Band Edge Energetics of Heterostructured Nanorods: Photoemission Spectroscopy and Waveguide Spectroelectrochemistry of Au-Tipped CdSe Nanorod Monolayers

Ehamparam, Ramanan; Pavlopoulos, Nicholas G.; Liao, Michael W.; Hill, Lawrence J.; Armstrong, Neal R.; Pyun, Jeffrey; Saavedra, S. Scott

doi:10.1021/acsnano.5b01720

Title: Band Edge Energetics of Heterostructured Nanorods: Photoemission Spectroscopy and Waveguide Spectroelectrochemistry of Au-Tipped CdSe Nanorod Monolayers

Journal Article · Thu Aug 20 00:00:00 EDT 2015 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b01720· OSTI ID:1369928

Ehamparam, Ramanan ^[1]; Pavlopoulos, Nicholas G. ^[1]; Liao, Michael W. ^[1]; Hill, Lawrence J. ^[1]; Armstrong, Neal R. ^[1]; Pyun, Jeffrey ^[2]; Saavedra, S. Scott ^[1]

Univ. of Arizona, Tucson, AZ (United States)
Univ. of Arizona, Tucson, AZ (United States); Seoul National Univ. (Korea, Republic of)

Conduction and valence band energies (E_CB, E_VB) for CdSe nanorods (NRs) functionalized with Au nanoparticle (NP) tips are reported here, referenced to the vacuum scale. We use (a) UV photoemission spectroscopy (UPS) to measure E_VB for NR films, utilizing advanced approaches to secondary electron background correction, satellite removal to enhance spectral contrast, and correction for shifts in local vacuum levels; and (b) waveguide-based spectroelectrochemistry to measure E_CB from onset potentials for electron injection into NR films tethered to ITO. For untipped CdSe NRs, both approaches show E_VB = 5.9–6.1 eV and E_CB = 4.1–4.3 eV. Addition of Au tips alters the NR band edge energies and introduces midgap states, in ways that are predicted to influence the efficiency of these nanomaterials as photoelectrocatalysts. UPS results show that Au tipping shifts E_VB closer to vacuum by up to 0.4 eV, shifts the apparent Fermi energy toward the middle of the band gap, and introduces additional states above E_VB. Spectroelectrochemical results determine these trends: Au tipping shifts E_CB closer to vacuum, by 0.4–0.6 eV, and introduces midgap states below E_CB, which are assigned as metal–semiconductor interface (MSI) states. Characterization of these band edge energies and understanding the origins of MSI states is needed to design energy conversion systems with proper band alignment between the light absorbing NR, the NP catalyst, and solution electron donors and acceptors. Furthermore, the complementary characterization protocols presented here should be applicable to a wide variety of thin films of heterogeneous photoactive nanomaterials, aiding in the identification of the most promising material combinations for photoelectrochemical energy conversion.

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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); National Science Foundation (NSF)

Grant/Contract Number:: SC0001084; FG03-02ER15753; DMR-130792

OSTI ID:: 1369928

Journal Information:: ACS Nano, Vol. 9, 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 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Band Edge Energetics of Heterostructured Nanorods: Photoemission Spectroscopy and Waveguide Spectroelectrochemistry of Au-Tipped CdSe Nanorod Monolayers

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