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- ItemPatterning and control of the nanostructure in plasma thin films with acoustic waves: mechanical vs. electrical polarization effects(Cambridge : RSC Publ., 2021) García-Valenzuela, Aurelio; Fakhfouri, Armaghan; Oliva-Ramírez, Manuel; Rico-Gavira, Victor; Rojas, Teresa Cristina; Alvarez, Rafael; Menzel, Siegfried B.; Palmero, Alberto; Winkler, Andreas; González-Elipe, Agustín R.Nanostructuration and 2D patterning of thin films are common strategies to fabricate biomimetic surfaces and components for microfluidic, microelectronic or photonic applications. This work presents the fundamentals of a surface nanotechnology procedure for laterally tailoring the nanostructure and crystalline structure of thin films that are plasma deposited onto acoustically excited piezoelectric substrates. Using magnetron sputtering as plasma technique and TiO2 as case example, it is demonstrated that the deposited films depict a sub-millimetre 2D pattern that, characterized by large lateral differences in nanostructure, density (up to 50%), thickness, and physical properties between porous and dense zones, reproduces the wave features distribution of the generated acoustic waves (AW). Simulation modelling of the AW propagation and deposition experiments carried out without plasma and under alternative experimental conditions reveal that patterning is not driven by the collision of ad-species with mechanically excited lattice atoms of the substrate, but emerges from their interaction with plasma sheath ions locally accelerated by the AW-induced electrical polarization field developed at the substrate surface and growing film. The possibilities of the AW activation as a general approach for the tailored control of nanostructure, pattern size, and properties of thin films are demonstrated through the systematic variation of deposition conditions and the adjustment of AW operating parameters.
- ItemErratum: Exploring the 3D structure and defects of a self-assembled gold mesocrystal by coherent X-ray diffraction imaging (Nanoscale (2021) DOI: 10.1039/D1NR01806J)(Cambridge : RSC Publ., 2021) Carnis, Jerome; Kirner, Felizitas; Lapkin, Dmitry; Sturm, Sebastian; Kim, Young Yong; Baburin, Igor A.; Khubbutdinov, Ruslan; Ignatenko, Alexandr; Iashina, Ekaterina; Mistonov, Alexander; Steegemans, Tristan; Wieck, Thomas; Gemming, Thomas; Lubk, Axel; Lazarev, Sergey; Sprung, Michael; Vartanyants, Ivan A.; Sturm, Elena V.Correction for ‘Exploring the 3D structure and defects of a self-assembled gold mesocrystal by coherent X-ray diffraction imaging’ by Jerome Carnis et al., Nanoscale, 2021, DOI: 10.1039/D1NR01806J.
- ItemColloidal PbS nanoplatelets synthesized via cation exchange for electronic applications(Cambridge : RSC Publ., 2019) Sonntag, Luisa; Shamraienko, Volodymyr; Fan, Xuelin; Samadi Khoshkhoo, Mahdi; Kneppe, David; Koitzsch, Andreas; Gemming, Thomas; Hiekel, Karl; Leo, Karl; Lesnyak, Vladimir; Eychmüller, AlexanderIn this work, we present a new synthetic approach to colloidal PbS nanoplatelets (NPLs) utilizing a cation exchange (CE) strategy starting from CuS NPLs synthesized via the hot-injection method. Whereas the thickness of the resulting CuS NPLs was fixed at approx. 5 nm, the lateral size could be tuned by varying the reaction conditions, such as time from 6 to 16 h, the reaction temperature (120 °C, 140 °C), and the amount of copper precursor. In a second step, Cu+ cations were replaced with Pb2+ ions within the crystal lattice via CE. While the shape and the size of parental CuS platelets were preserved, the crystal structure was rearranged from hexagonal covellite to PbS galena, accompanied by the fragmentation of the monocrystalline phase into polycrystalline one. Afterwards a halide mediated ligand exchange (LE) was carried out in order to remove insulating oleic acid residues from the PbS NPL surface and to form stable dispersions in polar organic solvents enabling thin-film fabrication. Both CE and LE processes were monitored by several characterization techniques. Furthermore, we measured the electrical conductivity of the resulting PbS NPL-based films before and after LE and compared the processing in ambient to inert atmosphere. Finally, we fabricated field-effect transistors with an on/off ratio of up to 60 and linear charge carrier mobility for holes of 0.02 cm2 V−1 s−1.
