# Temporally ordered collective creep and dynamic transition in the charge-density-wave conductor NbSe3

## Abstract

We have observed an unusual form of creep at low temperatures in the charge-density-wave (CDW) conductor NbSe<sub>3</sub>. This creep develops when CDW motion becomes limited by thermally-activated phase advance past individual impurities, demonstrating the importance of local pinning and related short-length-scale dynamics. Unlike in vortex lattices, elastic collective dynamics on longer length scales results in temporally ordered motion and a finite threshold field. A first-order dynamic phase transition from creep to high-velocity sliding produces “switching” in the velocity-field characteristic.

Interaction between internal degrees of freedom and disorder determines the dynamical properties of driven periodic media, a class of systems that includes vortex lattices in type II superconductors , Wigner crystals , magnetic bubble arrays , and charge-density waves (CDWs), the low-temperature phase of quasi-one-dimensional conductors . While the interplay between quenched disorder and elastic deformations is relatively well understood, a complete description of the role of thermal disorder and plastic deformations, which may result in disordered dynamical phases such as driven glass, smectic and liquid states , has not yet been achieved.

CDWs have long been regarded as a prototypical system for the study of many-degree-of-freedom dynamics, both because of their relative theoretical simplicity and because CDW materials like NbSe<sub>3</sub> exhibit collective phenomena with remarkable clarity. A CDW consists of coupled modulations of the electronic density $`n=n_0+n_1\mathrm{cos}[Q_cx+\varphi (x)]`$ and of the positions of the lattice ions . Applied electric fields $`E`$ greater than a threshold field $`E_T`$ cause the CDW to depin from impurities and slide relative to the host lattice, resulting in a non-linear dc current density $`j_c`$ proportional to the CDW’s sliding velocity. The impurities cause the CDW to move nonuniformly in both space and time, and the elastic collective dynamics leads to oscillations (“narrow-band noise”) in $`j_c(t)`$. The frequency $`\nu `$ of these oscillations is proportional to the dc component of $`j_c`$, and their $`Q=\nu /\mathrm{\Delta }\nu `$ can exceed 30,000 in high-quality NbSe<sub>3</sub> crystals.

Despite these simplifying features, most aspects of CDW transport at low temperatures remain poorly understood. At temperatures $`T>2T_P`$/3, $`j_c`$ above $`E_T`$ is a smooth, asymptotically linear function of $`E`$. However, at low temperatures $`j_c(E)`$ changes drastically, as illustrated in Fig. 1. CDW conduction still begins at $`E_T`$ but $`j_c`$ is small and freezes out with decreasing temperature for fields less than a second characteristic field $`E_T^{}>E_T`$. At $`E_T^{}`$ $`j_c`$ increases by several orders of magnitude to a more nearly temperature-independent value, often by an abrupt, hysteretic ”switch.” Similar behavior is observed in all widely studied CDW materials and is thus a fundamental aspect of CDW dynamics .

We have characterized the sliding CDW’s transport and structural properties in the low-temperature regime of extremely high quality NbSe<sub>3</sub> crystals. For $`E_T<E<E_T^{}`$, we find that $`j_c`$ is activated in temperature and increases exponentially with field. Contrary to previous observations in driven periodic media, this creep-like collective motion exhibits temporal order. Our results illuminate the relation between local and collective pinning and indicate that dynamics on lengths much shorter than the Fukuyama-Lee-Rice (FLR) length — neglected in most theoretical treatments — play a central role. They imply revised interpretations for “switching” at $`E_T^{}`$, the low-frequency dielectric response, low-field relaxation, and nearly every other aspect of the CDW response at low temperatures.

High purity ($`r_R400`$) whisker-like NbSe<sub>3</sub> single crystals with typical cross-sectional dimensions of $``$3 by $``$0.8 $`\mu `$m were mounted on arrays of 2 $`\mu `$m wide gold-topped chromium wires . The total current density $`j_{tot}`$ is a sum of the CDW and single-particle current densities, $`j_c`$ and $`j_s`$. $`j_c`$ is orders of magnitude smaller than $`j_s`$ in the range $`E_T<E<E_T^{}`$ (except at relatively high temperatures and very close to $`E_T^{}`$ ). $`j_c(E)`$ cannot be directly measured and its form in the low-velocity branch of NbSe<sub>3</sub> has not previously been determined. As shown in the inset to Figure 2, our high-quality crystals  exhibit voltage oscillations with Q’s as large as 130 in this regime. Consequently, we are able to determine $`j_c`$ by measuring the oscillation frequency $`\nu =(Q_c/2\pi en_c)j_c`$, where $`e`$ is the electronic charge and $`n_c`$ is the condensed carrier density. $`j_c(E)`$ was independently estimated by alternating the applied current’s direction and measuring resistance transients $`R(t)`$ associated with transients in the distribution of CDW strain $`ϵ(x)=(1/Q_c)(\varphi /x)`$ between the current contacts .

