Browsing by Author "Ramesh, Ramamoorthy"
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Item Emergent chirality in a polar meron to skyrmion phase transition(Springer Nature, 2023) Shao, Yu-Tsun; Das, Sujit; Hong, Zijian; Xu, Ruijuan; Chandrika, Swathi; Gómez-Ortiz, Fernando; García-Fernández, Pablo; Chen, Long-Qing; Hwang, Harold Y.; Junquera, Javier; Martin, Lane W.; Ramesh, Ramamoorthy; Muller, David A.Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of −1) to a two-dimensional, tetratic lattice of merons (with topological charge of −1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8 membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). We show how scanning electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and phase-field simulations.Item Non-volatile magnon transport in a single domain multiferroic(Springer Nature, 2024) Husain, Sajid; Harris, Isaac; Meisenheimer, Peter; Mantri, Sukriti; Li, Xinyan; Ramesh, Maya; Behera, Piush; Taghinejad, Hossein; Kim, Jaegyu; Kavle, Pravin; Zhou, Shiyu; Kim, Tae Yeon; Zhang, Hongrui; Stevenson, Paul; Analytis, James G.; Schlom, Darrell; Salahuddin, Sayeef; Íñiguez-González, Jorge; Xu, Bin; Martin, Lane W.; Caretta, Lucas; Han, Yimo; Bellaiche, Laurent; Yao, Zhi; Ramesh, Ramamoorthy; Rice Advanced Materials InstituteAntiferromagnets have attracted significant attention in the field of magnonics, as promising candidates for ultralow-energy carriers for information transfer for future computing. The role of crystalline orientation distribution on magnon transport has received very little attention. In multiferroics such as BiFeO3 the coupling between antiferromagnetic and polar order imposes yet another boundary condition on spin transport. Thus, understanding the fundamentals of spin transport in such systems requires a single domain, a single crystal. We show that through Lanthanum (La) substitution, a single ferroelectric domain can be engineered with a stable, single-variant spin cycloid, controllable by an electric field. The spin transport in such a single domain displays a strong anisotropy, arising from the underlying spin cycloid lattice. Our work shows a pathway to understanding the fundamental origins of magnon transport in such a single domain multiferroic.Item Optical Control of Adaptive Nanoscale Domain Networks(Wiley, 2024) Zajac, Marc; Zhou, Tao; Yang, Tiannan; Das, Sujit; Cao, Yue; Guzelturk, Burak; Stoica, Vladimir; Cherukara, Mathew J.; Freeland, John W.; Gopalan, Venkatraman; Ramesh, Ramamoorthy; Martin, Lane W.; Chen, Long-Qing; Holt, Martin V.; Hruszkewycz, Stephan O.; Wen, Haidan; Rice Advanced Materials InstituteAdaptive networks can sense and adjust to dynamic environments to optimize their performance. Understanding their nanoscale responses to external stimuli is essential for applications in nanodevices and neuromorphic computing. However, it is challenging to image such responses on the nanoscale with crystallographic sensitivity. Here, the evolution of nanodomain networks in (PbTiO3)n/(SrTiO3)n superlattices (SLs) is directly visualized in real space as the system adapts to ultrafast repetitive optical excitations that emulate controlled neural inputs. The adaptive response allows the system to explore a wealth of metastable states that are previously inaccessible. Their reconfiguration and competition are quantitatively measured by scanning x-ray nanodiffraction as a function of the number of applied pulses, in which crystallographic characteristics are quantitatively assessed by assorted diffraction patterns using unsupervised machine-learning methods. The corresponding domain boundaries and their connectivity are drastically altered by light, holding promise for light-programable nanocircuits in analogy to neuroplasticity. Phase-field simulations elucidate that the reconfiguration of the domain networks is a result of the interplay between photocarriers and transient lattice temperature. The demonstrated optical control scheme and the uncovered nanoscopic insights open opportunities for the remote control of adaptive nanoscale domain networks.Item Phase Transformation Driven by Oxygen