Rapid Bimolecular and Defect-Assisted Carrier Recombination in Hexagonal Boron Nitride

Hexagonal boron nitride (hBN) is a wide, indirect bandgap semiconductor that holds great promise for optoelectronic devices in the ultraviolet and mid-infrared spectral regimes. The efficiency of optoelectronic devices is dominated by the dynamic behavior of photogenerated carriers. Here we report o...

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Published in:	Journal of physical chemistry. C Vol. 123; no. 23; pp. 14689 - 14695
Main Authors:	Chatzakis, Ioannis, Davidson, Roderick B, Dunkelberger, Adam D, Liu, Song, Freitas, Jaime, Culbertson, James, Edgar, J. H, Ratchford, Daniel C, Ellis, Chase T, Grafton, Andrea B, Giles, Alexander J, Tischler, Joseph G, Caldwell, Joshua D, Owrutsky, Jeffrey C
Format:	Journal Article
Language:	English
Published:	American Chemical Society 13-06-2019
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Abstract	Hexagonal boron nitride (hBN) is a wide, indirect bandgap semiconductor that holds great promise for optoelectronic devices in the ultraviolet and mid-infrared spectral regimes. The efficiency of optoelectronic devices is dominated by the dynamic behavior of photogenerated carriers. Here we report on the dynamics of photoexcited free carriers in exfoliated 10B-enriched (99%) hBN at room temperature. Through implementation of ultrafast ultraviolet-pump–infrared-probe transient transmission spectroscopy, we identify two characteristic recombination rates. Initially, at high free carrier density, the pump fluence dependence is bimolecular with a characteristic rate constant of ∼2.0 × 10–7 cm3/s. This is followed by an exponential recombination of the free carriers at a rate of ∼2.3 × 109 s–1, which we assign to the influence of the impurities and defects in the lattice. These initial results offer insight into the radiative recombination processes for deep ultraviolet optoelectronic devices and toward realizing active control of mid-IR nanophotonic responses.
AbstractList	Hexagonal boron nitride (hBN) is a wide, indirect bandgap semiconductor that holds great promise for optoelectronic devices in the ultraviolet and mid-infrared spectral regimes. The efficiency of optoelectronic devices is dominated by the dynamic behavior of photogenerated carriers. Here we report on the dynamics of photoexcited free carriers in exfoliated 10B-enriched (99%) hBN at room temperature. Through implementation of ultrafast ultraviolet-pump–infrared-probe transient transmission spectroscopy, we identify two characteristic recombination rates. Initially, at high free carrier density, the pump fluence dependence is bimolecular with a characteristic rate constant of ∼2.0 × 10–7 cm3/s. This is followed by an exponential recombination of the free carriers at a rate of ∼2.3 × 109 s–1, which we assign to the influence of the impurities and defects in the lattice. These initial results offer insight into the radiative recombination processes for deep ultraviolet optoelectronic devices and toward realizing active control of mid-IR nanophotonic responses.
Author	Davidson, Roderick B Culbertson, James Liu, Song Caldwell, Joshua D Ellis, Chase T Dunkelberger, Adam D Freitas, Jaime Grafton, Andrea B Tischler, Joseph G Chatzakis, Ioannis Owrutsky, Jeffrey C Edgar, J. H Giles, Alexander J Ratchford, Daniel C
AuthorAffiliation	ASEE Postdoctoral Fellow (residing at NRL, Washington, DC) Tim Taylor Department of Chemical Engineering Department of Mechanical Engineering Vanderbilt University NRC Postdoctoral Fellow (residing at NRL, Washington, DC)
AuthorAffiliation_xml	– name: ASEE Postdoctoral Fellow (residing at NRL, Washington, DC) – name: Department of Mechanical Engineering – name: Tim Taylor Department of Chemical Engineering – name: Vanderbilt University – name: NRC Postdoctoral Fellow (residing at NRL, Washington, DC)
Author_xml	– sequence: 1 givenname: Ioannis orcidid: 0000-0002-3568-2174 surname: Chatzakis fullname: Chatzakis, Ioannis organization: ASEE Postdoctoral Fellow (residing at NRL, Washington, DC) – sequence: 2 givenname: Roderick B surname: Davidson fullname: Davidson, Roderick B – sequence: 3 givenname: Adam D surname: Dunkelberger fullname: Dunkelberger, Adam D – sequence: 4 givenname: Song surname: Liu fullname: Liu, Song organization: Tim Taylor Department of Chemical Engineering – sequence: 5 givenname: Jaime surname: Freitas fullname: Freitas, Jaime – sequence: 6 givenname: James surname: Culbertson fullname: Culbertson, James – sequence: 7 givenname: J. H orcidid: 0000-0003-0918-5964 surname: Edgar fullname: Edgar, J. H organization: Tim Taylor Department of Chemical Engineering – sequence: 8 givenname: Daniel C orcidid: 0000-0001-7015-5305 surname: Ratchford fullname: Ratchford, Daniel C – sequence: 9 givenname: Chase T orcidid: 0000-0002-6718-6511 surname: Ellis fullname: Ellis, Chase T – sequence: 10 givenname: Andrea B surname: Grafton fullname: Grafton, Andrea B organization: NRC Postdoctoral Fellow (residing at NRL, Washington, DC) – sequence: 11 givenname: Alexander J surname: Giles fullname: Giles, Alexander J – sequence: 12 givenname: Joseph G surname: Tischler fullname: Tischler, Joseph G – sequence: 13 givenname: Joshua D orcidid: 0000-0003-0374-2168 surname: Caldwell fullname: Caldwell, Joshua D email: josh.caldwell@vanderbilt.edu organization: Vanderbilt University – sequence: 14 givenname: Jeffrey C orcidid: 0000-0003-3216-7270 surname: Owrutsky fullname: Owrutsky, Jeffrey C email: jeff.owrutsky@nrl.navy.mil
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Title	Rapid Bimolecular and Defect-Assisted Carrier Recombination in Hexagonal Boron Nitride
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