Vacancy relaxation in cuprous oxide (Cu2–xO1–y)

Frazer, Laszlo; Chang, Kelvin B.; Schaller, Richard D.; Poeppelmeier, Kenneth R.; Ketterson, John B.

doi:10.1016/j.jlumin.2016.11.011

Title: Vacancy relaxation in cuprous oxide (Cu_2–xO_1–y)

Abstract

Phonons are produced when an excited vacancy in cuprous oxide (Cu₂O) relaxes. Time resolved luminescence was used to find the excited copper vacancy (acceptor) and oxygen vacancy (donor) trap levels and lifetimes. It was also used to determine the typical energy and number of phonons in the phonon pulses emitted by vacancies. The vacancy properties of cuprous oxide are controlled by several synthesis parameters and by the temperature. We directly demonstrate the absorption of light by oxygen vacancies with transient absorption. Copper and oxygen vacancies behave differently, in part because the two kinds of traps capture carriers from different states. For example, the copper vacancy luminescence lifetime is around 25 times greater at low temperature. Moreover, both kinds of vacancy luminescence are consistent with a Poissonian multiple phonon emission model.

Authors:

Frazer, Laszlo ^[1]; Chang, Kelvin B. ^[2]; Schaller, Richard D. ^[3]; Poeppelmeier, Kenneth R. ^[3]; Ketterson, John B. ^[2]

Temple Univ., Philadelphia, PA (United States); UNSW, Sydney, NSW (Australia)
Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Mon Nov 14 00:00:00 EST 2016

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Inverse Design (CID)

Sponsoring Org.:: Institute for Sustainability and Energy at Northwestern (ISEN); Argonne National Laboratory, Laboratory Directed Research and Development (LDRD); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences, and Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)

OSTI Identifier:: 1364756

Alternate Identifier(s):: OSTI ID: 1396574

Grant/Contract Number:: AC02-06CH11357; AC36-08GO28308

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Luminescence

Additional Journal Information:: Journal Volume: 183; Journal Issue: C; Journal ID: ISSN 0022-2313

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bound exciton; cuprous oxide; exciton; phonon; stoichiometry; vacancy

Citation Formats


                    Frazer, Laszlo, Chang, Kelvin B., Schaller, Richard D., Poeppelmeier, Kenneth R., and Ketterson, John B. Vacancy relaxation in cuprous oxide (Cu2–xO1–y).  United States: N. p., 2016. 
Web.  doi:10.1016/j.jlumin.2016.11.011.

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                    Frazer, Laszlo, Chang, Kelvin B., Schaller, Richard D., Poeppelmeier, Kenneth R., & Ketterson, John B. Vacancy relaxation in cuprous oxide (Cu2–xO1–y).  United States.  https://doi.org/10.1016/j.jlumin.2016.11.011

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                    Frazer, Laszlo, Chang, Kelvin B., Schaller, Richard D., Poeppelmeier, Kenneth R., and Ketterson, John B. Mon .  
"Vacancy relaxation in cuprous oxide (Cu2–xO1–y)".  United States.  https://doi.org/10.1016/j.jlumin.2016.11.011.  https://www.osti.gov/servlets/purl/1364756.

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@article{osti_1364756,

  title        = {Vacancy relaxation in cuprous oxide (Cu2–xO1–y)},

  author       = {Frazer, Laszlo and Chang, Kelvin B. and Schaller, Richard D. and Poeppelmeier, Kenneth R. and Ketterson, John B.},

  abstractNote = {Phonons are produced when an excited vacancy in cuprous oxide (Cu2O) relaxes. Time resolved luminescence was used to find the excited copper vacancy (acceptor) and oxygen vacancy (donor) trap levels and lifetimes. It was also used to determine the typical energy and number of phonons in the phonon pulses emitted by vacancies. The vacancy properties of cuprous oxide are controlled by several synthesis parameters and by the temperature. We directly demonstrate the absorption of light by oxygen vacancies with transient absorption. Copper and oxygen vacancies behave differently, in part because the two kinds of traps capture carriers from different states. For example, the copper vacancy luminescence lifetime is around 25 times greater at low temperature. Moreover, both kinds of vacancy luminescence are consistent with a Poissonian multiple phonon emission model.},

  doi          = {10.1016/j.jlumin.2016.11.011},

  journal      = {Journal of Luminescence},

  number       = C,

  volume       = 183,

  place        = {United States},

  year         = {Mon Nov 14 00:00:00 EST 2016},

  month        = {Mon Nov 14 00:00:00 EST 2016}

}

Copy to clipboard

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https://doi.org/10.1016/j.jlumin.2016.11.011

