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Motional narrowing of the nuclear magnetic resonance line by the sliding of spin-density waves
E. Barthel, G. Quirion, P. Wzietek, D. Jérome, J. Christensen, M. Jørgensen, K. Bechgaard
To cite this version:
E. Barthel, G. Quirion, P. Wzietek, D. Jérome, J. Christensen, et al.. Motional narrowing of the
nuclear magnetic resonance line by the sliding of spin-density waves. Journal de Physique I, EDP
Sciences, 1993, 3 (7), pp.1501-1505. �10.1051/jp1:1993195�. �jpa-00246809�
Classification Physics Abstracts 75.30F 72.15N
Short Communication
Motional narrowing of the nuclear magnetic
resonanceline by the
sliding of spin-density
wavesE. Barthel
I'),
G.Quirion I'),
P. WzietekI'),
D. Jdrome(~),
J. B. Christensen(~),
M.
J#rgensen (~)
and K.Bechgaard (~)
(~) Laboratoire de
Physique
des Solides, UniversitdParis-Sud-CNRS,
F-91405Orsay,
France(~)
CISMI,University
ofCopenhagen, Blegdamsvej
21, DK-2100Copenhagen,
Denmark(Received
18 January 1993,accepted
4May1993)
Abstract. We report on a
study
of the electricalconductivity
and~~C-NMR
in the nonlinearconductivity regime
in thespin-density
wave(SbW) phase
of(TMTSF)2PF6 (TMTSF
stands fortetramethyltetraselenafulvalene).
Thenarrowing
of the NMR line demonstrates that there is a bulk motion of the SDW. We find aqualitative
agreement between the nonlinear currentand the minimum current necessary to narrow the NMR line in the
simplest
model of SDW conduction.The
anisotropic organic
conductor(TMTSF)2PF6 Ill
is in severalrespect
theprototype
mate- rial for thestudy
of theproperties
of the one dimensional(I-D)
electron gas. A verystriking signature
of I-Dphysics
is thecompetition
between electron-electron and electron-holepairing
instabilities.
Due to the
stcechiometry
of the salt and itscrystalline structure, (TMTSF)2PF6
isformally
a half-filled band I-D conductor. This
system
is sensitive to electronic instabilities. At am- bient pressure, the most stable state is aground
stateexhibiting
a finite modulation of themagnetization
orspin-density
wave(SDW) [2].
Thedivergence
towards the SDW state is dominant aslong
as the interchaincoupling
remainssufficiently
small.Hence,
theapplication
of a
high
pressure, which enhances the transversecoupling
makessuperconductivity
the moststable state at 9 kbar [3].
The SDW state is
phenomenologically antiferromagnetic,
as demonstratedby susceptibility anisotropy
[4] data andantiferromagnetic
resonance[5].
The main difference between aregular antiferromagnetic phase
and the SDWphase
lies in the wave vector of the modulation. It wasclearly
shown from theanalysis
of~SR
[6] andproton
NMR[7,
8]spectra
that the wave vector in(TMTSF)~PFS
is incommensurate with the lattice.One of the most
spectacular properties
of thiscompound
is thesharp
increase ofconductivity
above a low threshold field
[9].
It iswidely
believed that the incommensurate character of the1502 JOURNAL DE
PHYSIQUE
I N°7SDW
ground
state is at theorigin
of a zerofrequency
collectivemode,
which in nonlinear response amounts to asliding
of the overall electron-hole condensate.Pinning
of the SDW toimpurities
accounts for the nonzero threshold field.The same nonlinear
conductivity
is found incharge-density
waves(CDW).
In the NMRspectrum,
the presence of the CDW induces a broadfrequency
distribution because of thespatial
distribution of the electric fieldgradient.
In the nonlinearconductivity regime,
this line is narrowed[10].
Thisclearly
demonstrates that the additionalconductivity
induces a fastmodulation of the local
field,
thussupporting
the notion ofsliding.
A
~H-NMR study
of thesliding
SDW in thequenched
SDW state of(TMTSF)2Cl04
has beenreported recently [ill. However,
theprotons
aredipolarly coupled
in four distinctmethyl
groups, and
give
rise toa very
complex
structure. The'~C-NMR
at the carbon sites at the center of the TMTSF molecule are much better suited for thesestudies,
because thespectrum
issimpler,
and thecoupling
of these nuclei to the SDW isstronger
than thecoupling
ofprotons.
We demonstrated in a
previous
paper[12]
that the'~C-NMR
line in(TMTSF)2PF6
is alsoconsiderably
broadened in the SDW state.In this
communication,
wereport
thepreliminary
results of astudy
of the electrical con-ductivity
and~~C-NMR
in the nonlinearconductivity regime
of(TMTSF)2PF6. Narrowing
of the NMR line demonstrates that there is a bulk motion of the SDW. We find a
qualitative agreement
between theinjected
current and the minimum current necessary to narrow the line in the mostsimple
model ofsliding.
