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- ItemEngineering new limits to magnetostriction through metastability in iron-gallium alloys([London] : Nature Publishing Group UK, 2021) Meisenheimer, P.B.; Steinhardt, R.A.; Sung, S.H.; Williams, L.D.; Zhuang, S.; Nowakowski, M.E.; Novakov, S.; Torunbalci, M.M.; Prasad, B.; Zollner, C. J.; Wang, Z.; Dawley, N.M.; Schubert, J.; Hunter, A.H.; Manipatruni, S.; Nikonov, D.E.; Young, I.A.; Chen, L.Q.; Bokor, J.; Bhave, S.A.; Ramesh, R.; Hu, J.-M.; Kioupakis, E.; Hovden, R.; Schlom, D.G.; Heron, J.T.Magnetostrictive materials transduce magnetic and mechanical energies and when combined with piezoelectric elements, evoke magnetoelectric transduction for high-sensitivity magnetic field sensors and energy-efficient beyond-CMOS technologies. The dearth of ductile, rare-earth-free materials with high magnetostrictive coefficients motivates the discovery of superior materials. Fe1−xGax alloys are amongst the highest performing rare-earth-free magnetostrictive materials; however, magnetostriction becomes sharply suppressed beyond x = 19% due to the formation of a parasitic ordered intermetallic phase. Here, we harness epitaxy to extend the stability of the BCC Fe1−xGax alloy to gallium compositions as high as x = 30% and in so doing dramatically boost the magnetostriction by as much as 10x relative to the bulk and 2x larger than canonical rare-earth based magnetostrictors. A Fe1−xGax − [Pb(Mg1/3Nb2/3)O3]0.7−[PbTiO3]0.3 (PMN-PT) composite magnetoelectric shows robust 90° electrical switching of magnetic anisotropy and a converse magnetoelectric coefficient of 2.0 × 10−5 s m−1. When optimally scaled, this high coefficient implies stable switching at ~80 aJ per bit.
- ItemOptoelectronic properties and ultrafast carrier dynamics of copper iodide thin films([London] : Nature Publishing Group UK, 2022) Li, Zhan Hua; He, Jia Xing; Lv, Xiao Hu; Chi, Ling Fei; Egbo, Kingsley O.; Li, Ming-De; Tanaka, Tooru; Guo, Qi Xin; Yu, Kin Man; Liu, Chao PingAs a promising high mobility p-type wide bandgap semiconductor, copper iodide has received increasing attention in recent years. However, the defect physics/evolution are still controversial, and particularly the ultrafast carrier and exciton dynamics in copper iodide has rarely been investigated. Here, we study these fundamental properties for copper iodide thin films by a synergistic approach employing a combination of analytical techniques. Steady-state photoluminescence spectra reveal that the emission at ~420 nm arises from the recombination of electrons with neutral copper vacancies. The photogenerated carrier density dependent ultrafast physical processes are elucidated with using the femtosecond transient absorption spectroscopy. Both the effects of hot-phonon bottleneck and the Auger heating significantly slow down the cooling rate of hot-carriers in the case of high excitation density. The effect of defects on the carrier recombination and the two-photon induced ultrafast carrier dynamics are also investigated. These findings are crucial to the optoelectronic applications of copper iodide.
- ItemThe multi-photon induced Fano effect([London] : Nature Publishing Group UK, 2021) Litvinenko, K.L.; Le, Nguyen H.; Redlich, B.; Pidgeon, C.R.; Abrosimov, N.V.; Andreev, Y.; Huang, Zhiming; Murdin, B.N.The ordinary Fano effect occurs in many-electron atoms and requires an autoionizing state. With such a state, photo-ionization may proceed via pathways that interfere, and the characteristic asymmetric resonance structures appear in the continuum. Here we demonstrate that Fano structure may also be induced without need of auto-ionization, by dressing the continuum with an ordinary bound state in any atom by a coupling laser. Using multi-photon processes gives complete, ultra-fast control over the interference. We show that a line-shape index q near unity (maximum asymmetry) may be produced in hydrogenic silicon donors with a relatively weak beam. Since the Fano lineshape has both constructive and destructive interference, the laser control opens the possibility of state-selective detection with enhancement on one side of resonance and invisibility on the other. We discuss a variety of atomic and molecular spectroscopies, and in the case of silicon donors we provide a calculation for a qubit readout application.
- ItemNanometer-thick lateral polyelectrolyte micropatterns induce macrosopic electro-osmotic chaotic fluid instabilities([London] : Macmillan Publishers Limited, part of Springer Nature, 2014) Wessling, M.; Morcillo, L. Garrigós; Abdu, S.Electro-convective vortices in ion concentration polarization under shear flow have been of practical relevance for desalination processes using electrodialysis. The phenomenon has been scientifically disregarded for decades, but is recently embraced by a growing fluid dynamics community due its complex superposition of multi-scale gradients in electrochemical potential and space charge interacting with emerging complex fluid momentum gradients. While the visualization, quantification and fundamental understanding of the often-chaotic fluid dynamics is evolving rapidly due to sophisticated simulations and experimentation, little is known whether these instabilities can be induced and affected by chemical topological heterogeneity in surface properties. In this letter, we report that polyelectrolyte layers applied as micropatterns on ion exchange membranes induce and facilitate the electro-osmotic fluid instabilities. The findings stimulate a variety of fundamental questions comparable to the complexity of today's turbulence research.
