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Title: 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:
 [1];  [2];  [1];  [3];  [3];  [2];  [1]
  1. Marquette Univ., Milwaukee, WI (United States)
  2. Lanzhou Univ., Gansu (People's Republic of China)
  3. 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}
}

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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
  • DOI: 10.1021/nl801817d

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
  • DOI: 10.1063/1.331858

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
  • DOI: 10.1039/b211104g

Phase transition and anomalous electronic behavior in the layered superconductor CuS probed by NQR
journal, February 2009


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
  • DOI: 10.1063/1.2991441

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
  • DOI: 10.1038/nmat3004

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
  • DOI: 10.1021/cm401366q

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
  • DOI: 10.1039/b606226a

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
  • DOI: 10.1021/ic900201p

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
  • DOI: 10.1002/adfm.200600245

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
  • DOI: 10.1021/ja805655b

Mechanisms for optical nonlinearities and ultrafast carrier dynamics in Cu x S nanocrystals
journal, September 1996


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
  • DOI: 10.1002/chem.200601368

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
  • DOI: 10.1021/ja106254h

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
  • DOI: 10.1021/am504615x

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
  • DOI: 10.1021/nl202587b

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
  • DOI: 10.1063/1.2903599

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
  • DOI: 10.1039/c3tc00639e

Probing the structural and electronic properties of boron cluster anions doped with one or two aluminum atoms
journal, December 2014


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
  • DOI: 10.1021/jp4013027

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
  • DOI: 10.1039/c2ee22681b

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
  • DOI: 10.1021/ja8034637

Works referencing / citing this record:

Direct electrodeposition of carboxymethyl cellulose based on coordination deposition method
journal, November 2017


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
  • DOI: 10.1039/c7nr03182c

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
  • DOI: 10.1039/c7nr03828c

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
  • DOI: 10.1002/admi.201801771

Green synthesis of multifunctional copper sulfide for efficient adsorption and photocatalysis
journal, April 2019


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
  • DOI: 10.1039/c7ta04071g

One‐Step Transformation from Cu 2 S Nanocrystal to CuS Nanocrystal with Photocatalytic Properties
journal, July 2019


Near infrared light induced plasmonic hot hole transfer at a nano-heterointerface
journal, June 2018


Near infrared light induced plasmonic hot hole transfer at a nano-heterointerface
journal, June 2018