Abstract
Correlated-electron systems have long been an important platform for various interesting phenomena and fundamental questions in condensed matter physics. As a pivotal process in these systems, d-d transitions have been suggested as a key factor toward realizing optical spin control in two-dimensional (2D) magnets. However, it remains unclear how d-d excitations behave in quasi-2D systems with strong electronic correlation and spin-charge coupling. Here, we present a systematic electronic Raman spectroscopy investigation on d-d transitions in a 2D antiferromagnet-NiPS3, from bulk to atomically thin samples. Two electronic Raman modes originating from the scattering of incident photons with d electrons in Ni2+ ions are observed at ~1.0 eV. This electronic process persists down to trilayer flakes and exhibits insensitivity to the spin ordering of NiPS3. Our study demonstrates the utility of electronic Raman scattering in investigating the unique electronic structure and its coupling to magnetism in correlated 2D magnets.
| Original language | English |
|---|---|
| Article number | eabl7707 |
| Journal | Science Advances |
| Volume | 8 |
| Issue number | 2 |
| DOIs | |
| State | Published - Jan 2022 |
Funding
This material is based upon work supported by the National Science Foundation (NSF) under grant no. 1945364. X.W. and X.L. acknowledge the financial support from Boston University. X.L. acknowledges the membership of the Boston University Photonics Center. L.L. acknowledges computational resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC05-00OR22725. A portion of this research (DFT calculations) used resources at the Center for Nanophase Materials Sciences, which is a U.S. Department of Energy Office of Science User Facility. A.C., A.H., and S.S. acknowledge financial support from the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) Early Career Program under award no. DESC0018080. We acknowledge the computational resources through the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI-1548562, and 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. W.X. acknowledges the National Natural Science Foundation of China (21873048) and the Natural Science Foundation of Jiangsu Province (BK20180319). Z.L. and D.S. acknowledge support from the U.S. Department of Energy (no. DE-FG02-07ER46451) for high-field magnetospectroscopy measurements performed at National High Magnetic Field Laboratory, which is supported by the National Science Foundation through NSF/DMR-1644779 and the state of Florida. K.S.B. is grateful for the support of the Office of Naval Research under award number N00014-20-1-2308.
| Funders | Funder number |
|---|---|
| CADES | |
| Data Environment for Science | |
| National Science Foundation | 1945364 |
| Office of Naval Research | N00014-20-1-2308 |
| U.S. Department of Energy | DE-AC05-00OR22725 |
| Division of Materials Research | -1644779 |
| Office of Science | DE-AC02-05CH11231 |
| Basic Energy Sciences | ACI-1548562, DESC0018080 |
| Boston University | |
| National Energy Research Scientific Computing Center | |
| National Natural Science Foundation of China | 21873048 |
| Natural Science Foundation of Jiangsu Province | BK20180319, DE-FG02-07ER46451 |