Vacancy Redistribution as the Mechanism of Ferroelectric Hf0.5Zr0.5O2 Fatigue(Wiley, 2024) Zhang, Zimeng; Craig, Isaac; Zhou, Tao; Holt, Martin; Flores, Raul; Sheridan, Evan; Inzani, Katherine; Huang, Xiaoxi; Nag, Joyeeta; Prasad, Bhagwati; Griffin, Sinéad M.; Ramesh, RamamoorthyAs a promising candidate for nonvolatile memory devices, the hafnia-based ferroelectric system has recently been a hot research topic. Although significant progress has been made over the past decade, the endurance problem is still an obstacle to its final application. In perovskite-based ferroelectrics, such as the well-studied Pb[ZrxTi1−x]O3 (PZT) family, polarization fatigue has been discussed within the framework of the interaction of charged defects (such as oxygen vacancies) with the moving domains during the switching process, particularly at the electrode-ferroelectric interface. Armed with this background, a hypothesis is set out to test that a similar mechanism can be in play with the hafnia-based ferroelectrics. The conducting perovskite La-Sr-Mn-O is used as the contact electrode to create La0.67Sr0.33MnO3 / Hf0.5Zr0.5O2 (HZO)/ La0.67Sr0.33MnO3 capacitor structures deposited on SrTiO3-Si substrates. Nanoscale X-ray diffraction is performed on single capacitors, and a structural phase transition from polar o-phase toward non-polar m-phase is demonstrated during the bipolar switching process. The energy landscape of multiphase HZO has been calculated at varying oxygen vacancy concentrations. Based on both theoretical and experimental results, it is found that a polar to non-polar phase transformation caused by oxygen vacancy redistribution during electric cycling is a likely explanation for fatigue in HZO.Item Roadmap on low-power electronics(AIP Publishing, 2024) Ramesh, Ramamoorthy; Salahuddin, Sayeef; Datta, Suman; Diaz, Carlos H.; Nikonov, Dmitri E.; Young, Ian A.; Ham, Donhee; Chang, Meng-Fan; Khwa, Win-San; Lele, Ashwin Sanjay; Binek, Christian; Huang, Yen-Lin; Sun, Yuan-Chen; Chu, Ying-Hao; Prasad, Bhagwati; Hoffmann, Michael; Hu, Jia-Mian; Yao, Zhi (Jackie); Bellaiche, Laurent; Wu, Peng; Cai, Jun; Appenzeller, Joerg; Datta, Supriyo; Camsari, Kerem Y.; Kwon, Jaesuk; Incorvia, Jean Anne C.; Asselberghs, Inge; Ciubotaru, Florin; Couet, Sebastien; Adelmann, Christoph; Zheng, Yi; Lindenberg, Aaron M.; Evans, Paul G.; Ercius, Peter; Radu, Iuliana P.Item Size-Induced Ferroelectricity in Antiferroelectric Oxide Membranes(Wiley, 2023) Xu, Ruijuan; Crust, Kevin J.; Harbola, Varun; Arras, Rémi; Patel, Kinnary Y.; Prosandeev, Sergey; Cao, Hui; Shao, Yu-Tsun; Behera, Piush; Caretta, Lucas; Kim, Woo Jin; Khandelwal, Aarushi; Acharya, Megha; Wang, Melody M.; Liu, Yin; Barnard, Edward S.; Raja, Archana; Martin, Lane W.; Gu, X. Wendy; Zhou, Hua; Ramesh, Ramamoorthy; Muller, David A.; Bellaiche, Laurent; Hwang, Harold Y.Despite extensive studies on size effects in ferroelectrics, how structures and properties evolve in antiferroelectrics with reduced dimensions still remains elusive. Given the enormous potential of utilizing antiferroelectrics for high-energy-density storage applications, understanding their size effects will provide key information for optimizing device performances at small scales. Here, the fundamental intrinsic size dependence of antiferroelectricity in lead-free NaNbO3 membranes is investigated. Via a wide range of experimental and theoretical approaches, an intriguing antiferroelectric-to-ferroelectric transition upon reducing membrane thickness is probed. This size effect leads to a ferroelectric single-phase below 40 nm, as well as a mixed-phase state with ferroelectric and antiferroelectric orders coexisting above this critical thickness. Furthermore, it is shown that the antiferroelectric and ferroelectric orders are electrically switchable. First-principle calculations further reveal that the observed transition is driven by the structural distortion arising from the membrane surface. This work provides direct experimental evidence for intrinsic size-driven scaling in antiferroelectrics and demonstrates enormous potential of utilizing size effects to drive emergent properties in