Journal
NANO LETTERS
Volume 11, Issue 9, Pages 3855-3861Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nl201944h
Keywords
Carrier dynamics; electronic structure; interfacial charge transfer; nanostructure; oxide heterostructure
Categories
Funding
- U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy
- Sandia National Laboratories
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
- Basic Energy Sciences Division of the U.S. Department of Energy [DE-FG02-ER46232]
- W.M. Keck Center for Nanoscale Optofluidics at UCSC
- Department of Defense (DoD)
- National Science Foundation (NSF)
- Center on Nanostructuring for Efficient Energy Conversion, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001060, DE-AC02-05CH11231]
- MEXT, Japan
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Direct experimental observation of spontaneous electron enrichment of metal d orbitals in a new transition metal oxide heterostructure with nanoscale dimensionality is reported. Aqueous chemical synthesis and vapor phase deposition are combined to fabricate oriented arrays of high-interfacial-area hetero-nanostructures comprised of titanium oxide and iron oxide nanomaterials. Synchrotron-based soft X-ray spectroscopy techniques with high spectral resolution are utilized to directly probe the titanium and oxygen orbital character of the interfacial region's occupied and unoccupied densities of states. These data demonstrate the interface to possess electrons in Ti 3d bands and an emergent degree of orbital hybridization that is absent in parent oxide reference crystals. The carrier dynamics of the hetero-nanostructures are studied by ultrafast transient absorption spectroscopy, which reveals the presence of a dense manifold of states, the relaxations from which exhibit multiple exponential decays whose magnitudes depend on their energetic positions within the electronic structure.
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