrant

») regime

in

figure

4a with

T~

~ 35

K,

where the isotherms all possess inflection

points

and exhibit a wait time

dependence

indicative of

nonequilibrium

processes and describable

analytically by

the

superposition

of a stretched

exponential

and a

constant term as in

equation (I),

and

(b)

a

high

temperature («

ferromagnetic ») regime

in

figure

4b with

T~~35K,

where

aging

effects are

negligible

and where the

decay

is

incompatible

with a stretched

exponential representation,

but is consistent with a weak power law

dependence

of the form

M~(t)

=

Mo

+

Mj t-m, (2)

(a) (b)

~~ Tm(K)

, so

~ ~~~ ~~

f

~

70

80

uo

io ioo 1

tog t

Fig.

4.-(a)

Decay

of the thermoremanent

magnetization

at several

representative

temperatures

T~

within the reentrant

phase

of the

Aug~fej~ ferromagnet,

for a wait time t~ = 60 s,

plotted

on a

logarithmic

time scale. The vertical arrows mark the locations of the inflection

points.

(b) Decay of the thermoremanent

magnetization

for t~ = 60s at Several

representative

temperatures T~ within the

ferromagnetic phase

of

Aug~Fej7.

(9)

symptomatic

of relaxation fron~ a

fully equilibrated

field cooled state.

Figure

5

provides

a

typical

illustration of the

quality

of th± fits for selected isotherms in each of the two relaxation

regimes.

and tables II and III list all the relevant

experimental

parameters,

including

the best fit values of the constants

Mo,

n, r, and m in

equations (I

and

(2).

Based on a

comparison

with the relaxation

dynamics

of a pure

spin glass,

as defined

by figure

2 and table I, the

magnitude

and variation of the stretched

exponential

parameters n and r in table II are

completely

consistent with

orientationally

random

spin freezing

within the low

temperature

reentrant

regime. However,

the constraints

imposed

on the

experimental cooling

rates

by

the

necessity

to cool the system over

relatively large

temperature intervals

T~ T~

are

responsible

fur some apparent

systematic discrepancies

; in

particular,

while the

experimental cooling technique

is unable to

distinguish

bet~N.een

cooling

intervals

differing by typically

A

(TR T~ )/T~

0. I, so

that the nominal

experimental

age t~+t~ of the system is

essentially independent

of

measurement temperature

T~

within the reentrant

phase,

the location of the inflection

point

t~n~ = r

(see

vertical arrows in

Fig. 4a),

and hence the true age of the system, exhibits an

obvious inverse correlation to

T~, shifting

from t,n~ ~ t~ + t~ to t,n~ ~ t~ + t~ with

increasing

measurement temperature. This behaviour

is,

however,

entirely

consistent with the absence of

aging

observed

throughout

the

ferromagnetic phase,

and

merely

confirms that the system is

continuously

in

equilibrium throughout

the initial

portion

of the

cooling interval,

and that

aging

processes do not commence until the system has been cooled

through

some effective reference temperature

Ti

which lies well below

T~

but close to the

ferromagnetic-reentrant phase boundary (although

fine

tendency

for t~n~ to exceed all of the obvious

experimental

time

(a) (b)

5emu/g

M~

05emu/g

70K

90K

~2 3 4 2 3 4

log t

Fig.

5. -(a)

Typical

fits (solid curves) of

Eq.

(I) to some of the reentrant relaAtion isotherms of

Aug~fej~

for two different wait times t~ = 60 s(.) and t~ = 7 200 s (A). The vertical arrows mark the locations of the inflect:on points, and the zero magnetization levels of the relaxation curves have been shifted by arbitrary amounts for clarity of

presentation,

so that only, the scale of the relaxation has been indicated in the lower left of the figure. (b)

Typical

fits (solid curves) of

equation

(2) to some of the

ferromagnetic

relaxation isotherms of

Aug~fej~.

As in

figure

a,

only

the scale of the relaxation has been indicated in the upper

right

of the

figure.

(10)

Table II.

Au~~Fei7

reentrant

phase.

t~(S) t~+t~(s) tan(s) ~s) n (s)

16 60 900 3500+1000 2860+l10 0.77+0.01 2.98+0.01 6-10'

17.5 60 900 3000+1000 2330+l10 0.83+0.01 2.92+0.01 5~10'

20 60 960 2500+500 2560+140 0.88+0.01 2.37+0.01 5-10'

20 7200 8220 > 10' (1.9+0.9)x10~ 0.87+0.01 2.75+0.03 6~10'

21.6 60 1200 1600+600 1800+180 0.91+0.01 2.82a0.01 6~10'

22.5 60 1260 1200+300 1000+70 0.92+0.01 2.80a0.02 5-10'

22.5 7200 8260 4000+1000 4800+300 0.89+0.01 2.7l+0.02 5~10'

23 60 l160 1200+500 1760+50 0.93+0.01 2.78+0.01 5~2.7x10'

23 7200 8220 > 10' (5.4+0.3)x10' 0.89+0.01 2.77a0.03 5~l.5x10'

23.5 60 1200 < 10 7.0a2.0 0.96+0.01 2.68+0.03 5-10'

Table III.

Au83Fe17 ferromagnetic phase.

