Physical Origins of the Transient Absorption Spectra and Dynamics in Thin-Film Semiconductors: The Case of BiVO4
Abstract
Transient absorption (TA) spectroscopy is uniquely suited for understanding kinetic processes initiated by light over vast ranges of time. In combination with white light probes, the recorded differential absorption spectra can contain spectroscopic signatures characteristic of specific charge carrier population densities. However, disentangling the often-complex and convoluted spectra is made challenging without robust analysis methods relating the underlying physical mechanisms to the spectral components. In this work, we address the origin of the transient spectra of a model system of emerging solar energy harvesting materials using a monoclinic BiVO4 thin film. Using ground-state optical properties of the semiconductor, we find the main derivative-like spectral response to be related to shifting and broadening of oscillators, rather than specific carrier-related transitions. However, by using the Drude optical model of free carriers, we also identify the transient response related to free-hole density. Importantly, sample heating from the optical pumping, which begins at ~10 ps and plateaus by ~200 ps, dominates the overall spectral response at longer times. On the basis of a physical model of the spectral response, a kinetic model is developed that describes the pump power dependence of the free-hole density, as well as the temporal evolution of the spectral changesmore »
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis, Chemical Sciences Division
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics; Univ. Andres Bello, Santiago (Chile). Dept. de Ciencias Físicas
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics, and Kavli Energy NanoSciences Inst.
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis, Chemical Sciences Division; Technische Univ. München, Garching (Germany). Walter Schottky Institut and Physik Dept.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1506360
- Grant/Contract Number:
- AC02-05CH11231; SC0004993
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 36; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Cooper, Jason K., Reyes-Lillo, Sebastian E., Hess, Lucas H., Jiang, Chang-Ming, Neaton, Jeffrey B., and Sharp, Ian D. Physical Origins of the Transient Absorption Spectra and Dynamics in Thin-Film Semiconductors: The Case of BiVO4. United States: N. p., 2018.
Web. doi:10.1021/acs.jpcc.8b06645.
Cooper, Jason K., Reyes-Lillo, Sebastian E., Hess, Lucas H., Jiang, Chang-Ming, Neaton, Jeffrey B., & Sharp, Ian D. Physical Origins of the Transient Absorption Spectra and Dynamics in Thin-Film Semiconductors: The Case of BiVO4. United States. https://doi.org/10.1021/acs.jpcc.8b06645
Cooper, Jason K., Reyes-Lillo, Sebastian E., Hess, Lucas H., Jiang, Chang-Ming, Neaton, Jeffrey B., and Sharp, Ian D. Mon .
"Physical Origins of the Transient Absorption Spectra and Dynamics in Thin-Film Semiconductors: The Case of BiVO4". United States. https://doi.org/10.1021/acs.jpcc.8b06645. https://www.osti.gov/servlets/purl/1506360.
@article{osti_1506360,
title = {Physical Origins of the Transient Absorption Spectra and Dynamics in Thin-Film Semiconductors: The Case of BiVO4},
author = {Cooper, Jason K. and Reyes-Lillo, Sebastian E. and Hess, Lucas H. and Jiang, Chang-Ming and Neaton, Jeffrey B. and Sharp, Ian D.},
abstractNote = {Transient absorption (TA) spectroscopy is uniquely suited for understanding kinetic processes initiated by light over vast ranges of time. In combination with white light probes, the recorded differential absorption spectra can contain spectroscopic signatures characteristic of specific charge carrier population densities. However, disentangling the often-complex and convoluted spectra is made challenging without robust analysis methods relating the underlying physical mechanisms to the spectral components. In this work, we address the origin of the transient spectra of a model system of emerging solar energy harvesting materials using a monoclinic BiVO4 thin film. Using ground-state optical properties of the semiconductor, we find the main derivative-like spectral response to be related to shifting and broadening of oscillators, rather than specific carrier-related transitions. However, by using the Drude optical model of free carriers, we also identify the transient response related to free-hole density. Importantly, sample heating from the optical pumping, which begins at ~10 ps and plateaus by ~200 ps, dominates the overall spectral response at longer times. On the basis of a physical model of the spectral response, a kinetic model is developed that describes the pump power dependence of the free-hole density, as well as the temporal evolution of the spectral changes associated with shifting and broadening of oscillators. First-principles density functional theory calculations are used to rationalize experimental measurements. Here, this comprehensive approach to analyzing and modeling the TA spectra offers a generalizable basis for understanding the complex pump-probe data, reveals thermal heating artifacts that are frequently erroneously assigned to long-lived photocarriers, and offers a path to eliminating ambiguity in analysis of photocarrier dynamics in solid-state systems.},
doi = {10.1021/acs.jpcc.8b06645},
journal = {Journal of Physical Chemistry. C},
number = 36,
volume = 122,
place = {United States},
year = {Mon Aug 20 00:00:00 EDT 2018},
month = {Mon Aug 20 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
Attosecond band-gap dynamics in silicon
journal, December 2014
- Schultze, M.; Ramasesha, K.; Pemmaraju, C. D.
