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Register a new userCoherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
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Added by
Prashant Padmanabhan
Publication date
2020
fields
Physics
and research's language is
English
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The discovery of two-dimensional (2D) systems hosting intrinsic long-range magnetic order represents a seminal addition to the rich physical landscape of van der Waals (vdW) materials. CrI3 has emerged as perhaps the most salient example, as the interdependence of crystalline structure and magnetic order, along with strong light-matter interactions provides a promising platform to explore the optical control of magnetic, vibrational, and charge degrees of freedom at the 2D limit. However, the fundamental question of how this relationship between structure and magnetism manifests on their intrinsic timescales has rarely been explored. Here, we use ultrafast optical spectroscopy to probe magnetic and vibrational dynamics in CrI3, revealing demagnetization dynamics governed by spin-flip scattering and remarkably, a strong transient exchange-mediated interaction between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the helicity of the driving pulse in the magnetically ordered phase. Our results shed light on the nature of spin-lattice coupling in vdW magnets on ultrafast timescales and highlight their potential for applications requiring non-thermal, high-speed control of magnetism at the nanoscale.
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We report structural, physical properties and electronic structure of van der Waals (vdW) crystal VI3. Detailed analysis reveals that VI3 exhibits a structural transition from monoclinic C2/m to rhombohedral R-3 at Ts ~ 79 K, similar to CrX3 (X = Cl, Br, I). Below Ts, a long-range ferromagnetic (FM) transition emerges at Tc ~ 50 K. The local moment of V in VI3 is close to the high-spin state V3+ ion (S = 1). Theoretical calculation suggests that VI3 may be a Mott insulator with the band gap of about 0.84 eV. In addition, VI3 has a relative small interlayer binding energy and can be exfoliated easily down to few layers experimentally. Therefore, VI3 is a candidate of two-dimensional FM semiconductor. It also provides a novel platform to explore 2D magnetism and vdW heterostructures in S = 1 system.
Van der Waals (vdW) heterostructures, stacking different two-dimensional materials, have opened up unprecedented opportunities to explore new physics and device concepts. Especially interesting are recently discovered two-dimensional magnetic vdW materials, providing new paradigms for spintronic applications. Here, using density functional theory (DFT) calculations, we investigate the spin-dependent electronic transport across vdW magnetic tunnel junctions (MTJs) composed of Fe3GeTe2 ferromagnetic electrodes and a graphene or hexagonal boron nitride (h-BN) spacer layer. For both types of junctions, we find that the junction resistance changes by thousands of percent when the magnetization of the electrodes is switched from parallel to antiparallel. Such a giant tunneling magnetoresistance (TMR) effect is driven by dissimilar electronic structure of the two spin-conducting channels in Fe3GeTe2, resulting in a mismatch between the incoming and outgoing Bloch states in the electrodes and thus suppressed transmission for an antiparallel-aligned MTJ. The vdW bounding between electrodes and a spacer layer makes this result virtually independent of the type of the spacer layer, making the predicted giant TMR effect robust with respect to strain, lattice mismatch, interface distance and other parameters which may vary in the experiment. We hope that our results will further stimulate experimental studies of vdW MTJs and pave the way for their applications in spintronics.
Raman scattering is a ubiquitous phenomenon in light-matter interactions which reveals a materials electronic, structural and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe2 monolayer with materials such as SiO2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons which are either traditionally inactive or weak. This Raman scattering can be amplified by nearly two orders of magnitude when a foreign phonon mode is resonantly coupled to the A exciton in WSe2 directly, or via an A1 optical phonon from WSe2. We further showed that the interfacial Raman scattering is distinct between hBN-encapsulated and hBN-sandwiched WSe2 sample geometries. This cross-platform electron-phonon coupling, as well as the sensitivity of 2D excitons to their phononic environments, will prove important in the understanding and engineering of optoelectronic devices based on vdW heterostructures.
Superconductor-ferromagnet (S-F) interfaces in two-dimensional (2D) heterostructures present a unique opportunity to study the interplay between superconductivity and ferromagnetism. The realization of such nanoscale heterostructures in van der Waals (vdW) crystals remains largely unexplored due to the challenge of making an atomically-sharp interface from their layered structures. Here, we build a vdW ferromagnetic Josephson junction (JJ) by inserting a few-layer ferromagnetic insulator Cr2Ge2Te6 into two layers of superconductor NbSe2. Owing to the remanent magnetic moment of the barrier, the critical current and the corresponding junction resistance exhibit a hysteretic and oscillatory behavior against in-plane magnetic fields, manifesting itself as a strong Josephson coupling state. Through the control of this hysteresis, we can effectively trace the magnetic properties of atomic Cr2Ge2Te6 in response to the external magnetic field. Also, we observe a central minimum of critical current in some thick JJ devices, evidencing the coexistence of 0 and {pi} phase coupling in the junction region. Our study paves the way to exploring the sensitive probes of weak magnetism and multifunctional building blocks for phase-related superconducting circuits with the use of vdW heterostructures.
Magnetic phase transitions often occur spontaneously at specific critical temperatures. The presence of more than one critical temperature (Tc) has been observed in several compounds where the coexistence of competing magnetic orders highlights the importance of phase separation driven by different factors such as pressure, temperature and chemical composition. However, it is unknown whether recently discovered two-dimensional (2D) van der Walls (vdW) magnetic materials show such intriguing phenomena that can result in rich phase diagrams with novel magnetic features to be explored. Here we show the existence of three magnetic phase transitions at different Tcs in 2D vdW magnet CrI3 revealed by a complementary suite of muon spin relaxation-rotation, superconducting quantum interference device magnetometry, and large-scale atomistic simulations including higher-order exchange interactions. We find that the traditionally identified Curie temperature of bulk CrI3 at 61 K does not correspond to the long-range order in the full volume (VM) of the crystal but rather a partial transition with less than 25% of VM being magnetically spin-ordered. This transition is composed of highly disordered domains with the easy-axis component of the magnetization Sz not being fully spin-polarized but disordered by in-plane components (Sx, Sy) over the entire layer. As the system cools down, two additional phase transitions at 50 K and 25 K drive the system to 80% and nearly 100% of the magnetically ordered volume, respectively, where the ferromagnetic ground state has a marked Sz character yet also displaying finite contributions of Sx and Sy to the total magnetization. Our results indicate that volume-wise competing electronic phases play an important role in the magnetic properties of CrI3 which set a much lower threshold temperature for exploitation in magnetic device-platforms than initially considered.
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