- ItemHuman spermbots for patient-representative 3D ovarian cancer cell treatment(Cambridge : RSC Publ., 2020) Xu, Haifeng; Medina-Sánchez, Mariana; Zhang, Wunan; Seaton, Melanie P. H.; Brison, Daniel R.; Edmondson, Richard J.; Taylor, Stephen S.; Nelson, Louisa; Zeng, Kang; Bagley, Steven; Ribeiro, Carla; Restrepo, Lina P.; Lucena, Elkin; Schmidt, Christine K.; Schmidt, Oliver G.Cellular micromotors are attractive for locally delivering high concentrations of drug, and targeting hard-to-reach disease sites such as cervical cancer and early ovarian cancer lesions by non-invasive means. Spermatozoa are highly efficient micromotors perfectly adapted to traveling up the female reproductive system. Indeed, bovine sperm-based micromotors have shown potential to carry drugs toward gynecological cancers. However, due to major differences in the molecular make-up of bovine and human sperm, a key translational bottleneck for bringing this technology closer to the clinic is to transfer this concept to human material. Here, we successfully load human sperm with Doxorubicin (DOX) and perform treatment of 3D cervical cancer and patient-representative ovarian cancer cell cultures, resulting in strong anticancer cell effects. Additionally, we define the subcellular localization of the chemotherapeutic drug within human sperm, using high-resolution optical microscopy. We also assess drug effects on sperm motility and viability over time, employing sperm samples from healthy donors as well as assisted reproduction patients. Finally, we demonstrate guidance and release of human drug-loaded sperm onto cancer tissues using magnetic microcaps, and show the sperm microcap loaded with a second anticancer drug, camptothecin (CPT), which unlike DOX is not suitable for directly loading into sperm due to its hydrophobic nature. This co-drug delivery approach opens up novel targeted combinatorial drug therapies for future applications. © 2020 The Royal Society of Chemistry.
- ItemTailoring the stoichiometry of C3N4 nanosheets under electron beam irradiation(Cambridge : RSC Publ., 2021) Mendes, Rafael G.; Ta, Huy Q.; Yang, Xiaoqin; Bachmatiuk, Alicja; Praus, Petr; Mamakhel, Aref; Iversen, Bo B.; Su, Ren; Gemming, Thomas; Rümmeli, Mark H.Two-dimensional polymeric graphitic carbon nitride (g-C3N4) is a low-cost material with versatile properties that can be enhanced by the introduction of dopant atoms and by changing the degree of polymerization/stoichiometry, which offers significant benefits for numerous applications. Herein, we investigate the stability of g-C3N4 under electron beam irradiation inside a transmission electron microscope operating at different electron acceleration voltages. Our findings indicate that the degradation of g-C3N4 occurs with N species preferentially removed over C species. However, the precise nitrogen group from which N is removed from g-C3N4 (C–N–C, [double bond, length as m-dash]NH or –NH2) is unclear. Moreover, the rate of degradation increases with decreasing electron acceleration voltage, suggesting that inelastic scattering events (radiolysis) dominate over elastic events (knock-on damage). The rate of degradation by removing N atoms is also sensitive to the current density. Hence, we demonstrate that both the electron acceleration voltage and the current density are parameters with which one can use to control the stoichiometry. Moreover, as N species were preferentially removed, the d-spacing of the carbon nitride structure increased. These findings provide a deeper understanding of g-C3N4.
