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- ItemOrganic carbon burial is paced by a ∼173-ka obliquity cycle in the middle to high latitudes(Washington, DC [u.a.] : Assoc., 2021) Huang, He; Gao, Yuan; Ma, Chao; Jones, Matthew M.; Zeeden, Christian; Ibarra, Daniel E.; Wu, Huaichun; Wang, ChengshanEarth’s climate system is complex and inherently nonlinear, which can induce some extraneous cycles in paleoclimatic proxies at orbital time scales. The paleoenvironmental consequences of these extraneous cycles are debated owing to their complex origin. Here, we compile high-resolution datasets of total organic carbon (TOC) and stable carbon isotope (δ13Corg) datasets to investigate organic carbon burial processes in middle to high latitudes. Our results document a robust cyclicity of ~173 thousand years (ka) in both TOC and δ13Corg. The ~173-ka obliquity–related forcing signal was amplified by internal climate feedbacks of the carbon cycle under different geographic and climate conditions, which control a series of sensitive climatic processes. In addition, our new and compiled records from multiple proxies confirm the presence of the obliquity amplitude modulation (AM) cycle during the Mesozoic and Cenozoic and indicate the usefulness of the ~173-ka cycle as geochronometer and for paleoclimatic interpretation.
- ItemVoltage control of magnetic order in RKKY coupled multilayers(Washington, DC [u.a.] : Assoc., 2023) Kossak, Alexander E.; Huang, Mantao; Reddy, Pooja; Wolf, Daniel; Beach, Geoffrey S. D.In the field of antiferromagnetic (AFM) spintronics, there is a substantial effort present to make AFMs viable active components for efficient and fast devices. Typically, this is done by manipulating the AFM Néel vector. Here, we establish a method of enabling AFM active components by directly controlling the magnetic order. We show that magneto-ionic gating of hydrogen enables dynamic control of the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction in solid-state synthetic AFM multilayer devices. Using a gate voltage, we tune the RKKY interaction to drive continuous transitions from AFM to FM and vice versa. The switching is submillisecond at room temperature and fully reversible. We validate the utility of this method by demonstrating that magneto-ionic gating of the RKKY interaction allows for 180° field-free deterministic switching. This dynamic method of controlling a fundamental exchange interaction can engender the manipulation of a broader array of spin textures, e.g., chiral domain walls and skyrmions.
- ItemQuantitative hyperspectral coherent diffractive imaging spectroscopy of a solid-state phase transition in vanadium dioxide(Washington, DC [u.a.] : Assoc., 2021) Johnson, Allan S.; Conesa, Jordi Valls; Vidas, Luciana; Perez-Salinas, Daniel; Günther, Christian M.; Pfau, Bastian; Hallman, Kent A.; Haglund, Richard F.; Eisebitt, Stefan; Wall, SimonSolid-state systems can host a variety of thermodynamic phases that can be controlled with magnetic fields, strain, or laser excitation. Many phases that are believed to exhibit exotic properties only exist on the nanoscale, coexisting with other phases that make them challenging to study, as measurements require both nanometer spatial resolution and spectroscopic information, which are not easily accessible with traditional x-ray spectromicroscopy techniques. Here, we use coherent diffractive imaging spectroscopy (CDIS) to acquire quantitative hyperspectral images of the prototypical quantum material vanadium oxide across the vanadium L2,3 and oxygen K x-ray absorption edges with nanometer-scale resolution. We extract the full complex refractive indices of the monoclinic insulating and rutile conducting phases of VO2 from a single sample and find no evidence for correlation-driven phase transitions. CDIS will enable quantitative full-field x-ray spectromicroscopy for studying phase separation in time-resolved experiments and other extreme sample environments where other methods cannot operate.