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Title: Vacancy relaxation in cuprous oxide (Cu2–xO1–y)

Abstract

Citation Formats

Photocurrent Enhancement of n-Type Cu 2 O Electrodes Achieved by Controlling Dendritic Branching Growth journal, February 2009

Evaluation of defects in cuprous oxide through exciton luminescence imaging journal, March 2015

Population dynamics of a Bose gas near saturation journal, March 1989

Dynamics associated with Bose-Einstein statistics of orthoexcitons generated by resonant excitations in cuprous oxide journal, November 1997

High resolution spectroscopy of yellow 1S excitons in Cu2O journal, April 2005

First-Principles Predictions of the Structure, Stability, and Photocatalytic Potential of Cu 2 O Surfaces journal, September 2013

Correlated lifetimes of free paraexcitons and excitons trapped at oxygen vacancies in cuprous oxide journal, February 2013

Transition to a Bose–Einstein condensate and relaxation explosion of excitons at sub-Kelvin temperatures journal, May 2011

Bose–Einstein condensation of excitons in Cu 2 O: progress over 30 years journal, October 2014

Third-harmonic generation in cuprous oxide: efficiency determination journal, January 2014

Green Luminescence Band in ZnO: Fine Structures, Electron−Phonon Coupling, and Temperature Effect journal, June 2006

Analysis of Wavelength Derivative Spectra of Exciton in Cu 2 O journal, July 1975

Femtosecond spectroscopy of condensed phases with chirped supercontinuum probing journal, March 1999

Optical Absorption of Cuprous Oxide journal, January 1961

Highly Mobile Paraexcitons in Cuprous Oxide journal, March 1984

Study of Orthoexciton-to-Paraexciton Conversion in C u 2 O by Excitonic Lyman Spectroscopy journal, January 2005

Symmetry of Excitons in Cu 2 O journal, October 1961

Removal of Copper Vacancies in Cuprous Oxide Single Crystals Grown by the Floating Zone Method journal, October 2013

Modeling of the thermalization of trapped paraexcitons in Cu 2 O at ultralow temperatures journal, August 2014

Free exciton motion in crystals and exciton-phonon interaction journal, October 1966

Electrodeposited Cu 2 O as Photoelectrodes with Controllable Conductivity Type for Solar Energy Conversion journal, November 2015

Engineering of optically defect free Cu_2O enabling exciton luminescence at room temperature journal, January 2013

Epitaxial stabilization of orthorhombic cuprous oxide films on MgO(110) journal, April 2001

Appearance of coherent artifact signals in femtosecond transient absorption spectroscopy in dependence on detector design journal, January 2007

Experimental and theoretical studies of Cu2O solar cells journal, December 1982

Unexpectedly slow two particle decay of ultra-dense excitons in cuprous oxide journal, September 2013

Giant Rydberg excitons in the copper oxide Cu2O journal, October 2014

Oxygen vacancy in N-doped Cu 2 O crystals: A density functional theory study journal, August 2012

Cupric oxide inclusions in cuprous oxide crystals grown by the floating zone method journal, June 2015

Electronic Structure of Pure and Doped Cuprous Oxide with Copper Vacancies: Suppression of Trap States journal, January 2013

Carrier thermalization in Cu 2 O: Phonon emission by excitons journal, August 1991

Study of photoluminescence in Cu 2 O journal, September 1975

The red luminescence spectrum of brown diamonds: vibronic coupling journal, March 1986

Indirect generation of quadrupole polaritons from dark excitons in Cu 2 O journal, February 2008

Undoped n -Type Cu 2 O: Fact or Fiction? journal, August 2010

Growth and microstructural control of single crystal cuprous oxide Cu2O journal, August 1974

Mechanisms behind green photoluminescence in ZnO phosphor powders journal, May 1996

Photoionization cross section of 1 s orthoexcitons in cuprous oxide journal, June 2014

Relaxation of localized excitons by phonon emission at oxygen vacancies in Cu2O journal, November 2014

Signatures of coherent propagation of blue polaritons in Cu 2 O journal, June 2013

The search for Bose–Einstein condensation of excitons in Cu 2 O: exciton-Auger recombination versus biexciton formation journal, December 2014

Potentiostatic electrodeposition of cuprous oxide thin films for photovoltaic applications journal, May 2011

Detailed Examination of Relaxation Processes of Excitons in Photoluminescence Spectra of Cu 2 O journal, July 1997

Thermodynamic Assessment of the Silver-Oxygen System journal, December 1997

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Title: Vacancy relaxation in cuprous oxide (Cu_2–xO_1–y)

Photocurrent Enhancement of n-Type Cu ₂ O Electrodes Achieved by Controlling Dendritic Branching Growth
journal, February 2009