- Science, Vol. 346, Issue 6215
Semiconductor interfacial carrier dynamics via photoinduced electric fields
journal, November 2015
- Yang, Y.; Gu, J.; Young, J. L.
- Science, Vol. 350, Issue 6264
Cobalt–phosphate complexes catalyze the photoelectrochemical water oxidation of BiVO4 electrodes
journal, January 2011
- Jeon, Tae Hwa; Choi, Wonyong; Park, Hyunwong
- Physical Chemistry Chemical Physics, Vol. 13, Issue 48
Enhanced Stability and Activity for Water Oxidation in Alkaline Media with Bismuth Vanadate Photoelectrodes Modified with a Cobalt Oxide Catalytic Layer Produced by Atomic Layer Deposition
journal, November 2013
- Lichterman, Michael F.; Shaner, Matthew R.; Handler, Sheila G.
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 23
Indirect Bandgap and Optical Properties of Monoclinic Bismuth Vanadate
journal, January 2015
- Cooper, Jason K.; Gul, Sheraz; Toma, Francesca M.
- The Journal of Physical Chemistry C, Vol. 119, Issue 6
Atomic layer deposition of CdO and CdxZn1−xO films
journal, July 2013
- Bakke, Jonathan R.; Hägglund, Carl; Jung, Hee Joon
- Materials Chemistry and Physics, Vol. 140, Issue 2-3
Multiple oscillator models for the optical constants of polycrystalline zinc oxide thin films over a wide wavelength range
journal, July 2014
- Khoshman, J. M.; Hilfiker, J. N.; Tabet, N.
- Applied Surface Science, Vol. 307
Influence of the exchange screening parameter on the performance of screened hybrid functionals
journal, December 2006
- Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F.
- The Journal of Chemical Physics, Vol. 125, Issue 22
Green’s-function approach to linear response in solids
journal, May 1987
- Baroni, Stefano; Giannozzi, Paolo; Testa, Andrea
- Physical Review Letters, Vol. 58, Issue 18
Electron–Phonon Coupling Dynamics at Oxygen Evolution Sites of Visible-Light-Driven Photocatalyst: Bismuth Vanadate
journal, May 2013
- Aiga, Norihiro; Jia, Qingxin; Watanabe, Kazuya
- The Journal of Physical Chemistry C, Vol. 117, Issue 19
Unraveling the Carrier Dynamics of BiVO 4 : A Femtosecond to Microsecond Transient Absorption Study
journal, November 2014
- Ravensbergen, Janneke; Abdi, Fatwa F.; van Santen, Judith H.
- The Journal of Physical Chemistry C, Vol. 118, Issue 48
Dynamics of Photogenerated Charge Carriers in WO 3 /BiVO 4 Heterojunction Photoanodes
journal, August 2015
- Grigioni, Ivan; Stamplecoskie, Kevin G.; Selli, Elena
- The Journal of Physical Chemistry C, Vol. 119, Issue 36
Atomic Insight into the W-Doping Effect on Carrier Dynamics and Photoelectrochemical Properties of BiVO 4 Photoanodes
journal, January 2016
- Pattengale, Brian; Ludwig, John; Huang, Jier
- The Journal of Physical Chemistry C, Vol. 120, Issue 3
Rational Interpretation of Correlated Kinetics of Mobile and Trapped Charge Carriers: Analysis of Ultrafast Carrier Dynamics in BiVO 4
journal, August 2017
- Suzuki, Yohichi; Murthy, Dharmapura H. K.; Matsuzaki, Hiroyuki
- The Journal of Physical Chemistry C, Vol. 121, Issue 35
Electronic Structure of Monoclinic BiVO 4
journal, September 2014
- Cooper, Jason K.; Gul, Sheraz; Toma, Francesca M.
- Chemistry of Materials, Vol. 26, Issue 18
Third-derivative modulation spectroscopy with low-field electroreflectance
journal, June 1973
- Aspnes, D. E.
