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- Item(BB)-Carboryne Complex of Ruthenium: Synthesis by Double B-H Activation at a Single Metal Center(Washington, DC : ACS Publications, 2016) Eleazer, Bennett J.; Smith, Mark D.; Popov, Alexey A.; Peryshkov, Dmitry V.The first example of a transition metal (BB)-carboryne complex containing two boron atoms of the icosahedral cage connected to a single exohedral metal center (POBBOP)Ru(CO)2 (POBBOP = 1,7-OP(i-Pr)2-2,6-dehydro-m-carborane) was synthesized by double B-H activation within the strained m-carboranyl pincer framework. Theoretical calculations revealed that the unique three-membered (BB)>Ru metalacycle is formed by two bent B-Ru σ-bonds with the concomitant increase of the bond order between the two metalated boron atoms. The reactivity of the highly strained electron-rich (BB)-carboryne fragment with small molecules was probed by reactions with electrophiles. The carboryne-carboranyl transformations reported herein represent a new mode of cooperative metal-ligand reactivity of boron-based complexes.
- ItemExtremely large magnetoresistance from electron-hole compensation in the nodal-loop semimetal ZrP2(Woodbury, NY : Inst., 2021) Bannies, J.; Razzoli, E.; Michiardi, M.; Kung, H.-H.; Elfimov, I.S.; Yao, M.; Fedorov, A.; Fink, J.; Jozwiak, C.; Bostwick, A.; Rotenberg, E.; Damascelli, A.; Felser, C.Several early transition metal dipnictides (TMDPs) have been found to host topological semimetal states and exhibit large magnetoresistance (MR). In this paper, we use angle-resolved photoemission spectroscopy (ARPES) and magnetotransport to study the electronic properties of a TMDP ZrP2. We find that ZrP2 exhibits an extremely large and unsaturated MR of up to 40 000% at 2 K, which originates from an almost perfect electron-hole (e-h) compensation. Our band structure calculations further show that ZrP2 hosts a topological nodal loop in proximity to the Fermi level. Based on the ARPES measurements, we confirm the results of our calculations and determine the surface band structure. This paper establishes ZrP2 as a platform to investigate near-perfect e-h compensation and its interplay with topological band structures.
- ItemSpin pumping at interfaces with ferro- and paramagnetic Fe60Al40films acting as spin source and spin sink(Melville, NY : American Inst. of Physics, 2022) Strusch, T.; Lenz, K.; Meckenstock, R.; Bali, R.; Ehrler, J.; Lindner, J.; Fassbender, J.; Farle, M.; Potzger, K.; Semisalova, A.We present a study of spin pumping efficiency and determine the spin mixing conductance and spin diffusion length in thin bilayer films based on 3d transition metal alloy Fe60Al40. Due to its magnetostructural phase transition, Fe60Al40 can be utilized as a ferromagnetic (FM) or paramagnetic (PM) material at the same temperature depending on its structural order; thus a thin Fe60Al40 film can act as a spin source or a spin sink when interfaced with a paramagnet or a ferromagnet, respectively. Ferromagnetic resonance measurements were performed in a frequency range of 5-35 GHz on bilayer films composed of FM-Fe60Al40/Pd and PM-Fe60Al40/Ni80Fe20 (permalloy). The increase in damping with the thickness of the paramagnetic layer was interpreted as a result of spin pumping into the paramagnet. We determine the spin mixing conductance g P d ↑↓ = (3.8 ± 0.5) × 10 18 m - 2 at the FM-Fe60Al40/Pd interface and the spin diffusion length λ P d = 9.1 ± 2.0 nm in Pd. For the PM-Fe60Al40/permalloy interface, we find a spin mixing conductance g F e A l ↑↓ = (2.1 ± 0.2) × 10 18 m - 2 and a spin diffusion length λ F e A l = 11.9 ± 0.2 nm for PM-Fe60Al40. The demonstrated bi-functionality of the Fe60Al40 alloy in spin pumping structures may be promising for spintronic applications.