- ItemAtomic Sn–enabled high-utilization, large-capacity, and long-life Na anode(Washington, DC [u.a.] : Assoc., 2022) Xu, Fei; Qu, Changzhen; Lu, Qiongqiong; Meng, Jiashen; Zhang, Xiuhai; Xu, Xiaosa; Qiu, Yuqian; Ding, Baichuan; Yang, Jiaying; Cao, Fengren; Yang, Penghui; Jiang, Guangshen; Kaskel, Stefan; Ma, Jingyuan; Li, Liang; Zhang, Xingcai; Wang, HongqiangConstructing robust nucleation sites with an ultrafine size in a confined environment is essential toward simultaneously achieving superior utilization, high capacity, and long-term durability in Na metal-based energy storage, yet remains largely unexplored. Here, we report a previously unexplored design of spatially confined atomic Sn in hollow carbon spheres for homogeneous nucleation and dendrite-free growth. The designed architecture maximizes Sn utilization, prevents agglomeration, mitigates volume variation, and allows complete alloying-dealloying with high-affinity Sn as persistent nucleation sites, contrary to conventional spatially exposed large-size ones without dealloying. Thus, conformal deposition is achieved, rendering an exceptional capacity of 16 mAh cm−2 in half-cells and long cycling over 7000 hours in symmetric cells. Moreover, the well-known paradox is surmounted, delivering record-high Na utilization (e.g., 85%) and large capacity (e.g., 8 mAh cm−2) while maintaining extraordinary durability over 5000 hours, representing an important breakthrough for stabilizing Na anode.
- ItemHighly efficient modulation doping: A path toward superior organic thermoelectric devices(Washington, DC [u.a.] : Assoc., 2022) Wang, Shu-Jen; Panhans, Michel; Lashkov, Ilia; Kleemann, Hans; Caglieris, Federico; Becker-Koch, David; Vahland, Jörn; Guo, Erjuan; Huang, Shiyu; Krupskaya, Yulia; Vaynzof, Yana; Büchner, Bernd; Ortmann, Frank; Leo, KarlWe investigate the charge and thermoelectric transport in modulation-doped large-area rubrene thin-film crystals with different crystal phases. We show that modulation doping allows achieving superior doping efficiencies even for high doping densities, when conventional bulk doping runs into the reserve regime. Modulation-doped orthorhombic rubrene achieves much improved thermoelectric power factors, exceeding 20 μW m−1 K−2 at 80°C. Theoretical studies give insight into the energy landscape of the heterostructures and its influence on qualitative trends of the Seebeck coefficient. Our results show that modulation doping together with high-mobility crystalline organic semiconductor films is a previosly unexplored strategy for achieving high-performance organic thermoelectrics.
- ItemIntermolecular charge transfer enhances the performance of molecular rectifiers(Washington, DC [u.a.] : Assoc., 2022) Sullivan, Ryan P.; Morningstar, John T.; Castellanos-Trejo, Eduardo; Bradford, Robert W.; Hofstetter, Yvonne J.; Vaynzof, Yana; Welker, Mark E.; Jurchescu, Oana D.Molecular-scale diodes made from self-assembled monolayers (SAMs) could complement silicon-based technologies with smaller, cheaper, and more versatile devices. However, advancement of this emerging technology is limited by insufficient electronic performance exhibited by the molecular current rectifiers. We overcome this barrier by exploiting the charge-transfer state that results from co-assembling SAMs of molecules with strong electron donor and acceptor termini. We obtain a substantial enhancement in current rectification, which correlates with the degree of charge transfer, as confirmed by several complementary techniques. These findings provide a previously enexplored method for manipulating the properties of molecular electronic devices by exploiting donor/acceptor interactions. They also serve as a model test platform for the study of doping mechanisms in organic systems. Our devices have the potential for fast widespread adoption due to their low-cost processing and self-assembly onto silicon substrates, which could allow seamless integration with current technologies.