T~O~) ~(s) m

40 60 0.06+0.01 1.69+0.01

45 60 0.06+0.01 1,64+0.01

60 60 0.04+0.01 lA7+0.02

65 60 0.04+0.01 lA6+0.01

60 60 0.04+0.01 1.38+0.01

60 7200 0.04+0.01 1.38+0.01

65 60 0.06+0.01 1.37+0.01

70 60 0.06+0.01 1.30+0.01

70 7200 0.04+0.01 1.30+0.01

75 60 0.08+0.01 1.27+0.01

80 60 0.07+0.01 1.18+0.01

80 7200 0.06+0.01 1.18+0.01

86 60 0.06+0.01 1.12+0.01

90 60 0.08+0.01 1.05+0.01

100 60 0.08+0.01 0.85±0.01

constants at the lower measurement

temperatures

is further evidence that slow

cooling

rates

distort the

anticipated correspondence

between t~ + t~ and tin~,

and,

in

fact,

accelerate the

aging process).

As mentioned

earlier,

the zero field

equilibrium (t~

=

co)

relaxation in

spin glasses

is

expected,

on the basis of both Monte Carlo simulations

[16]

as well as critical fractal-cluster model calculations

[17],

to be characterized

by

a slow

power-law decay

below

Ts~,

and this

expectation

is

supported by

both static and

dynamic

measurements of the relaxation rate S in various canonical

spin glass systems [17].

In

ferromagnets,

remanent relaxation has

traditionally

been attributed to domain rotation and wall

motion,

and models

[18]

which invoke activation processes over a smooth distribution of barrier

heights predict logarithmic

time

(11)

dependences. However,

more recent theoretical

investigations

of

Ising ferromagnets, specifi- cally

those with

quenched

random

exchange disorder,

suggest

[8]

that power law

decay

is also

a feature of the

equilibrium dynamics

of random

ferromagnets. Apparently,

the low

frequency, long length

scale fluctuations in the ordered

phase

of such systems with

spontaneously

broken discrete symmetry are

droplets

of

coherently

reversed

spins

surrounded

by

domain walls which

are

pinned

to the disorder, so that

droplet

annihilation

requires

thermal activation over

large free-energy

barriers which grow with

length

scale. In

fact,

the

long-time

behaviour of the

spatially averaged temporal spin

autocorrelation function C

(t)

w

(S,(0) Sj(t)) (S,)~)

,

where

(.. )

denotes an infinite-time average and

(.. )

~

a

configuration

average, is dominated

by droplet

excitations with

anomalously long

relaxation times

which,

in random

ferromagnets (through

a combination of activated

droplet

lifetimes and Boltzmann

droplet

excitation

probabilities [8]),

are

exponentially

i-are in

in

t,

yielding

a power law

decay

:

c

(t j

~- kiln ti

~ ~- tiT)

(3j

for random

exchange

where y = I.

(This

result appears not to be

specific

to

Ising spins,

since

recent models

[15]

for activated relaxation of

dispersive

excitations on a

percolation

distribution of fixed finite-sized

domains,

which are based on

quite general geometric

considerations

independent

of such

specifics

as

spin dimensionality,

and which have been

applied successfully

to pure

Heisenberg ferromagnets [19], yield

the same

asymptotic behaviour.)

Moreover, Fisher and Huse have

pointed

out

[8]

that the

region

of

validity

of the

predicted asymptotic equilibrium decay (3) expands

to include

progressively

shorter obser- vation times as the bond disorder becomes more extreme, so that

nearly

tricritical

ferromagnets

should represent the best

experimental

candidates for

assessing

the

applicability

of

equation (3).

Since these are

precisely

the conditions which favour reentrant

ferromagnetism,

it follows that the behaviour of the relaxation isotherms within the

ferromagnetic phase

of the

reentrant

Aug~fei~ alloy (viz.,

a weak power law

decay

with an exponent m 0.04

0.08,

and

negligible

wait time

effects)

may be

interpreted

as direct confirmation of the theoretical

predictions.

In summary, measurements of the low field thermoremanent relaxation on either side of the tricritical

point

in the Aufe system have revealed the existence of a

temperature-driven

crossover between two distinct relaxation

regimes

in

ferromagnets

where the

exchange

bond

disorder is sufficient to generate

sequential (or

« reentrant

»)

behaviour one of the

regimes

is coincident with the «

high

temperature »

ferromagnetic phase,

and, within the

slow-cooling

constraints of the current

investigation,

is characterized

by

an

extremely rapid approach

to

equilibrium

and

by

a weak power law

temporal decay

of the thermoremanent

magnetization

consistent with the

predictions

of

droplet

fluctuation models

[8]

of random

Ising ferromagnets,

while the other

regime

coincides with the

« low

temperature

» reentrant

phase,

and exhibits

nonequilibrium, age-dependent

relaxation

dynamics

which are

virtually indistinguishable

from those in the « pure »

spin glass phase,

and which are describable

by

a common relaxation

function which has been linked to a

mesoscopic picture [10]

of

growth

and

fragmentation

of

spin glass

domains.

Acknowledgements.

This work has been

supported

in part

by

a grant from the Natural Sciences and

Engineering

Research Council of Canada.

(12)

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JOURNAL DE PHYSIQUE I T 2, N' 12, DECEMBER J992 83

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