Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}

Point defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the nonequilibrium dynamics of the charge states of these defects at ultrafast (subnanosecond) timescales are rare....

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Main Authors: Arjan Singh, Okan Koksal, Nicholas Tanen, Jonathan McCandless, Debdeep Jena, Huili (Grace) Xing, Hartwin Peelaers, Farhan Rana
Format: Article
Language:English
Published: American Physical Society 2021-05-01
Series:Physical Review Research
Online Access:http://doi.org/10.1103/PhysRevResearch.3.023154
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author Arjan Singh
Okan Koksal
Nicholas Tanen
Jonathan McCandless
Debdeep Jena
Huili (Grace) Xing
Hartwin Peelaers
Farhan Rana
author_facet Arjan Singh
Okan Koksal
Nicholas Tanen
Jonathan McCandless
Debdeep Jena
Huili (Grace) Xing
Hartwin Peelaers
Farhan Rana
author_sort Arjan Singh
collection DOAJ
description Point defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the nonequilibrium dynamics of the charge states of these defects at ultrafast (subnanosecond) timescales are rare. We present results from ultrafast optical-pump supercontinuum-probe spectroscopy measurements on β-Ga_{2}O_{3}. The probe absorption spectra shows defect absorption peaks at two energies, ∼2.20eV and ∼1.63eV, within the 1.3–2.5 eV probe energy bandwidth. The strength of the absorption associated with each peak is time dependent and the spectral weight shifts from the lower energy peak to the higher energy peak with pump-probe delay. Further, maximum defect absorption is seen for probes polarized along the crystal c axis. The time-dependent probe absorption spectra and the observed dynamics for all probe wavelengths at all pump-probe delays can be fit with a set of rate equations for a single multilevel defect. Based on first-principles calculations within hybrid density-functional theory, we attribute the observed absorption features to optical transitions from the valence band to different charge states of Gallium vacancies. Our results demonstrate that broadband ultrafast supercontinuum spectroscopy can be a useful tool to explore charge states of defects and defect dynamics in semiconductors.
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spelling doaj.art-c0c3a965f83a4c3c888a2d95ccd27f432024-04-12T17:10:16ZengAmerican Physical SocietyPhysical Review Research2643-15642021-05-013202315410.1103/PhysRevResearch.3.023154Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}Arjan SinghOkan KoksalNicholas TanenJonathan McCandlessDebdeep JenaHuili (Grace) XingHartwin PeelaersFarhan RanaPoint defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the nonequilibrium dynamics of the charge states of these defects at ultrafast (subnanosecond) timescales are rare. We present results from ultrafast optical-pump supercontinuum-probe spectroscopy measurements on β-Ga_{2}O_{3}. The probe absorption spectra shows defect absorption peaks at two energies, ∼2.20eV and ∼1.63eV, within the 1.3–2.5 eV probe energy bandwidth. The strength of the absorption associated with each peak is time dependent and the spectral weight shifts from the lower energy peak to the higher energy peak with pump-probe delay. Further, maximum defect absorption is seen for probes polarized along the crystal c axis. The time-dependent probe absorption spectra and the observed dynamics for all probe wavelengths at all pump-probe delays can be fit with a set of rate equations for a single multilevel defect. Based on first-principles calculations within hybrid density-functional theory, we attribute the observed absorption features to optical transitions from the valence band to different charge states of Gallium vacancies. Our results demonstrate that broadband ultrafast supercontinuum spectroscopy can be a useful tool to explore charge states of defects and defect dynamics in semiconductors.http://doi.org/10.1103/PhysRevResearch.3.023154
spellingShingle Arjan Singh
Okan Koksal
Nicholas Tanen
Jonathan McCandless
Debdeep Jena
Huili (Grace) Xing
Hartwin Peelaers
Farhan Rana
Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}
Physical Review Research
title Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}
title_full Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}
title_fullStr Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}
title_full_unstemmed Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}
title_short Ultrafast dynamics of gallium vacancy charge states in β-Ga_{2}O_{3}
title_sort ultrafast dynamics of gallium vacancy charge states in β ga 2 o 3
url http://doi.org/10.1103/PhysRevResearch.3.023154
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