- ItemA thrombin-triggered self-regulating anticoagulant strategy combined with anti-inflammatory capacity for blood-contacting implants(Washington, DC [u.a.] : Assoc., 2022) Wang, Yanan; Wu, Haoshuang; Zhou, Zhongyi; Maitz, Manfred F.; Liu, Kunpeng; Zhang, Bo; Yang, Li; Luo, Rifang; Wang, YunbingInterrelated coagulation and inflammation are impediments to endothelialization, a prerequisite for the longterm function of cardiovascular materials. Here, we proposed a self-regulating anticoagulant coating strategy combined with anti-inflammatory capacity, which consisted of thrombin-responsive nanogels with anticoagulant and anti-inflammatory components. As an anticoagulant, rivaroxaban was encapsulated in nanogels cross-linked by thrombin-cleavable peptide and released upon the trigger of environmental thrombin, blocking the further coagulation cascade. The superoxide dismutase mimetic Tempol imparted the antioxidant property. Polyphenol epigallocatechin gallate (EGCG), in addition to its anti-inflammatory function in synergy with Tempol, also acted as a weak cross-linker to stabilize the coating. The effectiveness and versatility of this coating were validated using two typical cardiovascular devices as models, biological valves and vascular stents. It was demonstrated that the coating worked as a precise strategy to resist coagulation and inflammation, escorted reendothelialization on the cardiovascular devices, and provided a new perspective for designing endothelium-like functional coatings.
- ItemUltrafast optically induced spin transfer in ferromagnetic alloys(Washington, DC [u.a.] : Assoc., 2020) Hofherr, M.; Häuser, S.; Dewhurst, J.K.; Tengdin, P.; Sakshath, S.; Nembach, H.T.; Weber, S.T.; Shaw, J.M.; Silva, T.J.; Kapteyn, H.C.; Cinchetti, M.; Rethfeld, B.; Murnane, M.M.; Steil, D.; Stadtmüller, B.; Sharma, S.; Aeschlimann, M.; Mathias, S.The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.
- ItemStrongly enhanced and tunable photovoltaic effect in ferroelectric-paraelectric superlattices(Washington, DC [u.a.] : Assoc., 2021) Yun, Yeseul; Mühlenbein, Lutz; Knoche, David S.; Lotnyk, Andriy; Bhatnagar, AkashEver since the first observation of a photovoltaic effect in ferroelectric BaTiO3, studies have been devoted to analyze this effect, but only a few attempted to engineer an enhancement. In conjunction, the steep progress in thin-film fabrication has opened up a plethora of previously unexplored avenues to tune and enhance material properties via growth in the form of superlattices. In this work, we present a strategy wherein sandwiching a ferroelectric BaTiO3 in between paraelectric SrTiO3 and CaTiO3 in a superlattice form results in a strong and tunable enhancement in photocurrent. Comparison with BaTiO3 of similar thickness shows the photocurrent in the superlattice is 103 times higher, despite a nearly two-thirds reduction in the volume of BaTiO3. The enhancement can be tuned by the periodicity of the superlattice, and persists under 1.5 AM irradiation. Systematic investigations highlight the critical role of large dielectric permittivity and lowered bandgap.
- ItemFingerprint of volcanic forcing on the ENSO-Indian monsoon coupling(Washington, DC [u.a.] : Assoc., 2020) Singh, M.; Krishnan, R.; Goswami, B.; Choudhury, A. D.; Swapna, P.; Vellore, R.; Prajeesh, A. G.; Sandeep, N.; Venkataraman, C.; Donner, R. V.; Marwan, N.; Kurths, J.Coupling of the El Niño-Southern Oscillation (ENSO) and Indian monsoon (IM) is central to seasonal summer monsoon rainfall predictions over the Indian subcontinent, although a nonstationary relationship between the two nonlinear phenomena can limit seasonal predictability. Radiative effects of volcanic aerosols injected into the stratosphere during large volcanic eruptions (LVEs) tend to alter ENSO evolution; however, their impact on ENSO-IM coupling remains unclear. Here, we investigate how LVEs influence the nonlinear behavior of the ENSO and IM dynamical systems using historical data, 25 paleoclimate reconstructions, last-millennium climate simulations, large-ensemble targeted climate sensitivity experiments, and advanced analysis techniques. Our findings show that LVEs promote a significantly enhanced phase-synchronization of the ENSO and IM oscillations, due to an increase in the angular frequency of ENSO. The results also shed innovative insights into the physical mechanism underlying the LVE-induced enhancement of ENSO-IM coupling and strengthen the prospects for improved seasonal monsoon predictions.