Development of a tunnelling model of charge-density-wve depinning

Development of a tunnelling model of charge-density-wve depinning

Synthetic Metals, 19 (1987) 1-6 DEVELOPMENT 1 OF A TUNNELING MODEL OF CHARGE-DENSITY-WAVE DEPINNING JOHN BARDEEN Department Urbana, of Physics, ...

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Synthetic Metals, 19 (1987) 1-6

DEVELOPMENT

1

OF A TUNNELING MODEL OF CHARGE-DENSITY-WAVE

DEPINNING

JOHN BARDEEN Department Urbana,

of Physics,

IL 6|801

University

of Illinois at Urbana-Champaign,

(U.S.A.)

J.W. LYDING, W.G. LYONS, J.H. MILLER, Jr., R.E. THORNE and J.R. TUCKER Department

of Electrical

Laboratory,

University

and Computer Engineering

of Illinois,

Urbana,

and Coordinated

IL 61801

Science

(U.S.A.)

ABSTRACT The tunneling model of transport by charge-density dimensional metals has been developed and experiment. condensate suggested

Deplnning

by the field dependence

initiated at Illinois successful

from a close interaction between theory

by coherent

in many parallel chains,

Zener tunneling of electrons

characteristic.

of the dc current.

to study detection,

Reagor

for a wide

et al. of a(~) in the

to account for CDW metals with high

such as (TaSe4)21 and the alloys Tal_xNbxS3.-

low-frequency

ac response

can be derived from parameters

frequencies.

The theory accounts

measured

The de and

measured at high

for the "narrow band" noise that accompanies

dc current flow and the subharmonic

DEVELOPMENT

tunneling theory accounts

by Gr~ner,

range i-I00 GHz suggested a modification

characteristic

In 1981, a program

mixing and harmonic generation was

The only inputs are a scaling parameter and the dc I-V

Recent measurements

pinning frequencies,

in the CDW

first applied to NbSe 3 and TaS3, was

in showing that photon-assisted

range of phenomena.

waves in quasi-one-

steps of constant current in the dc I-V

in the presence of an applied ac.

OF CONCEPTS

Recent observations

indicate that Fr~hlich conduction by moving charge-

density waves occurs in the organic transfer salt TTF-TCNQ below the Peierls transition [I]; Since the phenomena may occur in other organic metals, worthwhile

to review the background

of FrShllch conduction as developed

for inorganic metals.

Normally pinned to the lattice by impurities incommensurate

(DW's gradually become depinnned

0379-6779/87/$3.50

it may be

and current status of the tunneling theory

or lattice imperfections, and move through the lattice

© Elsevier Sequoia/Printed in The Netherlands

2 when a threshold

field is exceeded and contribute

to the current flow.

Following the discovery of FrShllch conduction in NbSe 3 in 1975, many other inorganic quasi-one-dlmensional

metals have been found that exhibit the

phenomena. Competing theories, systems[2]

one based on treating

and another as massive

freedom have been developed. development

CDW metals as macroscopic

classical systems[3] with internal degrees of

The quantum approach has undergone

in both theory and experiment,

particularly

considerable

during the past year, so

that it is now capable of accounting for a wide range of GDW phenomena quantitative

quantum

detail with a theory based on only a few measurable

While we will not go into the details of the derivation, results and how they compare with recent experiment.

in

parameters.

we will describe

It is believed

the

that

remaining problems will be resolved within the quantum approach. It was not until the remarkable

field- and frequency-dependent

was observed below Tp in NbSe 3 by Monceau, conduction was discovered. approximately

They found that the dc current could be expressed

in the form i = OaE + ObE exp[-Eo/E],

where E is the electric

field and the second term is the CDW contribution.

The exponential

suggested Zener tunneling through a small pinning gap. account for CDW depinnlng

conductivity

Ong and Portis that true Fr&~llch

form

Early attempts

to

on this basis, or by creation of solltons in an

electric field, were abandoned when it was found the required energy gap is ~ IO-4kBT. In 1979 it was pointed out that such theories are viable if the CDW is a macroscopic

quantum system with one thermal degree of freedom in a volume

containing perhaps

106 parallel

atomic chains of atoms.

Tunneling

electrons would then add coherently in this volume, as do electrons through an insulating

layer in the Josephson

relate the depinning field,

effect.

were made of o(~) in the megahertz

that if tunneling is involved, tunneling

tunneling

An attempt was made to

Eo, with the pinning frequency.

The expression

given for E o is close to that in the present version of the theory. after measurements

of individual

In 1980,

region, it was suggested

it should be possible to apply photon-asslsted

(PAT) theory to derive the ac response from the de.

One consequence

is that o(~) should scale with idc/E , so that the CDW response is o(~) = abexp(-~s/m),

where u s is the scaling frequency.