environmentally benign lead-free oxides with the membrane platform.Item Spin disorder control of topological spin texture(Springer Nature, 2024) Zhang, Hongrui; Shao, Yu-Tsun; Chen, Xiang; Zhang, Binhua; Wang, Tianye; Meng, Fanhao; Xu, Kun; Meisenheimer, Peter; Chen, Xianzhe; Huang, Xiaoxi; Behera, Piush; Husain, Sajid; Zhu, Tiancong; Pan, Hao; Jia, Yanli; Settineri, Nick; Giles-Donovan, Nathan; He, Zehao; Scholl, Andreas; N’Diaye, Alpha; Shafer, Padraic; Raja, Archana; Xu, Changsong; Martin, Lane W.; Crommie, Michael F.; Yao, Jie; Qiu, Ziqiang; Majumdar, Arun; Bellaiche, Laurent; Muller, David A.; Birgeneau, Robert J.; Ramesh, Ramamoorthy; Rice Advanced Materials InstituteStabilization of topological spin textures in layered magnets has the potential to drive the development of advanced low-dimensional spintronics devices. However, achieving reliable and flexible manipulation of the topological spin textures beyond skyrmion in a two-dimensional magnet system remains challenging. Here, we demonstrate the introduction of magnetic iron atoms between the van der Waals gap of a layered magnet, Fe3GaTe2, to modify local anisotropic magnetic interactions. Consequently, we present direct observations of the order-disorder skyrmion lattices transition. In addition, non-trivial topological solitons, such as skyrmioniums and skyrmion bags, are realized at room temperature. Our work highlights the influence of random spin control of non-trivial topological spin textures.Item Switching the spin cycloid in BiFeO3 with an electric field(Springer Nature, 2024) Meisenheimer, Peter; Moore, Guy; Zhou, Shiyu; Zhang, Hongrui; Huang, Xiaoxi; Husain, Sajid; Chen, Xianzhe; Martin, Lane W.; Persson, Kristin A.; Griffin, Sinéad; Caretta, Lucas; Stevenson, Paul; Ramesh, Ramamoorthy; Rice Advanced Materials InstituteBismuth ferrite (BiFeO3) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO3 are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements. Using nitrogen vacancy-based diamond magnetometry, we observe the magnetic spin cycloid structure of BiFeO3 in real space. This structure is magnetoelectrically coupled through symmetry to the ferroelectric polarization and this relationship is maintained through electric field switching. Through a combination of in-plane and out-of-plane electrical switching, coupled with ab initio studies, we have discovered that the epitaxy from the substrate imposes a magnetoelastic anisotropy on the spin cycloid, which establishes preferred cycloid propagation directions. The energy landscape of the cycloid is shaped by both the ferroelectric degree of freedom and strain-induced anisotropy, restricting the spin spiral propagation vector to changes to specific switching events.Item The emergence of three-dimensional chiral domain walls in polar vortices(Springer Nature, 2023) Susarla, Sandhya; Hsu, Shanglin; Gómez-Ortiz, Fernando; García-Fernández, Pablo; Savitzky, Benjamin H.; Das, Sujit; Behera, Piush; Junquera, Javier; Ercius, Peter; Ramesh, Ramamoorthy; Ophus, ColinChirality or handedness of a material can be used as an order parameter to uncover the emergent electronic properties for quantum information science. Conventionally, chirality is found in naturally occurring biomolecules and magnetic materials. Chirality can be engineered in a topological polar vortex ferroelectric/dielectric system via atomic-scale symmetry-breaking operations. We use four-dimensional scanning transmission electron microscopy (4D-STEM) to map out the topology-driven three-dimensional domain walls, where the handedness of two neighbor topological domains change or remain the same. The nature of the domain walls is governed by the interplay of the local perpendicular (lateral) and parallel (axial) polarization with respect to the tubular vortex structures. Unique symmetry-breaking operations and the finite nature of domain walls result in a triple point formation at the junction of chiral and achiral domain walls. The unconventional nature of the domain walls with triple point pairs may result in unique electrostatic and magnetic properties potentially useful for quantum sensing applications.