- Surface Science, Vol. 37
Photoreflectance and electroreflectance in silicon
journal, June 1969
- Cerdeira, F.; Cardona, Manuel
- Solid State Communications, Vol. 7, Issue 12
Band-gap renormalization in photoexcited semiconductor quantum-wire structures in the approximation
journal, July 1998
- Hwang, E. H.; Das Sarma, S.
- Physical Review B, Vol. 58, Issue 4
Phonon renormalization effects in photoexcited quantum wires
journal, January 1995
- Güven, K.; Tanatar, B.
- Physical Review B, Vol. 51, Issue 3
Combined Charge Carrier Transport and Photoelectrochemical Characterization of BiVO 4 Single Crystals: Intrinsic Behavior of a Complex Metal Oxide
journal, July 2013
- Rettie, Alexander J. E.; Lee, Heung Chan; Marshall, Luke G.
- Journal of the American Chemical Society, Vol. 135, Issue 30
The Origin of Slow Carrier Transport in BiVO 4 Thin Film Photoanodes: A Time-Resolved Microwave Conductivity Study
journal, July 2013
- Abdi, Fatwa F.; Savenije, Tom J.; May, Matthias M.
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 16
Direct Time-Resolved Observation of Carrier Trapping and Polaron Conductivity in BiVO 4
journal, October 2016
- Ziwritsch, Manuel; Müller, Sönke; Hempel, Hannes
- ACS Energy Letters, Vol. 1, Issue 5
Crystal growth and structure of BiVO4
journal, December 1979
- Sleight, A. W.; Chen, H. -y.; Ferretti, A.
- Materials Research Bulletin, Vol. 14, Issue 12
Density functional theory study on the electronic and optical properties of three crystalline phases of BiVO4
journal, March 2013
- Ding, Kaining; Chen, Bin; Fang, Zhenxing
- Theoretical Chemistry Accounts, Vol. 132, Issue 5
Electronic structure and optical properties of monoclinic clinobisvanite BiVO4
journal, January 2011
- Zhao, Zongyan; Li, Zhaosheng; Zou, Zhigang
- Physical Chemistry Chemical Physics, Vol. 13, Issue 10
Observation of a hot-phonon bottleneck in lead-iodide perovskites
journal, October 2015
- Yang, Ye; Ostrowski, David P.; France, Ryan M.
- Nature Photonics, Vol. 10, Issue 1
Effect of heavy doping on the optical properties and the band structure of silicon
journal, June 1984
- Viña, L.; Cardona, M.
- Physical Review B, Vol. 29, Issue 12
Electronic and nuclear contributions to time-resolved optical and X-ray absorption spectra of hematite and insights into photoelectrochemical performance
journal, January 2016
- Hayes, Dugan; Hadt, Ryan G.; Emery, Jonathan D.
- Energy & Environmental Science, Vol. 9, Issue 12
The temperature dependence of the LO(T) and TO(T) phonons in GaAs and InP
journal, May 1996
- Irmer, G.; Wenzel, M.; Monecke, J.
- physica status solidi (b), Vol. 195, Issue 1
Physical mechanisms of coherent acoustic phonons generation by ultrafast laser action
journal, February 2015
- Ruello, Pascal; Gusev, Vitalyi E.
- Ultrasonics, Vol. 56
Carrier dynamics in α‐Fe2O3 (0001) thin films and single crystals probed by femtosecond transient absorption and reflectivity
journal, March 2006
- Joly, Alan G.; Williams, Joshua R.; Chambers, Scott A.
- Journal of Applied Physics, Vol. 99, Issue 5
Coherent Longitudinal Acoustic Phonon Approaching THz Frequency in Multilayer Molybdenum Disulphide
journal, July 2014
- Ge, Shaofeng; Liu, Xuefeng; Qiao, Xiaofen
- Scientific Reports, Vol. 4, Issue 1
Excitation-wavelength-dependent small polaron trapping of photoexcited carriers in α-Fe2O3
journal, July 2017
- Carneiro, Lucas M.; Cushing, Scott K.; Liu, Chong
- Nature Materials, Vol. 16, Issue 8
Role of Hydrogen in Defining the n-Type Character of BiVO 4 Photoanodes
journal, August 2016
- Cooper, Jason K.; Scott, Soren B.; Ling, Yichuan
- Chemistry of Materials, Vol. 28, Issue 16
Works referencing / citing this record:
Influence of shape on the carrier relaxation dynamics of CsPbBr 3 perovskite nanocrystals
journal, January 2019
- Ghosh, Goutam; Jana, Bikash; Sain, Sumanta
- Physical Chemistry Chemical Physics, Vol. 21, Issue 35