Figure 2 shows the CDW current density $`j_c(E)=\nu \times 0.32`$ pA/$`\mu `$m<sup>2</sup>Hz  calculated from the measured oscillation frequency $`\nu (E)`$ for $`E_T<E<E_T^{}`$ at four temperatures. The CDW moves extremely slowly throughout this field and temperature range: the smallest measured $`\nu `$ values at $`T`$=20.7 K correspond to CDW motion of roughly one wavelength or 14 Å per second and to $`j_c10^9j_{tot}`$. Between T$``$40 K and T$``$20 K, $`j_c`$ at fixed $`E<E_T^{}`$ is temperature activated, decreasing by roughly 7 orders of magnitude. $`j_c`$ jumps abruptly at $`E_T^{}`$, with $`j_c(E=1.1E_T^{})/j_c(E=0.9E_T^{})`$ increasing from $``$ 10<sup>3</sup> to $``$ 10<sup>6</sup> as $`T`$ decreases from 28 to 20 K.

The current density $`j_c\nu `$ can be fit by a modified form for thermal creep 

$$j_c(E,T)=\sigma _0[EE_T]\mathrm{exp}\left[\frac{T_0}{T}\right]\mathrm{exp}\left[\alpha \frac{E}{T}\right].$$
(1)   
where the $`[EE_T]`$ term describes the fact that the current drops to zero at a threshold $`E_T`$ that remains large even at high temperatures. The solid lines in Fig. 2 indicate a fit with $`T_0=505`$ K, $`\alpha =136`$ K V<sup>-1</sup> cm, and $`\sigma _0=350`$ $`\mathrm{\Omega }^1\mu `$m<sup>-1</sup>. The value of $`T_0`$ is insensitive to the assumed field dependence and corresponds to 0.6 times the single-particle gap $`2\mathrm{\Delta }`$ , consistent with measurements of delayed conduction  and of $`\sigma _c`$ near $`E_T^{}`$ above 30 K . Although creep is observed in other systems, the coherent oscillations imply that the creep in this case is highly unusual: it exhibits temporal order.

Figure 3 shows $`j_c(E)`$ at $`T`$=20.5 K obtained from transient measurements . These data agree closely with $`j_c(E)`$ deduced from $`\nu (E)`$ over nearly three decades in $`j_c`$ . Combining the two measurements yields $`j_c/\nu =0.22`$ pA/$`\mu `$m<sup>2</sup>Hz, consistent with the expected value of $`j_c/\nu =0.32`$ pA/$`\mu `$m<sup>2</sup>Hz  within the factor-of-two uncertainty in the value of $`j_c`$ determined from transient measurements. This rules out significant filamentary conduction, observed in the low temperature regime of other CDW materials, and implies that the entire crystal cross section or at least a significant fraction of it is involved in coherent conduction.

Figure 4 shows the results of high-resolution x-ray diffraction measurements of the CDW’s transverse structure versus electric field. The CDW creates superlattice peaks in the diffraction pattern, and the half-width of each peak is inversely related to the CDW phase-phase correlation length. For $`E<E_T`$, the resolution-corrected inverse half-width is $`l4100`$ Å, comparable to the crystal dimension in this direction. For $`E>E_T`$, $`l`$ decreases monotonically with increasing $`E`$, remaining greater than $`2500`$ Å for $`E_T<E<E_T^{}`$. $`l`$ does not show any abrupt change at $`E_T^{}`$ despite the several orders-of-magnitude increase in $`j_c`$ there. Similar results were obtained in other directions perpendicular to $`𝐐_𝐜`$ (e.g. \[1 0 3\] and \[1 0 2̄\]) and at higher temperatures.

Several different models have been proposed to account for the low-temperature properties of CDW conductors. In K<sub>0.3</sub>MoO<sub>3</sub> and TaS<sub>3</sub>, whose Fermi surfaces are completely gapped by CDW formation, the activation energies for the single-particle conductivity $`\sigma _s`$ and the CDW conductivity $`\sigma _c`$ in the low-velocity branch are both comparable to the CDW gap so that $`\sigma _c(T)\sigma _s(T)`$ . Motivated by this observation, Littlewood  suggested that dissipation caused by single-particle screening of CDW deformations limits CDW motion in the low-velocity branch, and that an abrupt, hysteretic transition to the high-velocity branch occurs at a frequency $`\nu `$ comparable to the dielectric relaxation frequency $`\nu _1\sigma _s`$ when this screening becomes ineffective. The predicted value of $`\nu `$ at the discontinuity for K<sub>0.3</sub>MoO<sub>3</sub> and TaS<sub>3</sub> is four orders of magnitude too large , and for NbSe<sub>3</sub> at $`T`$=20.7 K $`\nu `$ is 13 orders of magnitude too large. Levy et al.  showed that a related model exhibits a hysteretic transition from the pinned state to a fast sliding state when $`\sigma _s`$ is small even if high-frequency screening effects are neglected. Neither model can explain the low-temperature CDW properties of partially-gapped NbSe<sub>3</sub>, for which $`\sigma _s`$ remains metallic and increases with decreasing temperature below 50 K.

