2017, He, Hongkun, Rahimi, Khosrow, Zhong, Mingjiang, Mourran, Ahmed, Luebke, David R., Nulwala, Hunaid B., Möller, Martin, Matyjaszewski, Krzysztof

Cubosomes 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.

2021, Kublitski, Jonas, Fischer, Axel, Xing, Shen, Baisinger, Lukasz, Bittrich, Eva, Spoltore, Donato, Benduhn, Johannes, Vandewal, Koen, Leo, Karl

Detection 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.

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.

2022, Zanotto, Simone, Biasiol, Giorgio, Santos, Paulo V., Pitanti, Alessandro

Wave 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.

2021, Ruf, J.P., Paik, H., Schreiber, N.J., Nair, H.P., Miao, L., Kawasaki, J.K., Nelson, J.N., Faeth, B.D., Lee, Y., Goodge, B.H., Pamuk, B., Fennie, C.J., Kourkoutis, L.F., Schlom, D.G., Shen, K.M.

Superconductivity is among the most fascinating and well-studied quantum states of matter. Despite over 100 years of research, a detailed understanding of how features of the normal-state electronic structure determine superconducting properties has remained elusive. For instance, the ability to deterministically enhance the superconducting transition temperature by design, rather than by serendipity, has been a long sought-after goal in condensed matter physics and materials science, but achieving this objective may require new tools, techniques and approaches. Here, we report the transmutation of a normal metal into a superconductor through the application of epitaxial strain. We demonstrate that synthesizing RuO2 thin films on (110)-oriented TiO2 substrates enhances the density of states near the Fermi level, which stabilizes superconductivity under strain, and suggests that a promising strategy to create new transition-metal superconductors is to apply judiciously chosen anisotropic strains that redistribute carriers within the low-energy manifold of d orbitals.

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.

2021, Tschernig, Konrad, Jimenez-Galán, Álvaro, Christodoulides, Demetrios N., Ivanov, Misha, Busch, Kurt, Bandres, Miguel A., Perez-Leija, Armando

Topological insulators combine insulating properties in the bulk with scattering-free transport along edges, supporting dissipationless unidirectional energy and information flow even in the presence of defects and disorder. The feasibility of engineering quantum Hamiltonians with photonic tools, combined with the availability of entangled photons, raises the intriguing possibility of employing topologically protected entangled states in optical quantum computing and information processing. However, while two-photon states built as a product of two topologically protected single-photon states inherit full protection from their single-photon “parents”, a high degree of non-separability may lead to rapid deterioration of the two-photon states after propagation through disorder. In this work, we identify physical mechanisms which contribute to the vulnerability of entangled states in topological photonic lattices. Further, we show that in order to maximize entanglement without sacrificing topological protection, the joint spectral correlation map of two-photon states must fit inside a well-defined topological window of protection.

2019, Scotti, A., Bochenek, S., Brugnoni, M., Fernandez-Rodriguez, M.A., Schulte, M.F., Houston, J.E., Gelissen, A.P.H., Potemkin, I.I., Isa, L., Richtering, W.

Microgels are solvent-swollen nano- and microparticles that show prevalent colloidal-like behavior despite their polymeric nature. Here we study ultra-low crosslinked poly(N-isopropylacrylamide) microgels (ULC), which can behave like colloids or flexible polymers depending on dimensionality, compression or other external stimuli. Small-angle neutron scattering shows that the structure of the ULC microgels in bulk aqueous solution is characterized by a density profile that decays smoothly from the center to a fuzzy surface. Their phase behavior and rheological properties are those of soft colloids. However, when these microgels are confined at an oil-water interface, their behavior resembles that of flexible macromolecules. Once monolayers of ultra-low crosslinked microgels are compressed, deposited on solid substrate and studied with atomic-force microscopy, a concentration-dependent topography is observed. Depending on the compression, these microgels can behave as flexible polymers, covering the substrate with a uniform film, or as colloidal microgels leading to a monolayer of particles.

2021, Ayuso, David, Ordonez, Andres F., Decleva, Piero, Ivanov, Misha, Smirnova, Olga

Structured light, which exhibits nontrivial intensity, phase, and polarization patterns in space, has key applications ranging from imaging and 3D micromanipulation to classical and quantum communication. However, to date, its application to molecular chirality has been limited by the weakness of magnetic interactions. Here we structure light’s local handedness in space to introduce and realize an enantio-sensitive interferometer for efficient chiral recognition without magnetic interactions, which can be seen as an enantio-sensitive version of Young’s double slit experiment. Upon interaction with isotropic chiral media, such chirality-structured light effectively creates chiral emitters of opposite handedness, located at different positions in space. We show that if the distribution of light’s handedness breaks left-right symmetry, the interference of these chiral emitters leads to unidirectional bending of the emitted light, in opposite directions in media of opposite handedness, even if the number of the left-handed and right-handed emitters excited in the medium is exactly the same. Our work introduces the concepts of polarization of chirality and chirality-polarized light, exposes the immense potential of sculpting light’s local chirality, and offers novel opportunities for efficient chiral discrimination, enantio-sensitive optical molecular fingerprinting and imaging on ultrafast time scales.

2018, Richter, Clemens, Hollas, Daniel, Saak, Clara-Magdalena, Förstel, Marko, Miteva, Tsveta, Mucke, Melanie, Björneholm, Olle, Sisourat, Nicolas, Slavíček, Petr, Hergenhahn, Uwe

Intermolecular Coulombic decay (ICD) is a ubiquitous relaxation channel of electronically excited states in weakly bound systems, ranging from dimers to liquids. As it is driven by electron correlation, it was assumed that it will dominate over more established energy loss mechanisms, for example fluorescence. Here, we use electron–electron coincidence spectroscopy to determine the efficiency of the ICD process after 2a1 ionization in water clusters. We show that this efficiency is surprisingly low for small water clusters and that it gradually increases to 40–50% for clusters with hundreds of water units. Ab initio molecular dynamics simulations reveal that proton transfer between neighboring water molecules proceeds on the same timescale as ICD and leads to a configuration in which the ICD channel is closed. This conclusion is further supported by experimental results from deuterated water. Combining experiment and theory, we infer an intrinsic ICD lifetime of 12–52 fs for small water clusters.