Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks
Abstract
CuS nanocrystals are potential materials for developing low-cost solar energy conversion devices. Understanding the underlying dynamics of photoinduced carriers in CuS nanocrystals is essential to improve their performance in these devices. In this work, we investigated the photoinduced hole dynamics in CuS nanodisks (NDs) using the combination of transient optical (OTA) and X-ray (XTA) absorption spectroscopy. OTA results show that the broad transient absorption in the visible region is attributed to the photoinduced hot and trapped holes. The hole trapping process occurs on a subpicosecond time scale, followed by carrier recombination (~100 ps). The nature of the hole trapping sites, revealed by XTA, is characteristic of S or organic ligands on the surface of CuS NDs. Lastly, these results not only suggest the possibility to control the hole dynamics by tuning the surface chemistry of CuS but also represent the first time observation of hole dynamics in semiconductor nanocrystals using XTA.
- Authors:
-
- Marquette Univ., Milwaukee, WI (United States)
- Lanzhou Univ., Gansu (People's Republic of China)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division; Marquette University; National Natural Science Foundation of China (NSFC); Argonne National Laboratory, Advanced Photon Source
- OSTI Identifier:
- 1376714
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 14; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; CuS nanodisks; energy conversion; optical transient absorption spectroscopy; X-ray transient absorption spectroscopy
Citation Formats
Ludwig, John, An, Li, Pattengale, Brian, Kong, Qingyu, Zhang, Xiaoyi, Xi, Pinxian, and Huang, Jier. Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks. United States: N. p., 2015.
Web. doi:10.1021/acs.jpclett.5b01078.
Ludwig, John, An, Li, Pattengale, Brian, Kong, Qingyu, Zhang, Xiaoyi, Xi, Pinxian, & Huang, Jier. Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks. United States. https://doi.org/10.1021/acs.jpclett.5b01078
Ludwig, John, An, Li, Pattengale, Brian, Kong, Qingyu, Zhang, Xiaoyi, Xi, Pinxian, and Huang, Jier. Mon .
"Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks". United States. https://doi.org/10.1021/acs.jpclett.5b01078. https://www.osti.gov/servlets/purl/1376714.
@article{osti_1376714,
title = {Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks},
author = {Ludwig, John and An, Li and Pattengale, Brian and Kong, Qingyu and Zhang, Xiaoyi and Xi, Pinxian and Huang, Jier},
abstractNote = {CuS nanocrystals are potential materials for developing low-cost solar energy conversion devices. Understanding the underlying dynamics of photoinduced carriers in CuS nanocrystals is essential to improve their performance in these devices. In this work, we investigated the photoinduced hole dynamics in CuS nanodisks (NDs) using the combination of transient optical (OTA) and X-ray (XTA) absorption spectroscopy. OTA results show that the broad transient absorption in the visible region is attributed to the photoinduced hot and trapped holes. The hole trapping process occurs on a subpicosecond time scale, followed by carrier recombination (~100 ps). The nature of the hole trapping sites, revealed by XTA, is characteristic of S or organic ligands on the surface of CuS NDs. Lastly, these results not only suggest the possibility to control the hole dynamics by tuning the surface chemistry of CuS but also represent the first time observation of hole dynamics in semiconductor nanocrystals using XTA.},
doi = {10.1021/acs.jpclett.5b01078},
journal = {Journal of Physical Chemistry Letters},
number = 14,
volume = 6,
place = {United States},
year = {Mon Jun 22 00:00:00 EDT 2015},
month = {Mon Jun 22 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Synthesis and Photovoltaic Application of Copper(I) Sulfide Nanocrystals
journal, August 2008
- Wu, Yue; Wadia, Cyrus; Ma, Wanli
- Nano Letters, Vol. 8, Issue 8
Degradation of a Cu x S/CdS solar cell in hot, moist air and recovery in hydrogen and air
journal, November 1983
- Partain, L. D.; McLeod, P. S.; Duisman, J. A.
- Journal of Applied Physics, Vol. 54, Issue 11
Evaluation of the photoinduced electron relaxation dynamics of Cu1.8S quantum dots
journal, February 2003
- Lou, Yongbing; Samia, Anna C. S.; Cowen, Jonathan
- Physical Chemistry Chemical Physics, Vol. 5, Issue 6
Metallic-like Stoichiometric Copper Sulfide Nanocrystals: Phase- and Shape-Selective Synthesis, Near-Infrared Surface Plasmon Resonance Properties, and Their Modeling
journal, July 2013
- Xie, Yi; Carbone, Luigi; Nobile, Concetta
- ACS Nano, Vol. 7, Issue 8
Phase transition and anomalous electronic behavior in the layered superconductor CuS probed by NQR
journal, February 2009
- Gainov, R. R.; Dooglav, A. V.; Pen’kov, I. N.
