# MAGNETIC AND CHARGE FLUCTUATIONS IN HIGH-𝑇_𝑐 SUPERCONDUCTORS

## I INTRODUCTION

Neutron scattering measurements continue to provide information of direct relevance to some of the most important issues in the high-$`T_c`$ cuprate superconductors. The magnetic excitations of these materials are the spin fluctuations, and recent measurements have shown that the low-energy spin fluctuations in YBa<sub>2</sub>Cu<sub>3</sub>O<sub>6.6</sub> (YBCO<sub>6.6</sub>) are incommensurate in nature while a commensurate excitation that is relatively sharp in energy called a resonance is found at about 35 meV . The incommensurability was originally discovered by the filter integration technique  that integrates over the outgoing neutron energy in a direction along $`c^{}`$ and thus provides a high data collection rate for the study of lower dimensional excitations. The disadvantage of the technique is that no discrete energy information is available. Thus when a discovery is made by the integration technique further measurements are made by triple-axis or time-of-flight techniques to determine the energy spectrum. Figure 1a shows the direction of the integrating scan that is made through the point $`(\pi ,\pi )`$ to observe the incommensurate fluctuations shown by the dots at the position $`\delta /2`$ from the commensurate position. Such a scan employs high resolution along the scan direction, but coarse resolution perpendicular to the scan direction and thus cannot determine the exact wave vector position of the incommensurate peaks. The result of the scan for YBCO<sub>6.6</sub> is shown in Fig. 1b. The $`(\pi ,\pi )`$ position is at (0.5, 0.5) in reciprocal lattice units (r.l.u.).

A recent measurement using a pulsed spallation source with time-of-flight energy determination has used a two-dimensional position-sensitive detector bank to determine the wave vector and energy of the YBCO<sub>6.6</sub> incommensurate peaks . The peaks are found to be along the $`(0,\pi )`$ and $`(\pi ,0)`$ directions as shown in Fig. 1a. The peaks are therefore not exactly on the scan direction shown in Fig. 1a, but are above and below it being observed in the integrated scan through the relaxed vertical resolution. The peaks in the scan in Fig. 1b are found at about 0.055 on either side of the commensurate point. The wave vector of the incommensurate scattering is then $`\sqrt{2}`$ times 0.055 from the geometry in Fig. 1 and this value must be multiplied by $`\sqrt{2}`$ again as the scan is in units of $`(h,h)`$ giving $`\delta /2=0.11`$ or $`\delta =0.22`$. The number determined from the time-of-flight measurement is $`0.21\pm 0.02`$ r.l.u.. This incommensurability is essentially identical to that observed in similarly doped  La<sub>1-x</sub>Sr<sub>x</sub>CuO<sub>4</sub> (214). It was found that the intensities and the correlation lengths are also very similar in the (214) single-layer and YBCO (123) bilayer materials, thus the low energy spin fluctuations appear to be universal for the high-Tc cuprate materials measured to date.

## II MAGNETIC FLUCTUATIONS IN BSSCO

Bi<sub>2</sub>Sr<sub>2</sub>CaCu<sub>2</sub>O<sub>8</sub> (BSSCO) or (2212) is a high temperature superconductor of considerable importance as one can cleave the material easily to obtain a good surface for photoemission measurements and other surface sensitive techniques. Unfortunately it is difficult to obtain the large single crystals needed for neutron scattering for the BSSCO composition. We were successful in growing rods of the material which have a $`[110]`$ reciprocal lattice direction along the rod direction (using the same definition of $`a`$ and $`b`$ as for YBCO). It was then possible to align a number of these rods together to form a sample of 35 grams for neutron studies. We have a crystal with one set of the  directions aligned and this permits some information to be obtained.

A difficulty with the sample for the study of magnetic excitations is that the material has bilayers similar to those in YBCO and thus we expect that the magnetic fluctuations are coupled in a similar way. In this case the low energy magnetic fluctuations have no structure factor unless a finite value of $`c^{}`$ is used and $`c^{}`$ is randomly orientated perpendicular to the aligned direction of the crystal. One must then set the spectrometer to sample a point off the  direction which means that only some of the $`c^{}`$ values desired fall within the resolution volume of the spectrometer, considerably reducing the magnetic signal.

One might expect that a resonance excitation might exist in BSSCO in a similar way as for YBCO and one can search for it in the same way  using a triple-axis spectrometer. Our sample of BSSCO has an oxygen composition near optimum doping and we expect that the resonance will not be observable much above $`T_c`$ in this case. The simplest experiment is thus to scan energy at the momentum value where the resonance is expected and take the difference between data taken well below $`T_c`$ and data taken above $`T_c`$. This works in YBCO, but fails in BSCCO for two related reasons. The first is that the signal is small relative to the phonons as we cannot achieve the full magnetic intensity that would be available at a fixed value for $`c^{}`$. The second problem is the phonons are much more temperature sensitive in BSSCO than they are in YBCO so that the difference in data at high and low temperatures strongly reflects the phonon differences. The only way to circumvent these difficulties is to use a polarized neutron beam to isolate the magnetic scattering. This unfortunately results in even less intensity as polarized beams are much weaker than unpolarized ones. Nevertheless, after considerable counting reasonable results were obtained. Momentum values near (0.5, 0.5) and (1.5, 1.5,) were both tried and similar patterns were obtained with the magnetic scattering near (1.5, 1.5) being considerably weaker because of the magnetic form factor. The results are shown in Fig. 2. A peak in energy about 10 meV wide, which is equal to the energy resolution of the experiment, is observed at 10 K while the result at 100 K appears rather featureless. The peak is only found in the spin flip channel guaranteeing that it is magnetic. The peak is observed at about 37 meV which is near the value expected if the $`T_c`$ of the BSSCO of 84K is scaled to that of YBCO for the same doping level. The results strongly suggest that BSSCO has a resonance excitation rather similar to that of YBCO. However, the results should be checked with single crystals when they become available.