Evaluation of defects in cuprous oxide through exciton luminescence imaging
journal, March 2015

Population dynamics of a Bose gas near saturation
journal, March 1989

Dynamics associated with Bose-Einstein statistics of orthoexcitons generated by resonant excitations in cuprous oxide
journal, November 1997

High resolution spectroscopy of yellow 1S excitons in Cu2O
journal, April 2005

First-Principles Predictions of the Structure, Stability, and Photocatalytic Potential of Cu ₂ O Surfaces
journal, September 2013

Correlated lifetimes of free paraexcitons and excitons trapped at oxygen vacancies in cuprous oxide
journal, February 2013

Transition to a Bose–Einstein condensate and relaxation explosion of excitons at sub-Kelvin temperatures
journal, May 2011

Bose–Einstein condensation of excitons in Cu ₂ O: progress over 30 years
journal, October 2014

Third-harmonic generation in cuprous oxide: efficiency determination
journal, January 2014

Green Luminescence Band in ZnO: Fine Structures, Electron−Phonon Coupling, and Temperature Effect
journal, June 2006

Analysis of Wavelength Derivative Spectra of Exciton in Cu ₂ O
journal, July 1975

Femtosecond spectroscopy of condensed phases with chirped supercontinuum probing
journal, March 1999

Optical Absorption of Cuprous Oxide
journal, January 1961

Highly Mobile Paraexcitons in Cuprous Oxide
journal, March 1984

Study of Orthoexciton-to-Paraexciton Conversion in ${C u}_{2} O$ by Excitonic Lyman Spectroscopy
journal, January 2005

Symmetry of Excitons in ${Cu}_{2}$ O
journal, October 1961

Removal of Copper Vacancies in Cuprous Oxide Single Crystals Grown by the Floating Zone Method
journal, October 2013

Modeling of the thermalization of trapped paraexcitons in ${Cu}_{2} O$ at ultralow temperatures
journal, August 2014

Free exciton motion in crystals and exciton-phonon interaction
journal, October 1966

Electrodeposited Cu ₂ O as Photoelectrodes with Controllable Conductivity Type for Solar Energy Conversion
journal, November 2015

Engineering of optically defect free Cu_2O enabling exciton luminescence at room temperature
journal, January 2013

Epitaxial stabilization of orthorhombic cuprous oxide films on MgO(110)
journal, April 2001

Appearance of coherent artifact signals in femtosecond transient absorption spectroscopy in dependence on detector design
journal, January 2007

Experimental and theoretical studies of Cu2O solar cells
journal, December 1982

Unexpectedly slow two particle decay of ultra-dense excitons in cuprous oxide
journal, September 2013

Giant Rydberg excitons in the copper oxide Cu2O
journal, October 2014

Oxygen vacancy in N-doped Cu ₂ O crystals: A density functional theory study
journal, August 2012

Cupric oxide inclusions in cuprous oxide crystals grown by the floating zone method
journal, June 2015

Electronic Structure of Pure and Doped Cuprous Oxide with Copper Vacancies: Suppression of Trap States
journal, January 2013

Carrier thermalization in ${Cu}_{2}$ O: Phonon emission by excitons
journal, August 1991

Study of photoluminescence in ${Cu}_{2}$ O
journal, September 1975

The red luminescence spectrum of brown diamonds: vibronic coupling
journal, March 1986

Indirect generation of quadrupole polaritons from dark excitons in ${Cu}_{2} O$
journal, February 2008

Undoped n -Type Cu ₂ O: Fact or Fiction?
journal, August 2010

Growth and microstructural control of single crystal cuprous oxide Cu2O
journal, August 1974

Mechanisms behind green photoluminescence in ZnO phosphor powders
journal, May 1996

Photoionization cross section of $1 s$ orthoexcitons in cuprous oxide
journal, June 2014

Relaxation of localized excitons by phonon emission at oxygen vacancies in Cu2O
journal, November 2014

Signatures of coherent propagation of blue polaritons in Cu $_{2}$ O
journal, June 2013

The search for Bose–Einstein condensation of excitons in Cu ₂ O: exciton-Auger recombination versus biexciton formation
journal, December 2014

Potentiostatic electrodeposition of cuprous oxide thin films for photovoltaic applications
journal, May 2011

Detailed Examination of Relaxation Processes of Excitons in Photoluminescence Spectra of Cu ₂ O
journal, July 1997

Thermodynamic Assessment of the Silver-Oxygen System
journal, December 1997

Oxygen vacancy rich Cu ₂ O based composite material with nitrogen doped carbon as matrix for photocatalytic H ₂ production and organic pollutant removal
journal, January 2018