- Physical Review B, Vol. 79, Issue 7
Fabrication and microstructure of p-type transparent conducting CuS thin film and its application in dye-sensitized solar cell
journal, September 2008
- Yuan, K. D.; Wu, J. J.; Liu, M. L.
- Applied Physics Letters, Vol. 93, Issue 13
Localized surface plasmon resonances arising from free carriers in doped quantum dots
journal, April 2011
- Luther, Joseph M.; Jain, Prashant K.; Ewers, Trevor
- Nature Materials, Vol. 10, Issue 5, p. 361-366
Biomolecule-Assisted, Environmentally Friendly, One-Pot Synthesis of CuS/Reduced Graphene Oxide Nanocomposites with Enhanced Photocatalytic Performance
journal, August 2012
- Zhang, Yingwei; Tian, Jingqi; Li, Haiyan
- Langmuir, Vol. 28, Issue 35
Evolution of Hierarchical Hexagonal Stacked Plates of CuS from Liquid−Liquid Interface and its Photocatalytic Application for Oxidative Degradation of Different Dyes under Indoor Lighting
journal, July 2010
- Basu, Mrinmoyee; Sinha, Arun Kumar; Pradhan, Mukul
- Environmental Science & Technology, Vol. 44, Issue 16
Routes to Nanostructured Inorganic Materials with Potential for Solar Energy Applications
journal, July 2013
- Ramasamy, Karthik; Malik, Mohammad Azad; Revaprasadu, Neerish
- Chemistry of Materials, Vol. 25, Issue 18
Large scale synthesis of uniform CuS nanotubes in ethylene glycol by a sacrificial templating method under mild conditions
journal, January 2006
- Wu, Chunyan; Yu, Shu-Hong; Chen, Shaofeng
- Journal of Materials Chemistry, Vol. 16, Issue 32
Fast Synthesis, Formation Mechanism, and Control of Shell Thickness of CuS Hollow Spheres
journal, July 2009
- Zhu, Haitao; Wang, Jixin; Wu, Daxiong
- Inorganic Chemistry, Vol. 48, Issue 15
Nanometer-Sized Copper Sulfide Hollow Spheres with Strong Optical-Limiting Properties
journal, April 2007
- Yu, X. -L.; Cao, C. -B.; Zhu, H. -S.
- Advanced Functional Materials, Vol. 17, Issue 8
Plasmonic Cu 2− x S Nanocrystals: Optical and Structural Properties of Copper-Deficient Copper(I) Sulfides
journal, April 2009
- Zhao, Yixin; Pan, Hongcheng; Lou, Yongbing
- Journal of the American Chemical Society, Vol. 131, Issue 12
Femtosecond Spectroscopic Investigation of the Carrier Lifetimes in Digenite Quantum Dots and Discrimination of the Electron and Hole Dynamics via Ultrafast Interfacial Electron Transfer †
journal, November 2003
- Lou, Yongbing; Chen, Xiaobo; Samia, Anna C.
- The Journal of Physical Chemistry B, Vol. 107, Issue 45
Mechanisms for optical nonlinearities and ultrafast carrier dynamics in S nanocrystals
journal, September 1996
- Klimov, Victor I.; Karavanskii, Vladimir A.
- Physical Review B, Vol. 54, Issue 11
Shape-Controlled Synthesis and Self-Assembly of Hexagonal Covellite (CuS) Nanoplatelets
journal, April 2007
- Du, Weimin; Qian, Xuefeng; Ma, Xiaodong
- Chemistry - A European Journal, Vol. 13, Issue 11
Cu 2 Se Nanoparticles with Tunable Electronic Properties Due to a Controlled Solid-State Phase Transition Driven by Copper Oxidation and Cationic Conduction
journal, February 2011
- Riha, Shannon C.; Johnson, Derek C.; Prieto, Amy L.