The
sample
comes from the same batch ofselectively ~~C
enrichedcrystals [13]
we used in ourprevious
measurements[12].
Theoccupation probability
for each of the central sites(labelled (3)
and(13)
in[14])
is 5il.
Its size was 3.0 x 0.25 x 0.3mm~,
with a cross-section of 6 x10~~ mm~
anda mass of 0.35 mg. All measurements were
performed
in the 9.3 T NMR field. For thecontacts,
we did not use silverpaint,
because it is notorious forcracking
uponcooldown,
but twoclamped
contactsapplied
on thegold-plated
b-c faces of thesample.
Nojump
in theresistivity
was observed uponcooldown,
and the residualresistivity
at 15 K was 0.9 Q. The 18 Q resistance at 4.2 K is thus almostentirely
due to thesample,
inagreement
with the very
large
transversemagnetoresistance
of the SDWphase [15].
At 4.2
K,
in the SDWphase,
weclearly
observe a threshold field of 5mV/cm
in the current-voltage (I-V)
characteristics(Fig. I),
which is consistent with the usual values[16].
We obtained the NMRspectra (Fig. 2) by
an echo sequence with a Bruker MSL400spectrometer.
At 9.3
T,
the'~C frequency
is 99.67 MHz. At zerocurrent,
thespectrum
exhibits two very wideU-shaped
structures which aretypical
of theinhomogeneous broadening
due to thesinusoidally spatially
modulatedmagnetization.
Each one is associated with one of the twoinequivalent
sites. The contribution of the other carbons is
negligible
because of the small'~C
concentration andlong
relaxation time.Under
current,
two narrowpeaks
grow out of the broad distributions. Theirintensity
in-creases with
increasing
current.However,
even at ImA,
there remains a reminiscence of thezerc-current
spectrum.
We believe this is due to theinhomogeneity
of the currentdensity
in thesample. Therefore,
there is a substantial fraction of thesample
in which no SDW current flows. We estimate this fraction as 75il
at 0.5mA,
and as 60it
at I mA.At the same
time,
the presence of a static fractionclearly
demonstrates that the appearance of the twopeaks
in the nonlinearconductivity regime
is not due toheating
of thesample
abovethe
phase
transition. We also stress that ifheating
wereinvolved,
theintensity
of the NMRsignal
should decreaseby
at least a factor of3,
which is not observed.These results confirm the
sliding
SDWpicture. However,
the exact nature of thesliding
mode can be characterized further
by
the ratio of the SDW current perchain, jsDw,
to the localphase
oscillationfrequency
vj(phase winding rate).
Thisratio,
in thesimplest
modelzo
(
~
j
~
O-S
l~ ("
$ ~
Q~ °'°
~
~l,oa
0 0
ectric field mV/cm)
Fig,
I.Sample
resistance as a funtion of electric field(T
= 4.2
K).
Inset: nonlinear SDW currentISDW " I
V/R(E
-
0)
as a function of the total current 1.1=imA
i=o.5mA
1=omA
-400 400 800
shift
(ppm)
Fig.2.
NMR spectra in the SDWphase
as a functionif
the total samplecurrent I at T
= 4.2 K.
1504 JOURNAL DE
PHYSIQUE
I N°7[17],
isexpected
to be:jsDw/v4
= 2e(I)
It can be
indirectly
determinedby measuring
thefrequency
of the conduction noise which appears in the nonlinearconductivity regime
versus current.Up
to now, these determinations[18]
haveyielded
a ratio which is between 8 and 20 times smaller thanexpected
fromequation (I). Although
it is not clear whether the noisefrequency
isequal
to thephase winding
rate or twicelarger,
these datasuggested
alarge discrepancy
with thetheory.
It isusually
assumed that this arises as astrongly inhomogeneous depinning,
which leads to an erroneous estimate of the effectivesliding
cross-section.We estimate the SDW current from
IsDw=I-V/R,
where R is the low electric field resistance
(Fig. I, inset). Then, using
a chain cross section of 100i~
anda
depinned
fraction inferred from the NMRspectra,
we find fromequation (I)
a mean
phase winding
rate of 30 kHz ata total current of 0.5
mA,
and 56 kHz at I mA. The simulations show that suchfrequencies
arehigh enough
toyield
a substantialnarrowing
of the line.Therefore,
we cannotexclude,
on the basis of thesedata,
that thejsDw/vj
ratio isconsiderably
smaller thanexpected. However,
this is not necessary.We conclude that there are
large amplitude
localphase
fluctuations in the non linear con-ductivity regime
in(TMTSF)2PF6.