- ItemCubosomes from hierarchical self-assembly of poly(ionic liquid) block copolymers([London] : Nature Publishing Group UK, 2017) He, Hongkun; Rahimi, Khosrow; Zhong, Mingjiang; Mourran, Ahmed; Luebke, David R.; Nulwala, Hunaid B.; Möller, Martin; Matyjaszewski, KrzysztofCubosomes are micro- and nanoparticles with a bicontinuous cubic two-phase structure, reported for the self-assembly of low molecular weight surfactants, for example, lipids, but rarely formed by polymers. These objects are characterized by a maximum continuous interface and high interface to volume ratio, which makes them promising candidates for efficient adsorbents and host-guest applications. Here we demonstrate self-assembly to nanoscale cuboidal particles with a bicontinuous cubic structure by amphiphilic poly(ionic liquid) diblock copolymers, poly(acrylic acid)-block-poly(4-vinylbenzyl)-3-butyl imidazolium bis(trifluoromethylsulfonyl)imide, in a mixture of tetrahydrofuran and water under optimized conditions. Structure determining parameters include polymer composition and concentration, temperature, and the variation of the solvent mixture. The formation of the cubosomes can be explained by the hierarchical interactions of the constituent components. The lattice structure of the block copolymers can be transferred to the shape of the particle as it is common for atomic and molecular faceted crystals.
- ItemReply to Ruhl and Craig: Assessing and governing extreme climate risks needs to be legitimate and democratic(Washington, DC : National Acad. of Sciences, 2022) Kemp, Luke; Xu, Chi; Depledge, Joanna; Ebi, Kristie L.; Gibbins, Goodwin; Kohler, Timothy A.; Rockström, Johan; Scheffer, Marten; Schellnhuber, Hans Joachim; Steffen, Will; Lenton, Timothy M.[No abstract available]
- 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.
- ItemOn-chip generation and dynamic piezo-optomechanical rotation of single photons([London] : Nature Publishing Group UK, 2022) Bühler, Dominik D.; Weiß, Matthias; Crespo-Poveda, Antonio; Nysten, Emeline D. S.; Finley, Jonathan J.; Müller, Kai; Santos, Paulo V.; de Lima Jr., Mauricio M.; Krenner, Hubert J.Integrated photonic circuits are key components for photonic quantum technologies and for the implementation of chip-based quantum devices. Future applications demand flexible architectures to overcome common limitations of many current devices, for instance the lack of tuneabilty or built-in quantum light sources. Here, we report on a dynamically reconfigurable integrated photonic circuit comprising integrated quantum dots (QDs), a Mach-Zehnder interferometer (MZI) and surface acoustic wave (SAW) transducers directly fabricated on a monolithic semiconductor platform. We demonstrate on-chip single photon generation by the QD and its sub-nanosecond dynamic on-chip control. Two independently applied SAWs piezo-optomechanically rotate the single photon in the MZI or spectrally modulate the QD emission wavelength. In the MZI, SAWs imprint a time-dependent optical phase and modulate the qubit rotation to the output superposition state. This enables dynamic single photon routing with frequencies exceeding one gigahertz. Finally, the combination of the dynamic single photon control and spectral tuning of the QD realizes wavelength multiplexing of the input photon state and demultiplexing it at the output. Our approach is scalable to multi-component integrated quantum photonic circuits and is compatible with hybrid photonic architectures and other key components for instance photonic resonators or on-chip detectors.
- ItemMetamaterial-enabled asymmetric negative refraction of GHz mechanical waves([London] : Nature Publishing Group UK, 2022) Zanotto, Simone; Biasiol, Giorgio; Santos, Paulo V.; Pitanti, AlessandroWave refraction at an interface between different materials is a basic yet fundamental phenomenon, transversal to several scientific realms – electromagnetism, gas and fluid acoustics, solid mechanics, and possibly also matter waves. Under specific circumstances, mostly enabled by structuration below the wavelength scale, i.e., through the metamaterial approach, waves undergo negative refraction, eventually enabling superlensing and transformation optics. However, presently known negative refraction systems are symmetric, in that they cannot distinguish between positive and negative angles of incidence. Exploiting a metamaterial with an asymmetric unit cell, we demonstrate that the aforementioned symmetry can be broken, ultimately relying on the specific shape of the Bloch mode isofrequency curves. Our study specialized upon a mechanical metamaterial operating at GHz frequency, which is by itself a building block for advanced technologies such as chip-scale hybrid optomechanical and electromechanical devices. However, the phenomenon is based on general wave theory concepts, and it applies to any frequency and time scale for any kind of linear waves, provided that a suitable shaping of the isofrequency contours is implemented.
- ItemEnhancing sub-bandgap external quantum efficiency by photomultiplication for narrowband organic near-infrared photodetectors([London] : Nature Publishing Group UK, 2021) Kublitski, Jonas; Fischer, Axel; Xing, Shen; Baisinger, Lukasz; Bittrich, Eva; Spoltore, Donato; Benduhn, Johannes; Vandewal, Koen; Leo, KarlDetection of electromagnetic signals for applications such as health, product quality monitoring or astronomy requires highly responsive and wavelength selective devices. Photomultiplication-type organic photodetectors have been shown to achieve high quantum efficiencies mainly in the visible range. Much less research has been focused on realizing near-infrared narrowband devices. Here, we demonstrate fully vacuum-processed narrow- and broadband photomultiplication-type organic photodetectors. Devices are based on enhanced hole injection leading to a maximum external quantum efficiency of almost 2000% at −10 V for the broadband device. The photomultiplicative effect is also observed in the charge-transfer state absorption region. By making use of an optical cavity device architecture, we enhance the charge-transfer response and demonstrate a wavelength tunable narrowband photomultiplication-type organic photodetector with external quantum efficiencies superior to those of pin-devices. The presented concept can further improve the performance of photodetectors based on the absorption of charge-transfer states, which were so far limited by the low external quantum efficiency provided by these devices.
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