Abstract
The interplay between charge, structure, and magnetism gives rise to rich phase diagrams in complex materials with exotic properties emerging when phases compete. Molecule-based materials are particularly advantageous in this regard due to their low energy scales, flexible lattices, and chemical tunability. Here, we bring together high pressure Raman scattering, modeling, and first principles calculations to reveal the pressure-temperature-magnetic field phase diagram of Mn[N(CN)2]2. We uncover how hidden soft modes involving octahedral rotations drive two pressure-induced transitions triggering the low → high magnetic anisotropy crossover and a unique reorientation of exchange planes. These magnetostructural transitions and their mechanisms highlight the importance of spin-lattice interactions in establishing phases with novel magnetic properties in Mn(II)-containing systems.
| Original language | English |
|---|---|
| Article number | 65 |
| Journal | npj Quantum Materials |
| Volume | 2 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 1 2017 |
Funding
This work was supported by the National Science Foundation [DMR-1707846 (JLM, UT) and DMR-1703003 (JLM, EWU)], the Petroleum Research Fund [52052-ND10 (JLM, UT)], and the Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (RF). The research at UNIST (JHL, MSK) was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning (2015R1C1A1A01055760) and Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2017M3D1A1040828). Work at the National Synchrotron Light Source at Brookhaven National Laboratory was funded by the Department of Energy (DE-AC98-06CH10886). The use of the U2A beamline was supported by COMPRES under NSF Cooperative Agreement EAR 11-57758 and CDAC (DE-FC03-03N00144). This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
| Funders | Funder number |
|---|---|
| CDAC | DE-FC03-03N00144 |
| COMPRES | |
| DOE Office of Science | |
| Ministry of Science and ICT | 2017M3D1A1040828, DE-AC98-06CH10886 |
| National Science Foundation | 1703003, EAR 11-57758, 1707846, DMR-1707846, DMR-1703003 |
| U.S. Department of Energy | |
| Office of Science | |
| Basic Energy Sciences | |
| American Chemical Society Petroleum Research Fund | 52052-ND10 |
| Division of Materials Sciences and Engineering | |
| Ulsan National Institute of Science and Technology | |
| Ministry of Science, ICT and Future Planning | 2015R1C1A1A01055760 |
| National Research Foundation of Korea |