- Journal of the American Chemical Society, Vol. 133, Issue 5
Influence of Cu Vacancy on Knit Coir Mat Structured CuS as Counter Electrode for Quantum Dot Sensitized Solar Cells
journal, October 2014
- Savariraj, A. Dennyson; Viswanathan, Kodakkal Kannan; Prabakar, Kandasamy
- ACS Applied Materials & Interfaces, Vol. 6, Issue 22
Visible Light Photocatalytic H 2 -Production Activity of CuS/ZnS Porous Nanosheets Based on Photoinduced Interfacial Charge Transfer
journal, November 2011
- Zhang, Jun; Yu, Jiaguo; Zhang, Yimin
- Nano Letters, Vol. 11, Issue 11
Effect of sulfurization conditions on structural and electrical properties of copper sulfide films
journal, April 2008
- Kundu, Manisha; Hasegawa, Tsuyoshi; Terabe, Kazuya
- Journal of Applied Physics, Vol. 103, Issue 7
Quantitative X-ray absorption and emission spectroscopies: electronic structure elucidation of Cu2S and CuS
journal, January 2013
- Kumar, Prashant; Nagarajan, Rajamani; Sarangi, Ritimukta
- Journal of Materials Chemistry C, Vol. 1, Issue 13
Probing the structural and electronic properties of boron cluster anions doped with one or two aluminum atoms
journal, December 2014
- Gu, Jianbing; Wang, Chenju; Cheng, Yan
- Computational and Theoretical Chemistry, Vol. 1049
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
In situ probe of photocarrier dynamics in water-splitting hematite (α-Fe2O3) electrodes
journal, January 2012
- Huang, Zhuangqun; Lin, Yongjing; Xiang, Xu
- Energy & Environmental Science, Vol. 5, Issue 10
Mechanism of Photocatalytic Water Splitting in TiO 2 . Reaction of Water with Photoholes, Importance of Charge Carrier Dynamics, and Evidence for Four-Hole Chemistry
journal, October 2008
- Tang, Junwang; Durrant, James R.; Klug, David R.
- Journal of the American Chemical Society, Vol. 130, Issue 42
Works referencing / citing this record:
Metallic CuCo 2 S 4 nanosheets of atomic thickness as efficient bifunctional electrocatalysts for portable, flexible Zn-air batteries
journal, January 2018
- Li, Yuxuan; Yin, Jie; An, Li
- Nanoscale, Vol. 10, Issue 14
Constructing hyperbranched polymers as a stable elastic framework for copper sulfide nanoplates for enhancing sodium-storage performance
journal, January 2019
- Qin, Aiqiong; Wu, Hao; Chen, Jie
- Nanoscale, Vol. 11, Issue 15
Enhancement of Hydrogen Productions by Accelerating Electron-Transfers of Sulfur Defects in the CuS@CuGaS2 Heterojunction Photocatalysts
journal, January 2019
- Son, Namgyu; Heo, Jun; Youn, Young-Sang
- Catalysts, Vol. 9, Issue 1
Direct electrodeposition of carboxymethyl cellulose based on coordination deposition method
journal, November 2017
- Wang, Yifeng; Zhang, Zheng; Wang, Ming
- Cellulose, Vol. 25, Issue 1
High-index faceted CuFeS 2 nanosheets with enhanced behavior for boosting hydrogen evolution reaction
journal, January 2017
- Li, Yuxuan; Wang, Yu; Pattengale, Brian
- Nanoscale, Vol. 9, Issue 26
Diversified copper sulfide (Cu 2−x S) micro-/nanostructures: a comprehensive review on synthesis, modifications and applications
journal, January 2017
- Sun, Shaodong; Li, Pengju; Liang, Shuhua
- Nanoscale, Vol. 9, Issue 32
Probing Interfacial Surface State Excitons in Nanoscale Synthesized Cu x S/MoS 2 Heterostructure
journal, January 2019
- Shahzad, Rauf; Mun, Jihun; Kim, Tae Wan
- Advanced Materials Interfaces, Vol. 6, Issue 6
Green synthesis of multifunctional copper sulfide for efficient adsorption and photocatalysis
journal, April 2019
- Li, Ye-Hua; Wang, Zheng
- Chemical Papers, Vol. 73, Issue 9
Hierarchical design of Cu 1−x Ni x S nanosheets for high-performance asymmetric solid-state supercapacitors
journal, January 2017
- Balamurugan, Jayaraman; Li, Chao; Thanh, Tran Duy
- Journal of Materials Chemistry A, Vol. 5, Issue 37
One‐Step Transformation from Cu 2 S Nanocrystal to CuS Nanocrystal with Photocatalytic Properties
journal, July 2019
- Wan, Mengli; Zhang, Yingying; Wei, Wutao
- ChemistrySelect, Vol. 4, Issue 25
Near infrared light induced plasmonic hot hole transfer at a nano-heterointerface
journal, June 2018
- Lian, Zichao; Sakamoto, Masanori; Matsunaga, Hironori
- Nature Communications, Vol. 9, Issue 1
Near infrared light induced plasmonic hot hole transfer at a nano-heterointerface
journal, June 2018
- Lian, Zichao; Sakamoto, Masanori; Matsunaga, Hironori
- Nature Communications, Vol. 9, Issue 1