skip to main content

This content will become publicly available on May 1, 2024

Title: Spin–phonon interactions and magnetoelectric coupling in Co4B2O9 ( B = Nb, Ta)
In order to explore the consequences of spin–orbit coupling on spin–phonon interactions in a set of chemically similar mixed metal oxides, we measured the infrared vibrational properties of Co4B2O9 (B = Nb, Ta) as a function of temperature and compared our findings with lattice dynamics calculations and several different models of spin–phonon coupling. Frequency vs temperature trends for the Co2+ shearing mode near 150 cm−1 reveal significant shifts across the magnetic ordering temperature that are especially large in relative terms. Bringing these results together and accounting for noncollinearity, we obtain spin–phonon coupling constants of −3.4 and −4.3 cm−1 for Co4Nb2O9 and the Ta analog, respectively. Analysis reveals that these coupling constants are derived from interlayer (rather than intralayer) exchange interactions and that the interlayer interactions contain competing antiferromagnetic and ferromagnetic contributions. At the same time, beyond-Heisenberg terms are minimized due to fortuitous symmetry considerations, different from most other 4d- and 5d-containing oxides. Comparison with other contemporary oxides shows that spin–phonon coupling in this family of materials is among the strongest ever reported, suggesting an origin for magnetoelectric coupling.  more » « less
Award ID(s):
2103625 1954856
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Applied Physics Letters
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Due to the coexistence of many emergent phenomena, including 2D superconductivity and a large Rashba spin‐orbit coupling, 5d transition metal oxides‐based two‐dimensional electron systems (2DESs) have been prospected as one of the potential intrants for modern electronics. However, despite the lighter electron mass, the mobility of carriers, a key requisite for high‐performance devices, in 5d‐oxides devices remains far behind their 3d‐oxides analogs. The carriers’ mobility in these oxides is significantly hampered by the inevitable presence of defects. Here, very high mobility (≈22 650 cm2V−1s−1) of 5d‐2DES confined at the LaAlO3/KTaO3interface is reported. The high mobility, which is beyond the values observed in SrTiO32DESs in the same carrier‐density range, is achieved using the ionic‐liquid gating at room temperature. The authors postulate that the ionic‐liquid gating affects the oxygen vacancies and efficiently reduces any disorder at the interface. Investigating density and mobility in a broad range of back‐gate voltage, the authors reveal that the mobility follows the power‐law µ ∝ n1.2, indicating the very high quality of ionic‐liquid‐gated LaAlO3/KTaO3devices, consistent with the postulate. Furthermore, the analysis of the quantum oscillations confirms that the high‐mobility electrons occupy the electronic sub‐bands emerging from the Ta:5d orbitals of KTaO3.

    more » « less
  2. Abstract

    Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI3, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm−1. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by ~50% and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI3. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors.

    more » « less
  3. null (Ed.)
    We used a combination of polarized Raman spectroscopy experiment and model magnetism–phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet CrI 3 . We reveal a layered-magnetism–assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in N -layer CrI 3 . We resolve in data and by calculations that the first-order A g phonon of the monolayer splits into an N -fold multiplet in N -layer CrI 3 due to the interlayer coupling ( N ≥ 2 ) and that the phonons within the multiplet show distinct magnetic field dependence because of their different layered-magnetism–phonon coupling. We further find that such a layered-magnetism–phonon coupled Raman scattering mechanism extends beyond first-order to higher-order multiphonon scattering processes. Our results on the magneto-Raman effect of the first-order phonons in the multiplet and the higher-order multiphonons in N -layer CrI 3 demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underline the unique opportunities of spin–phonon physics in van der Waals layered magnets. 
    more » « less
  4. Abstract

    The formation of a “spin polaron” stems from strong spin-charge-lattice interactions in magnetic oxides, which leads to a localization of carriers accompanied by local magnetic polarization and lattice distortion. For example, cupric oxide (CuO), which is a promising photocathode material and shares important similarities with highTcsuperconductors, conducts holes through spin polaron hopping with flipped spins at Cu atoms where a spin polaron has formed. The formation of these spin polarons results in an activated hopping conduction process where the carriers must not only overcome strong electron−phonon coupling but also strong magnetic coupling. Collectively, these effects cause low carrier conduction in CuO and hinder its applications. To overcome this fundamental limitation, we demonstrate from first-principles calculations how doping can improve hopping conduction through simultaneous improvement of hole concentration and hopping mobility in magnetic oxides such as CuO. Specifically, using Li doping as an example, we show that Li has a low ionization energy that improves hole concentration, and lowers the hopping barrier through both the electron−phonon and magnetic couplings' reduction that improves hopping mobility. Finally, this improved conduction predicted by theory is validated through the synthesis of Li-doped CuO electrodes which show enhanced photocurrent compared to pristine CuO electrodes. We conclude that doping with nonmagnetic shallow impurities is an effective strategy to improve hopping conductivities in magnetic oxides.

    more » « less
  5. Ultrashort light pulses can selectively excite charges, spins, and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge-density wave (CDW) material 1T-TaSe2. After exciting the material with a femtosecond pulse, fast spatial smearing of the laser-excited electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This finding is in contrast to all previous observations in multiple materials to date, where the electron temperature decreases monotonically via electron–phonon scattering. By tuning the laser fluence, the magnitude of the electron temperature modulation changes from ∼200 K in the case of weak excitation, to ∼1,000 K for strong laser excitation. We also observe a phase change of π in the electron temperature modulation at a critical fluence of 0.7 mJ/cm2, which suggests a switching of the dominant coupling mechanism between the coherent phonon and electrons. Our approach opens up routes for coherently manipulating the interactions and properties of two-dimensional and other quantum materials using light.

    more » « less