Study of the Cu-spin correlation is indispensable in elucidating the mechanism of superconductivity in high-Tc cuprates. In the hole-doped cuprates, neutron-scattering [1] and muon-spin-relaxation (μSR) [2] measurements revealed that the antiferromagnetic (AF) spin correlation weakened with overdoping of holes and disappeared in the non-superconducting (SC) heavily overdoped regime, suggesting the intimate relation between the AF spin correlation and superconductivity. In the electron-doped cuprate Pr1-xLaCexCuO4, on the other hand, neutron-scattering experiments suggested the robust AF correlation in non-SC heavily overdoped regime [3], whereas μSR measurements suggested the disappearance of the development of Cu-spin correlation together with superconductivity in the heavily overdoped regime [4]. However, details remain unclear because of predominant effects of the Pr3+ moment on the μSR spectra.
In this study, to clarify the relationship between the Cu-spin correlation and superconductivity in the electron-doped cuprates, we performed transport and μSR measurements of La2-xCexCuO4 (LCCO) without rare-earth moments.
Overdoped LCCO (x = 0.13, 0.17) target samples were prepared by solid-state reaction [5]. Thin films were fabricated on the SrTiO3 substrate by the pulsed-laser deposition method using a third harmonic of Nd:YAG laser (wavelength : 355 nm) as a light source, which is different from the previous report [6]. By varying the oxygen partial pressure and reduction annealing conditions, LCCO thin films with x = 0.13 and 0.17 having Tc = 20 K and 3 K were fabricated, respectively. μSR measurements using low-energy muons were performed at the MuE4 beamline at the Paul Scherrer Institut in Switzerland.
Figures show zero-field μSR spectra of optimally reduced LCCO with x = 0.13 and 0.17. Fast relaxation of muon spins is observed at low temperatures in both samples, indicating the development of the Cu-spin correlation. As the temperature dependence of the spectra is almost identical between x = 0.13 and 0.17, this suggests that the development of the Cu-spin correlation is less doping-dependent, which is different from the results of Pr1-xLaCexCuO4 [4]. The development of the Cu-spin correlation at x = 0.17, where superconductivity is almost suppressed, may be related to a recently proposed ferromagnetic order [7].
[1] S. Wakimoto et al., Phys. Rev. Lett. 72, 064521 (2005).
[2] Risdiana et al., Phys. Rev. B 77, 054516 (2008).
[3] M. Fujita et al., Phys. Rev. Lett. 101, 107003 (2008).
[4] M. A. Baqiya et al., Phys. Rev. B 100, 064514 (2019).
[5] T. Yamada et al., Jpn. J. Appl. Phys. 33, L168 (1994).
[6] A. Sawa et al., Phys. Rev. B 66, 014531 (2002).
[7] T. Sarkar et al., Science 368, 532 (2020).
Helpful advises on the preparation of LCCO thin films by A. Maeda, F. Nabeshima, I. Tsukada are gratefully acknowledged. A part of the resistivity and Hall measurements were performed by using the commercial apparatus (PPMS) at the CROSS-user laboratory.
Figure 1. Zero-field μSR spectra of La2-xCexCuO4 with (a) x = 0.13 and (b) x = 0.17.
Keywords: High-Tc superconducting cuprate, Thin film, Spin correlation, Muon spin relaxation