skip to main content


Title: Local lattice distortions and dynamics in extremely overdoped superconducting YSr 2 Cu 2.75 Mo 0.25 O 7.54

A common characteristic of many “overdoped” cuprates prepared with high-pressure oxygen isTcvalues ≥ 50 K that often exceed that of optimally doped parent compounds, despite O stoichiometries that place the materials at the edge or outside of the conventional boundary between superconducting and normal Fermi liquid states. X-ray absorption fine-structure (XAFS) measurements at 52 K on samples of high-pressure oxygen (HPO) YSr2Cu2.75Mo0.25O7.54,Tc= 84 K show that the Mo is in the (VI) valence in an unusually undistorted octahedral geometry with predominantly Mo neighbors that is consistent with its assigned substitution for Cu in the chain sites of the structure. Perturbations of the Cu environments are minimal, although the Cu X-ray absorption near-edge structure (XANES) differs from that in other cuprates. The primary deviation from the crystal structure is therefore nanophase separation into Mo- and Cu-enriched domains. There are, however, indications that the dynamical attributes of the structure are altered relative to YBa2Cu3O7, including a shift of the Cu-apical O two-site distribution from the chain to the plane Cu sites. Another effect that would influenceTcis the possibility of multiple bands at the Fermi surface caused by the presence of the second phase and the lowering of the Fermi level.

 
more » « less
Award ID(s):
1928874
NSF-PAR ID:
10135230
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Proceedings of the National Academy of Sciences
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
117
Issue:
9
ISSN:
0027-8424
Page Range / eLocation ID:
p. 4559-4564
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. null (Ed.)
    A crucial issue in cuprates is the extent and mechanism of the coupling of the lattice to the electrons and the superconductivity. Here we report Cu K edge extended X-ray absorption fine structure measurements elucidating the internal quantum tunneling polaron (iqtp) component of the dynamical structure in two heavily overdoped superconducting cuprate compounds, tetragonal YSr 2 Cu 2.75 Mo 0.25 O 7.54 with superconducting critical temperature, T c = 84 K and hole density p = 0.3 to 0.5 per planar Cu, and the tetragonal phase of Sr 2 CuO 3.3 with T c = 95 K and p = 0.6. In YSr 2 Cu 2.75 Mo 0.25 O 7.54 changes in the Cu-apical O two-site distribution reflect a sequential renormalization of the double-well potential of this site beginning at T c , with the energy difference between the two minima increasing by ∼6 meV between T c and 52 K. Sr 2 CuO 3.3 undergoes a radically larger transformation at T c , >1-Å displacements of the apical O atoms. The principal feature of the dynamical structure underlying these transformations is the strongly anharmonic oscillation of the apical O atoms in a double-well potential that results in the observation of two distinct O sites whose Cu–O distances indicate different bonding modes and valence-charge distributions. The coupling of the superconductivity to the iqtp that originates in this nonadiabatic coupling between the electrons and lattice demonstrates an important role for the dynamical structure whereby pairing occurs even in a system where displacements of the atoms that are part of the transition are sufficiently large to alter the Fermi surface. The synchronization and dynamic coherence of the iqtps resulting from the strong interactions within a crystal would be expected to influence this process. 
    more » « less
  2. The local structure of the highly “overdoped” 95 K superconductor Sr2CuO3.3determined by Cu K X-ray absorption fine structure (XAFS) at 62 K in magnetically oriented samples shows that 1) the magnetization is perpendicular to thecaxis; 2) at these levels of precision the Cu sublattice is tetragonal in agreement with the crystal structure; the O sublattice has 3) continuous -Cu-O- chains that orient perpendicular to an applied magnetic field; 4) approximately half-filled -Cu-O- chains that orient parallel to this field; 5) a substantial number of apical O vacancies; 6) O ions at some apical positions with expanded Cu-O distances; and 7) interstitial positions that imply highly displaced Sr ions. These results contradict the universally accepted features of cuprates that require intact CuO2planes, magnetization along thecaxis, and a termination of the superconductivity when the excess charge on the CuO2Cu ions exceeds 0.27. These radical differences in charge and structure demonstrate that this compound constitutes a separate class of Cu-O–based superconductors in which the superconductivity originates in a different, more complicated structural unit than CuO2planes while retaining exceptionally high transition temperatures.

     
    more » « less
  3. Abstract

    Control of surface functionalization of MXenes holds great potential, and in particular, may lead to tuning of magnetic and electronic order in the recently reported magnetic Cr2TiC2Tx. Here, vacuum annealing experiments of Cr2TiC2Txare reported with in situ electron energy loss spectroscopy and novel in situ Cr K‐edge extended energy loss fine structure analysis, which directly tracks the evolution of the MXene surface coordination environment. These in situ probes are accompanied by benchmarking synchrotron X‐ray absorption fine structure measurements and density functional theory calculations. With the etching method used here, the MXene has an initial termination chemistry of Cr2TiC2O1.3F0.8. Annealing to 600 °C results in the complete loss of F, but O termination is thermally stable up to (at least) 700 °C. These findings demonstrate thermal control of F termination in Cr2TiC2Txand offer a first step toward termination engineering this MXene for magnetic applications. Moreover, this work demonstrates high energy electron spectroscopy as a powerful approach for surface characterization in 2D materials.

     
    more » « less
  4. In the physics of condensed matter, quantum critical phenomena and unconventional superconductivity are two major themes. In electron-doped cuprates, the low critical field (HC2) allows one to study the putative quantum critical point (QCP) at low temperature and to understand its connection to the long-standing problem of the origin of the high-TCsuperconductivity. Here we present measurements of the low-temperature normal-state thermopower (S) of the electron-doped cuprate superconductor La2−xCexCuO4(LCCO) fromx= 0.11–0.19. We observe quantum criticalS/Tversusln(1/T)behavior over an unexpectedly wide doping rangex= 0.15–0.17 above the QCP (x= 0.14), with a slope that scales monotonically with the superconducting transition temperature (TCwith H = 0). The presence of quantum criticality over a wide doping range provides a window on the criticality. The thermopower behavior also suggests that the critical fluctuations are linked withTC. Above the superconductivity dome, atx= 0.19, a conventional Fermi-liquidSTbehavior is found forT40 K.

     
    more » « less
  5. Abstract

    The mechanism of unconventional superconductivity in correlated materials remains a great challenge in condensed matter physics. The recent discovery of superconductivity in infinite-layer nickelates, as an analog to high-Tccuprates, has opened a new route to tackle this challenge. By growing 8 nm Pr0.8Sr0.2NiO2films on the (LaAlO3)0.3(Sr2AlTaO6)0.7substrate, we successfully raise the superconducting onset transition temperatureTcin the widely studied SrTiO3-substrated nickelates from 9 K into 15 K, which indicates compressive strain is an efficient protocol to further enhance superconductivity in infinite-layer nickelates. Additionally, the x-ray absorption spectroscopy, combined with the first-principles and many-body simulations, suggest a crucial role of the hybridization between Ni and O orbitals in the unconventional pairing. These results also suggest the increase ofTcbe driven by the change of charge-transfer nature that would narrow the origin of general unconventional superconductivity in correlated materials to the covalence of transition metals and ligands.

     
    more » « less