The same BSSCO sample was employed to search for magnetic incommensurate fluctuations. The integration technique was used in the same way as for YBCO<sub>6.6</sub>. The experiment works in a similar manner except that the integration now takes place over the directions perpendicular to the  direction and thus is only partly along $`c^{}`$. For two-dimensional scattering from bilayers this results in an intensity loss in the magnetic signal. However, we see from Fig. 1 the magnetic signal in the integration technique is substantial so that an intensity loss may be tolerated. The results of the measurement are shown in Fig. 3. Fig. 3a shows data presented in the same way as for the YBCO<sub>6.6</sub> in Fig 1. The results suggest the possibility of small incommensurate peaks although the counting errors are larger than desired. The data shown are from a number of runs averaged together. Fig. b-d show one of the satellite peaks measured at different temperatures. In this case the background was obtained by a 30 deg. rotation of the sample relative to the position where the scan is performed. The magnetic signal is expected to be small in the 30 deg rotation case which samples reciprocal space well removed from (0.5, 0.5). The signal decreases with temperature as would be expected for a magnetic excitation. The peak is broad so the center is hard to determine accurately with the errors involved, however, the peak appears to be centered at about 0.42 r.l.u. or 0.08 r.l.u. units from the (0.5, 0.5) position. If the magnetic satellites are arranged as in Fig. 1, $`\delta `$ would be about 0.32. The value of $`\delta `$ for fully doped 214 materials is about 0.25 so the $`\delta `$ value for BSSCO appears to be somewhat larger than for the 214 materials assuming the same type of incommensurability. However, the BSCCO measurement has sizable counting errors and we do not know the actual pattern of the incommensurability. A measurement on a single crystal is needed for a more accurate determination. Until such an experiment is performed the present result suggests that BSSCO has low energy incommensurate fluctuations which may be similar to those found in 123 and 214 materials.

## III CHARGE FLUCTUATIONS IN YBCO

Neutrons cannot measure charge directly, but can observe a change in the mass density that is either static or dynamic. One can assume that static mass displacements reflect static charge ordering and such effects have been observed in the 214 cuprate materials in special cases . Dynamic charge ordering has not been observed so far and the present results serve as an indication that this occurs in the YBCO materials. We have made measurements on the same YBCO<sub>6.6</sub> sample in which the incommensurate magnetic fluctuations are observed. Again we start with the integration technique except we examine the region around the peaks of the reciprocal lattice stemming from the atoms rather than from the magnetism. Fig. 4 shows scans around the (1, 0) reciprocal lattice peak. Data are again shown that use a measurement at 300K as a background. As the sample is cooled distinct peaks form on both sides of the (1, 0) peak that we assume reflects a dynamic incommensurate mass fluctuation that can be considered to stem from an incommensurate charge fluctuation. However, we have not completely ruled out magnetic effects. We note the peaks are small, being an order of magnitude smaller than the magnetic satellite peaks shown in Fig. 1. The scan is along the (h, 0) reciprocal lattice or the $`(\pi ,0)`$ direction and thus is along the direction of the magnetic incommensurate scattering. The charge fluctuation peaks are about 0.22 in r.l.u. units from the commensurate position so that the $`\delta /2`$ value for them is 0.22 or twice the wave vector of the incommensurate magnetic satellites. However, the absolute direction of the incommensurate wave vector cannot be determined with the integration technique and the peaks could be at a wave vector off of the $`(\pi ,0)`$ direction. Fig. 4d shows an identical measurement for YBCO<sub>6.35</sub> which has a much lower oxygen content. No peaks are visible at 0.22 r.l.u. for this material.

Work has been underway with triple-axis spectrometry to determine the energy spectra of the charge fluctuations, but that work is still incomplete. It has been noted however, that certain phonon branches show anomalies at the wave vector of the charge fluctuations. The origin of the charge fluctuations is not clear. It would seem extremely likely that the magnetic and charge fluctuations stem from the same source. Obviously the observation of charge fluctuations strongly suggest a dynamic striped phase in YBCO<sub>6.6</sub>. However, other possibilities exist including Fermi surface effects or dynamic charge density waves. The next step is to determine the energy spectra and absolute wave vector of the incommensurate charge scattering.

## IV CONCLUSION

We have shown new neutron scattering results for the cuprate superconductors. Measurements on a BSCCO sample of crystals with a  direction aligned show strong evidence for a resonance excitation and indications of incommensurate magnetic fluctuations. It would be good to have these results confirmed by a high quality single crystal. For YBCO<sub>6.6</sub> clear dynamic incommensurate peaks are observed at low temperatues on either side of the (1, 0) reciprocal lattice peak. Since these are found at positions relative to the crystal reciprocal lattice they are assumed to stem from mass fluctuations driven by charge fluctuations. No such peaks are found for a YBCO<sub>6.35</sub> sample. The wave vector of the charge fluctuation peaks is twice that of the magnetic fluctuations if we assume the charge peaks are on the $`(0,\pi )`$ direction. It would seem likely the magnetic and charge excitations are related. The results give support to a dynamic striped phase model for the cuprate superconductors.

This research was supported by the US DOE under Contract No. DE-AC05-96OR22464 with Lockheed Martin Energy Research, Inc.