- ItemTunable charge transfer properties in metal-phthalocyanine heterojunctions(Cambridge : Royal Society of Chemistry, 2016) Siles, P.F.; Hahn, T.; Salvan, G.; Knupfer, M.; Zhu, F.; Zahn, D.R.T.; Schmidt, O.G.Organic materials such as phthalocyanine-based systems present a great potential for organic device applications due to the possibility of integrating films of different organic materials to create organic heterostructures which combine the electrical capabilities of each material. This opens the possibility to precisely engineer and tune new electrical properties. In particular, similar transition metal phthalocyanines demonstrate hybridization and charge transfer properties which could lead to interesting physical phenomena. Although, when considering device dimensions, a better understanding and control of the tuning of the transport properties still remain in the focus of research. Here, by employing conductive atomic force microscopy techniques, we provide an insight about the nanoscale electrical properties and transport mechanisms of MnPc and fluorinated phthalocyanines such as F16CuPc and F16CoPc. We report a transition from typical diode-like transport mechanisms for pure MnPc thin films to space-charge-limited current transport regime (SCLC) for Pc-based heterostructures. The controlled addition of fluorinated phthalocyanine also provides highly uniform and symmetric-polarized transport characteristics with conductance enhancements up to two orders of magnitude depending on the polarization. We present a method to spatially map the mobility of the MnPc/F16CuPc structures with a nanoscale resolution and provide theoretical calculations to support our experimental findings. This well-controlled nanoscale tuning of the electrical properties for metal transition phthalocyanine junctions stands as key step for future phthalocyanine-based electronic devices, where the low dimension charge transfer, mediated by transition metal atoms could be intrinsically linked to a transfer of magnetic moment or spin.
- ItemSubstrate Developments for the Chemical Vapor Deposition Synthesis of Graphene(Weinheim : Wiley-VCH Verlag, 2020) Shi, Q.; Tokarska, K.; Ta, H.Q.; Yang, X.; Liu, Y.; Ullah, S.; Liu, L.; Trzebicka, B.; Bachmatiuk, A.; Sun, J.; Fu, L.; Liu, Z.; Rümmeli, M.H.Since the isolation of graphene and numerous demonstrations of its unique properties, the expectations for this material to be implemented in many future commercial applications have been enormous. However, to date, challenges still remain. One of the key challenges is the fabrication of graphene in a manner that satisfies processing requirements. While transfer of graphene can be used, this tends to damage or contaminate it, which degrades its performance. Hence, there is an important drive to grow graphene directly over a number of technologically important materials, viz., different substrate materials, so as to avoid the need for transfer. One of the more successful approaches to synthesis graphene is chemical vapor deposition (CVD), which is well established. Historically, transition metal substrates are used due to their catalytic properties. However, in recent years this has developed to include many nonmetal substrate systems. Moreover, both solid and molten substrate forms have also been demonstrated. In addition, the current trend to progress flexible devices has spurred interest in graphene growth directly over flexible materials surfaces. All these aspects are presented in this review which presents the developments in available substrates for graphene fabrication by CVD, with a focus primarily on large area graphene.
- ItemThe interplay between spin densities and magnetic superexchange interactions: Case studies of monoand trinuclear bis(oxamato)-type complexes(Frankfurt am Main : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017) Aliabadi, A.; Büchner, B.; Kataev, V.; Rüffer, T.For future molecular spintronic applications the possibility to modify and tailor the magnetic properties of transition-metal complexes is very promising. One of such possibilities is given by the countless derivatization offered by carbon chemistry. They allow for altering chemical structures and, in doing so, to tune magnetic properties of molecular spin-carrying compounds. With emphasis on the interplay of the spin density distribution of mononuclear and magnetic superexchange couplings of trinuclear bis(oxamato)- type complexes we review on efforts on such magneto-structural correlations.
