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Title: Integer Charge Transfer and Hybridization at an Organic Semiconductor/Conductive Oxide Interface

Journal Article · · Journal of Physical Chemistry. C
DOI: https://doi.org/10.1021/jp512153b · OSTI ID:1210375
 [1];  [2];  [3];  [1];  [4];  [4];  [4];  [1];  [5];  [1];  [2]
  1. Friedrich Schiller Univ. Jena (Germany). Inst. für Festkörperphysik
  2. Univ. of Arizona, Tucson, AZ (United States)
  3. Georgia Inst. of Technology, Atlanta, GA (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. Georgia Inst. of Technology, Atlanta, GA (United States); King Abdullah Univ. of Science and Technology (KAUST), Thuwal (Kingdom of Saudi Arabia)
+ Show Author Affiliations

In this work we investigate the prototypical hybrid interface formed between PTCDA and conductive $$n$$-doped ZnO films by means of complementary optical and electronic spectroscopic techniques. We demonstrate that shallow donors in the vicinity of the ZnO surface cause an integer charge transfer to PTCDA, which is clearly restricted to the first monolayer. By means of DFT calculations, we show that the experimental signatures of the anionic PTCDA species can be understood in terms of strong hybridization with localized states (the shallow donors) in the substrate and charge back-donation, resulting in an effectively integer charge transfer across the interface. Charge transfer is thus not merely a question of locating the Fermi level above the PTCDA electron-transport level but requires rather an atomistic understanding of the interfacial interactions. The study reveals that defect sites and dopants can have a significant influence on the specifics of interfacial coupling and thus on carrier injection or extraction.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Interface Science: Solar Electric Materials (CISSEM)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); German Research Foundation (DFG); National Science Foundation (NSF)
Grant/Contract Number:
SC0001084; FR875/9-3; CHE0946869
OSTI ID:
1210375
Journal Information:
Journal of Physical Chemistry. C, Vol. 119, Issue 9; Related Information: CISSEM partners with the University of Arizona (lead); Georgia Institute of Technology; National Renewable Energy Laboratory; Princeton University; University of Washington; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 53 works
Citation information provided by
Web of Science

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Cited By (6)

Hybridization-Induced Carrier Localization at the C 60 /ZnO Interface journal November 2015
The Impact of Dipolar Layers on the Electronic Properties of Organic/Inorganic Hybrid Interfaces journal May 2019
The role of initial and final states in molecular spectroscopies journal January 2019
Spectroscopy and control of near-surface defects in conductive thin film ZnO journal February 2016
Tailoring the growth and electronic structures of organic molecular thin films journal September 2019
Doping-Induced Electron Transfer at Organic/Oxide Interfaces: Direct Evidence from Infrared Spectroscopy text January 2020

Figures / Tables (5)

ϵ" spectra of 1 MLE PTCDA on inert mica, 1 MLE of PTCDA partially potassium-doped providing pronounced new features of PTCDA radical anions at low photon energies (investigated in detail previously), polycrystalline (pc) PTCDA and the dramatically broadened spectra of 1 MLE of PTCDA on Au(111) and Ag(111) are shown in the bottom panel. b) ΔDRS of PTCDA on quartz glass for nominal thicknesses ranging from submonolayers up to 1 MLE. The graphs are labeled according to the scheme (m +1) - m referring to eq. (2)." data-ostiid="1210375">
Figure 1(p. 9)figure Figure 1
Figure 2(p. 13)figure Figure 2
Table 1(p. 15)table Table 1
Figure 3(p. 16)figure Figure 3
Figure 4(p. 19)figure Figure 4

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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