This result is consistent with theaccepted picture
of asliding spin-density
wave.Although
a smalljsDw/vj
ratio is not in contradiction with ourresults,
it is not necessary toexplain
our data.Obviously,
combined conduction noise andNMR measurements are needed to solve this
problem.
After this work was
performed
we learned that W. H.Wong
and coworkers[19]
had also observedsliding
SDW in(TMTSF)2PF6 by ~H-NMR
in lowmagnetic
fields.Acknowledgments.
Useful discussions with G. Kriza are
acknowledged.
We aregrateful
to J. C. Ameline forbuilding
the NMRprobe
andtogether
with G.Tevanian,
for decisivehelp
with the contactsystem.
E. B.acknowledges support
from the Et~des Doctorales de l'EcolePolytechniq~e.
References
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E.M.,
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K.,Phys.
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R. V.,Chiang
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K., Phys. Rev. Lent. 62(1989)
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Thorup N.,
RindorfG., Soling
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M.,
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1507-1508 JULY 1993, PAGE 1507Corrigendum and addendum to section 3 of "Level spacing
functions and
nonlinear differential equations"
G. Mahoux and M.L. Mehta
J.
PlJys.
I. France 3(1993)
fi97-715.In the above reference we missed to note that the functions
A,
w, ~, u, andif
inequations
(3.ll)-(3.21)
are real for real r, so that the absolute value ofya~(T)
isunity
for real T. In otherwords,
if we set ya2 "exp(2ip), p(T)
is real for real T, satisfies the(non linear)
differentialequation
p"
+
~'~ ~)
tan pp'~
+ 4 = 0(3.28)
T
and near T = 0 has the
expansion
p(T)
= -2TJ (T
+o(T~)1 (3.29)
Thus
equation (3.5)
should be corrected asya2 = exp
(-4iT
+4i(T~
+O(T~))
= 4iT +
4(I( 2)T~
+ 16(
~~ T~ +O(T~). (3.5')
3
Also it was shown that each of the four functions Re
S(T),
ImS(T), A(T), B(T)
can beexpressed
in terms of a fifth Painlevd transcendent(P5),
and one ofthem, namely B(T),
also in terms of a third Painlevd transcendent(P3). Actually, according
to Gromak(see
the referencebelow),
each of theremaining
three functions can also beexpressed
in terms of a P3. In otherwords,
as the P5 withequation (3.5')
is related to the P3 withequation (3.8),
so the P5 withequations (3.2), (3.3)
and(3A)
are related to the P3 withrespectively
(1)a=-I, fl=3, 1=1, b=-I;andforT«I,
Y(T)
--1+ 3 1)
T +
(-I
+
<1
T~ +
(3.30)
(2)cY=-I, fl=3,1=1, b=-I;andforT«I,
y(~~ ~~~~ (T~
3
I $
~(3.31)
and
(3)cY=I, fl=I, i=I, b=-I;andforT«1,
~3 Y+(~)
" ~~ +(~~
j
+ '(3.32)
or another
possible
choicey_
(T)
=( (~
T +
(3.33)
T 3
Here are the necessary details. This addendum is
supposed
to be read with theoriginal
reference.
Consider the
couple
ofequations
~ R~
T
~~' ~)
'
~
f~1 ~~'~ ~) ~~'~~~
Eliminating f
onegets equation (3.10),
whileeliminating
R onegets f"
=
)f'~ ( $~
+
f(f~ -1). (3.35)
Set
f
=1t/(1t 1),
or ~ =f~/( f~ I),
so that'~~~ i~~1L
-~l)
'~~~ ~~~
~'~ ~~~ ~'~ ~~ ~~~
This is
again
almost a PS with b=
0,
and becomes a standard PS ontaking
T~ as the newindependent
variable.Consider now the
couple
ofequations
~
~~ ~' ~~'
~ TIL'~~1L
1)
~~ ~~~Eliminating
uJ, onegets (3.36),
whileeliminating
1t onegets
a P3 for uJ with cY=
-I, fl
=
3, 1=1,
b= -I.
In
equation (3.21)
if one writesf
=(y~ 1)/(2iy),
then onegets
Y" "
~ ~
+
(y~
+I)
+y~
,
(3.38)
a P3 with o
=
l~ fl
=I,
i =I,
b = -I.Expressing
y in termsoff,
y+ =
it
+-, (3.39)
one
gets equation (3.32)
or(3.33).
Some
one-parameter
families of solutions of theseequations
areknown,
but none of them satisfies our conditions at T = 0.Reference