- ItemFermi surface nesting in several transition metal dichalcogenides(Milton Park : Taylor & Francis, 2008) Inosov, D.S.; Zabolotnyy, V.B.; Evtushinsky, D.V.; Kordyuk, A.A.; Büchner, B.; Follath, R.; Berger, H.; Borisenko, S.V.By means of high-resolution angle-resolved photoelectron spectroscopy (ARPES), we have studied the fermiology of 2H transition metal dichalcogenide polytypes TaSe2, NbSe2 and Cu0.2NbS 2. The tight-binding model of the electronic structure, extracted from ARPES spectra for all three compounds, was used to calculate the Lindhard function (bare spin susceptibility), which reflects the propensity to charge density wave (CDW) instabilities observed in TaSe2 and NbSe 2. We show that though the Fermi surfaces of all three compounds possess an incommensurate nesting vector in the close vicinity of the CDW wave vector, the nesting and ordering wave vectors do not exactly coincide, and there is no direct relationship between the magnitude of the susceptibility at the nesting vector and the CDW transition temperature. The nesting vector persists across the incommensurate CDW transition in TaSe2 as a function of temperature despite the observable variations of the Fermi surface geometry in this temperature range. In Cu0.2NbS2, the nesting vector is present despite different doping levels, which leads us to expect a possible enhancement of the CDW instability with Cu intercalation in the Cu xNbS2 family of materials.
- ItemNonlocal dielectric function and nested dark excitons in MoS2(London : Nature Publishing Group, 2019) Koitzsch, A.; Pawlik, A.-S.; Habenicht, C.; Klaproth, T.; Schuster, R.; Büchner, B.; Knupfer, M.Their exceptional optical properties are a driving force for the persistent interest in atomically thin transition metal dichalcogenides such as MoS2. The optical response is dominated by excitons. Apart from the bright excitons, which directly couple to light, it has been realized that dark excitons, where photon absorption or emission is inhibited by the spin state or momentum mismatch, are decisive for many optical properties. However, in particular the momentum dependence is difficult to assess experimentally and often remains elusive or is investigated by indirect means. Here we study the momentum dependent electronic structure experimentally and theoretically. We use angle-resolved photoemission as a one-particle probe of the occupied valence band structure and electron energy loss spectroscopy as a two-particle probe of electronic transitions across the gap to benchmark a single-particle model of the dielectric function ϵ(q, ω) against momentum dependent experimental measurements. This ansatz captures key aspects of the data surprisingly well. In particular, the energy region where substantial nesting occurs, which is at the origin of the strong light–matter interaction of thin transition metal dichalcogenides and crucial for the prominent C-exciton, is described well and spans a more complex exciton landscape than previously anticipated. Its local maxima in (q≠0,ω) space can be considered as dark excitons and might be relevant for higher order optical processes. Our study may lead to a more complete understanding of the optical properties of atomically thin transition metal dichalcogenides.
- ItemFate of density waves in the presence of a higher-order van Hove singularity(College Park, MD : APS, 2023) Zervou, Alkistis; Efremov, Dmitry V.; Betouras, Joseph J.Topological transitions in electronic band structures, resulting in van Hove singularities in the density of states, can considerably affect various types of orderings in quantum materials. Regular topological transitions (of neck formation or collapse) lead to a logarithmic divergence of the electronic density of states (DOS) as a function of energy in two dimensions. In addition to the regular van Hove singularities, there are higher-order van Hove singularities (HOVHS) with a power-law divergence in DOS. By employing renormalization group techniques, we study the fate of a spin-density wave phase formed by nested parts of the Fermi surface, when a HOVHS appears in parallel. We find that the phase formation can be boosted by the presence of the singularity, with the critical temperature increasing by orders of magnitude, under certain conditions. We discuss possible applications of our findings to a range of quantum materials such as Sr3Ru2O7, Sr2RuO4, and transition metal dichalcogenides.