A program was initiated in 1981 to study detection, and harmonic generation

to test predictions

found to be in good quantitative

mixing,

of the PAT theory.

or semi-quantltative

harmonic mixing Results were

agreement when biased

above threshold or if the frequency to be detected

is above a critical value.

In some cases results were qualitatively

from those expected from

classical models.

A phenomenological

range of phenomena when the frequency

different

theory was developed

to account for a

is lower than the critical value, called

the ac-dc decoupling

frequency.

In this region the expected

compensated

at least in part by polarization

THEORETICAL

BACKGROUND

When a CDW moves with a drift velocity, to -kF+q, kF+q, where Nq = my d. the current

response

is

fields.

Vd, the ID Fermi surface, ~kF, moves

The Peierls gaps move with the Fermi sea and

flow is the same as if the gaps were not present.

The total kinetic

energy is (I/2)(m + MF)V~, where M F >> m is that associated with the moving ions that accompany

the wave.

Changes in electron density ~nd in v d can be described by a phase ~(x,t) such that the electron density

is

(2)

P = Po + 01 c°s[2kFX + ~(x,t)]

For uniform flow, ~ = -~d t, where ~d = 2kFVd is the frequency of the macroscopically difference

occupied phonon that accompanies

the wave.

between opposite sides of the FS is ~ d "

density are proportional

~o(X),

More generally,

changes in

to ~#/Sx and drift velocity to - ~ / ~ t .

In the Fukuyama-Lee-Rice deformations,

The energy

theory of weak impurity pinning,

change the phase to minimize

fluctuations.

The phase is adjusted

deformations

with an average wavelength

static

the energy from impurity

in regions of average length, Ld, by lp = 2L d = 2~Co/~p, where

c o = m/~7~F v F is the phason velocity and ~p/2~ the pinning frequency.

More than

half the pinning energy can be maintained with current flow if the phase oscillates

between two space variations

in the sign of the space variations.

~A(X) and ~B(X) = ~ - ~A(X) that differ

In an idealized model,

#A =

-(~/2)cos(~X/Ld) , giving the minimum energy when the space-average 8 = <#> = 0 (mod 2~). (mod 2w).

When a current

flows and 8 changes in time, the system oscillates

between 8 A and 8 B for each change w in 8. maintained

phase

The state 8 B gives the minimum energy when =

In the model (Fig.

i) the phase is

at -~/2 for x = n2L d as 8 goes from 0 to -w and at -(3w/2)

x = (2n + I)L d as e goes from -~ to -2~.

at

The variation of the pinning energy

with phase would then be V(8) = -V o - Vlcos8 j (see Fig. lb). The phase variations Eg = (2/~)4MF/m ~ p

8 A and 8 B give rise to a pinning gap

at the Fermi surface.

The reason for the gap is that the

charge added in going from 8 A to 8 B must be localized within 2L d. is that required to add 2k F to the wave-vector acceleration antlsoliton

step.

In the idealized model,

of the electrons

The energy E g

in an

this is the energy of a ~-soliton-

pair, where a ~-soliton corresponds

to half a state, or, when doubly

occupied,

to a charge e per chain.

The Zener expression

for the probability

tunneling

through the pinning gap is P(E) = exp(-Eo/E) , where

of

A

2~'-

/i-'--'--,,~ B

",., t

-@(x)

~. .

.

.

.

_L--

-_!

_~_- -

o

(a)

X/Ld----,-

t v(8) 0

7r/2

3~r/2

5rr/2

777/2

__.

(b) Figure 1.

w -w. (a) Phase variations for e = 0, - ~,

(b) Pinning energy as

function of B ffi <@(x,t)>.

wE 2 M~u2 E ° =----g--= P 4~vFe wmvFe

(2)

The equation for the acceleration is dq ~-=

dVd m dt

m eEF(E) mF

(3)

where m/M F is the probability that the added momentum goes to the electrons rather than the macroscopic phonons.

When integrated over a relaxation time 3*,

m

~u d ffi 2~kFV d = 2VF~ q ~ F

(4)

eE2VFT*P(E)

where VFT* ~ Co/U p and o b = ne2~*/M.

The scaling frequency is the drift

frequency for free acceleration in a field Eo, or [~u

m

s ffi ~

(5)

eEo2VF T*

These expressions for Eo and u s are in good agreement with experiment for "pure" NbSe 3 and TaS3, but require modification when the pinning frequency is very high, as in the alloy Tal_xNbxS 3 and (TaSe4)21.

For the latter, it is

necessary to take into account the relaxation time between electrons and macroscoplcally occupied phonons.

