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Title: Orbital Character Effects in the Photon Energy and Polarization Dependence of Pure C60 Photoemission

Abstract

We report that recent direct experimental observation of multiple highly dispersive C60 valence bands has allowed for a detailed analysis of the unusual photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C60 molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C60 band manifolds which allow for a more precise determination of the orbital character within the third highest occupied molecular orbital (HOMO-2). In conclusion, our observations and analysis provide important considerations for the connection between molecular and crystalline C60 electronic structure, past and future band structure studies, and for increasingly popular C60 electronic device applications, especially those making use of heterostructures.

Authors:
 [1]; ORCiD logo [2];  [3];  [2];  [1];  [4]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. California State Univ. (CalState), Long Beach, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
California State Univ. (CalState), Long Beach, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1782491
Alternate Identifier(s):
OSTI ID: 1581081; OSTI ID: 1595116
Grant/Contract Number:  
SC0018154; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; C60; angle resolved photoemission spectroscopy; polarization-dependent photoemission; molecular solid; orbital character; photoemission; light; energy; polarization; oscillation; C60, angle resolved photoemission spectroscopy, polarization-dependent photoemission, molecular solid, orbital character

Citation Formats

Latzke, Drew W., Ojeda-Aristizabal, Claudia, Denlinger, Jonathan D., Reno, Ryan, Zettl, Alex, and Lanzara, Alessandra. Orbital Character Effects in the Photon Energy and Polarization Dependence of Pure C60 Photoemission. United States: N. p., 2019. Web. doi:10.1021/acsnano.9b04536.
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Latzke, Drew W., Ojeda-Aristizabal, Claudia, Denlinger, Jonathan D., Reno, Ryan, Zettl, Alex, & Lanzara, Alessandra. Orbital Character Effects in the Photon Energy and Polarization Dependence of Pure C60 Photoemission. United States. https://doi.org/10.1021/acsnano.9b04536
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Latzke, Drew W., Ojeda-Aristizabal, Claudia, Denlinger, Jonathan D., Reno, Ryan, Zettl, Alex, and Lanzara, Alessandra. Tue . "Orbital Character Effects in the Photon Energy and Polarization Dependence of Pure C60 Photoemission". United States. https://doi.org/10.1021/acsnano.9b04536. https://www.osti.gov/servlets/purl/1782491.
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@article{osti_1782491,
title = {Orbital Character Effects in the Photon Energy and Polarization Dependence of Pure C60 Photoemission},
author = {Latzke, Drew W. and Ojeda-Aristizabal, Claudia and Denlinger, Jonathan D. and Reno, Ryan and Zettl, Alex and Lanzara, Alessandra},
abstractNote = {We report that recent direct experimental observation of multiple highly dispersive C60 valence bands has allowed for a detailed analysis of the unusual photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C60 molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C60 band manifolds which allow for a more precise determination of the orbital character within the third highest occupied molecular orbital (HOMO-2). In conclusion, our observations and analysis provide important considerations for the connection between molecular and crystalline C60 electronic structure, past and future band structure studies, and for increasingly popular C60 electronic device applications, especially those making use of heterostructures.},
doi = {10.1021/acsnano.9b04536},
journal = {ACS Nano},
number = 11,
volume = 13,
place = {United States},
year = {Tue Oct 22 00:00:00 EDT 2019},
month = {Tue Oct 22 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsnano.9b04536
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Figures / Tables:

FIG. 1 FIG. 1: (a) Geometry of the experimental setup indicating incoming light polarization, outgoing photoelectrons, and Brillouin zone. High resolution constant energy maps of $C$60 (5 nm) on Bi2Se3 with cuts through the energies near the (b) HOMO top, (c) HOMO bottom, (d) HOMO-1 top, and (e) HOMO-1 bottom. Upper andmore » lower images are taken with out-of-plane light polarization (⊥, blue) and in-plane light polarization (‖, red), respectively. The first Brillouin zone of $C$60 (Bi2Se3) is indicated by a thick black (gray) hexagon with the high-symmetry points labeled in panel (b). Higher order Brillouin zones are indicated by dashed hexagons. ($hν$ = 45 eV, $T$ = 20 K).« less
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    Signatures of an Atomic Crystal in the Band Structure of a Molecular Thin Film
    text, January 2020

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      FIG. 3 (p. 11)figure
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