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Photoexcited Small Polaron Formation in Goethite (α-FeOOH) Nanorods Probed by Transient Extreme Ultraviolet Spectroscopy

Porter, Ilana J. and Cushing, Scott K. and Carneiro, Lucas M. and Lee, Angela and Ondry, Justin C. and Dahl, Jakob C. and Chang, Hung-Tzu and Alivisatos, A. Paul and Leone, Stephen R. (2018) Photoexcited Small Polaron Formation in Goethite (α-FeOOH) Nanorods Probed by Transient Extreme Ultraviolet Spectroscopy. Journal of Physical Chemistry Letters, 9 (14). pp. 4120-4124. ISSN 1948-7185.

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Small polaron formation limits the mobility and lifetimes of photoexcited carriers in metal oxides. As the ligand field strength increases, the carrier mobility decreases, but the effect on the photoexcited small polaron formation is still unknown. Extreme ultraviolet transient absorption spectroscopy is employed to measure small polaron formation rates and probabilities in goethite (α-FeOOH) crystalline nanorods at pump photon energies from 2.2 to 3.1 eV. The measured polaron formation time increases with excitation photon energy from 70 ± 10 fs at 2.2 eV to 350 ± 30 fs at 2.6 eV, whereas the polaron formation probability (85 ± 10%) remains constant. By comparison to hematite (α-Fe_2O_3), an oxide analogue, the role of ligand composition and metal center density in small polaron formation time is discussed. This work suggests that incorporating small changes in ligands and crystal structure could enable the control of photoexcited small polaron formation in metal oxides.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Porter, Ilana J.0000-0001-8692-9950
Cushing, Scott K.0000-0003-3538-2259
Lee, Angela0000-0001-5388-8400
Ondry, Justin C.0000-0001-9113-3420
Chang, Hung-Tzu0000-0001-7378-8212
Alivisatos, A. Paul0000-0001-6895-9048
Leone, Stephen R.0000-0003-1819-1338
Additional Information:© 2018 American Chemical Society. Received: May 14, 2018; Accepted: July 9, 2018; Published: July 9, 2018. This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05-CH11231, within the Physical Chemistry of Inorganic Nanostructures Program (KC3103). S.K.C. acknowledges support by the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Solar Energy Technologies Office. H.-T.C. acknowledges support by the Air Force Office of Scientific Research (AFOSR) (FA9550-15-1-0037). J.C.D. acknowledges support by the National Science Foundation Graduate Research Fellowship under DGE 1752814. The authors declare no competing financial interest.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-05-CH11231
Air Force Office of Scientific Research (AFOSR)FA9550-15-1-0037
NSF Graduate Research FellowshipDGE-1752814
Issue or Number:14
Record Number:CaltechAUTHORS:20180918-112320426
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Official Citation:Photoexcited Small Polaron Formation in Goethite (α-FeOOH) Nanorods Probed by Transient Extreme Ultraviolet Spectroscopy. Ilana J. Porter, Scott K. Cushing, Lucas M. Carneiro, Angela Lee, Justin C. Ondry, Jakob C. Dahl, Hung-Tzu Chang, A. Paul Alivisatos, and Stephen R. Leone. The Journal of Physical Chemistry Letters 2018 9 (14), 4120-4124. DOI: 10.1021/acs.jpclett.8b01525
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:89701
Deposited By: Tony Diaz
Deposited On:18 Sep 2018 18:49
Last Modified:03 Oct 2019 20:18

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