- ItemEndohedral metal-nitride cluster ordering in metallofullerene-NiII(OEP) complexes and crystals : A theoretical study(Cambridge : RSC Publ., 2019) Dubrovin, Vasilii; Gan, Li-Hua; Büchner, Bernd; Popov, Alexey A.; Avdoshenko, Stanislav M.The ordering of endohedral clusterfullerenes Sc3N@C80 and YSc2N@C80 co-crystallized with Ni(OEP) and isolated complexes with Ni(OEP) have been investigated theoretically. Having used multiple orientations of M3N clusters inside the cages with Fibonacci sampling, we describe the effect of intermolecular interactions on the orientation of the endohedral cluster. © the Owner Societies.
- ItemMixed dysprosium-lanthanide nitride clusterfullerenes DyM2N@C80-: I h and Dy2MN@C80- i h (M = Gd, Er, Tm, and Lu): Synthesis, molecular structure, and quantum motion of the endohedral nitrogen atom(Cambridge : RSC Publ., 2019) Schlesier, C.; Liu, F.; Dubrovin, V.; Spree, L.; Büchner, B.; Avdoshenko, S.M.; Popov, A.A.Systematic exploration of the synthesis of mixed-metal Dy-M nitride clusterfullerenes (NCFs, M = Gd, Er, Tm, Lu) is performed, and the impact of the second metal on the relative yield is evaluated. We demonstrate that the ionic radius of the metal appears to be the main factor allowing explanation of the relative yields in Dy-M mixed-metal systems with M = Sc, Lu, Er, and Gd. At the same time, Dy-Tm NCFs show anomalously low yields, which is not consistent with the relatively small ionic radius of Tm3+ but can be explained by the high third ionization potential of Tm. Complete separation of Dy-Gd and Dy-Er, as well as partial separation of Dy-Lu M3N@C80 nitride clusterfullerenes, is accomplished by recycling HPLC. The molecular structures of DyGd2N@C80 and DyEr2N@C80 are analyzed by means of single-crystal X-ray diffraction. A remarkable ordering of mixed-metal nitride clusters is found despite similar size and electronic properties of the metals. Possible pyramidalization of the nitride clusters in these and other nitride clusterfullerenes is critically analyzed with the help of DFT calculations and reconstruction of the nitrogen inversion barrier in M3N@C80 molecules is performed. Although a double-well potential with a pyramidal cluster structure is found to be common for most of them, the small size of the inversion barrier often leads to an apparent planar structure of the cluster. This situation is found for those M3N@C80 molecules in which the energy of the lowest vibrational level exceeds that of the inversion barrier, including Dy3N@C80 and DyEr2N@C80. The genuine pyramidal structure can be observed by X-ray diffraction only when the lowest vibrational level is below the inversion barrier, such as those found in Gd3N@C80 and DyGd2N@C80. The quantum nature of molecular vibrations becomes especially apparent when the size of the inversion barrier is comparable to the energy of the lowest vibrational levels.
- ItemInfluence of 4f filling on electronic and magnetic properties of rare earth-Au surface compounds(Cambridge : RSC Publ., 2020) Fernandez, L.; Blanco-Rey, M.; Castrillo-Bodero, R.; Ilyn, M.; Ali, K.; Turco, E.; Corso, M.; Ormaza, M.; Gargiani, P.; Valbuena, M.A.; Mugarza, A.; Moras, P.; Sheverdyaeva, P.M.; Kundu, Asish K.; Jugovac, M.; Laubschat, C.; Ortega, J.E.; Schiller, F.One-atom-thick rare-earth/noble metal (RE-NM) compounds are attractive materials to investigate two-dimensional magnetism, since they are easy to synthesize into a common RE-NM2 structure with high crystal perfection. Here we perform a comparative study of the GdAu2, HoAu2, and YbAu2 monolayer compounds grown on Au(111). We find the same atomic lattice quality and moiré superlattice periodicity in the three cases, but different electronic properties and magnetism. The YbAu2 monolayer reveals the characteristic electronic signatures of a mixed-valence configuration in the Yb atom. In contrast, GdAu2 and HoAu2 show the trivalent character of the rare-earth and ferromagnetic transitions below 22 K. Yet, the GdAu2 monolayer has an in-plane magnetic easy-axis, versus the out-of-plane one in HoAu2. The electronic bands of the two trivalent compounds are very similar, while the divalent YbAu2 monolayer exhibits different band features. In the latter, a strong 4f-5d hybridization is manifested in neatly resolved avoided crossings near the Fermi level. First principles theory points to a residual presence of empty 4f states, explaining the fluctuating valence of Yb in the YbAu2 monolayer. © The Royal Society of Chemistry.
