• Control of the dipole layer of polar organic molecules adsorbed on metal surfaces via different charge-transfer channels

      Lin, Meng-Kai; Nakayama, Yasuo; Zhuang, Ying-Jie; Su, Kai-Jun; Wang, Chin-Yung; Pi, Tun-Wen; Metz, Sebastian; Papadopoulos, Theodoros A.; Chiang, Tai-Chang; Ishii, Hisao; et al. (American Physical Society, 2017-02-17)
      Organic molecules with a permanent electric dipole moment have been widely used as a template for further growth of molecular layers in device structures. Key properties of the resulting organic films such as energy level alignment (ELA), work function, and injection/collection barrier are linked to the magnitude and direction of the dipole moment at the interface. Using angle-resolved photoemission spectroscopy (ARPES), we have systematically investigated the coverage-dependent work function and spectral line shapes of occupied molecular energy states (MES) of chloroaluminium-phthalocyanine (ClAlPc) grown on Ag(111). We demonstrate that the dipole orientation of the first ClAlPc layer can be controlled by adjusting the deposition rate and post annealing conditions; the ELA at the interface differs by ~0.4 eV between the Cl-up and -down configurations of the adsorbed ClAlPc molecules. These observations are rationalized by density-functional-theory (DFT) calculations based on a realistic model of the ClAlPc/Ag(111) interface, which reveal that the different orientations of the ClAlPc dipole layer lead to different charge-transfer channels between the adsorbed ClAlPc and Ag(111) substrate. Our findings provide a useful framework towards method development for ELA tuning.
    • Trion formation in a two-dimensional hole-doped electron gas

      Spink, Graham G.; López Ríos, Pablo; Drummond, Neil D.; Needs, Richard J.; University of Cambridge; University of Chester; Lancaster University (American Physical Society, 2016-07-22)
      The interaction between a single hole and a two-dimensional, paramagnetic, homogeneous electron gas is studied using diffusion quantum Monte Carlo simulations. Electron-hole relaxation energies, pair-correlation functions, and electron-hole center-of-mass momentum densities are reported for a range of electron-hole mass ratios and electron densities. We find numerical evidence of a crossover from a collective excitonic state to a trion-dominated state in a density range in agreement with that found in recent experiments on quantum-well heterostructures.