Title: Dipolar Spin Ice Regime Proximate to an All-In-All-Out Néel Ground State in the Dipolar-Octupolar Pyrochlore ${\mathrm{Ce}}_2{\mathrm{Sn}}_2{\mathrm{O}}_7$

Abstract

The dipolar-octupolar (DO) pyrochlores, R₂M₂O₇ (R ¼ Ce; Sm; Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce₂Sn₂O₇, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce₂Sn₂O₇ using the near-neighbor XYZ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce₂Sn₂O₇ samples, we place Ce₂Sn₂O₇’s ground state within the ordered dipolar all-in-all-out (AIAO) N´eel phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce₂Sn₂O₇ powders show a broad signal at low scattering wave vectors, reminiscent of a dipolar spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic octupoles and suggested an octupolarmore » quantum spin ice state. We conclude that new hydrothermally grown Ce₂Sn₂O₇ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO Néel order.« less

Authors:

Yahne, D. R.; Placke, B. ;

• Search DOE PAGES for author "Placke, B."
• Search DOE PAGES for ORCID "0000-0002-9975-7120"

Schäfer, R.; Benton, O. ;

• Search DOE PAGES for author "Benton, O."
• Search DOE PAGES for ORCID "0000-0001-9345-632X"

Moessner, R.; Powell, M. ;

• Search DOE PAGES for author "Powell, M."
• Search DOE PAGES for ORCID "0000-0002-5590-0693"

Kolis, J. W.; Pasco, C. M. ;

• Search DOE PAGES for author "Pasco, C. M."
• Search DOE PAGES for ORCID "0000-0003-3837-6858"

May, A. F.; Frontzek, M. D. ;

• Search DOE PAGES for author "Frontzek, M. D."
• Search DOE PAGES for ORCID "0000-0001-8704-8928"

Smith, E. M. ;

• Search DOE PAGES for author "Smith, E. M."
• Search DOE PAGES for ORCID "0000-0002-2054-3585"

Gaulin, B. D.; Calder, S. ;

• Search DOE PAGES for author "Calder, S."
• Search DOE PAGES for ORCID "0000-0001-8402-3741"

Ross, K. A.

Publication Date:

Tue Jan 16 00:00:00 EST 2024

Research Org.:

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Oak Ridge Institute for Science and Education (ORISE), Oak Ridge, TN (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

OSTI Identifier:

2281437

Alternate Identifier(s):

OSTI ID: 2305796

Grant/Contract Number:  

SC0014664; SC0020071; AC05-00OR22725

Resource Type:

Published Article

Journal Name:

Physical Review. X

Additional Journal Information:

Journal Name: Physical Review. X Journal Volume: 14 Journal Issue: 1; Journal ID: ISSN 2160-3308

Publisher:

American Physical Society

Country of Publication:

United States

Language:

English

Subject:

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; frustrated magnetism; magnetic interactions; phase diagrams; spin ice; pyrochlores; exact diagonalization; Monte Carlo methods; neutron diffraction; specific heat measurements