- ItemDirect imaging of nanoscale field-driven domain wall oscillations in Landau structures(Cambridge : RSC Publ., 2022) Singh, Balram; Ravishankar, Rachappa; Otálora, Jorge A.; Soldatov, Ivan; Schäfer, Rudolf; Karnaushenko, Daniil; Neu, Volker; Schmidt, Oliver G.Linear oscillatory motion of domain walls (DWs) in the kHz and MHz regime is crucial when realizing precise magnetic field sensors such as giant magnetoimpedance devices. Numerous magnetically active defects lead to pinning of the DWs during their motion, affecting the overall behavior. Thus, the direct monitoring of the domain wall's oscillatory behavior is an important step to comprehend the underlying micromagnetic processes and to improve the magnetoresistive performance of these devices. Here, we report an imaging approach to investigate such DW dynamics with nanoscale spatial resolution employing conventional table-top microscopy techniques. Time-averaged magnetic force microscopy and Kerr imaging methods are applied to quantify the DW oscillations in Ni81Fe19 rectangular structures with Landau domain configuration and are complemented by numeric micromagnetic simulations. We study the oscillation amplitude as a function of external magnetic field strength, frequency, magnetic structure size, thickness and anisotropy and understand the excited DW behavior as a forced damped harmonic oscillator with restoring force being influenced by the geometry, thickness, and anisotropy of the Ni81Fe19 structure. This approach offers new possibilities for the analysis of DW motion at elevated frequencies and at a spatial resolution of well below 100 nm in various branches of nanomagnetism.
- ItemMg3(Bi,Sb)2 single crystals towards high thermoelectric performance(Cambridge : RSC Publ., 2020) Pan, Yu; Yao, Mengyu; Hong, Xiaochen; Zhu, Yifan; Fan, Fengren; Imasato, Kazuki; He, Yangkun; Hess, Christian; Fink, Jörg; Yang, Jiong; Büchner, Bernd; Fu, Chenguang; Snyder, G. Jeffrey; Felser, ClaudiaThe rapid growth of the thermoelectric cooler market makes the development of novel room temperature thermoelectric materials of great importance. Ternary n-type Mg3(Bi,Sb)2 alloys are promising alternatives to the state-of-the-art Bi2(Te,Se)3 alloys but grain boundary resistance is the most important limitation. n-type Mg3(Bi,Sb)2 single crystals with negligible grain boundaries are expected to have particularly high zT but have rarely been realized due to the demanding Mg-rich growth conditions required. Here, we report, for the first time, the thermoelectric properties of n-type Mg3(Bi,Sb)2 alloyed single crystals grown by a one-step Mg-flux method using sealed tantalum tubes. High weighted mobility ∼140 cm2 V−1 s−1 and a high zT of 0.82 at 315 K are achieved in Y-doped Mg3Bi1.25Sb0.75 single crystals. Through both experimental angle-resolved photoemission spectroscopy and theoretical calculations, we denote the origin of the high thermoelectric performance from a point of view of band widening effect and electronegativity, as well as the necessity to form high Bi/Sb ratio ternary Mg3(Bi,Sb)2 alloys. The present work paves the way for further development of Mg3(Bi,Sb)2 for near room temperature thermoelectric applications.