Various forms of CDW plasticity including phase slip at isolated defects  and shear between two-dimensional CDW sheets  have been suggested to account for the properties of the low-velocity branch and the transition at $`E_T^{}`$. Our observation of highly coherent oscillations in high-quality crystals and earlier results rule out models based on slip at rare isolated defects and contacts, and our x-ray measurements rule out the form of shear plasticity discussed in Ref. .

Brazovskii and Larkin have focused on the CDW’s local interaction with defects. At low temperatures CDW phase advance past rare defects occurs via thermally-activated soliton generation, and motion becomes much more rapid at large fields when the effective barrier to soliton generation vanishes. This interpretation has appealing features, but the suggested form for the $`j_c(E)`$ relation at low temperatures does not reproduce the two branches separated by an abrupt hysteretic transition or the field dependence in either branch observed experimentally in NbSe<sub>3</sub>. Furthermore, the predicted $`E_T^{}`$ is determined by the soliton energy and should be independent of crystal size. Experimentally, in NbSe<sub>3</sub> both $`E_T`$ and $`E_T^{}`$ vary as $`1/t`$ for crystal thicknesses $`t`$ less than $``$ 20 $`\mu `$m . The thickness dependence of $`E_T`$ results because transverse CDW correlations are limited by $`t`$ so that collective pinning is two-dimensional . Consequently, the thickness dependence of $`E_T^{}`$ implies that it, too, is determined by collective effects.

CDW creep of a fundamentally different character is observed in thin NbSe<sub>3</sub> crystals at high temperatures . Near T<sub>P</sub>, $`E_T`$ is rounded, nonlinear conduction can extend to near E=0, and highly coherent oscillations below the nominal $`E_T`$ are not observed. This incoherent creep occurs when $`k_BT`$ approaches the collective pinning energy ($`\mathrm{\Delta }(T)^2t`$) of the phase-correlated FLR domains, which in NbSe<sub>3</sub> have micrometer dimensions. The temporally-ordered creep observed in relatively thick crystals at low temperatures above a sharp threshold $`E_T`$ must involve barriers that are much smaller than those of collective pinning and that are not rare, and a length scale that is much smaller than that of the collective dynamics responsible for the narrow-band noise.

Motivated by earlier ideas , we suggest that the low-velocity branch develops when CDW motion becomes limited by thermally-activated phase advance by $``$ 2$`\pi `$ past individual impurities. Although collective pinning is weak , the phase of the $`Q_c=2k_F`$ oscillations is fixed at each impurity so that phase advance requires CDW amplitude collapse and a finite barrier $`\mathrm{\Delta }`$ . Collective dynamics within volumes containing enormous numbers of impurities (set by the FLR length) then generates the finite threshold $`E_T`$ and coherent oscillations, as in the high-temperature regime. Unlike in vortex lattices, long-length-scale CDW dynamics is largely elastic and thus retains temporal order even though the short-length-scale dynamics is stochastic.

The $`EE_T`$ prefactor  and the remaining terms in Eq. 1 follow naturally from this combination of long and short length-scale processes. The measured barrier $`T_0`$ is consistent with the expected pinning barrier per impurity of $``$ $`\mathrm{\Delta }`$ . An applied electric field should reduce this barrier by $``$ $`en_cV\lambda E`$, and using a condensate density $`n_c=2\times 10^{21}`$ cm<sup>-3</sup> , a CDW wavelength $`\lambda =14\AA `$ and the measured $`\alpha `$ value yields a volume $`V`$ involved in each thermally-activated event of $`V4.2\times 10^{17}`$ cm<sup>3</sup>. Using the scale factor expected for typical impurities , the bulk residual resistance ratio of $``$ 400 for our crystals corresponds to a concentration $`n_i2.5\times 10^{16}`$ cm<sup>-3</sup>. The volume per impurity $`1/n_i4\times 10^{17}`$ cm<sup>3</sup> is thus in excellent agreement with $`V`$ deduced from creep measurements.

The present experiments together with those of Ref.  rule out all previous explanations of the “switching” between low and high velocity branches at $`E_T^{}`$ in NbSe<sub>3</sub>. We suggest that switching occurs via a first-order dynamic phase transition. The long-length-scale dynamics exhibits temporal order in both branches, but in the high-velocity branch dynamic fluctuations produced as the CDW moves past impurities may become more important than thermal fluctuations in overcoming impurity barriers . The transition’s abruptness, hysteresis, and temperature dependence shown in Fig. 1, the CDW’s tendency to fragment near the transition into distinct conducting regions , and the field and temperature-dependent time delays required for the transition’s completion  are all consistent with this explanation.

Finally, we note that local temporal order has very recently been observed in the creep regime of a vortex lattice .

We thank C.L. Henley, M. B. Weissman, M. C. Marchetti, A. A. Middleton, and S. Brazovskii for fruitful discussions. This work was supported by NSF Grants DMR97-05433 and DMR-98-01792. S.G.L. acknowledges additional support from NSERC. The x-ray data were collected using beam line X20A at the National Synchrotron Light Source (NSLS). Sample holders were prepared at the Cornell Nanofabrication Facility.