Ultrafast charge carrier separation in Potassium-intercalated endohedral metallofullerene Sc3_3N@C80_{80} thin films

Molecular materials have emerged as highly tunable materials for photovoltaic and light-harvesting applications. The most severe challenge of this class of materials is the trapping of charge carriers in bound electron-hole pairs, which severely limits the free charge carrier generation. Here, we demonstrate a significant modification of the exciton dynamics of thin films of endohedral metallofullerene complexes upon alkali metal intercalation. For the exemplary case of Sc$_3$N@C$_{80}$ thin films, we show that potassium intercalation results in an additional relaxation channel for the optically excited charge-transfer excitons that prevents the trapping of excitons in a long-lived Frenkel exciton-like state. Instead, K intercalation leads to an ultrafast exciton dissociation coinciding most likely with the generation of free charge carriers. In this way, we propose alkali metal doping of molecular films as a novel approach to enhance the light to-charge carrier conversion efficiency in photovoltaic materials

Topological States on the Gold Surface

Gold surfaces host special electronic states that have been understood as a prototype of Shockley surface states (SSs). These SSs are commonly employed to benchmark the capability of angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling spectroscopy. We find that these Shockley SSs can be reinterpreted as topologically derived surface states (TDSSs) of a topological insulator (TI), a recently discovered quantum state. Based on band structure calculations, the Z2 topological invariant can be well defined to characterize the nontrivial features of gold that we detect by ARPES. The same TDSSs are also recognized on surfaces of other well-known noble metals (e.g., silver, copper, platinum, and palladium). Besides providing a new understanding of noble metal SSs, finding topological states on late transition metals provokes interesting questions on the role of topological effects in surface-related processes, such as adsorption and catalysis.Comment: 21 pages, 3 figure

Tailoring the ferromagnetic surface potential landscape by a templating two-dimensional metal-organic porous network

Two-dimensional metal-organic porous networks (2D-MOPNs) have been identified as versatile nanoarchitectures to tailor surface electronic and magnetic properties on noble metals. In this context, we propose a protocol to redecorate a ferromagnetic surface potential landscape using a 2D-MOPN. Ultrathin cobalt (Co) films grown on Au(111) exhibit a well-ordered surface triangular reconstruction. On the ferromagnetic surface, the adsorbed 2,4,6-tris(4-pyridyl)-1,3,5triazine (T4PT) molecules can coordinate with the native Co atoms to form a large-scale Co-T4PT porous network. The Co-T4PT network with periodic nanocavities serves as a templating layer to reshape the ferromagnetic surface potential. The subsequently deposited C60 molecules are steered by the network porous potential and the neighboring C60 interactions. The prototype of the ferromagnetic-supported 2D-MOPN is a promising template for the tailoring of molecular electronic and spin properties

Vertical bonding distances and interfacial band structure of PTCDA on a Sn-Ag surface alloy

Molecular materials enable a vast variety of functionalities for novel electronic and spintronic devices. The unique possibility to alter or substitute organic molecules or metallic substrates offers the opportunity to modify and optimize interfacial properties for almost any desired field of application. For this reason, we extend the successful approach to control molecular interfaces by surface alloying. We present a comprehensive characterization of the structural and electronic properties of the interface formed between the prototypical molecule PTCDA and a Sn-Ag surface alloy grown on an Ag(111) single crystal surface. We monitor the changes of adsorption height of the surface alloy atoms and electronic valence band structure upon adsorption of one layer of PTCDA using the normal incidence x-ray standing wave technique in combination with momentum-resolved photoelectron spectroscopy. We find that the vertical buckling and the surface band structure of the SnAg$_2$ surface alloy is not altered by the adsorption of one layer of PTCDA, in contrast to our recent study of PTCDA on a PbAg$_2$ surface alloy [Phys. Rev. Lett. 117, 096805 (2016)] . In addition, the vertical adsorption geometry of PTCDA and the interfacial energy level alignment indicate the absence of any chemical interaction between the molecule and the surface alloy. We attribute the different interactions at these PTCDA/surface alloy interfaces to the presence or absence of local $\sigma$-bonds between the PTCDA oxygen atoms and the surface atoms. Combining our findings with results from literature, we are able to propose an empiric rule for engineering the surface band structure of alloys by adsorption of organic molecules

Coherent and incoherent magnons induced by strong ultrafast demagnetization in thin permalloy films

Understanding spin dynamics on femto- and picosecond timescales offers new opportunities for faster and more efficient spintronic devices. Here, we experimentally investigate the coherent spin dynamics after ultrashort laser excitation by time-resolved magneto optical Kerr effect (TR-MOKE) in thin Ni80Fe20 films. We provide a detailed study of the magnetic field and pump fluence dependence of the coherent precessional dynamics. We show that the coherent precession lifetime increases with the applied external magnetic field which cannot be understood by viscous Gilbert damping of the coherent magnons. Instead, it can be explained by nonlinear magnon interactions and by the change in the fraction of incoherent magnons. This interpretation is in agreement with the observed trends of the coherent magnon amplitude and lifetime as a function of the exciting laser fluence. Our results provide a new insight into the magnetization relaxation processes in ferromagnetic thin films, which is of great importance for further spintronic applications.Comment: 8 pages, 7 figure

a route towards defined surface functionalization

We investigate the surface-catalyzed dissociation of the archetypal molecular switch azobenzene on the Cu(111) surface. Based on X-ray photoelectron spectroscopy, normal incidence X-ray standing waves and density functional theory calculations a detailed picture of the coverage-induced formation of phenyl nitrene from azobenzene is presented. Furthermore, a comparison to the azobenzene/Ag(111) interface provides insight into the driving force behind the dissociation on Cu(111). The quantitative decay of azobenzene paves the way for the creation of a defect free, covalently bonded monolayer. Our work suggests a route of surface functionalization via suitable azobenzene derivatives and the on surface synthesis concept, allowing for the creation of complex immobilized molecular systems

Equivalence of RABBITT and streaking delays in attosecond-time-resolved photoemission spectroscopy at solid surfaces

Gebauer A, Neb S, Enns W, Stadtmüller B, Aeschlimann M, Pfeiffer W. Equivalence of RABBITT and streaking delays in attosecond-time-resolved photoemission spectroscopy at solid surfaces. Applied Sciences. 2019;9(3): 592.The dynamics of the photoelectric effect in solid-state systems can be investigated via attosecond-time-resolved photoelectron spectroscopy. This article provides a comparison of delay information accessible by the two most important techniques, attosecond streaking spectroscopy and reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) at solid surfaces, respectively. The analysis is based on simulated time-resolved photoemission spectra obtained by solving the time-dependent Schrödinger equation in a single-active-electron approximation. We show a continuous transition from the few-cycle RABBITT regime to the streaking regime as two special cases of laser-assisted photoemission. The absolute delay times obtained by both methods agree with each other, within the uncertainty limits for kinetic energies >10 eV. Moreover, for kinetic energies >10 eV, both streaking delay time and RABBITT delay time coincide with the classical time of flight for an electron propagating from the emitter atom to the bulk-vacuum interface, with only small deviations of less than 4 as due to quantum mechanical interference effects