Search

We report anomalies observed in photoelectron spectroscopy measurements performed on α-(BEDT-TTF)2I3 crystals. In particular, above its metal-insulator transition temperature (T = 135 K), we observe the lack of a sharp Fermi edge in contradiction with the metallic transport properties exhibited by this quasi-bidimensional organic material. We interpret these unusual results as a signature of a one-dimensional electronic behavior confirmed by DFT band structure calculations. Using photoelectron spectroscopy we probe a Luttinger liquid with a large correlation parameter (α > 1) that we interpret to be caused by the chain-like electronic structure of α-(BEDT-TTF)2I3 surface doped by iodine defects. These new surface effects are inaccessible by bulk sensitive measurements of electronic transport techniques., We acknowledge A. Santander-Syro, M. Gabay and P. Auban- Senzier for fruitful discussions. Work in Spain was supported by the Spanish Ministerio de Econom a y Competitividad (Grants FIS2015-64886-C5-4-P and CTQ2015-64579-C3-3-P) and Generalitat de Catalunya (2017SGR1506, 2017SGR1289 and XRQTC). E.C. acknowledges support of the Spanish MINECO through the Severo Ochoa Centers of Excellence Program under Grant SEV-2015-0496. P.A. acknowledges support from the Maria de Maeztu Units of Excellence Program under Grant MDM-2017-0767.

The O 1s x-ray photoelectron spectroscopy spectrum for Al(111)/O at 300 K shows two components whose behavior as a function of time and variation of detection angle are consistent with either (a) a surface species represented by the higher binding-energy (BE) component and a subsurface species represented by the lower BE component, or (b) small close-packed oxygen islands with the interior atoms represented by the lower BE component and the perimeter atoms by the higher BE component. We have modeled both situations using ab initio Hartree-Fock wave functions for clusters of Al and O atoms. For an O atom in a threefold site, it was found that a below-surface position gave a higher O 1s BE than an above-surface position, incompatible with interpretation (a). This change in the O 1s BE could arise because the bond for O to Al may have a more covalent character when the O is below the surface than when it is above the surface. We present evidence consistent with this view. An O adatom island with all the O atoms in threefold sites gives calculated O 1s BE's which are significantly higher for the perimeter O atoms. Further, the results for an isolated O island without the Al substrate present also give higher BE¿s for the perimeter atoms. Both these results are consistent with interpretation (b). Published scanning-tunneling-microscopy data supports the suggestion that the chemisorbed state consists of small, close-packed islands, whereas the presence of two vibrational modes in high-resolution electron-energy-loss spectroscopy data has been interpreted as representing surface and subsurface oxygen atoms. In light of the present results, we suggest that a vibrational interpretation in terms of interior and perimeter adatoms should be considered.