If T = Tel_p h + T* is the total relaxation

time for momentum added to the electrons,

the revised expressions

for E o and u s

are

E' = o

m' = T4~W/~ m S s

(T/T*)Eo

EXPERIMENTAL

RESULTS

Careful experiments excellent

(6)

agreement[4]

on well-prepared

specimens

with the predictions

Zener form and the magnitudes

of E o and m s.

form holds for fields as large as I00 E T. agreement

of NbSe 3 and TaS 3 are in

of the tunneling theory for both the In NbSe 3 below TI, the exponential The revised expressions

for the alloy and the iodide as long as temperatures

thermally activated

region.

The expressions

are in good

are above the

are expected to be valid up to

fields as high as m d ~ ~MF/m m , or to l/T, the upper frequency cut-off on the P CDW response. The expression

(4) for the ~m d is similar to that for the overdamped

oscillator model, but with a field dependent

relaxation time, T*P(E).

E is the total field, E = Eappl + Epo I (O) where Epo I is proportional -~V(O)/~0.

The potential

to

V(O) has a rich harmonic content that differs markedly

from that of the sinusoidal

variation of the sine-Gordon model generally

in the overdamped oscillator model. oscillating

The field

At high fields,

taken

Eappl >> E o, the

current density from Epol, with O = mdt , is

ipo I = ObEpol(mdt)

(7)

A Fourier expansion of -~V(8)/~e decreases

indicates

that the amplitude of the harmonics

as I/n, consistent with experiment.

Because of rounding at the breaks

between 8 A and 8B, there is some decrease in harmonic content at high fields. Further confirmation

of the form for V(8) comes from the subharmonic

constant current observed when the dc I-V characteristic presence of an applied ac current. rational fractions

Measurements

p/q occur for integers

at UCLA have shown that all

less than about 12.

steps can be estimated by a simple argument.

The width of the

If it is assumed that the only

currents present are the applied dc and ac currents,

8 = -mdt

steps of

is measured in the

the phase is

mI m cosmt + 8 °

(s)

where e o is an adjustable current flow.

phase that may depend on the magnitude

With this expression

have dc components

corresponding

rational fraction p/q.

of the dc

for 8, the Fourier expansion of Epol(t) will

to a drift frequency m d = (p/q)m for every

Thus the total dc field E = Eappl + Epol(8o)dc

can

remain constant at the value required for the p/q step for a range of values of

Eappl extending from E - Em to E + Em, where Em is the maximum value of Epol(eb)dc as eo is varied.

This method has been used[5] to calculate the step

width for the rational fractions p/q.

The relative step widths are in good

agreement with experiment, although the magnitudes are smaller than predicted. Experiments on field dependence of current, harmonic content of narrow band noise and the subharmonlc steps all indicate that pinning energy is maintained to very high fields.

This is strong evidence for the quantum tunneling model of

deplnnlng, but is contrary to the basic assumption of the classical model of Sneddon, Cross and Fisher[3]. The latter assume that at high fields the CDW is essentially free and treat interaction with impurities by perturbation theory. At low temperatures, particularly in TaS3, (TaSe4)21 and K0.3MoO 3, the response is thermally activated.

While threshold fields are not far from

predicted values, the magnitudes of the currents are much smaller than predicted and scaling of the PAT theory no longer applies.

It is believed[13] that what is

involved is time to screen the COW fluctuations in the eA ÷ e B deplnnlng process by the normal conductivity from electrons and holes thermally excited across the Pelerls gap.

The theory as given above omits Coulomb forces from density

fluctuations and is valid only at high temperatures when the screening is complete. ACKNOWLEDGEMENTS The authors express gratitude for the close interaction with George Gr~ner and his students, S. E. Brown, M. Makl, G. Mozurkewlch, D. Reagor and S. Srldhar, that has been essential for the work described here to be carried out.

RET wishes to acknowledge support provided by an NSERC (Canada)

Postgraduate Scholarship and JHM for an IBM Fellowship. Funds were provided by the U.S. Joint Services Electronics Program under contract No. N00014-84-C-0149.

REFERENCES 1

R. C. Lacoe, H. J. Schulz, D. J~r~me, K. Bechgaard and L. Johannsen./ PhTs. Rev. Lett., 55

2

(1985) 2351.

R. E. Thorne, J. H. Miller, Jr., W. G. Lyons, J. W. Lydlng and J. R. Tucker, Phys. Rev. Lett., 5 5

(1985) 1006; J. Bardeen, Phys. Rev. Lett., 55 (1985) 1010

and references therein. 3

L. Sneddon, M. C. Cross and D. S. Fisher, Phys. Rev. Lett., 49 (1982) 292. D. S. Fisher, Phys. Rev. B,31 (1985) 1396.

4

R. E. Thorne, W. E. Lyons, J. H. Miller, Jr., J. W. Lydlng and J. R. Tucker, to be published.

5

R. E. Thorne, J. R. Tucker, J. Bardeen, S. E. Brown and G. Gr~ner, PhTs. Rev. B, 33 (May 15) (1986).

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J.R. Tucker, Proc. Yamada Conference, to be published in Physica B, December 1986