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- ItemTime-resolved structural evolution during the collapse of responsive hydrogels: The microgel-to-particle transition(Washington, DC [u.a.] : Assoc., 2018) Keidel, Rico; Ghavami, Ali; Lugo, Dersy M.; Lotze, Gudrun; Virtanen, Otto; Beumers, Peter; Pedersen, Jan Skov; Bardow, Andre; Winkler, Roland G.; Richtering, WalterAdaptive hydrogels, often termed smart materials, are macromolecules whose structure adjusts to external stimuli. Responsive micro- and nanogels are particularly interesting because the small length scale enables very fast response times. Chemical cross-links provide topological constraints and define the three-dimensional structure of the microgels, whereas their porous structure permits fast mass transfer, enabling very rapid structural adaption of the microgel to the environment. The change of microgel structure involves a unique transition from a flexible, swollen finite-size macromolecular network, characterized by a fuzzy surface, to a colloidal particle with homogeneous density and a sharp surface. In this contribution, we determine, for the first time, the structural evolution during the microgel-to-particle transition. Time-resolved small-angle x-ray scattering experiments and computer simulations unambiguously reveal a two-stage process: In a first, very fast process, collapsed clusters form at the periphery, leading to an intermediate, hollowish core-shell structure that slowly transforms to a globule. This structural evolution is independent of the type of stimulus and thus applies to instantaneous transitions as in a temperature jump or to slower stimuli that rely on the uptake of active molecules from and/or exchange with the environment. The fast transitions of size and shape provide unique opportunities for various applications as, for example, in uptake and release, catalysis, or sensing.
- ItemA photonic platform for donor spin qubits in silicon(Washington, DC [u.a.] : Assoc., 2017) Morse, Kevin J.; Abraham, Rohan J. S.; DeAbreu, Adam; Bowness, Camille; Richards, Timothy S.; Riemann, Helge; Abrosimov, Nikolay V.; Becker, Peter; Pohl, Hans-Joachim; Thewalt, Michael L. W.; Simmons, StephanieDonor spins in silicon are highly competitive qubits for upcoming quantum technologies, offering complementary metal-oxide semiconductor compatibility, coherence (T2) times of minutes to hours, and simultaneous initialization, manipulation, and readout fidelities near ~99.9%. This allows for many quantum error correction protocols, which will be essential for scale-up. However, a proven method of reliably coupling spatially separated donor qubits has yet to be identified. We present a scalable silicon-based platform using the unique optical properties of “deep” chalcogen donors. For the prototypical 77Se+ donor, we measure lower bounds on the transition dipole moment and excited-state lifetime, enabling access to the strong coupling limit of cavity quantum electrodynamics using known silicon photonic resonator technology and integrated silicon photonics. We also report relatively strong photon emission from this same transition. These results unlock clear pathways for silicon-based quantum computing, spin-to-photon conversion, photonic memories, integrated single-photon sources, and all-optical switches.
- 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.
- ItemSingle “Swiss-roll” microelectrode elucidates the critical role of iron substitution in conversion-type oxides(Washington, DC [u.a.] : Assoc., 2022) Liu, Lixiang; Huang, Shaozhuan; Shi, Wujun; Sun, Xiaolei; Pang, Jinbo; Lu, Qiongqiong; Yang, Ye; Xi, Lixia; Deng, Liang; Oswald, Steffen; Yin, Yin; Liu, Lifeng; Ma, Libo; Schmidt, Oliver G.; Shi, Yumeng; Zhang, LinAdvancing the lithium-ion battery technology requires the understanding of electrochemical processes in electrode materials with high resolution, accuracy, and sensitivity. However, most techniques today are limited by their inability to separate the complex signals from slurry-coated composite electrodes. Here, we use a three-dimensional “Swiss-roll” microtubular electrode that is incorporated into a micrometer-sized lithium battery. This on-chip platform combines various in situ characterization techniques and precisely probes the intrinsic electrochemical properties of each active material due to the removal of unnecessary binders and additives. As an example, it helps elucidate the critical role of Fe substitution in a conversion-type NiO electrode by monitoring the evolution of Fe2O3 and solid electrolyte interphase layer. The markedly enhanced electrode performances are therefore explained. Our approach exposes a hitherto unexplored route to tracking the phase, morphology, and electrochemical evolution of electrodes in real time, allowing us to reveal information that is not accessible with bulk-level characterization techniques.
- 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.